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Light-matter interaction from first principles: new developments in nonadiabatic dynamics with applications in energy (production, saving, storage) and medical research

Gesuchsteller/in Tavernelli Ivano
Nummer 146396
Förderungsinstrument Projektförderung (Abt. I-III)
Forschungseinrichtung IBM Research GmbH
Hochschule EPF Lausanne - EPFL
Hauptdisziplin Physikalische Chemie
Beginn/Ende 01.04.2013 - 30.11.2016
Bewilligter Betrag 208'672.00
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Alle Disziplinen (4)

Disziplin
Physikalische Chemie
Materialwissenschaften
Andere Gebiete der Physik
Anorganische Chemie

Keywords (11)

First-principles excited state dynamics; Density functional theory; Photo-induced water splitting; Spin-orbit couplings and intersystem crossing; OLED technology; Photo-induced drug delivery; Nuclear quantum (de-)coherence and dephasing; Time dependent density functional theory; Energy production; Cancer therapy; Nonadiabatic dynamics

Lay Summary (Französisch)

Lead
Interaction entre la lumière et la matière à partir de principes premiers: nouveaux développements en dynamique non-adiabatique avec applications à l'énergie (production, économie et stockage) et à la recherche médicale.
Lay summary

L'objectif principal de ce projet est d'améliorer et de dériver des nouveaux moyens théoriques, basés sur les principes premiers de la mécanique quantique, pour l'étude de l'interaction entre la lumière (notamment les radiations solaires) et des dispositifs moléculaires ou à l'état solide pouvant être utilisés pour la production et le stockage d'énergie . Nous avons récemment montré que des calculs de structure électronique pour l'obtention de propriétés de l'état fondamental et d'états excités, basés sur la théorie de la fonctionnelle de la densité (DFT) et la théorie de la fonctionnelle de la densité dépendante du temps (TDDFT), peuvent être combinés à des méthodes de dynamique moléculaire (MD) non-adiabatique afin de décrire divers phénomènes photophysiques et photochimiques en solution ou à l'état solide. Dans la première partie de ce projet nous visons à développer d'avantage notre méthode de MD avec des trajectoires avec sauts de surface (TSH), basée sur la TDDFT, qui atteint un bon équilibre entre la précision et l'efficacité numérique. Tous les logiciels développés seront mis à disposition de la communauté scientifique gratuitement, sur le site www.cpmd.org.

En plus du développement théorique décrit précédemment, le projet comporte aussi un partie d'application de la théorie à deux problèmes majeurs liés à la conversion d'énergie solaire et à l'économie d'énergie. En premier lieu nous allons nous intéresser à la conception de nouveaux dispositifs pour le craquage de l'eau, et en particulier au « design » de catalyseurs pour la production d'hydrogène à partir de l'énergie solaire. Nous allons aussi nous intéresser au développement de technologies d'éclairage plus efficaces basées sur les diodes électroluminescentes organiques (OLEDs), notamment ceux basés sur les complexes d'iridium, dont nous visons à optimiser le spectre d'absorption et émission (« spectral tuning »).

Direktlink auf Lay Summary Letzte Aktualisierung: 08.04.2013

Verantw. Gesuchsteller/in und weitere Gesuchstellende

Mitarbeitende

Publikationen

Publikation
Decoherence, control and attosecond probing of XUV-induced charge migration in biomolecules. A theoretical outlook
(2016), Decoherence, control and attosecond probing of XUV-induced charge migration in biomolecules. A theoretical outlook, in faraday Discussions, 194, 41.
Conditional Born–Oppenheimer Dynamics: Quantum Dynamics Simulations for the Model Porphine
(2015), Conditional Born–Oppenheimer Dynamics: Quantum Dynamics Simulations for the Model Porphine, in J. Phys, Chem. Lett., 6, 1529.
Local Control Theory in Trajectory Surface Hopping Dynamics Applied to the Excited‐State Proton Transfer of 4‐Hydroxyacridine
(2015), Local Control Theory in Trajectory Surface Hopping Dynamics Applied to the Excited‐State Proton Transfer of 4‐Hydroxyacridine, in ChemPhysChem, 16, 2127.
Nonadiabatic dynamics with intersystem crossing: A time-dependent density functional theory implementation
(2015), Nonadiabatic dynamics with intersystem crossing: A time-dependent density functional theory implementation, in The Journal of Chemical Physics, 143, 224105.
Nonadiabatic molecular dynamics simulations: Synergies between theory and experiments
(2015), Nonadiabatic molecular dynamics simulations: Synergies between theory and experiments, in Accounts of Chemical Research, 48, 792.
Probing wavepacket dynamics using ultrafast x-ray spectroscopy
(2015), Probing wavepacket dynamics using ultrafast x-ray spectroscopy, in Journal of Physics B, 48, 214001.
Derivation of spin-orbit couplings in collinear linear response TDDFT: A rigorous folmulation
(2014), Derivation of spin-orbit couplings in collinear linear response TDDFT: A rigorous folmulation, in The journal of Chemical Physics, 140, 144103.
Nonadiabatic molecular dynamics based on trajectories
(2013), Nonadiabatic molecular dynamics based on trajectories, in Entropy, 62-85.

Zusammenarbeit

Gruppe / Person Land
Formen der Zusammenarbeit
Prof. Majed Chergui, EPFL Schweiz (Europa)
- vertiefter/weiterführender Austausch von Ansätzen, Methoden oder Resultaten
- Publikation
Group of Dr. Etienne Baranoff at University of Birmingham Grossbritannien und Nordirland (Europa)
- vertiefter/weiterführender Austausch von Ansätzen, Methoden oder Resultaten
Prof. Fernando Martin, Universitad Autonoma de Madrid Spanien (Europa)
- vertiefter/weiterführender Austausch von Ansätzen, Methoden oder Resultaten
- Publikation
Alessandro Curioni, IBM, Zuerich Schweiz (Europa)
- Industrie/Wirtschaft/weitere anwendungs-orientierte Zusammenarbeit
Prof. Giovanni Ciccotti, Dep. of Physics University of Rome "La Sapienza", Rome Italien (Europa)
- vertiefter/weiterführender Austausch von Ansätzen, Methoden oder Resultaten

Wissenschaftliche Veranstaltungen

Aktiver Beitrag

Titel Art des Beitrags Titel des Artikels oder Beitrages Datum Ort Beteiligte Personen
Seminar at the Department de Quimica Fisica and Institut de Quimica Teorica i Computational. Vortrag im Rahmen einer Tagung TDDFT-based mixed quantum-classical dynamics 17.11.2016 Barcelona, Spanien Tavernelli Ivano;
7th International school and workshop on TDDFT Vortrag im Rahmen einer Tagung TDDFT-based nonadiabatic molecular dynamic with relativistic e ects 12.09.2016 Benasque, Spanien Tavernelli Ivano;
CECAM Workshop on ultrafast phenomena Vortrag im Rahmen einer Tagung TDDFT-based nonadiabatic molecular dynamic for ultrafast phenomena 11.04.2016 Lausanne, Schweiz Tavernelli Ivano;
XLIC Conference, Queen's University Vortrag im Rahmen einer Tagung TDDFT-based local control theory: controlling molecular reactions 10.04.2016 Belfast, Irland Tavernelli Ivano;
APS March meeting Vortrag im Rahmen einer Tagung Nonadiabatic dynamics with spin-orbit couplings 10.03.2016 Baltimore, Vereinigte Staaten von Amerika Tavernelli Ivano;
Thomas Young Center Colloquia Vortrag im Rahmen einer Tagung Nonadidbatic quantum dynamics with CPMD 03.03.2016 London, Grossbritannien und Nordirland Tavernelli Ivano;
Seminar at the Condensed Matter & Statistical Physics Section, ICTP Vortrag im Rahmen einer Tagung TDDFT-based mixed quantum-classical dynamics 02.12.2015 Trieste, Italien Tavernelli Ivano;
Swiss Chemical Society, Fall meeting 2015 Vortrag im Rahmen einer Tagung Molecular Dynamics with inter-system crossing and nonadiabatic effects 04.09.2015 EPFL Lausanne, Schweiz Miraglia Franco de Carvalho Felipe; Tavernelli Ivano;
Summer School of the Max-Planck-EPFL Center for Molecular Nanoscience and Technology Vortrag im Rahmen einer Tagung Trajectory-based nonadiabatic molecular dynamics: A TDDFT approach 27.07.2015 Schloss Ringberg, Deutschland Tavernelli Ivano;
Psi-k 2015 Conference (Invited talk). Vortrag im Rahmen einer Tagung TDDFT-based nonadiabatic dynamics with relativistic e ects 15.06.2015 San Sebastian, Spanien Tavernelli Ivano;
CECAM workshop on \Molecular Quantum Dynamics Methods: Benchmarks and State of the Art". Vortrag im Rahmen einer Tagung Nonadiabatic dynamics with trajectories 15.06.2015 Lausanne, Schweiz Tavernelli Ivano;
C4 Seminar Vortrag im Rahmen einer Tagung Nonadiabatic dynamics of complex molecular systems using time-dependent density functional theory 06.11.2014 Zurich, Schweiz Tavernelli Ivano;
Workshop at the European Theoretical Spectroscopy Facility (ETSF) Vortrag im Rahmen einer Tagung TDDFT-based nonadiabatic molecular dynamics with relativistic e ects 23.09.2014 Zaragoza, Spanien Tavernelli Ivano;
Science@FELs 2014 conference. PSI Poster Inter-system crossing and internal conversion with TDDFT 15.09.2014 Villigen, Schweiz Miraglia Franco de Carvalho Felipe; Tavernelli Ivano;
50th Symposium on Theoretical Chemistry Vortrag im Rahmen einer Tagung TDDFT-based nonadiabatic molecular dynamics with relativistic e ects 14.09.2014 Vienna, Oesterreich Tavernelli Ivano;
Swiss Chemical Society, Fall meeting 2014 Poster Inter-system crossing with TDDFT: Jablonski diagrams from theory 11.09.2014 ETH Zurich, Schweiz Miraglia Franco de Carvalho Felipe; Tavernelli Ivano;
Max-Planck Institute workshop on excited state dynamics Vortrag im Rahmen einer Tagung Nonadiabatic dynamics with trajectories 16.07.2014 Halle, Deutschland Tavernelli Ivano;
TSRC workshop on Excited States. Vortrag im Rahmen einer Tagung TDDFT-based nonadiabatic dynamics with relativistic e ects 13.07.2014 Telluride (CO), Vereinigte Staaten von Amerika Tavernelli Ivano;
Conference on New Frontiers in Multiscale Modelling of Advanced Materials Vortrag im Rahmen einer Tagung Nonadiabatic dynamics and material design 17.06.2014 Trento, Italien Tavernelli Ivano;
CECAM workshop on \Recent progress in adiabatic and non-adiabatic methods in quantum dynamics Vortrag im Rahmen einer Tagung Electron-phonon coupling from time-dependent density functional theory 12.05.2014 Lausanne, Schweiz Tavernelli Ivano;
COST Action MP 1006 workshop Vortrag im Rahmen einer Tagung Nonadiabatic molecular dynamics with classical and quantum trajectories 05.05.2014 Bad Hamburg, Deutschland Tavernelli Ivano;
APS March meeting Vortrag im Rahmen einer Tagung TDDFT-based local control theory: controlling molecular reactions 09.03.2014 Baltimore, Vereinigte Staaten von Amerika Tavernelli Ivano;
6th Time-Dependent Density-Functional Theory workshop and school Prospective and Applications. Vortrag im Rahmen einer Tagung Nonadiabatic dynamics and local control theory 04.01.2014 Benasque, Spanien Tavernelli Ivano;
Time-Dependent Density-Functional Theory: Prospects and Applications, 6th International Workshop and School Poster Spin-orbit coupling with TDDFT 04.01.2014 Benasque , Spanien Tavernelli Ivano; Miraglia Franco de Carvalho Felipe;
Seminar at the Physics Department of the University of Milano Vortrag im Rahmen einer Tagung TDDFT-based nonadiabatic dynamics of complex molecular systems 18.12.2013 Milan, Italien Tavernelli Ivano;
COST Action XLIC. WG2 meeting Vortrag im Rahmen einer Tagung TDDFT-based nonadiabatic dynamics of complex molecular systems 27.04.2013 Fruska Gora, Serbien Tavernelli Ivano;


Veranstaltungen zum Wissenstransfer

Aktiver Beitrag

Titel Art des Beitrags Titel des Artikels oder Beitrages Datum Ort Beteiligte Personen
CECAM workshop on \Molecular Quantum Dynamics Methods: Benchmarks and State of the Art" Vortrag 12.06.2015 Lausanne, Schweiz


Abstract

The principal aim of this project is to improve on and to derive new theoretical first-principles techniques for the investigation of the interaction of light (and in particular the solar radiation) with molecular and solid state devices that can be used for energy production and conversion, or that can replace old, energy inefficient apparatus. Recently, we showed that density functional theory (DFT) and time-dependent DFT (TDDFT) based electronic structure calculations for ground and excited state properties combined with suitable nonadiabatic molecular dynamics (MD) schemes offer an adequate description of many types of photochemical and photophysical processes in both solution and the solid phase. Therefore, in the first part of this project we plan to further develop our recently proposed TDDFT-based trajectory surface (TSH) molecular dynamics (MD) scheme [1], which offers an advantageous balance of accuracy and numerical efficiency. Among others, the main developments include: (i) a theory for the calculation of spin-orbit couplings in the framework od DFT and TDDFT, (ii) the implementation of more accurate DFT functionals and TDDFT kernels, and (iii) the design of a model for the coupling of the electronic and quantum nuclear degrees of freedom with the environment that goes beyond the classical QM/MM scheme and that therefore allows the study of phenomena like quantum dephasing and entanglement. Furthermore, in order to improve the description of the nuclear quantum effects within this formalism, we propose a new theoretical development based on quantum hydrodynamics (or quantum Bohmian dynamics), which introduces quantum (de-)coherence between the ‘quantum’ trajectories used to propagate the nuclear wavefunction. Starting from our recent development in reference [2], we plan to extend our TDDFT-based nonadiabatic Bohmian dynamics MD scheme to treat realistic systems of the size and complexity that are relevant for the applications addressed in this proposal. All this theoretical and software development will be made available to the scientific community, free of charge, from the address: www.cpmd.org [3].In parallel to the theoretical development, we will also address two main problems related to solar energy conversion and energy-saving, namely the design of improved light-induced water splitting devices and development of more efficient illumination technologies based on organic light-emitting-diodes (OLED). Instead of the direct conversion of solar energy into electric power (by means of a solar cell device), it was proposed to store this energy in chemical form, for instance, with the production of molecular hydrogen (H2). The simplest way to achieve such an energy conversion is by splitting water using solar radiation. To run this process efficiently, robust water oxidation catalysts are required to produce oxygen efficiently, that is, with high rates and using only a small (or better no) over-potential. The design of better catalysts is therefore key to the development of this technology and the use of adequate and predictive theoretical methods (like the ones developed in this proposal) is of enormous importance. Concerning energy-saving, our aim is to improve and design new kinds of OLEDs (mainly based on iridium dopants, but not exclusively) with desired absorption and emission properties and protection against photodegradation. By means of a theoretical investigation it is possible to optimally tune the absorption spectrum of a compound by selective mutation of the ligands attached to the central metal (spectral tuning). In conjunction with nonadiabatic MD it will be possible to shed lights on the excited state dynamics identifying for instance, intersystem crossings (via spin-orbit coupling), and also to locate potential energy minima on the excited PESs from which the OLED is emitting. Finally, we believe that the advanced theoretical tools we have developed so far will allow us to address, with new insights, another major challenge facing our society in the domain of public health: cancer therapy. The purpose of this study is the design of a new class of anti-cancer drugs based upon the combination of nanoparticles with light-induced drug delivery. Nanoparticle accumulate in tumor tissue thanks to the defective angiogenesis of cancer tissues. Combining this efficient drug delivery vector with a cytotoxic drug that can be released upon irradiation with tunable light (in the UV of X-ray range) it is possible to obtain a new powerful nano-technological device that can selectively kill tumors. [1] E. Tapavicza, I. Tavernelli, and U. Rothlisberger, “Trajectory surface hopping within linear response time-dependent density-functional theory”, Phys. Rev. Lett. , 98, 023001 (2007).[2] I. Tavernelli, “Ab initio-driven trajectory-based quantum dynamics in phase space”, submitted to Phys. Rev. A, June 2012.[3] CPMD, http://www.cpmd.org. Copyright IBM Corp. 1990-2008, ?Copyright MPI für Festkörperforschung Stuttgart 1997-2001.
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