diff --git a/config/_default/params.yaml b/config/_default/params.yaml index 5f4a2d9..a1ac8c2 100644 --- a/config/_default/params.yaml +++ b/config/_default/params.yaml @@ -9,7 +9,7 @@ appearance: theme_day: minimal theme_night: minimal font: native - font_size: L + font_size: M # SEO diff --git a/content/people/index.md b/content/people/index.md index b7a9cd9..ade8014 100644 --- a/content/people/index.md +++ b/content/people/index.md @@ -7,17 +7,16 @@ date: 2024-01-30 Gianluca's portrait + style="width: 180px; height: 195px; float: left; margin-right: 20px;"> -

+

### Gianluca Levi Group leader Science Institute of the University of Iceland VR-III Hjarðarhagi 2, 107 Reykjavík -[ORCID](https://orcid.org/0000-0002-4542-0653)   [Web of Science](https://www.webofscience.com/wos/author/record/GYQ-9226-2022)   [Google Scholar](https://scholar.google.com/citations?user=HhElK98AAAAJ&hl=en)   [CV](../doc/cv_giale.pdf) -+354 8326622 -giale@hi.is +[ORCID](https://orcid.org/0000-0002-4542-0653)   [Web of Science](https://www.webofscience.com/wos/author/record/GYQ-9226-2022)   [Google Scholar](https://scholar.google.com/citations?user=HhElK98AAAAJ&hl=en)   [CV](../doc/cv_giale.pdf) ++354 8326622, giale@hi.is

@@ -33,9 +32,9 @@ elliselenius@hi.is Yorick's portrait + style="width: 180px; height: 220px; float: left; margin-right: 20px;"> -

+

### Yorick Leonard A. Schmerwitz PhD student (co-supervised, main supervisor: Prof. [Hannes Jónsson](https://hj.hi.is/indexE.html)) diff --git a/public/404.html b/public/404.html index b1475f7..e007406 100644 --- a/public/404.html +++ b/public/404.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/adi-natan/index.html b/public/author/adi-natan/index.html index 38657bb..ae435df 100644 --- a/public/author/adi-natan/index.html +++ b/public/author/adi-natan/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git "a/public/author/alec-e.-sigur\303\260arson/index.html" "b/public/author/alec-e.-sigur\303\260arson/index.html" index 7a113a1..0ac575c 100644 --- "a/public/author/alec-e.-sigur\303\260arson/index.html" +++ "b/public/author/alec-e.-sigur\303\260arson/index.html" @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git "a/public/author/alec-elias-sigur\303\260arson/index.html" "b/public/author/alec-elias-sigur\303\260arson/index.html" index dcfc97b..5c4f3b5 100644 --- "a/public/author/alec-elias-sigur\303\260arson/index.html" +++ "b/public/author/alec-elias-sigur\303\260arson/index.html" @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/aleksei-v.-ivanov/index.html b/public/author/aleksei-v.-ivanov/index.html index a677df5..50711f7 100644 --- a/public/author/aleksei-v.-ivanov/index.html +++ b/public/author/aleksei-v.-ivanov/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/alex-j.-w.-thom/index.html b/public/author/alex-j.-w.-thom/index.html index 1c97f31..04da404 100644 --- a/public/author/alex-j.-w.-thom/index.html +++ b/public/author/alex-j.-w.-thom/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/alireza-taghizadeh/index.html b/public/author/alireza-taghizadeh/index.html index fe10400..b75a6c1 100644 --- a/public/author/alireza-taghizadeh/index.html +++ b/public/author/alireza-taghizadeh/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/andreas-savin/index.html b/public/author/andreas-savin/index.html index baa9939..0c22eee 100644 --- a/public/author/andreas-savin/index.html +++ b/public/author/andreas-savin/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/andrew-m.-teale/index.html b/public/author/andrew-m.-teale/index.html index 29a026b..060321b 100644 --- a/public/author/andrew-m.-teale/index.html +++ b/public/author/andrew-m.-teale/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/andrew-peterson/index.html b/public/author/andrew-peterson/index.html index d3fcc6b..c7e4f97 100644 --- a/public/author/andrew-peterson/index.html +++ b/public/author/andrew-peterson/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/anubhab-haldar/index.html b/public/author/anubhab-haldar/index.html index 4acb55f..650f11f 100644 --- a/public/author/anubhab-haldar/index.html +++ b/public/author/anubhab-haldar/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git "a/public/author/asbj\303\270rn-moltke/index.html" "b/public/author/asbj\303\270rn-moltke/index.html" index 6b80847..d28d67f 100644 --- "a/public/author/asbj\303\270rn-moltke/index.html" +++ "b/public/author/asbj\303\270rn-moltke/index.html" @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/ask-hjorth-larsen/index.html b/public/author/ask-hjorth-larsen/index.html index b9bda1a..03ad1f6 100644 --- a/public/author/ask-hjorth-larsen/index.html +++ b/public/author/ask-hjorth-larsen/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/asmus-o-dohn/index.html b/public/author/asmus-o-dohn/index.html index d881636..58f7e55 100644 --- a/public/author/asmus-o-dohn/index.html +++ b/public/author/asmus-o-dohn/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/asmus-o.-dohn/index.html b/public/author/asmus-o.-dohn/index.html index f73fb99..2665715 100644 --- a/public/author/asmus-o.-dohn/index.html +++ b/public/author/asmus-o.-dohn/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/asmus-ougaard-dohn/index.html b/public/author/asmus-ougaard-dohn/index.html index 908bd90..5ebf7f2 100644 --- a/public/author/asmus-ougaard-dohn/index.html +++ b/public/author/asmus-ougaard-dohn/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/benedikt-o-birgisson/index.html b/public/author/benedikt-o-birgisson/index.html index 8df2724..a2bb018 100644 --- a/public/author/benedikt-o-birgisson/index.html +++ b/public/author/benedikt-o-birgisson/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/christian-schafer/index.html b/public/author/christian-schafer/index.html index 1b7343e..7172b7b 100644 --- a/public/author/christian-schafer/index.html +++ b/public/author/christian-schafer/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/christopher-j.-milne/index.html b/public/author/christopher-j.-milne/index.html index b387078..1d084df 100644 --- a/public/author/christopher-j.-milne/index.html +++ b/public/author/christopher-j.-milne/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/dagrun-k.-v.-tveiten/index.html b/public/author/dagrun-k.-v.-tveiten/index.html index 6074ff6..31352a7 100644 --- a/public/author/dagrun-k.-v.-tveiten/index.html +++ b/public/author/dagrun-k.-v.-tveiten/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/diana-b-zederkof/index.html b/public/author/diana-b-zederkof/index.html index a5c9b4c..5404d0b 100644 --- a/public/author/diana-b-zederkof/index.html +++ b/public/author/diana-b-zederkof/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/diana-bregenholt-zederkof/index.html b/public/author/diana-bregenholt-zederkof/index.html index 491e94d..5ee19c7 100644 --- a/public/author/diana-bregenholt-zederkof/index.html +++ b/public/author/diana-bregenholt-zederkof/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/dmitry-khakhulin/index.html b/public/author/dmitry-khakhulin/index.html index c17d3bc..864a17f 100644 --- a/public/author/dmitry-khakhulin/index.html +++ b/public/author/dmitry-khakhulin/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/donald-g.-truhlar/index.html b/public/author/donald-g.-truhlar/index.html index 3f3f20d..d0a78e0 100644 --- a/public/author/donald-g.-truhlar/index.html +++ b/public/author/donald-g.-truhlar/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/dumitru-sirbu/index.html b/public/author/dumitru-sirbu/index.html index 3dce365..0e700b9 100644 --- a/public/author/dumitru-sirbu/index.html +++ b/public/author/dumitru-sirbu/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/duncan-gowland/index.html b/public/author/duncan-gowland/index.html index 76f2ff7..57e3a19 100644 --- a/public/author/duncan-gowland/index.html +++ b/public/author/duncan-gowland/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/eduardo-maurina-morais/index.html b/public/author/eduardo-maurina-morais/index.html index 24a24a9..a910268 100644 --- a/public/author/eduardo-maurina-morais/index.html +++ b/public/author/eduardo-maurina-morais/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/elisa-biasin/index.html b/public/author/elisa-biasin/index.html index f9ade44..197198c 100644 --- a/public/author/elisa-biasin/index.html +++ b/public/author/elisa-biasin/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/elli-selenius/index.html b/public/author/elli-selenius/index.html index 2bb1f0a..5146f3a 100644 --- a/public/author/elli-selenius/index.html +++ b/public/author/elli-selenius/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/elvar-o-jonsson/index.html b/public/author/elvar-o-jonsson/index.html index 1ae995c..2e70649 100644 --- a/public/author/elvar-o-jonsson/index.html +++ b/public/author/elvar-o-jonsson/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/elvar-o.-jonsson/index.html b/public/author/elvar-o.-jonsson/index.html index 40084b3..2a32681 100644 --- a/public/author/elvar-o.-jonsson/index.html +++ b/public/author/elvar-o.-jonsson/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/elvar-orn-jonsson/index.html b/public/author/elvar-orn-jonsson/index.html index 92c9ea5..b9a13ef 100644 --- a/public/author/elvar-orn-jonsson/index.html +++ b/public/author/elvar-orn-jonsson/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/emmanuel-fromager/index.html b/public/author/emmanuel-fromager/index.html index e4c8efc..99ef0e4 100644 --- a/public/author/emmanuel-fromager/index.html +++ b/public/author/emmanuel-fromager/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/eric-d.-hermes/index.html b/public/author/eric-d.-hermes/index.html index 4d5c570..12e7160 100644 --- a/public/author/eric-d.-hermes/index.html +++ b/public/author/eric-d.-hermes/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/filippo-monti/index.html b/public/author/filippo-monti/index.html index fa6da4e..8e0c7aa 100644 --- a/public/author/filippo-monti/index.html +++ b/public/author/filippo-monti/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/frederico-a.-lima/index.html b/public/author/frederico-a.-lima/index.html index f763311..5e148d5 100644 --- a/public/author/frederico-a.-lima/index.html +++ b/public/author/frederico-a.-lima/index.html @@ -1,6 +1,6 @@ - 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+ @@ -206,7 +206,7 @@ - + diff --git a/public/author/gianluca-levi/index.html b/public/author/gianluca-levi/index.html index e65c43e..50956fc 100644 --- a/public/author/gianluca-levi/index.html +++ b/public/author/gianluca-levi/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/gyorgy-vanko/index.html b/public/author/gyorgy-vanko/index.html index 90d8f04..9ae68c5 100644 --- a/public/author/gyorgy-vanko/index.html +++ b/public/author/gyorgy-vanko/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/hannes-jonsson/index.html b/public/author/hannes-jonsson/index.html index a2c204b..c4b70a8 100644 --- a/public/author/hannes-jonsson/index.html +++ b/public/author/hannes-jonsson/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/hannu-hakkinen/index.html b/public/author/hannu-hakkinen/index.html index 909050a..58b5790 100644 --- a/public/author/hannu-hakkinen/index.html +++ b/public/author/hannu-hakkinen/index.html @@ -1,6 +1,6 @@ - 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+ @@ -206,7 +206,7 @@ - + diff --git a/public/author/jakub-szlachetko/index.html b/public/author/jakub-szlachetko/index.html index fa2aa40..6d713ba 100644 --- a/public/author/jakub-szlachetko/index.html +++ b/public/author/jakub-szlachetko/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/james-m.-glownia/index.html b/public/author/james-m.-glownia/index.html index af078f8..b8427fa 100644 --- a/public/author/james-m.-glownia/index.html +++ b/public/author/james-m.-glownia/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/jan-gerit-brandenburg/index.html b/public/author/jan-gerit-brandenburg/index.html index 8469bdd..ba63fb9 100644 --- a/public/author/jan-gerit-brandenburg/index.html +++ b/public/author/jan-gerit-brandenburg/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/jens-j.-mortensen/index.html b/public/author/jens-j.-mortensen/index.html index b79d592..3282611 100644 --- a/public/author/jens-j.-mortensen/index.html +++ b/public/author/jens-j.-mortensen/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git "a/public/author/jens-j\303\270rgen-mortensen/index.html" "b/public/author/jens-j\303\270rgen-mortensen/index.html" index 960c1c0..3eb0ea1 100644 --- "a/public/author/jens-j\303\270rgen-mortensen/index.html" +++ "b/public/author/jens-j\303\270rgen-mortensen/index.html" @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/jens-ulstrup/index.html b/public/author/jens-ulstrup/index.html index af68d02..1ed36fc 100644 --- a/public/author/jens-ulstrup/index.html +++ b/public/author/jens-ulstrup/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git a/public/author/jiban-kangsabanik/index.html b/public/author/jiban-kangsabanik/index.html index 4ed14d0..da7839d 100644 --- a/public/author/jiban-kangsabanik/index.html +++ b/public/author/jiban-kangsabanik/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + diff --git "a/public/author/joachim-s\303\270dequist/index.html" "b/public/author/joachim-s\303\270dequist/index.html" index ceb3e0d..912f648 100644 --- "a/public/author/joachim-s\303\270dequist/index.html" +++ "b/public/author/joachim-s\303\270dequist/index.html" @@ -1,6 +1,6 @@ - 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Schmerwitz PhD student (co-supervised, main supervisor: Prof. Hannes Jónsson)\nScience Institute of the University of Iceland VR-III Hjarðarhagi 2, 107 Reykjavík\nORCID Web of Science Google Scholar\nyla1@hi.is\nBenedikt Orri Birgisson PhD student (co-supervised, main supervisor: Prof. Hannes Jónsson)\nScience Institute of the University of Iceland VR-III Hjarðarhagi 2, 107 Reykjavík\nbob9@hi.is\nCollaborations University of Iceland Elvar Örn Jónsson Hannes Jónsson\nTechnical University of Denmark Asmus Ougaard Dohn Kristoffer Haldrup Luca Laraia Martin Meedom Nielsen\nUniversity of Erlangen–Nuremberg Philipp Hansmann\n","date":1706572800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1706572800,"objectID":"c1d17ff2b20dca0ad6653a3161942b64","permalink":"https://example.com/people/","publishdate":"2024-01-30T00:00:00Z","relpermalink":"/people/","section":"","summary":"Group Members Gianluca Levi Group leader Science Institute of the University of Iceland VR-III Hjarðarhagi 2, 107 Reykjavík\nORCID Web of Science Google Scholar CV +354 8326622\ngiale@hi.is\nElli Inkeri Selenius Postdoc Science Institute of the University of Iceland VR-III Hjarðarhagi 2, 107 Reykjavík","tags":null,"title":"","type":"page"},{"authors":["Natalia E Powers-Riggs","Benedikt O Birgisson","Sumana L Raj","Philipp Lenzen","Diana Bregenholt Zederkof","Morten Haubro","K V Dagrún Tveiten","Robert W Hartsock","Tim B Van Driel","Matthieu Chollet","Joseph S Robinson","Silke Nelson","Kristoffer Haldrup","Kasper Steen Pedersen","Gianluca Levi","Ougaard Dohn","Jónsson Hannes","Klaus Braagaard Møller","Adi Natan","Martin Meedom Nielsen","Kelly Gaffney"],"categories":null,"content":"","date":1704067200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1704067200,"objectID":"2d152bc3dff6d27b33a6849e5441f3e6","permalink":"https://example.com/publication/powers-riggs-2024/","publishdate":"2024-02-02T14:14:57.342234Z","relpermalink":"/publication/powers-riggs-2024/","section":"publication","summary":"Dimeric complexes composed of d8 square planar metal centers and rigid bridg- ing ligands provide model systems to understand the interplay between attractive dispersion forces and steric strain, in order to assist the development reliable meth- ods to model metal dimer complexes more broadly. [Ir2(dimen)4]2+ (dimen = para- diisocyanomenthane) presents a unique case study for such phenomena, as distortions of the optimal structure of a ligand with limited conformational flexibility counteracts the attractive dispersive forces from the metal and ligand to yield a complex with two ground state deformational isomers. Here, we use ultrafast X-ray solution scattering (XSS) and optical transient absorption spectroscopy (OTAS) to reveal the nature of the equilibrium distribution and the exchange rate between the deformational isomers. The two ground state isomers have spectrally distinct electronic excitations that enable the selective excitation of one isomer or the other using a femtosecond duration pulse of visible light. We then track the dynamics of the non-equilibrium depletion of the electronic ground state population – often termed the ground state hole – with ultra- fast XSS and OTAS, revealing a restoration of the ground state equilibrium in 2.3 ps. This experimental study provides a critical test of various density functional approx- imations in the description of bridged d8-d8 metal complexes. Our study shows that reproduction of the primary experimental observations requires a hybrid functional, which includes exact exchange, while also accounting for dispersion interactions.","tags":null,"title":"Characterization of deformational isomerization potential and interconversion dynamics with ultrafast x-ray solution scattering","type":"publication"},{"authors":["Jens Jørgen Mortensen","Ask Hjorth Larsen","Mikael Kuisma","Aleksei V. Ivanov","Alireza Taghizadeh","Andrew Peterson","Anubhab Haldar","Asmus Ougaard Dohn","Christian Schäfer","Elvar Örn Jónsson","Eric D. Hermes","Fredrik Andreas Nilsson","Georg Kastlunger","Gianluca Levi","Hannes Jónsson","Hannu Häkkinen","Jakub Fojt","Jiban Kangsabanik","Joachim Sødequist","Jouko Lehtomäki","Julian Heske","Jussi Enkovaara","Kirsten Trøstrup Winther","Marcin Dulak","Marko M. Melander","Martin Ovesen","Martti Louhivuori","Michael Walter","Morten Gjerding","Olga Lopez-Acevedo","Paul Erhart","Robert Warmbier","Rolf Würdemann","Sami Kaappa","Simone Latini","Tara Maria Boland","Thomas Bligaard","Thorbjørn Skovhus","Toma Susi","Tristan Maxson","Tuomas Rossi","Xi Chen","Yorick Leonard A. Schmerwitz","Jakob Schiøtz","Thomas Olsen","Karsten Wedel Jacobsen","Kristian Sommer Thygesen"],"categories":null,"content":"","date":1704067200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1704067200,"objectID":"fecc1f77629a5542cb287e6a321ca0e7","permalink":"https://example.com/publication/mortensen-2024/","publishdate":"2024-02-02T14:14:57.347699Z","relpermalink":"/publication/mortensen-2024/","section":"publication","summary":"We review the GPAW open-source Python package for electronic structure calculations. GPAW is based on the projector-augmented wave method and can solve the self-consistent density functional theory (DFT) equations using three different wave-function representations, namely real-space grids, plane waves, and numerical atomic orbitals. The three representations are complementary and mutually independent and can be connected by transformations via the real-space grid. This multi-basis feature renders GPAW highly versatile and unique among similar codes. By virtue of its modular structure, the GPAW code constitutes an ideal platform for implementation of new features and methodologies. Moreover, it is well integrated with the Atomic Simulation Environment (ASE) providing a flexible and dynamic user interface. In addition to ground-state DFT calculations, GPAW supports many-body GW band structures, optical excitations from the Bethe-Salpeter Equation (BSE), variational calculations of excited states in molecules and solids via direct optimization, and real-time propagation of the Kohn-Sham equations within time-dependent DFT. A range of more advanced methods to describe magnetic excitations and non-collinear magnetism in solids are also now available. In addition, GPAW can calculate non-linear optical tensors of solids, charged crystal point defects, and much more. Recently, support of GPU acceleration has been achieved with minor modifications of the GPAW code thanks to the CuPy library. We end the review with an outlook describing some future plans for GPAW.","tags":null,"title":"GPAW: open Python package for electronic-structure calculations","type":"publication"},{"authors":["Elli Selenius","Alec Elías Sigurðarson","Yorick L. A. Schmerwitz","Gianluca Levi"],"categories":null,"content":"","date":1704067200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1704067200,"objectID":"bcfa7e3c0f3c211313b854dd04c37fda","permalink":"https://example.com/publication/selenius-2024/","publishdate":"2024-02-02T14:14:57.334688Z","relpermalink":"/publication/selenius-2024/","section":"publication","summary":"A strategy is presented for variational orbital optimization in time-independent calculations of excited electronic states. The approach involves minimizing the energy while constraining the degrees of freedom corresponding to negative curvature on the electronic energy surface, followed by fully unconstrained optimization, thereby converging on a saddle point. Both steps of this freeze-and-release strategy are carried out via direct orbital optimization at a similar cost as ground state calculations. The approach is applied in orbital optimized density functional calculations and is shown to converge intramolecular charge transfer excited states where the common maximum overlap method is unable to prevent collapse to unphysical, charge-delocalized solutions. The constrained minimization can also be used to improve the estimate of the saddle point order of the target excited state solution, which is required as input for generalized mode following methods. Calculations with the local density approximation and the generalized gradient approximation functionals PBE and BLYP are carried out for a large set of charge transfer excitations in organic molecules using both direct optimization as well as the linear-response time-dependent density functional theory (TD-DFT) method. The time-independent approach is fully variational and provides a relaxed excited state electron density that can be used to quantify the extent of charge transfer. The TD-DFT calculations are found to generally overestimate the charge transfer distance compared to the orbital optimized calculations, even when the TD-DFT relaxed density is used. Furthermore, the orbital optimized calculations yield more accurate excitation energy values relative to the theoretical best estimates for the medium and long-range charge transfer distances, where the errors of TD-DFT are as large as 2 eV.","tags":null,"title":"Orbital optimized vs time-dependent density functional calculations of intramolecular charge transfer excited states","type":"publication"},{"authors":["Tetsuo Katayama","Tae Kyu Choi","Dmitry Khakhulin","Asmus O Dohn","Christopher J. Milne","György Vankó","Zoltán Németh","Frederico A. Lima","Jakub Szlachetko","Tokushi Sato","Shunsuke Nozawa","Shin Ichi Adachi","Makina Yabashi","Thomas J. Penfold","Wojciech Gawelda","Gianluca Levi"],"categories":null,"content":"","date":1672531200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1672531200,"objectID":"7a1d7777a963c4dc088cf764b88b8ccb","permalink":"https://example.com/publication/katayama-2023/","publishdate":"2024-02-02T14:14:57.353919Z","relpermalink":"/publication/katayama-2023/","section":"publication","summary":"Photochemical reactions in solution are governed by a complex interplay between transient intramolecular electronic and nuclear structural changes and accompanying solvent rearrangements. State-of-the-art time-resolved X-ray solution scattering has emerged in the last decade as a powerful technique to observe solute and solvent motions in real time. However, disentangling solute and solvent dynamics and how they mutually influence each other remains challenging. Here, we simultaneously measure femtosecond X-ray emission and scattering to track both the intramolecular and solvation structural dynamics following photoexcitation of a solvated copper photosensitizer. Quantitative analysis assisted by molecular dynamics simulations reveals a two-step ligand flattening strongly coupled to the solvent reorganization, which conventional optical methods could not discern. First, a ballistic flattening triggers coherent motions of surrounding acetonitrile molecules. In turn, the approach of acetonitrile molecules to the copper atom mediates the decay of intramolecular coherent vibrations and induces a further ligand flattening. These direct structural insights reveal that photoinduced solute and solvent motions can be intimately intertwined, explaining how the key initial steps of light harvesting are affected by the solvent on the atomic time and length scale. Ultimately, this work takes a step forward in understanding the microscopic mechanisms of the bidirectional influence between transient solvent reorganization and photoinduced solute structural dynamics.","tags":null,"title":"Atomic-scale observation of solvent reorganization influencing photoinduced structural dynamics in a copper complex photosensitizer","type":"publication"},{"authors":["Yorick L. A. Schmerwitz","Gianluca Levi","Hannes Jónsson"],"categories":null,"content":"","date":1672531200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1672531200,"objectID":"adade83911a8e286321fdbdc5fec7930","permalink":"https://example.com/publication/schmerwitz-2023/","publishdate":"2024-02-02T14:14:57.364513Z","relpermalink":"/publication/schmerwitz-2023/","section":"publication","summary":"Variational calculations of excited electronic states are carried out by finding saddle points on the surface that describes how the energy of the system varies as a function of the electronic degrees of freedom. This approach has several advantages over commonly used methods especially in the context of density functional calculations, as collapse to the ground state is avoided and yet, the orbitals are variationally optimized for the excited state. This optimization makes it possible to describe excitations with large charge transfer where calculations based on ground state orbitals are problematic, as in linear response time-dependent density functional theory. A generalized mode following method is presented where an $n^textth$-order saddle point is found by inverting the components of the gradient in the direction of the eigenvectors of the $n$ lowest eigenvalues of the electronic Hessian matrix. This approach has the distinct advantage of following a chosen excited state through atomic configurations where the symmetry of the single determinant wave function is broken, as demonstrated in calculations of potential energy curves for nuclear motion in the ethylene and dihydrogen molecules. The method is implemented using a generalized Davidson algorithm and an exponential transformation for updating the orbitals within a generalized gradient approximation of the energy functional. Convergence is found to be more robust than for a direct optimization approach previously shown to outperform standard self-consistent field approaches, as illustrated here for charge transfer excitations in nitrobenzene and N-phenylpyrrole, involving calculations of $4^textth$- and $6^textth$-order saddle points, respectively. Finally, calculations of a diplatinum and silver complex are presented, illustrating the applicability of the method to excited state energy curves of large molecules.","tags":null,"title":"Calculations of Excited Electronic States by Converging on Saddle Points Using Generalized Mode Following","type":"publication"},{"authors":["Aleksei V. Ivanov","Yorick L. A. Schmerwitz","Gianluca Levi","Hannes Jónsson"],"categories":null,"content":"","date":1672531200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1672531200,"objectID":"f0c990063c541ef724582297df162936","permalink":"https://example.com/publication/ivanov-2023/","publishdate":"2024-02-02T14:14:57.359243Z","relpermalink":"/publication/ivanov-2023/","section":"publication","summary":"Elucidation of the mechanism for optical spin initialization of point defects in solids in the context of quantum applications requires an accurate description of the excited electronic states involved. While variational density functional calculations have been successful in describing the ground state of a great variety of systems, doubts have been expressed in the literature regarding the ability of such calculations to describe electronic excitations of point defects. A direct orbital optimization method is used here to perform time-independent, variational density functional calculations of a prototypical defect, the negatively charged nitrogen-vacancy center in diamond. The calculations include up to 512 atoms subject to periodic boundary conditions and the excited state calculations require similar computational effort as ground state calculations. Contrary to some previous reports, the use of local and semi-local density functionals gives the correct ordering of the low-lying triplet and singlet states, namely 3A2 \u003c 1E \u003c 1A1 \u003c 3E. Furthermore, the more advanced meta generalized gradient approximation functionals give results that are in remarkably good agreement with high-level, many-body calculations as well as available experimental estimates, even for the excited singlet state which is often referred to as having multireference character. The lowering of the energy in the triplet excited state as the atom coordinates are optimized in accordance with analytical forces is also close to the experimental estimate and the resulting zero-phonon line triplet excitation energy is underestimated by only 0.15 eV. The approach used here is found to be a promising tool for studying electronic excitations of point defects in, for example, systems relevant for quantum technologies.","tags":null,"title":"Electronic excitations of the charged nitrogen-vacancy center in diamond obtained using time-independent variational density functional calculations","type":"publication"},{"authors":["Alec E. Sigurðarson","Yorick L. A. Schmerwitz","Dagrún K. V. Tveiten","Gianluca Levi","Hannes Jónsson"],"categories":null,"content":"","date":1672531200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1672531200,"objectID":"836f37ae37f0d784e4501f37149f9651","permalink":"https://example.com/publication/sigurdarson-2023/","publishdate":"2024-02-02T14:14:57.369903Z","relpermalink":"/publication/sigurdarson-2023/","section":"publication","summary":"Density functional calculations of Rydberg excited states up to high energy are carried out for several molecules using an approach where the orbitals are variationally optimized by converging on saddle points on the electronic energy surface within a real space grid representation. Remarkably good agreement with experimental estimates of the excitation energy is obtained using the generalized gradient approximation (GGA) functional of Perdew, Burke and Ernzerhof (PBE) when Perdew-Zunger self-interaction correction is applied in combination with complex-valued orbitals. Even without the correction, the PBE functional gives quite good results despite the fact that corresponding Rydberg virtual orbitals have positive energy in the ground state calculation. Results obtained using the TPSS and r2SCAN meta-GGA functionals are also presented, but they do not provide a systematic improvement over the results from the uncorrected PBE functional. The grid representation combined with the projector augmented-wave approach gives a simpler and better representation of the diffuse Rydberg orbitals than a linear combination of atomic orbitals with commonly used basis sets, the latter leading to an overestimation of the excitation energy due to confinement of the excited states.","tags":null,"title":"Orbital-optimized Density Functional Calculations of Molecular Rydberg Excited States with Real Space Grid Representation and Self-Interaction Correction","type":"publication"},{"authors":["Yorick L. A. Schmerwitz","Aleksei V. Ivanov","Elvar Ö. Jónsson","Hannes Jónsson","Gianluca Levi"],"categories":null,"content":"","date":1640995200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1640995200,"objectID":"4d759ea085a5cd97f187984ec9820cdd","permalink":"https://example.com/publication/schmerwitz-2022/","publishdate":"2024-02-02T14:14:57.375018Z","relpermalink":"/publication/schmerwitz-2022/","section":"publication","summary":"Theoretical studies of photochemical processes require a description of the energy surfaces of excited electronic states, especially near degeneracies, where transitions between states are most likely. Systems relevant to photochemical applications are typically too large for high-level multireference methods, and while time-dependent density functional theory (TDDFT) is efficient, it can fail to provide the required accuracy. A variational, time- independent density functional approach is applied to the twisting of the double bond and pyramidal distortion in ethylene, the quintessential model for photochemical studies. By allowing for symmetry breaking, the calculated energy surfaces exhibit the correct topology around the twisted-pyramidalized conical intersection even when using a semilocal functional approximation, and by including explicit self-interaction correction, the torsional energy curves are in close agreement with published multireference results. The findings of the present work point to the possibility of using a single determinant time-independent density functional approach to simulate nonadiabatic dynamics, even for large systems where multireference methods are impractical and TDDFT is often not accurate enough.","tags":null,"title":"Variational Density Functional Calculations of Excited States: Conical Intersection and Avoided Crossing in Ethylene Bond Twisting","type":"publication"},{"authors":["Aleksei V. Ivanov","Gianluca Levi","Elvar Ö. Jónsson","Hannes Jónsson"],"categories":null,"content":"","date":1625097600,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1625097600,"objectID":"cca8ea6afaf84782b5b5fad638f4082b","permalink":"https://example.com/publication/ivanov-2021/","publishdate":"2024-02-02T14:14:57.38003Z","relpermalink":"/publication/ivanov-2021/","section":"publication","summary":"A direct orbital optimization method is presented for density functional calculations of excited electronic states using either a real space grid or a plane-wave basis set. The method is variational, provides atomic forces in the excited states, and can be applied to Kohn−Sham (KS) functionals as well as orbital-density-dependent (ODD) functionals including explicit self-interaction correction. The implementation for KS functionals involves two nested loops: (1) An inner loop for finding a stationary point in a subspace spanned by the occupied and a few virtual orbitals corresponding to the excited state; (2) an outer loop for minimizing the energy in a tangential direction in the space of the orbitals. For ODD functionals, a third loop is used to find the unitary transformation that minimizes the energy functional among occupied orbitals only. Combined with the maximum overlap method, the algorithm converges in challenging cases where conventional self-consistent field algorithms tend to fail. The benchmark tests presented include two charge-transfer excitations in nitrobenzene and an excitation of CO to degenerate $π$* orbitals where the importance of complex orbitals is illustrated. The application of this method to several metal-to-ligand charge-transfer and metal-centered excited states of an Fe II photosensitizer complex is described, and the results are compared to reported experimental estimates. This method is also used to study the effect of the Perdew−Zunger self-interaction correction on valence and Rydberg excited states of several molecules, both singlet and triplet states, and the performance compared to semilocal and hybrid functionals.","tags":null,"title":"Method for Calculating Excited Electronic States Using Density Functionals and Direct Orbital Optimization with Real Space Grid or Plane-Wave Basis Set","type":"publication"},{"authors":["Gianluca Levi","Mauro Causà","Luciano Cortese","Piero Salatino","Osvalda Senneca"],"categories":null,"content":"","date":1606780800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1606780800,"objectID":"74bdc2d338660e8cf419719b32cbd3e8","permalink":"https://example.com/publication/levi-2020-aecs/","publishdate":"2024-02-02T14:14:57.394721Z","relpermalink":"/publication/levi-2020-aecs/","section":"publication","summary":"Understanding how the structure of carbonaceous materials changes upon oxidation at mild temperature as a function of the graphitic order is of great importance for the development of clean combustion technologies, such as carbon fuel cells. The micro- and nanostructures of a range of carbon materials at room temperature and upon mild oxidation at 300 °C have been analysed by means of mercury porosimetry, Nitrogen adsorption, X-Ray Diffraction, Raman spectroscopy and Electron Paramagnetic Resonance. The samples included carbons with increasing level of graphitic order: three chars derived from two bituminous coals and a lignite, a synthetic carbon and a graphitized coke. The experimental characterization allows to classify the materials according to different structural parameters, including porosity, surface area, degree of graphitization and paramagnetic activation of the carbonaceous surface. A correlation with the rank of the analysed materials is observed. For the graphitized coke, oxidation leads to more crystalline order and enhancement of the paramagnetic signal. A similar increase in the paramagnetic activity is observed for the Lignite char. On the other hand, for the higher rank, bituminous and synthetic chars, mild oxidation leads to a slight expansion of the amorphous carbon and loss of paramagnetic activity. The differences are rationalized in terms of formation of new carbon-oxygen complexes on the graphitized coke and on the Lignite char, and redistribution of already existing complexes for the higher-rank coals. This investigation complements previous X-ray photoelectron spectroscopy measurements.","tags":null,"title":"On how mild oxidation affects the structure of carbons: Comparative analysis by different techniques","type":"publication"},{"authors":["Jan Gerit Brandenburg","Kieron Burke","Emmanuel Fromager","Matteo Gatti","Sara Giarrusso","Nikitas I. Gidopoulos","Paola Gori-Giorgi","Duncan Gowland","Trygve Helgaker","Matthew J. P. Hodgson","Lionel Lacombe","Gianluca Levi","Pierre-François Loos","Neepa T. Maitra","Eduardo Maurina Morais","Nisha Mehta","Filippo Monti","Manasi R. Mulay","Katarzyna Pernal","Lucia Reining","Pina Romaniello","Matthew R. Ryder","Andreas Savin","Dumitru Sirbu","Andrew M. Teale","Alex J. W. Thom","Donald G. Truhlar","Jack Wetherell","Weitao Yang"],"categories":null,"content":"","date":1577836800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1577836800,"objectID":"b72db564e1732bb1b6bcaa7e122e8788","permalink":"https://example.com/publication/brandenburg-2020/","publishdate":"2024-02-02T14:14:57.404571Z","relpermalink":"/publication/brandenburg-2020/","section":"publication","summary":"","tags":null,"title":"New approaches to study excited states in density functional theory: general discussion","type":"publication"},{"authors":["Gianluca Levi","Elisa Biasin","Asmus Ougaard Dohn","Hannes Jónsson"],"categories":null,"content":"","date":1577836800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1577836800,"objectID":"9f5e994fe7cf1f3116f388dc6bfb72b5","permalink":"https://example.com/publication/levi-2020-pccp/","publishdate":"2024-02-02T14:14:57.385191Z","relpermalink":"/publication/levi-2020-pccp/","section":"publication","summary":"Copper(I) bis-phenanthroline complexes represent Earth-abundant alternatives to ruthenium-based sensitizers for solar energy conversion and photocatalysis. Improved understanding of the solvent- mediated excited-state structural dynamics can help optimize their photoconversion efficiency. Through direct dynamics simulations in acetonitrile and excited-state minimum energy path calculations in vacuum, we uncover the mechanism of the photoinduced flattening motion of the prototypical system [Cu(dmphen)2]+ (dmphen = 2,9-dimethyl-1,10-phenanthroline). We find that the ligand distortion is a two-step process in acetonitrile. The fast component (B110 fs) is due to spontaneous pseudo Jahn– Teller instability and is largely solvent independent, while the slow component (B1.2 ps) arises from the mutual interplay between solvent molecules closely approaching the metal center and rotation of the methyl substituents. These results shed new light on the influence of a donor solvent such as acetonitrile and methyl substituents on the flattening dynamics of [Cu(dmphen)2]+.","tags":null,"title":"On the interplay of solvent and conformational effects in simulated excited-state dynamics of a copper phenanthroline photosensitizer","type":"publication"},{"authors":["Gianluca Levi","Aleksei V. Ivanov","Hannes Jonsson"],"categories":null,"content":"","date":1577836800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1577836800,"objectID":"8eed2820e8ad15923c9e41ae4751aacd","permalink":"https://example.com/publication/levi-2020-fd/","publishdate":"2024-02-02T14:14:57.399805Z","relpermalink":"/publication/levi-2020-fd/","section":"publication","summary":"A direct optimization method for obtaining excited electronic states using density functionals is presented. It involves selective convergence on saddle points on the energy surface representing the variation of the energy as a function of the electronic degrees of freedom, thereby avoiding convergence to a minimum and corresponding variational collapse to the ground electronic state. The method is based on an exponential transformation of the molecular orbitals, making it possible to use efficient quasi-Newton optimization approaches. Direct convergence on a target nth-order saddle point is guided by an appropriate preconditioner for the optimization as well as the maximum overlap method. Results of benchmark calculations of 52 excited states of molecules indicate that the method is more robust than a standard self-consistent field (SCF) approach especially when degenerate or quasi-degenerate orbitals are involved. The method can overcome challenges arising from rearrangement of closely spaced orbitals in a charge-transfer excitation of the nitrobenzene molecule, a case where the SCF fails to converge. The formulation of the method is general and can be applied to non-unitary invariant functionals, such as self-interaction corrected functionals.","tags":null,"title":"Variational Calculations of Excited States Via Direct Optimization of Orbitals in DFT","type":"publication"},{"authors":["Gianluca Levi","Aleksei V. Ivanov","Hannes Jónsson"],"categories":null,"content":"","date":1577836800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1577836800,"objectID":"0a4c37cc04b4b4ccf826f7911bb6ad6f","permalink":"https://example.com/publication/levi-2020-jctc/","publishdate":"2024-02-02T14:14:57.389836Z","relpermalink":"/publication/levi-2020-jctc/","section":"publication","summary":"A direct optimization method for obtaining excited electronic states using density functionals is presented. A direct optimization method for obtaining excited electronic states using density functionals is presented. It involves selective convergence on saddle points on the energy surface representing the variation of the energy as a function of the electronic degrees of freedom, thereby avoiding convergence to a minimum and corresponding variational collapse to the ground electronic state. The method is based on an exponential transformation of the molecular orbitals, making it possible to use efficient quasi-Newton optimization approaches. Direct convergence on a target n th-order saddle point is guided by an appropriate preconditioner for the optimization as well as the maximum overlap method. Results of benchmark calculations of 52 excited states of molecules indicate that the method is more robust than a standard self-consistent field (SCF) approach especially when degenerate or quasi-degenerate orbitals are involved. The method can overcome challenges arising from rearrangement of closely spaced orbitals in a charge-transfer excitation of the nitrobenzene molecule, a case where the SCF fails to converge. The formulation of the method is general and can be applied to non-unitary invariant functionals, such as self-interaction corrected functionals.","tags":null,"title":"Variational Density Functional Calculations of Excited States via Direct Optimization","type":"publication"},{"authors":["Mostafa Abedi","Gianluca Levi","Diana B Zederkof","Niels Engholm Henriksen","Mátyás Pápai","Klaus B. Møller"],"categories":null,"content":"","date":1546300800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1546300800,"objectID":"02de12da87670c9d0e83987e4dfcda4b","permalink":"https://example.com/publication/abedi-2019/","publishdate":"2024-02-02T14:14:57.409517Z","relpermalink":"/publication/abedi-2019/","section":"publication","summary":"In this work, we investigate the excited-state solute and solvation structure of [Ru(bpy)3]2+, [Fe(bpy)3]2+, [Fe(bmip)2]2+ and [Cu(phen)2]+ (bpy = 2,2′-bipyridine; bmip = 2,6-bis(3-methyl-imidazole-1-ylidine)-pyridine; phen = 1,10-phenanthroline) transition metal complexes (TMCs) in terms of solute–solvent radial distribution functions (RDFs) and evaluate the performance of some of the most popular partial atomic charge (PAC) methods for obtaining these RDFs by molecular dynamics (MD) simulations. To this end, we compare classical MD of a frozen solute in water and acetonitrile (ACN) with quantum mechanics/molecular mechanics Born–Oppenheimer molecular dynamics (QM/MM BOMD) simulations. The calculated RDFs show that the choice of a suitable PAC method is dependent on the coordination number of the metal, denticity of the ligands, and type of solvent. It is found that this selection is less sensitive for water than ACN. Furthermore, a careful choice of the PAC method should be considered for TMCs that exhibit a free direct coordination site, such as [Cu(phen)2]+. The results of this work show that fast classical MD simulations with ChelpG/RESP or CM5 PACs can produce RDFs close to those obtained by QM/MM MD and thus, provide reliable solvation structures of TMCs to be used, e.g. in the analysis of scattering data.","tags":null,"title":"Excited-State Solvation Structure of Transition Metal Complexes from Molecular Dynamics Simulations and Assessment of Partial Atomic Charge Methods","type":"publication"},{"authors":["Mátyás Pápai","Mostafa Abedi","Gianluca Levi","Elisa Biasin","Martin M Nielsen","Klaus B Møller"],"categories":null,"content":"","date":1546300800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1546300800,"objectID":"5ae9ef61d5bf371804524fe0f61b6f87","permalink":"https://example.com/publication/papai-2019/","publishdate":"2024-02-02T14:14:57.414963Z","relpermalink":"/publication/papai-2019/","section":"publication","summary":"The solvent-mediated excited-state dynamics of the COOH- functionalized Fe-carbene photosensitizer [Fe(bmicp)2]2+ (bmicp = 2,6-bis(3- methyl-imidazole-1-ylidine)-4-carboxy-pyridine) is studied by time-dependent density functional theory, as well as classical and quantum dynamics simulations. We demonstrate the crucial role of the polar acetonitrile solvent in stabilizing the metal-to-ligand charge transfer (MLCT) states of the investigated molecule using the conductor polarizable continuum model. This leads to dynamics that avoid sub-ps back electron transfer to the metal and an exceptionally long-lived 1MLCT state that does not undergo sub-ps 1MLCT → 3MLCT intersystem crossing as it is energetically isolated. We identify two components of the excited-state solvent reorganization process: an initial rotation (∼300 fs) and diffusional dynamics within the local cage surrounding the rotated solvent molecule (∼2 ps). Finally, it is found that the relaxation of the solvent only slightly affects the excited-state population dynamics of [Fe(bmicp)2]2+.","tags":null,"title":"Theoretical Evidence of Solvent-Mediated Excited-State Dynamics in a Functionalized Iron Sensitizer","type":"publication"},{"authors":["Kristoffer Haldrup","Gianluca Levi","Elisa Biasin","Peter Vester","Mads Goldschmidt Laursen","Frederik Beyer","Kasper Skov Kjær","Tim Brandt Van Driel","Tobias Harlang","Asmus O. Dohn","Robert J. Hartsock","Silke Nelson","James M. Glownia","Henrik T. Lemke","Morten Christensen","Kelly J. Gaffney","Niels E. Henriksen","Klaus B. Møller","Martin M. Nielsen"],"categories":null,"content":"","date":1546300800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1546300800,"objectID":"9f7cdd69d5771d4d3eed5489d37f6dda","permalink":"https://example.com/publication/haldrup-2019/","publishdate":"2024-02-02T14:14:57.420255Z","relpermalink":"/publication/haldrup-2019/","section":"publication","summary":"We report x-ray free electron laser experiments addressing ground-state structural dynamics of the diplatinum anion Pt2POP4 following photoexcitation. The structural dynamics are tracked with \u003c100 fs time resolution by x-ray scattering, utilizing the anisotropic component to suppress contributions from the bulk solvent. The x-ray data exhibit a strong oscillatory component with period 0.28 ps and decay time 2.2 ps, and structural analysis of the difference signal directly shows this as arising from ground-state dynamics along the PtPt coordinate. These results are compared with multiscale Born-Oppenheimer molecular dynamics simulations and demonstrate how off-resonance excitation can be used to prepare a vibrationally cold excited-state population complemented by a structure-dependent depletion of the ground-state population which subsequently evolves in time, allowing direct tracking of ground-state structural dynamics.","tags":["doi:10.1103/PhysRevLett.122.063001 url:https://doi"],"title":"Ultrafast X-Ray Scattering Measurements of Coherent Structural Dynamics on the Ground-State Potential Energy Surface of a Diplatinum Molecule","type":"publication"},{"authors":["Elisa Biasin","Tim Brandt van Driel","Gianluca Levi","Mads G Laursen","Asmus O Dohn","Asbjørn Moltke","Peter Vester","Frederik B. K. Hansen","Kasper S Kjaer","Tobias Harlang","Robert Hartsock","Morten Christensen","Kelly J. Gaffney","Niels E. Henriksen","Klaus B. Møller","Kristoffer Haldrup","Martin M Nielsen"],"categories":null,"content":"","date":1514764800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1514764800,"objectID":"05b96af22f22012ad051feb8d8745c95","permalink":"https://example.com/publication/biasin-2018-a/","publishdate":"2024-02-02T14:14:57.425313Z","relpermalink":"/publication/biasin-2018-a/","section":"publication","summary":"Time-resolved X-ray scattering patterns from photoexcited molecules in solution are in many cases anisotropic at the ultrafast time scales accessible at X-ray free-electron lasers (XFELs). This anisotropy arises from the interaction of a linearly polarized UV–Vis pump laser pulse with the sample, which induces anisotropic structural changes that can be captured by femtosecond X-ray pulses. In this work, a method for quantitative analysis of the anisotropic scattering signal arising from an ensemble of molecules is described, and it is demonstrated how its use can enhance the structural sensitivity of the time-resolved X-ray scattering experiment. This method is applied on time-resolved X-ray scattering patterns measured upon photoexcitation of a solvated di-platinum complex at an XFEL, and the key parameters involved are explored. It is shown that a combined analysis of the anisotropic and isotropic difference scattering signals in this experiment allows a more precise determination of the main photoinduced structural change in the solute, i.e. the change in Pt—Pt bond length, and yields more information on the excitation channels than the analysis of the isotropic scattering only. Finally, it is discussed how the anisotropic transient response of the solvent can enable the determination of key experimental parameters such as the instrument response function.","tags":["anisotropic scattering","molecular structure","orientational selection","supporting information","this article has","time-resolved","ultrafast","xfel"],"title":"Anisotropy enhanced X-ray scattering from solvated transition metal complexes research papers","type":"publication"},{"authors":["Gianluca Levi","Matyas Papai","Niels E Henriksen","Asmus O Dohn","Klaus B Møller"],"categories":null,"content":"","date":1514764800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1514764800,"objectID":"8faa2201100adbd50abf74c4f2352cf6","permalink":"https://example.com/publication/levi-2018/","publishdate":"2024-02-02T14:14:57.430762Z","relpermalink":"/publication/levi-2018/","section":"publication","summary":"Recent ultrafast experiments have unveiled the time scales of vibrational cooling and decoherence upon photoexcitation of the diplatinum complex [Pt2(P2O5H2)4]4– in solvents. Here, we contribute to the understanding of the structure and dynamics of the lowest lying singlet excited state of the model photocatalyst by performing potential energy surface calculations and Born–Oppenheimer molecular dynamics simulations in the gas phase and in water. Solvent effects were treated using a multiscale quantum mechanics/molecular mechanics approach. Fast sampling was achieved with a modified version of delta self-consistent field implemented in the grid-based projector-augmented wave density functional theory code. The known structural parameters and the PESs of the first singlet and triplet excited states are correctly reproduced. Besides, the simulations deliver clear evidence that pseudorotation of the ligands in the excited state leads to symmetry lowering of the Pt2P8 core. Coherence decay of Pt–Pt stretching vibrations in solution was found to be governed by vibrational cooling, which is in agreement with previous ultrafast experiments. We also show that the flow of excess Pt–Pt vibrational energy is first directed toward vibrational modes involving the ligands, with the solvent favoring intramolecular vibrational energy redistribution. The results are supported by thorough vibrational analysis in terms of generalized normal modes.","tags":null,"title":"Solution structure and ultrafast vibrational relaxation of the PtPOP complex revealed by ∆SCF-QM/MM Direct Dynamics simulations","type":"publication"},{"authors":["Asmus O. Dohn","Elvar Ö Jónsson","Gianluca Levi","Jens J. Mortensen","Olga Lopez-Acevedo","Kristian S. Thygesen","Karsten W. Jacobsen","Jens Ulstrup","Niels E. Henriksen","Klaus B. Møller","Hannes Jónsson"],"categories":null,"content":"","date":1483228800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1483228800,"objectID":"eb182d4a31d0e08df42b0cb8f71d2e51","permalink":"https://example.com/publication/dohn-2017/","publishdate":"2024-02-02T14:14:57.440939Z","relpermalink":"/publication/dohn-2017/","section":"publication","summary":"A multiscale density functional theory–quantum mechanics/molecular mechanics (DFT-QM/MM) scheme is presented, based on an efficient electrostatic coupling between the electronic density obtained from a grid-based projector augmented wave (GPAW) implementation of density functional theory and a classical potential energy function. The scheme is implemented in a general fashion and can be used with various choices for the descriptions of the QM or MM regions. Tests on H2O clusters, ranging from dimer to decamer show that no systematic energy errors are introduced by the coupling that exceeds the differences in the QM and MM descriptions. Over 1 ns of liquid water, Born–Oppenheimer QM/MM molecular dynamics (MD) are sampled combining 10 parallel simulations, showing consistent liquid water structure over the QM/MM border. The method is applied in extensive parallel MD simulations of an aqueous solution of the diplatinum [Pt2(P2O5H2)4]4– complex (PtPOP), spanning a total time period of roughly half a nanosecond. An average Pt–Pt distance deviating only 0.01 Å from experimental results, and a ground-state Pt–Pt oscillation frequency deviating by \u003c2% from experimental results were obtained. The simulations highlight a remarkable harmonicity of the Pt–Pt oscillation, while also showing clear signs of Pt–H hydrogen bonding and directional coordination of water molecules along the Pt–Pt axis of the complex.","tags":null,"title":"Grid-Based Projector Augmented Wave (GPAW) Implementation of Quantum Mechanics/Molecular Mechanics (QM/MM) Electrostatic Embedding and Application to a Solvated Diplatinum Complex","type":"publication"},{"authors":["Gianluca Levi","Mauro Causà","Paolo Lacovig","Piero Salatino","Osvalda Senneca"],"categories":null,"content":"","date":1483228800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1483228800,"objectID":"3aaecbe51cf144a7f09a85d3fb47e5cc","permalink":"https://example.com/publication/levi-2017/","publishdate":"2024-02-02T14:14:57.435908Z","relpermalink":"/publication/levi-2017/","section":"publication","summary":"The present study investigates the coal char combustion by a combination of thermochemical and X-ray photoemission spectroscopy (XPS) analyses. Thermoanalytical methods (differential thermogravimetry, differential scanning calorimetry, and temperature-programmed desorption) are used to identify the key reactive steps that occur upon oxidation and heating of coal char (chemisorption, structural rearrangement and switchover of surface oxides, and desorption) and their energetics. XPS is used to reveal the chemical nature of the surface oxides that populate the char surface and to monitor their evolution throughout thermochemical processing. XPS spectra show the presence on the carbon surface of three main components. It is shown that the most abundant oxygen functionality in the raw char is epoxy. It decreases with preoxidation at 300 °C and even more at 500 °C, where carboxyl and ether oxygen functionalities prevail. The rearrangement of epoxy during preoxidation goes together with activation of the more stable and less reactive carbon sites. Results are in good agreement with semi-lumped kinetic models of carbon oxidation, which include (1) formation of “metastable” surface oxides, (2) complex switchover, and (3) desorption into CO and CO2.","tags":null,"title":"Mechanism and Thermochemistry of Coal Char Oxidation and Desorption of Surface Oxides","type":"publication"},{"authors":["Gianluca Levi","Osvalda Senneca","Mauro Causà","Piero Salatino","Paolo Lacovig","Silvano Lizzit"],"categories":null,"content":"","date":1438387200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1438387200,"objectID":"ae4d3b2177f80cbd89b1f1b25983509d","permalink":"https://example.com/publication/levi-2015/","publishdate":"2024-02-02T14:14:57.446228Z","relpermalink":"/publication/levi-2015/","section":"publication","summary":"Coal chars, like most solid carbons, have a pronounced tendency to chemisorb oxygen at low and moderate temperatures. Characterization by XPS of surface oxides on carbon has been accomplished with the aim of providing a better atomistic insight into: (a) reactions involved in molecular oxygen adsorption on coals and (b) the relations between the nanostructure of solid carbons and the chemistry of oxidation. High-resolution C 1s and O 1s core level and valence band XPS spectra effectively reflected the oxidative functionalization of different types of coals and synthetic carbons upon oxidation in air at moderate temperatures (300 and 500 ??C). More specifically, analysis of C 1s and valence band spectra could be directed to monitor the structural evolution of the carbons in terms of extension of sp2 versus sp3 conjugation, carbon vacancies and oxidized carbon. Comparison of the O 1s spectra, on the other hand, provided a tool to characterize the nature of oxygen bonding on carbon and to determine the relative abundance of carbon-oxygen species. Results underline the important role of epoxy groups in the early stages of oxidation, providing a mechanistic framework for the identification of the stable and metastable intermediates in the heterogeneous oxidation of coal by molecular oxygen.","tags":null,"title":"Probing the chemical nature of surface oxides during coal char oxidation by high-resolution XPS","type":"publication"},{"authors":null,"categories":null,"content":" Funding CNERGY: Ultrafast Charge and Energy Transfer in Sunlight Conversion 2021 - 2024 IRF Project Grant Gianluca Levi Efficient molecular photoswitches identified using simulations of ultrafast charge transfer and solvation dynamics 2023 - 2026 IRF Postdoctoral Fellowship Grant Elli Inkeri Selenius EQuanDo: Energy Transfer in Semiconductor Quantum Dots Studied Using Nonadiabatic Dynamics and Reaction Path Calculations 2021 - 2024 IRF Doctoral student Grant Yorick Leonard A. Schmerwitz Exploring the Reaction Paths of Solvated Iron Photosensitizers: a Multiscale Nudged Elastic Band Strategy 2020 - 2023 IRF Doctoral student Grant Benedikt Orri Birgisson Electron-Nuclear Dynamics in Iron-Sensitized Solar Cells: A Unified Model Description from Light Absorption to Charge Separation 2019 - 2022 IRF Postdoctoral Fellowship Grant Gianluca Levi ","date":-62135596800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":-62135596800,"objectID":"768afc3a053405c37420b437a94d4f97","permalink":"https://example.com/funding/","publishdate":"0001-01-01T00:00:00Z","relpermalink":"/funding/","section":"","summary":"Funding CNERGY: Ultrafast Charge and Energy Transfer in Sunlight Conversion 2021 - 2024 IRF Project Grant Gianluca Levi Efficient molecular photoswitches identified using simulations of ultrafast charge transfer and solvation dynamics 2023 - 2026 IRF Postdoctoral Fellowship Grant Elli Inkeri Selenius EQuanDo: Energy Transfer in Semiconductor Quantum Dots Studied Using Nonadiabatic Dynamics and Reaction Path Calculations 2021 - 2024 IRF Doctoral student Grant Yorick Leonard A.","tags":null,"title":"","type":"page"}] \ No newline at end of file + [{"authors":null,"categories":null,"content":" Group Members Gianluca Levi Group leader Science Institute of the University of Iceland VR-III Hjarðarhagi 2, 107 Reykjavík\nORCID Web of Science Google Scholar CV +354 8326622, giale@hi.is\nElli Inkeri Selenius Postdoc Science Institute of the University of Iceland VR-III Hjarðarhagi 2, 107 Reykjavík\nORCID Web of Science Google Scholar\nelliselenius@hi.is\nYorick Leonard A. Schmerwitz PhD student (co-supervised, main supervisor: Prof. Hannes Jónsson)\nScience Institute of the University of Iceland VR-III Hjarðarhagi 2, 107 Reykjavík\nORCID Web of Science Google Scholar\nyla1@hi.is\nBenedikt Orri Birgisson PhD student (co-supervised, main supervisor: Prof. Hannes Jónsson)\nScience Institute of the University of Iceland VR-III Hjarðarhagi 2, 107 Reykjavík\nbob9@hi.is\nCollaborations University of Iceland Elvar Örn Jónsson Hannes Jónsson\nTechnical University of Denmark Asmus Ougaard Dohn Kristoffer Haldrup Luca Laraia Martin Meedom Nielsen\nUniversity of Erlangen–Nuremberg Philipp Hansmann\n","date":1706572800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1706572800,"objectID":"c1d17ff2b20dca0ad6653a3161942b64","permalink":"https://example.com/people/","publishdate":"2024-01-30T00:00:00Z","relpermalink":"/people/","section":"","summary":"Group Members Gianluca Levi Group leader Science Institute of the University of Iceland VR-III Hjarðarhagi 2, 107 Reykjavík\nORCID Web of Science Google Scholar CV +354 8326622, giale@hi.is\nElli Inkeri Selenius Postdoc Science Institute of the University of Iceland VR-III Hjarðarhagi 2, 107 Reykjavík","tags":null,"title":"","type":"page"},{"authors":["Natalia E Powers-Riggs","Benedikt O Birgisson","Sumana L Raj","Philipp Lenzen","Diana Bregenholt Zederkof","Morten Haubro","K V Dagrún Tveiten","Robert W Hartsock","Tim B Van Driel","Matthieu Chollet","Joseph S Robinson","Silke Nelson","Kristoffer Haldrup","Kasper Steen Pedersen","Gianluca Levi","Ougaard Dohn","Jónsson Hannes","Klaus Braagaard Møller","Adi Natan","Martin Meedom Nielsen","Kelly Gaffney"],"categories":null,"content":"","date":1704067200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1704067200,"objectID":"2d152bc3dff6d27b33a6849e5441f3e6","permalink":"https://example.com/publication/powers-riggs-2024/","publishdate":"2024-02-02T14:14:57.342234Z","relpermalink":"/publication/powers-riggs-2024/","section":"publication","summary":"Dimeric complexes composed of d8 square planar metal centers and rigid bridg- ing ligands provide model systems to understand the interplay between attractive dispersion forces and steric strain, in order to assist the development reliable meth- ods to model metal dimer complexes more broadly. [Ir2(dimen)4]2+ (dimen = para- diisocyanomenthane) presents a unique case study for such phenomena, as distortions of the optimal structure of a ligand with limited conformational flexibility counteracts the attractive dispersive forces from the metal and ligand to yield a complex with two ground state deformational isomers. Here, we use ultrafast X-ray solution scattering (XSS) and optical transient absorption spectroscopy (OTAS) to reveal the nature of the equilibrium distribution and the exchange rate between the deformational isomers. The two ground state isomers have spectrally distinct electronic excitations that enable the selective excitation of one isomer or the other using a femtosecond duration pulse of visible light. We then track the dynamics of the non-equilibrium depletion of the electronic ground state population – often termed the ground state hole – with ultra- fast XSS and OTAS, revealing a restoration of the ground state equilibrium in 2.3 ps. This experimental study provides a critical test of various density functional approx- imations in the description of bridged d8-d8 metal complexes. Our study shows that reproduction of the primary experimental observations requires a hybrid functional, which includes exact exchange, while also accounting for dispersion interactions.","tags":null,"title":"Characterization of deformational isomerization potential and interconversion dynamics with ultrafast x-ray solution scattering","type":"publication"},{"authors":["Jens Jørgen Mortensen","Ask Hjorth Larsen","Mikael Kuisma","Aleksei V. Ivanov","Alireza Taghizadeh","Andrew Peterson","Anubhab Haldar","Asmus Ougaard Dohn","Christian Schäfer","Elvar Örn Jónsson","Eric D. Hermes","Fredrik Andreas Nilsson","Georg Kastlunger","Gianluca Levi","Hannes Jónsson","Hannu Häkkinen","Jakub Fojt","Jiban Kangsabanik","Joachim Sødequist","Jouko Lehtomäki","Julian Heske","Jussi Enkovaara","Kirsten Trøstrup Winther","Marcin Dulak","Marko M. Melander","Martin Ovesen","Martti Louhivuori","Michael Walter","Morten Gjerding","Olga Lopez-Acevedo","Paul Erhart","Robert Warmbier","Rolf Würdemann","Sami Kaappa","Simone Latini","Tara Maria Boland","Thomas Bligaard","Thorbjørn Skovhus","Toma Susi","Tristan Maxson","Tuomas Rossi","Xi Chen","Yorick Leonard A. Schmerwitz","Jakob Schiøtz","Thomas Olsen","Karsten Wedel Jacobsen","Kristian Sommer Thygesen"],"categories":null,"content":"","date":1704067200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1704067200,"objectID":"fecc1f77629a5542cb287e6a321ca0e7","permalink":"https://example.com/publication/mortensen-2024/","publishdate":"2024-02-02T14:14:57.347699Z","relpermalink":"/publication/mortensen-2024/","section":"publication","summary":"We review the GPAW open-source Python package for electronic structure calculations. GPAW is based on the projector-augmented wave method and can solve the self-consistent density functional theory (DFT) equations using three different wave-function representations, namely real-space grids, plane waves, and numerical atomic orbitals. The three representations are complementary and mutually independent and can be connected by transformations via the real-space grid. This multi-basis feature renders GPAW highly versatile and unique among similar codes. By virtue of its modular structure, the GPAW code constitutes an ideal platform for implementation of new features and methodologies. Moreover, it is well integrated with the Atomic Simulation Environment (ASE) providing a flexible and dynamic user interface. In addition to ground-state DFT calculations, GPAW supports many-body GW band structures, optical excitations from the Bethe-Salpeter Equation (BSE), variational calculations of excited states in molecules and solids via direct optimization, and real-time propagation of the Kohn-Sham equations within time-dependent DFT. A range of more advanced methods to describe magnetic excitations and non-collinear magnetism in solids are also now available. In addition, GPAW can calculate non-linear optical tensors of solids, charged crystal point defects, and much more. Recently, support of GPU acceleration has been achieved with minor modifications of the GPAW code thanks to the CuPy library. We end the review with an outlook describing some future plans for GPAW.","tags":null,"title":"GPAW: open Python package for electronic-structure calculations","type":"publication"},{"authors":["Elli Selenius","Alec Elías Sigurðarson","Yorick L. A. Schmerwitz","Gianluca Levi"],"categories":null,"content":"","date":1704067200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1704067200,"objectID":"bcfa7e3c0f3c211313b854dd04c37fda","permalink":"https://example.com/publication/selenius-2024/","publishdate":"2024-02-02T14:14:57.334688Z","relpermalink":"/publication/selenius-2024/","section":"publication","summary":"A strategy is presented for variational orbital optimization in time-independent calculations of excited electronic states. The approach involves minimizing the energy while constraining the degrees of freedom corresponding to negative curvature on the electronic energy surface, followed by fully unconstrained optimization, thereby converging on a saddle point. Both steps of this freeze-and-release strategy are carried out via direct orbital optimization at a similar cost as ground state calculations. The approach is applied in orbital optimized density functional calculations and is shown to converge intramolecular charge transfer excited states where the common maximum overlap method is unable to prevent collapse to unphysical, charge-delocalized solutions. The constrained minimization can also be used to improve the estimate of the saddle point order of the target excited state solution, which is required as input for generalized mode following methods. Calculations with the local density approximation and the generalized gradient approximation functionals PBE and BLYP are carried out for a large set of charge transfer excitations in organic molecules using both direct optimization as well as the linear-response time-dependent density functional theory (TD-DFT) method. The time-independent approach is fully variational and provides a relaxed excited state electron density that can be used to quantify the extent of charge transfer. The TD-DFT calculations are found to generally overestimate the charge transfer distance compared to the orbital optimized calculations, even when the TD-DFT relaxed density is used. Furthermore, the orbital optimized calculations yield more accurate excitation energy values relative to the theoretical best estimates for the medium and long-range charge transfer distances, where the errors of TD-DFT are as large as 2 eV.","tags":null,"title":"Orbital optimized vs time-dependent density functional calculations of intramolecular charge transfer excited states","type":"publication"},{"authors":["Tetsuo Katayama","Tae Kyu Choi","Dmitry Khakhulin","Asmus O Dohn","Christopher J. Milne","György Vankó","Zoltán Németh","Frederico A. Lima","Jakub Szlachetko","Tokushi Sato","Shunsuke Nozawa","Shin Ichi Adachi","Makina Yabashi","Thomas J. Penfold","Wojciech Gawelda","Gianluca Levi"],"categories":null,"content":"","date":1672531200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1672531200,"objectID":"7a1d7777a963c4dc088cf764b88b8ccb","permalink":"https://example.com/publication/katayama-2023/","publishdate":"2024-02-02T14:14:57.353919Z","relpermalink":"/publication/katayama-2023/","section":"publication","summary":"Photochemical reactions in solution are governed by a complex interplay between transient intramolecular electronic and nuclear structural changes and accompanying solvent rearrangements. State-of-the-art time-resolved X-ray solution scattering has emerged in the last decade as a powerful technique to observe solute and solvent motions in real time. However, disentangling solute and solvent dynamics and how they mutually influence each other remains challenging. Here, we simultaneously measure femtosecond X-ray emission and scattering to track both the intramolecular and solvation structural dynamics following photoexcitation of a solvated copper photosensitizer. Quantitative analysis assisted by molecular dynamics simulations reveals a two-step ligand flattening strongly coupled to the solvent reorganization, which conventional optical methods could not discern. First, a ballistic flattening triggers coherent motions of surrounding acetonitrile molecules. In turn, the approach of acetonitrile molecules to the copper atom mediates the decay of intramolecular coherent vibrations and induces a further ligand flattening. These direct structural insights reveal that photoinduced solute and solvent motions can be intimately intertwined, explaining how the key initial steps of light harvesting are affected by the solvent on the atomic time and length scale. Ultimately, this work takes a step forward in understanding the microscopic mechanisms of the bidirectional influence between transient solvent reorganization and photoinduced solute structural dynamics.","tags":null,"title":"Atomic-scale observation of solvent reorganization influencing photoinduced structural dynamics in a copper complex photosensitizer","type":"publication"},{"authors":["Yorick L. A. Schmerwitz","Gianluca Levi","Hannes Jónsson"],"categories":null,"content":"","date":1672531200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1672531200,"objectID":"adade83911a8e286321fdbdc5fec7930","permalink":"https://example.com/publication/schmerwitz-2023/","publishdate":"2024-02-02T14:14:57.364513Z","relpermalink":"/publication/schmerwitz-2023/","section":"publication","summary":"Variational calculations of excited electronic states are carried out by finding saddle points on the surface that describes how the energy of the system varies as a function of the electronic degrees of freedom. This approach has several advantages over commonly used methods especially in the context of density functional calculations, as collapse to the ground state is avoided and yet, the orbitals are variationally optimized for the excited state. This optimization makes it possible to describe excitations with large charge transfer where calculations based on ground state orbitals are problematic, as in linear response time-dependent density functional theory. A generalized mode following method is presented where an $n^textth$-order saddle point is found by inverting the components of the gradient in the direction of the eigenvectors of the $n$ lowest eigenvalues of the electronic Hessian matrix. This approach has the distinct advantage of following a chosen excited state through atomic configurations where the symmetry of the single determinant wave function is broken, as demonstrated in calculations of potential energy curves for nuclear motion in the ethylene and dihydrogen molecules. The method is implemented using a generalized Davidson algorithm and an exponential transformation for updating the orbitals within a generalized gradient approximation of the energy functional. Convergence is found to be more robust than for a direct optimization approach previously shown to outperform standard self-consistent field approaches, as illustrated here for charge transfer excitations in nitrobenzene and N-phenylpyrrole, involving calculations of $4^textth$- and $6^textth$-order saddle points, respectively. Finally, calculations of a diplatinum and silver complex are presented, illustrating the applicability of the method to excited state energy curves of large molecules.","tags":null,"title":"Calculations of Excited Electronic States by Converging on Saddle Points Using Generalized Mode Following","type":"publication"},{"authors":["Aleksei V. Ivanov","Yorick L. A. Schmerwitz","Gianluca Levi","Hannes Jónsson"],"categories":null,"content":"","date":1672531200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1672531200,"objectID":"f0c990063c541ef724582297df162936","permalink":"https://example.com/publication/ivanov-2023/","publishdate":"2024-02-02T14:14:57.359243Z","relpermalink":"/publication/ivanov-2023/","section":"publication","summary":"Elucidation of the mechanism for optical spin initialization of point defects in solids in the context of quantum applications requires an accurate description of the excited electronic states involved. While variational density functional calculations have been successful in describing the ground state of a great variety of systems, doubts have been expressed in the literature regarding the ability of such calculations to describe electronic excitations of point defects. A direct orbital optimization method is used here to perform time-independent, variational density functional calculations of a prototypical defect, the negatively charged nitrogen-vacancy center in diamond. The calculations include up to 512 atoms subject to periodic boundary conditions and the excited state calculations require similar computational effort as ground state calculations. Contrary to some previous reports, the use of local and semi-local density functionals gives the correct ordering of the low-lying triplet and singlet states, namely 3A2 \u003c 1E \u003c 1A1 \u003c 3E. Furthermore, the more advanced meta generalized gradient approximation functionals give results that are in remarkably good agreement with high-level, many-body calculations as well as available experimental estimates, even for the excited singlet state which is often referred to as having multireference character. The lowering of the energy in the triplet excited state as the atom coordinates are optimized in accordance with analytical forces is also close to the experimental estimate and the resulting zero-phonon line triplet excitation energy is underestimated by only 0.15 eV. The approach used here is found to be a promising tool for studying electronic excitations of point defects in, for example, systems relevant for quantum technologies.","tags":null,"title":"Electronic excitations of the charged nitrogen-vacancy center in diamond obtained using time-independent variational density functional calculations","type":"publication"},{"authors":["Alec E. Sigurðarson","Yorick L. A. Schmerwitz","Dagrún K. V. Tveiten","Gianluca Levi","Hannes Jónsson"],"categories":null,"content":"","date":1672531200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1672531200,"objectID":"836f37ae37f0d784e4501f37149f9651","permalink":"https://example.com/publication/sigurdarson-2023/","publishdate":"2024-02-02T14:14:57.369903Z","relpermalink":"/publication/sigurdarson-2023/","section":"publication","summary":"Density functional calculations of Rydberg excited states up to high energy are carried out for several molecules using an approach where the orbitals are variationally optimized by converging on saddle points on the electronic energy surface within a real space grid representation. Remarkably good agreement with experimental estimates of the excitation energy is obtained using the generalized gradient approximation (GGA) functional of Perdew, Burke and Ernzerhof (PBE) when Perdew-Zunger self-interaction correction is applied in combination with complex-valued orbitals. Even without the correction, the PBE functional gives quite good results despite the fact that corresponding Rydberg virtual orbitals have positive energy in the ground state calculation. Results obtained using the TPSS and r2SCAN meta-GGA functionals are also presented, but they do not provide a systematic improvement over the results from the uncorrected PBE functional. The grid representation combined with the projector augmented-wave approach gives a simpler and better representation of the diffuse Rydberg orbitals than a linear combination of atomic orbitals with commonly used basis sets, the latter leading to an overestimation of the excitation energy due to confinement of the excited states.","tags":null,"title":"Orbital-optimized Density Functional Calculations of Molecular Rydberg Excited States with Real Space Grid Representation and Self-Interaction Correction","type":"publication"},{"authors":["Yorick L. A. Schmerwitz","Aleksei V. Ivanov","Elvar Ö. Jónsson","Hannes Jónsson","Gianluca Levi"],"categories":null,"content":"","date":1640995200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1640995200,"objectID":"4d759ea085a5cd97f187984ec9820cdd","permalink":"https://example.com/publication/schmerwitz-2022/","publishdate":"2024-02-02T14:14:57.375018Z","relpermalink":"/publication/schmerwitz-2022/","section":"publication","summary":"Theoretical studies of photochemical processes require a description of the energy surfaces of excited electronic states, especially near degeneracies, where transitions between states are most likely. Systems relevant to photochemical applications are typically too large for high-level multireference methods, and while time-dependent density functional theory (TDDFT) is efficient, it can fail to provide the required accuracy. A variational, time- independent density functional approach is applied to the twisting of the double bond and pyramidal distortion in ethylene, the quintessential model for photochemical studies. By allowing for symmetry breaking, the calculated energy surfaces exhibit the correct topology around the twisted-pyramidalized conical intersection even when using a semilocal functional approximation, and by including explicit self-interaction correction, the torsional energy curves are in close agreement with published multireference results. The findings of the present work point to the possibility of using a single determinant time-independent density functional approach to simulate nonadiabatic dynamics, even for large systems where multireference methods are impractical and TDDFT is often not accurate enough.","tags":null,"title":"Variational Density Functional Calculations of Excited States: Conical Intersection and Avoided Crossing in Ethylene Bond Twisting","type":"publication"},{"authors":["Aleksei V. Ivanov","Gianluca Levi","Elvar Ö. Jónsson","Hannes Jónsson"],"categories":null,"content":"","date":1625097600,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1625097600,"objectID":"cca8ea6afaf84782b5b5fad638f4082b","permalink":"https://example.com/publication/ivanov-2021/","publishdate":"2024-02-02T14:14:57.38003Z","relpermalink":"/publication/ivanov-2021/","section":"publication","summary":"A direct orbital optimization method is presented for density functional calculations of excited electronic states using either a real space grid or a plane-wave basis set. The method is variational, provides atomic forces in the excited states, and can be applied to Kohn−Sham (KS) functionals as well as orbital-density-dependent (ODD) functionals including explicit self-interaction correction. The implementation for KS functionals involves two nested loops: (1) An inner loop for finding a stationary point in a subspace spanned by the occupied and a few virtual orbitals corresponding to the excited state; (2) an outer loop for minimizing the energy in a tangential direction in the space of the orbitals. For ODD functionals, a third loop is used to find the unitary transformation that minimizes the energy functional among occupied orbitals only. Combined with the maximum overlap method, the algorithm converges in challenging cases where conventional self-consistent field algorithms tend to fail. The benchmark tests presented include two charge-transfer excitations in nitrobenzene and an excitation of CO to degenerate $π$* orbitals where the importance of complex orbitals is illustrated. The application of this method to several metal-to-ligand charge-transfer and metal-centered excited states of an Fe II photosensitizer complex is described, and the results are compared to reported experimental estimates. This method is also used to study the effect of the Perdew−Zunger self-interaction correction on valence and Rydberg excited states of several molecules, both singlet and triplet states, and the performance compared to semilocal and hybrid functionals.","tags":null,"title":"Method for Calculating Excited Electronic States Using Density Functionals and Direct Orbital Optimization with Real Space Grid or Plane-Wave Basis Set","type":"publication"},{"authors":["Gianluca Levi","Mauro Causà","Luciano Cortese","Piero Salatino","Osvalda Senneca"],"categories":null,"content":"","date":1606780800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1606780800,"objectID":"74bdc2d338660e8cf419719b32cbd3e8","permalink":"https://example.com/publication/levi-2020-aecs/","publishdate":"2024-02-02T14:14:57.394721Z","relpermalink":"/publication/levi-2020-aecs/","section":"publication","summary":"Understanding how the structure of carbonaceous materials changes upon oxidation at mild temperature as a function of the graphitic order is of great importance for the development of clean combustion technologies, such as carbon fuel cells. The micro- and nanostructures of a range of carbon materials at room temperature and upon mild oxidation at 300 °C have been analysed by means of mercury porosimetry, Nitrogen adsorption, X-Ray Diffraction, Raman spectroscopy and Electron Paramagnetic Resonance. The samples included carbons with increasing level of graphitic order: three chars derived from two bituminous coals and a lignite, a synthetic carbon and a graphitized coke. The experimental characterization allows to classify the materials according to different structural parameters, including porosity, surface area, degree of graphitization and paramagnetic activation of the carbonaceous surface. A correlation with the rank of the analysed materials is observed. For the graphitized coke, oxidation leads to more crystalline order and enhancement of the paramagnetic signal. A similar increase in the paramagnetic activity is observed for the Lignite char. On the other hand, for the higher rank, bituminous and synthetic chars, mild oxidation leads to a slight expansion of the amorphous carbon and loss of paramagnetic activity. The differences are rationalized in terms of formation of new carbon-oxygen complexes on the graphitized coke and on the Lignite char, and redistribution of already existing complexes for the higher-rank coals. This investigation complements previous X-ray photoelectron spectroscopy measurements.","tags":null,"title":"On how mild oxidation affects the structure of carbons: Comparative analysis by different techniques","type":"publication"},{"authors":["Jan Gerit Brandenburg","Kieron Burke","Emmanuel Fromager","Matteo Gatti","Sara Giarrusso","Nikitas I. Gidopoulos","Paola Gori-Giorgi","Duncan Gowland","Trygve Helgaker","Matthew J. P. Hodgson","Lionel Lacombe","Gianluca Levi","Pierre-François Loos","Neepa T. Maitra","Eduardo Maurina Morais","Nisha Mehta","Filippo Monti","Manasi R. Mulay","Katarzyna Pernal","Lucia Reining","Pina Romaniello","Matthew R. Ryder","Andreas Savin","Dumitru Sirbu","Andrew M. Teale","Alex J. W. Thom","Donald G. Truhlar","Jack Wetherell","Weitao Yang"],"categories":null,"content":"","date":1577836800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1577836800,"objectID":"b72db564e1732bb1b6bcaa7e122e8788","permalink":"https://example.com/publication/brandenburg-2020/","publishdate":"2024-02-02T14:14:57.404571Z","relpermalink":"/publication/brandenburg-2020/","section":"publication","summary":"","tags":null,"title":"New approaches to study excited states in density functional theory: general discussion","type":"publication"},{"authors":["Gianluca Levi","Elisa Biasin","Asmus Ougaard Dohn","Hannes Jónsson"],"categories":null,"content":"","date":1577836800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1577836800,"objectID":"9f5e994fe7cf1f3116f388dc6bfb72b5","permalink":"https://example.com/publication/levi-2020-pccp/","publishdate":"2024-02-02T14:14:57.385191Z","relpermalink":"/publication/levi-2020-pccp/","section":"publication","summary":"Copper(I) bis-phenanthroline complexes represent Earth-abundant alternatives to ruthenium-based sensitizers for solar energy conversion and photocatalysis. Improved understanding of the solvent- mediated excited-state structural dynamics can help optimize their photoconversion efficiency. Through direct dynamics simulations in acetonitrile and excited-state minimum energy path calculations in vacuum, we uncover the mechanism of the photoinduced flattening motion of the prototypical system [Cu(dmphen)2]+ (dmphen = 2,9-dimethyl-1,10-phenanthroline). We find that the ligand distortion is a two-step process in acetonitrile. The fast component (B110 fs) is due to spontaneous pseudo Jahn– Teller instability and is largely solvent independent, while the slow component (B1.2 ps) arises from the mutual interplay between solvent molecules closely approaching the metal center and rotation of the methyl substituents. These results shed new light on the influence of a donor solvent such as acetonitrile and methyl substituents on the flattening dynamics of [Cu(dmphen)2]+.","tags":null,"title":"On the interplay of solvent and conformational effects in simulated excited-state dynamics of a copper phenanthroline photosensitizer","type":"publication"},{"authors":["Gianluca Levi","Aleksei V. Ivanov","Hannes Jonsson"],"categories":null,"content":"","date":1577836800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1577836800,"objectID":"8eed2820e8ad15923c9e41ae4751aacd","permalink":"https://example.com/publication/levi-2020-fd/","publishdate":"2024-02-02T14:14:57.399805Z","relpermalink":"/publication/levi-2020-fd/","section":"publication","summary":"A direct optimization method for obtaining excited electronic states using density functionals is presented. It involves selective convergence on saddle points on the energy surface representing the variation of the energy as a function of the electronic degrees of freedom, thereby avoiding convergence to a minimum and corresponding variational collapse to the ground electronic state. The method is based on an exponential transformation of the molecular orbitals, making it possible to use efficient quasi-Newton optimization approaches. Direct convergence on a target nth-order saddle point is guided by an appropriate preconditioner for the optimization as well as the maximum overlap method. Results of benchmark calculations of 52 excited states of molecules indicate that the method is more robust than a standard self-consistent field (SCF) approach especially when degenerate or quasi-degenerate orbitals are involved. The method can overcome challenges arising from rearrangement of closely spaced orbitals in a charge-transfer excitation of the nitrobenzene molecule, a case where the SCF fails to converge. The formulation of the method is general and can be applied to non-unitary invariant functionals, such as self-interaction corrected functionals.","tags":null,"title":"Variational Calculations of Excited States Via Direct Optimization of Orbitals in DFT","type":"publication"},{"authors":["Gianluca Levi","Aleksei V. Ivanov","Hannes Jónsson"],"categories":null,"content":"","date":1577836800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1577836800,"objectID":"0a4c37cc04b4b4ccf826f7911bb6ad6f","permalink":"https://example.com/publication/levi-2020-jctc/","publishdate":"2024-02-02T14:14:57.389836Z","relpermalink":"/publication/levi-2020-jctc/","section":"publication","summary":"A direct optimization method for obtaining excited electronic states using density functionals is presented. A direct optimization method for obtaining excited electronic states using density functionals is presented. It involves selective convergence on saddle points on the energy surface representing the variation of the energy as a function of the electronic degrees of freedom, thereby avoiding convergence to a minimum and corresponding variational collapse to the ground electronic state. The method is based on an exponential transformation of the molecular orbitals, making it possible to use efficient quasi-Newton optimization approaches. Direct convergence on a target n th-order saddle point is guided by an appropriate preconditioner for the optimization as well as the maximum overlap method. Results of benchmark calculations of 52 excited states of molecules indicate that the method is more robust than a standard self-consistent field (SCF) approach especially when degenerate or quasi-degenerate orbitals are involved. The method can overcome challenges arising from rearrangement of closely spaced orbitals in a charge-transfer excitation of the nitrobenzene molecule, a case where the SCF fails to converge. The formulation of the method is general and can be applied to non-unitary invariant functionals, such as self-interaction corrected functionals.","tags":null,"title":"Variational Density Functional Calculations of Excited States via Direct Optimization","type":"publication"},{"authors":["Mostafa Abedi","Gianluca Levi","Diana B Zederkof","Niels Engholm Henriksen","Mátyás Pápai","Klaus B. Møller"],"categories":null,"content":"","date":1546300800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1546300800,"objectID":"02de12da87670c9d0e83987e4dfcda4b","permalink":"https://example.com/publication/abedi-2019/","publishdate":"2024-02-02T14:14:57.409517Z","relpermalink":"/publication/abedi-2019/","section":"publication","summary":"In this work, we investigate the excited-state solute and solvation structure of [Ru(bpy)3]2+, [Fe(bpy)3]2+, [Fe(bmip)2]2+ and [Cu(phen)2]+ (bpy = 2,2′-bipyridine; bmip = 2,6-bis(3-methyl-imidazole-1-ylidine)-pyridine; phen = 1,10-phenanthroline) transition metal complexes (TMCs) in terms of solute–solvent radial distribution functions (RDFs) and evaluate the performance of some of the most popular partial atomic charge (PAC) methods for obtaining these RDFs by molecular dynamics (MD) simulations. To this end, we compare classical MD of a frozen solute in water and acetonitrile (ACN) with quantum mechanics/molecular mechanics Born–Oppenheimer molecular dynamics (QM/MM BOMD) simulations. The calculated RDFs show that the choice of a suitable PAC method is dependent on the coordination number of the metal, denticity of the ligands, and type of solvent. It is found that this selection is less sensitive for water than ACN. Furthermore, a careful choice of the PAC method should be considered for TMCs that exhibit a free direct coordination site, such as [Cu(phen)2]+. The results of this work show that fast classical MD simulations with ChelpG/RESP or CM5 PACs can produce RDFs close to those obtained by QM/MM MD and thus, provide reliable solvation structures of TMCs to be used, e.g. in the analysis of scattering data.","tags":null,"title":"Excited-State Solvation Structure of Transition Metal Complexes from Molecular Dynamics Simulations and Assessment of Partial Atomic Charge Methods","type":"publication"},{"authors":["Mátyás Pápai","Mostafa Abedi","Gianluca Levi","Elisa Biasin","Martin M Nielsen","Klaus B Møller"],"categories":null,"content":"","date":1546300800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1546300800,"objectID":"5ae9ef61d5bf371804524fe0f61b6f87","permalink":"https://example.com/publication/papai-2019/","publishdate":"2024-02-02T14:14:57.414963Z","relpermalink":"/publication/papai-2019/","section":"publication","summary":"The solvent-mediated excited-state dynamics of the COOH- functionalized Fe-carbene photosensitizer [Fe(bmicp)2]2+ (bmicp = 2,6-bis(3- methyl-imidazole-1-ylidine)-4-carboxy-pyridine) is studied by time-dependent density functional theory, as well as classical and quantum dynamics simulations. We demonstrate the crucial role of the polar acetonitrile solvent in stabilizing the metal-to-ligand charge transfer (MLCT) states of the investigated molecule using the conductor polarizable continuum model. This leads to dynamics that avoid sub-ps back electron transfer to the metal and an exceptionally long-lived 1MLCT state that does not undergo sub-ps 1MLCT → 3MLCT intersystem crossing as it is energetically isolated. We identify two components of the excited-state solvent reorganization process: an initial rotation (∼300 fs) and diffusional dynamics within the local cage surrounding the rotated solvent molecule (∼2 ps). Finally, it is found that the relaxation of the solvent only slightly affects the excited-state population dynamics of [Fe(bmicp)2]2+.","tags":null,"title":"Theoretical Evidence of Solvent-Mediated Excited-State Dynamics in a Functionalized Iron Sensitizer","type":"publication"},{"authors":["Kristoffer Haldrup","Gianluca Levi","Elisa Biasin","Peter Vester","Mads Goldschmidt Laursen","Frederik Beyer","Kasper Skov Kjær","Tim Brandt Van Driel","Tobias Harlang","Asmus O. Dohn","Robert J. Hartsock","Silke Nelson","James M. Glownia","Henrik T. Lemke","Morten Christensen","Kelly J. Gaffney","Niels E. Henriksen","Klaus B. Møller","Martin M. Nielsen"],"categories":null,"content":"","date":1546300800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1546300800,"objectID":"9f7cdd69d5771d4d3eed5489d37f6dda","permalink":"https://example.com/publication/haldrup-2019/","publishdate":"2024-02-02T14:14:57.420255Z","relpermalink":"/publication/haldrup-2019/","section":"publication","summary":"We report x-ray free electron laser experiments addressing ground-state structural dynamics of the diplatinum anion Pt2POP4 following photoexcitation. The structural dynamics are tracked with \u003c100 fs time resolution by x-ray scattering, utilizing the anisotropic component to suppress contributions from the bulk solvent. The x-ray data exhibit a strong oscillatory component with period 0.28 ps and decay time 2.2 ps, and structural analysis of the difference signal directly shows this as arising from ground-state dynamics along the PtPt coordinate. These results are compared with multiscale Born-Oppenheimer molecular dynamics simulations and demonstrate how off-resonance excitation can be used to prepare a vibrationally cold excited-state population complemented by a structure-dependent depletion of the ground-state population which subsequently evolves in time, allowing direct tracking of ground-state structural dynamics.","tags":["doi:10.1103/PhysRevLett.122.063001 url:https://doi"],"title":"Ultrafast X-Ray Scattering Measurements of Coherent Structural Dynamics on the Ground-State Potential Energy Surface of a Diplatinum Molecule","type":"publication"},{"authors":["Elisa Biasin","Tim Brandt van Driel","Gianluca Levi","Mads G Laursen","Asmus O Dohn","Asbjørn Moltke","Peter Vester","Frederik B. K. Hansen","Kasper S Kjaer","Tobias Harlang","Robert Hartsock","Morten Christensen","Kelly J. Gaffney","Niels E. Henriksen","Klaus B. Møller","Kristoffer Haldrup","Martin M Nielsen"],"categories":null,"content":"","date":1514764800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1514764800,"objectID":"05b96af22f22012ad051feb8d8745c95","permalink":"https://example.com/publication/biasin-2018-a/","publishdate":"2024-02-02T14:14:57.425313Z","relpermalink":"/publication/biasin-2018-a/","section":"publication","summary":"Time-resolved X-ray scattering patterns from photoexcited molecules in solution are in many cases anisotropic at the ultrafast time scales accessible at X-ray free-electron lasers (XFELs). This anisotropy arises from the interaction of a linearly polarized UV–Vis pump laser pulse with the sample, which induces anisotropic structural changes that can be captured by femtosecond X-ray pulses. In this work, a method for quantitative analysis of the anisotropic scattering signal arising from an ensemble of molecules is described, and it is demonstrated how its use can enhance the structural sensitivity of the time-resolved X-ray scattering experiment. This method is applied on time-resolved X-ray scattering patterns measured upon photoexcitation of a solvated di-platinum complex at an XFEL, and the key parameters involved are explored. It is shown that a combined analysis of the anisotropic and isotropic difference scattering signals in this experiment allows a more precise determination of the main photoinduced structural change in the solute, i.e. the change in Pt—Pt bond length, and yields more information on the excitation channels than the analysis of the isotropic scattering only. Finally, it is discussed how the anisotropic transient response of the solvent can enable the determination of key experimental parameters such as the instrument response function.","tags":["anisotropic scattering","molecular structure","orientational selection","supporting information","this article has","time-resolved","ultrafast","xfel"],"title":"Anisotropy enhanced X-ray scattering from solvated transition metal complexes research papers","type":"publication"},{"authors":["Gianluca Levi","Matyas Papai","Niels E Henriksen","Asmus O Dohn","Klaus B Møller"],"categories":null,"content":"","date":1514764800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1514764800,"objectID":"8faa2201100adbd50abf74c4f2352cf6","permalink":"https://example.com/publication/levi-2018/","publishdate":"2024-02-02T14:14:57.430762Z","relpermalink":"/publication/levi-2018/","section":"publication","summary":"Recent ultrafast experiments have unveiled the time scales of vibrational cooling and decoherence upon photoexcitation of the diplatinum complex [Pt2(P2O5H2)4]4– in solvents. Here, we contribute to the understanding of the structure and dynamics of the lowest lying singlet excited state of the model photocatalyst by performing potential energy surface calculations and Born–Oppenheimer molecular dynamics simulations in the gas phase and in water. Solvent effects were treated using a multiscale quantum mechanics/molecular mechanics approach. Fast sampling was achieved with a modified version of delta self-consistent field implemented in the grid-based projector-augmented wave density functional theory code. The known structural parameters and the PESs of the first singlet and triplet excited states are correctly reproduced. Besides, the simulations deliver clear evidence that pseudorotation of the ligands in the excited state leads to symmetry lowering of the Pt2P8 core. Coherence decay of Pt–Pt stretching vibrations in solution was found to be governed by vibrational cooling, which is in agreement with previous ultrafast experiments. We also show that the flow of excess Pt–Pt vibrational energy is first directed toward vibrational modes involving the ligands, with the solvent favoring intramolecular vibrational energy redistribution. The results are supported by thorough vibrational analysis in terms of generalized normal modes.","tags":null,"title":"Solution structure and ultrafast vibrational relaxation of the PtPOP complex revealed by ∆SCF-QM/MM Direct Dynamics simulations","type":"publication"},{"authors":["Asmus O. Dohn","Elvar Ö Jónsson","Gianluca Levi","Jens J. Mortensen","Olga Lopez-Acevedo","Kristian S. Thygesen","Karsten W. Jacobsen","Jens Ulstrup","Niels E. Henriksen","Klaus B. Møller","Hannes Jónsson"],"categories":null,"content":"","date":1483228800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1483228800,"objectID":"eb182d4a31d0e08df42b0cb8f71d2e51","permalink":"https://example.com/publication/dohn-2017/","publishdate":"2024-02-02T14:14:57.440939Z","relpermalink":"/publication/dohn-2017/","section":"publication","summary":"A multiscale density functional theory–quantum mechanics/molecular mechanics (DFT-QM/MM) scheme is presented, based on an efficient electrostatic coupling between the electronic density obtained from a grid-based projector augmented wave (GPAW) implementation of density functional theory and a classical potential energy function. The scheme is implemented in a general fashion and can be used with various choices for the descriptions of the QM or MM regions. Tests on H2O clusters, ranging from dimer to decamer show that no systematic energy errors are introduced by the coupling that exceeds the differences in the QM and MM descriptions. Over 1 ns of liquid water, Born–Oppenheimer QM/MM molecular dynamics (MD) are sampled combining 10 parallel simulations, showing consistent liquid water structure over the QM/MM border. The method is applied in extensive parallel MD simulations of an aqueous solution of the diplatinum [Pt2(P2O5H2)4]4– complex (PtPOP), spanning a total time period of roughly half a nanosecond. An average Pt–Pt distance deviating only 0.01 Å from experimental results, and a ground-state Pt–Pt oscillation frequency deviating by \u003c2% from experimental results were obtained. The simulations highlight a remarkable harmonicity of the Pt–Pt oscillation, while also showing clear signs of Pt–H hydrogen bonding and directional coordination of water molecules along the Pt–Pt axis of the complex.","tags":null,"title":"Grid-Based Projector Augmented Wave (GPAW) Implementation of Quantum Mechanics/Molecular Mechanics (QM/MM) Electrostatic Embedding and Application to a Solvated Diplatinum Complex","type":"publication"},{"authors":["Gianluca Levi","Mauro Causà","Paolo Lacovig","Piero Salatino","Osvalda Senneca"],"categories":null,"content":"","date":1483228800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1483228800,"objectID":"3aaecbe51cf144a7f09a85d3fb47e5cc","permalink":"https://example.com/publication/levi-2017/","publishdate":"2024-02-02T14:14:57.435908Z","relpermalink":"/publication/levi-2017/","section":"publication","summary":"The present study investigates the coal char combustion by a combination of thermochemical and X-ray photoemission spectroscopy (XPS) analyses. Thermoanalytical methods (differential thermogravimetry, differential scanning calorimetry, and temperature-programmed desorption) are used to identify the key reactive steps that occur upon oxidation and heating of coal char (chemisorption, structural rearrangement and switchover of surface oxides, and desorption) and their energetics. XPS is used to reveal the chemical nature of the surface oxides that populate the char surface and to monitor their evolution throughout thermochemical processing. XPS spectra show the presence on the carbon surface of three main components. It is shown that the most abundant oxygen functionality in the raw char is epoxy. It decreases with preoxidation at 300 °C and even more at 500 °C, where carboxyl and ether oxygen functionalities prevail. The rearrangement of epoxy during preoxidation goes together with activation of the more stable and less reactive carbon sites. Results are in good agreement with semi-lumped kinetic models of carbon oxidation, which include (1) formation of “metastable” surface oxides, (2) complex switchover, and (3) desorption into CO and CO2.","tags":null,"title":"Mechanism and Thermochemistry of Coal Char Oxidation and Desorption of Surface Oxides","type":"publication"},{"authors":["Gianluca Levi","Osvalda Senneca","Mauro Causà","Piero Salatino","Paolo Lacovig","Silvano Lizzit"],"categories":null,"content":"","date":1438387200,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":1438387200,"objectID":"ae4d3b2177f80cbd89b1f1b25983509d","permalink":"https://example.com/publication/levi-2015/","publishdate":"2024-02-02T14:14:57.446228Z","relpermalink":"/publication/levi-2015/","section":"publication","summary":"Coal chars, like most solid carbons, have a pronounced tendency to chemisorb oxygen at low and moderate temperatures. Characterization by XPS of surface oxides on carbon has been accomplished with the aim of providing a better atomistic insight into: (a) reactions involved in molecular oxygen adsorption on coals and (b) the relations between the nanostructure of solid carbons and the chemistry of oxidation. High-resolution C 1s and O 1s core level and valence band XPS spectra effectively reflected the oxidative functionalization of different types of coals and synthetic carbons upon oxidation in air at moderate temperatures (300 and 500 ??C). More specifically, analysis of C 1s and valence band spectra could be directed to monitor the structural evolution of the carbons in terms of extension of sp2 versus sp3 conjugation, carbon vacancies and oxidized carbon. Comparison of the O 1s spectra, on the other hand, provided a tool to characterize the nature of oxygen bonding on carbon and to determine the relative abundance of carbon-oxygen species. Results underline the important role of epoxy groups in the early stages of oxidation, providing a mechanistic framework for the identification of the stable and metastable intermediates in the heterogeneous oxidation of coal by molecular oxygen.","tags":null,"title":"Probing the chemical nature of surface oxides during coal char oxidation by high-resolution XPS","type":"publication"},{"authors":null,"categories":null,"content":" Funding CNERGY: Ultrafast Charge and Energy Transfer in Sunlight Conversion 2021 - 2024 IRF Project Grant Gianluca Levi Efficient molecular photoswitches identified using simulations of ultrafast charge transfer and solvation dynamics 2023 - 2026 IRF Postdoctoral Fellowship Grant Elli Inkeri Selenius EQuanDo: Energy Transfer in Semiconductor Quantum Dots Studied Using Nonadiabatic Dynamics and Reaction Path Calculations 2021 - 2024 IRF Doctoral student Grant Yorick Leonard A. Schmerwitz Exploring the Reaction Paths of Solvated Iron Photosensitizers: a Multiscale Nudged Elastic Band Strategy 2020 - 2023 IRF Doctoral student Grant Benedikt Orri Birgisson Electron-Nuclear Dynamics in Iron-Sensitized Solar Cells: A Unified Model Description from Light Absorption to Charge Separation 2019 - 2022 IRF Postdoctoral Fellowship Grant Gianluca Levi ","date":-62135596800,"expirydate":-62135596800,"kind":"page","lang":"en","lastmod":-62135596800,"objectID":"768afc3a053405c37420b437a94d4f97","permalink":"https://example.com/funding/","publishdate":"0001-01-01T00:00:00Z","relpermalink":"/funding/","section":"","summary":"Funding CNERGY: Ultrafast Charge and Energy Transfer in Sunlight Conversion 2021 - 2024 IRF Project Grant Gianluca Levi Efficient molecular photoswitches identified using simulations of ultrafast charge transfer and solvation dynamics 2023 - 2026 IRF Postdoctoral Fellowship Grant Elli Inkeri Selenius EQuanDo: Energy Transfer in Semiconductor Quantum Dots Studied Using Nonadiabatic Dynamics and Reaction Path Calculations 2021 - 2024 IRF Doctoral student Grant Yorick Leonard A.","tags":null,"title":"","type":"page"}] \ No newline at end of file diff --git a/public/index.xml b/public/index.xml index 11408f0..926c205 100644 --- a/public/index.xml +++ b/public/index.xml @@ -20,15 +20,14 @@ <h1 style="text-align: center;"> Group Members </h1> <p><img src="../images/gianluca_portrait.png" alt="Gianluca's portrait" -style="width: 240px; height: 260px; float: left; margin-right: 20px;"></p> -<p style="margin-top: 75px;"> +style="width: 180px; height: 195px; float: left; margin-right: 20px;"></p> +<p style="margin-top: 60px;"> <h3 id="gianluca-levi">Gianluca Levi</h3> <p><span style="color: #cb5041; font-weight: bold;">Group leader </span> <br> Science Institute of the University of Iceland <br> VR-III Hjarðarhagi 2, 107 Reykjavík<br> -<a href="https://orcid.org/0000-0002-4542-0653" target="_blank" rel="noopener">ORCID</a>   <a href="https://www.webofscience.com/wos/author/record/GYQ-9226-2022" target="_blank" rel="noopener">Web of Science</a>   <a href="https://scholar.google.com/citations?user=HhElK98AAAAJ&amp;hl=en" target="_blank" rel="noopener">Google Scholar</a>   <a href="../doc/cv_giale.pdf">CV</a> -+354 8326622<br> -<a href="mailto:giale@hi.is">giale@hi.is</a></p> +<a href="https://orcid.org/0000-0002-4542-0653" target="_blank" rel="noopener">ORCID</a>   <a href="https://www.webofscience.com/wos/author/record/GYQ-9226-2022" target="_blank" rel="noopener">Web of Science</a>   <a href="https://scholar.google.com/citations?user=HhElK98AAAAJ&amp;hl=en" target="_blank" rel="noopener">Google Scholar</a>   <a href="../doc/cv_giale.pdf">CV</a> <br> ++354 8326622, <a href="mailto:giale@hi.is">giale@hi.is</a></p> </p> <div style="clear: both;"></div> <h3 id="elli-inkeri-selenius">Elli Inkeri Selenius</h3> @@ -40,8 +39,8 @@ VR-III Hjarðarhagi 2, 107 Reykjavík<br> <div style="clear: both;"></div> <p><img src="../images/yorick_portrait.png" alt="Yorick's portrait" -style="width: 240px; height: 288px; float: left; margin-right: 20px;"></p> -<p style="margin-top: 65px;"> +style="width: 180px; height: 220px; float: left; margin-right: 20px;"></p> +<p style="margin-top: 45px;"> <h3 id="yorick-leonard-a-schmerwitz">Yorick Leonard A. Schmerwitz</h3> <p><span style="color: #cb5041; font-weight: bold;">PhD student </span> (co-supervised, main supervisor: Prof. <a href="https://hj.hi.is/indexE.html" target="_blank" rel="noopener">Hannes Jónsson</a>)<br> Science Institute of the University of Iceland <br> diff --git a/public/people/index.html b/public/people/index.html index 3bbbcee..a75197a 100644 --- a/public/people/index.html +++ b/public/people/index.html @@ -1,6 +1,6 @@ - + @@ -206,7 +206,7 @@ - + @@ -266,8 +266,7 @@ @@ -318,8 +317,7 @@ @@ -714,15 +712,14 @@

Group Members

Gianluca's portrait

-

+style="width: 180px; height: 195px; float: left; margin-right: 20px;">

+

Gianluca Levi

Group leader
Science Institute of the University of Iceland
VR-III Hjarðarhagi 2, 107 Reykjavík
-ORCID   Web of Science   Google Scholar   CV -+354 8326622
-giale@hi.is

+ORCID   Web of Science   Google Scholar   CV
++354 8326622, giale@hi.is

Elli Inkeri Selenius

@@ -734,8 +731,8 @@

Elli Inkeri Selenius

Yorick's portrait

-

+style="width: 180px; height: 220px; float: left; margin-right: 20px;">

+

Yorick Leonard A. Schmerwitz

PhD student (co-supervised, main supervisor: Prof. Hannes Jónsson)
Science Institute of the University of Iceland
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