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Computer simulations studies of the electronic structure of chemical species in their realistic condensed-phase environment

English title Computer simulations studies of the electronic structure of chemical species in their realistic condensed-phase environment
Applicant Wesolowski Tomasz
Number 172532
Funding scheme Project funding (Div. I-III)
Research institution Département de Chimie Physique Université de Genève
Institution of higher education University of Geneva - GE
Main discipline Physical Chemistry
Start/End 01.04.2017 - 30.09.2020
Approved amount 365'000.00
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Keywords (7)

solvatochromism; liminescence; UV/Vis absorption; Frozen-Density Embedding Theory; multi-scale simulations; electronic structure; materials science

Lay Summary (French)

Lead
Les simulations numériques basées sur les lois fondamentales de la physique de différents domaines comme la mécanique, l’électrodynamique, l’hydrodynamique, etc. sont des parties indispensables de la technologie et de la société d'aujourd'hui (prévisions météorologiques, ingénierie civile, industries aéronautiques, etc.). A l’échelle atomique et moléculaire, les lois correspondantes proviennent de la mécanique quantique. Malheureusement, la simulation des propriétés des matériaux, des biomolécules, des nanomatériaux, ne peuvent, à l’échelle atomique, mener à des prédictions aussi précises que dans les domaines, situés à l’échelle macroscopique, cités précédemment. La raison est une complication intrinsèque des lois physiques sous-jacentes. Notre proposition vise le développement d’un formalisme permettant une applicabilité générale.
Lay summary

Un grand nombre de méthodes ont été développées par la communauté de chimie computationnelle durant les dernières décennies.  Ces méthodes ciblent généralement des matériaux ou des propriétés spécifiques. Nous explorons l’idée que a) la division d’un système polyatomique compliqué en plusieurs sous-systèmes dont un seul est décrit par les lois de la mécanique quantique b) décrire les autres sous-systèmes en utilisant les lois physiques et les approximations appropriées c) prendre en compte des interactions entre les sous-systèmes au moyen d’un potentiel d’encapsulation  dépendant de la densité de charges. Cela a été proposé dans notre travail original publié déjà en 1993 par Wesolowski and Warshel, qui a été la première formulation de la théorie de l’encapsulation d’un système quantique en la densité gelée (FDET pour Frozen Density Embedding Theory). De cette formulation a débuté un large champ de recherche poursuivit par nous-mêmes ainsi que par de nombreux autres groupes afin de résoudre des problèmes mathématiques fondamentaux en lien avec FDET, de développer des approximations et des implémentations numériques efficientes, ou formuler les extensions de la formulation originale.

Nous planifions plusieurs applications spécifiques des outils développés à caractère novateur prédisant les propriétés spectroscopiques des molécules dans la phase condensée (molécules biologiques, molécules dans des solvants polaires ainsi que des complexes intermoléculaires). Ces applications sont prévues principalement  pour obtenir les informations détaillées non accessibles par les techniques expérimentales disponibles par nôtres collaborateurs. Ils sont planifies aussi comme une démonstration des utilité des méthodes développées jusqu’à maintenant.  Un objectif secondaire du projet consiste en l’amélioration des approximations faites dans les simulations pour élargir le domaine d’applicabilité des méthodes basées sur FDET.

Direct link to Lay Summary Last update: 17.07.2017

Responsible applicant and co-applicants

Employees

Project partner

Natural persons


Name Institute

Publications

Publication
On the Correlation Potential in Frozen-Density Embedding Theory
Wesolowski Tomasz A. (2020), On the Correlation Potential in Frozen-Density Embedding Theory, in Journal of Chemical Theory and Computation, acs.jctc.0-acs.jctc.0.
Embedding-theory-based simulations using experimental electron densities for the environment
Ricardi Niccolò, Ernst Michelle, Macchi Piero, Wesolowski Tomasz Adam (2020), Embedding-theory-based simulations using experimental electron densities for the environment, in Acta Crystallographica Section A Foundations and Advances, 76(5), 571-579.
OpenMolcas: From Source Code to Insight
Fdez. Galván Ignacio, Vacher Morgane, Alavi Ali, Angeli Celestino, Aquilante Francesco, Autschbach Jochen, Bao Jie J., Bokarev Sergey I., Bogdanov Nikolay A., Carlson Rebecca K., Chibotaru Liviu F., Creutzberg Joel, Dattani Nike, Delcey Mickaël G., Dong Sijia S., Dreuw Andreas, Freitag Leon, Frutos Luis Manuel, Gagliardi Laura, Gendron Frédéric, Giussani Angelo, González Leticia, Grell Gilbert, Guo Meiyuan, et al. (2019), OpenMolcas: From Source Code to Insight, in Journal of Chemical Theory and Computation, 15(11), 5925-5964.
The deconvolution analysis of ATR-FTIR spectra of diacetylene during UV exposure
Ortuso Roberto D., Ricardi Niccolò, Bürgi Thomas, Wesolowski Tomasz A., Sugihara Kaori (2019), The deconvolution analysis of ATR-FTIR spectra of diacetylene during UV exposure, in Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, 219, 23-32.
Origin of the Solvatochromism in Organic Fluorophores with Flexible Side Chains: A Case Study of Flugi-2
Wolff Franziska E., Höfener Sebastian, Elstner Marcus, Wesołowski Tomasz A. (2019), Origin of the Solvatochromism in Organic Fluorophores with Flexible Side Chains: A Case Study of Flugi-2, in The Journal of Physical Chemistry A, 123(21), 4581-4587.
Extension of frozen-density embedding theory for non-variational embedded wavefunctions
Zech Alexander, Dreuw Andreas, Wesolowski Tomasz A. (2019), Extension of frozen-density embedding theory for non-variational embedded wavefunctions, in The Journal of Chemical Physics, 150(12), 121101-121101.
Explicit vs. implicit electronic polarisation of environment of an embedded chromophore in frozen-density embedding theory
Ricardi Niccolò, Zech Alexander, Gimbal-Zofka Yann, Wesolowski Tomasz A. (2018), Explicit vs. implicit electronic polarisation of environment of an embedded chromophore in frozen-density embedding theory, in Physical Chemistry Chemical Physics, 20(41), 26053-26062.
Benchmark of Excitation Energy Shifts from Frozen-Density Embedding Theory: Introduction of a Density-Overlap-Based Applicability Threshold
Zech Alexander, Ricardi Niccolò, Prager Stefan, Dreuw Andreas, Wesolowski Tomasz A. (2018), Benchmark of Excitation Energy Shifts from Frozen-Density Embedding Theory: Introduction of a Density-Overlap-Based Applicability Threshold, in Journal of Chemical Theory and Computation, 14(8), 4028-4040.
Size extensivity of elastic properties of alkane fragments
Radiom Milad, Maroni Plinio, Wesolowski Tomasz A. (2018), Size extensivity of elastic properties of alkane fragments, in Journal of Molecular Modeling, 24(1), 36-36.
Nonadditive kinetic potentials from inverted Kohn-Sham problem
Banafsheh Mojdeh, Adam Wesolowski Tomasz (2018), Nonadditive kinetic potentials from inverted Kohn-Sham problem, in International Journal of Quantum Chemistry, 118(1), e25410-e25410.
Implementation and Application of the Frozen Density Embedding Theory with the Algebraic Diagrammatic Construction Scheme for the Polarization Propagator up to Third Order
Prager Stefan, Zech Alexander, Wesolowski Tomasz A., Dreuw Andreas (2017), Implementation and Application of the Frozen Density Embedding Theory with the Algebraic Diagrammatic Construction Scheme for the Polarization Propagator up to Third Order, in Journal of Chemical Theory and Computation, 13(10), 4711-4725.
Frontiers in Multiscale Modelling of Photoreceptor Proteins
Mroginski Maria-Andrea, Adam Suliman, Amoyal Gil S., Barnoy Avishai, Bondar Ana-Nocoleta, Borin Veniamin, Church Jonathan R., Domratcheva Tatiana, Ensig Bernd, Fanelli Francesca, Ferre Nicolas, Filiba Ofer, Gonzalez Laura P., Gonzalez Ronald, Gonzalez-Espinoza Cristina, Kar Rajiv K., Kemmler Lukas, Kim Seung Soo, Kongsted Jacob, Krylov Anna I., Lahav Yigal, Lazaratos Michalis, Nasser Edin Qays, Navizet Isabelle, Nemukhin Alexander, Olivucci Massimo, Olsen Jogvan M.H., Perez de Alba Ortiz Alberto, Pieri Elisa, Rao Adita G., Rhee Young Min, Ricardi Niccolo, Sen Saumik, Solovyov Ilia, De Vito Luca, Wesolowski Tomasz A., Wiebler Christian, Yang Xuchun, Schapiro Igor, Frontiers in Multiscale Modelling of Photoreceptor Proteins, in Photochemistry and Photobiology.

Collaboration

Group / person Country
Types of collaboration
Prof. Clemence Corminoeuf/EPFL Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
Prof. Daniel Borgis/ Laboratoire PASTEUR CNRS-UMR 8640 France (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
Dr. Igor Schapiro /Hebrew University Jerusalem Israel (Asia)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Exchange of personnel
Dr. Magdalena Kowalska/CERN Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
- Exchange of personnel
Prof. Leeor Kronik/Weizmann Institute of Science Israel (Asia)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
Prof. Martin Gander/University of Geneva Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Exchange of personnel

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
Multiscale simulations of soft matter: New method developments and mathematical foundations, Lausanne, Switzerland, Sept. 30-Oct. 2, 2020 Talk given at a conference Frozen Density Embedding Theory approach to multi-level simulations 30.09.2020 Lausanne (ZOOM conference), Switzerland Wesolowski Tomasz;
International Conference on Computational Materials Science for Nanoscale Modelling, Napoli, Italy, Feb. 11-12, 2020 Talk given at a conference Frozen-Density Embedding Theory approach to multi-level simulations of spectroscopic properties of molecules in condensed phase 11.02.2020 Napoli, Italy Wesolowski Tomasz;
Talk at the Faculty of Physics, Copernicus University Torun Individual talk Quantum Embedding Theory based on Hohenberg-Kohn Theorems 05.12.2019 Torun, Poland Wesolowski Tomasz;
Fall meeting of European Materials Research Society, Warsaw, Poland, Sept 16-19, 2019 Talk given at a conference Quantum embedding theory based on Hohenberg-Kohn Theorems for multi-level simulations 16.09.2019 Warsaw, Poland Wesolowski Tomasz;
CECAM Workshop: Frontiers in Multiscale Modelling of Photoreceptor Proteins 3-5 September 2019, Jerusalem, Israel Talk given at a conference Frozen-Density Embedding Theory based multi-level simulations: the formalism, approximations, and setting up practical simulation protocol 03.09.2019 Jerusalem, Israel Wesolowski Tomasz; Fu Mingxue;
Current Trends in Theoretical Chemistry VIII 1-5 September 2019, Kraków, Poland Talk given at a conference Frozen-Density Embedding Theory based methods for simulation of electronic structure of embedded species: what determines the accuracy? 01.09.2019 Krakow, Poland Wesolowski Tomasz; Fu Mingxue; Gimbal-Zofka Yann;
9th Molecular Quantum Mechanics Conference, Heidelberg, Germany, July 1- 5, 2019 Talk given at a conference Accuracy in Frozen-Density Embedding Theory based simulations 01.07.2019 Heidelberg, Germany Wesolowski Tomasz;
American Chemical Society Spring meeting, Orlando, Fl, March 31 - April 4, 2019 Talk given at a conference Frozen-Density Embedding Theory (FDET) based multi-level simulations of electronic structure: approximations, procedures, and benchmarking 31.03.2019 Orlando, United States of America Wesolowski Tomasz;
Symposium in Honour of Professor Arieh Warshel, Tromso, Norway, Sept. 25, 2018 Talk given at a conference Opening a Pandora's box with Professor Arieh Warshel: Frozen-Density Embedding Theory view on QM/MM methods 25.09.2018 Tromso, Norway Wesolowski Tomasz;
Multi-Scale Quantum Mechanical Analysis of Condensed Phase Systems: Methods and Applications, Telluride Workshop, July 23-27, 2018 Talk given at a conference Induction, dispersion, exchange-repulsion, where they are in Frozen-Density Embedding Theory based simulations? 23.07.2018 Telluride, United States of America Wesolowski Tomasz;
Developments in QM/MM and Embedding Models for Photochemical and Electron Transfer Processes, Telluride Workshop, July 9-13, 2018 Talk given at a conference Induction, dispersion, exchange-repulsion, where they are in Frozen-Density Embedding Theory based simulations? 09.07.2018 Telluride, United States of America Wesolowski Tomasz;
MDMM2018, Polanica Zdroj, Poland, June 24-28, 2018 Talk given at a conference Multi-level simulations based on Frozen-Density Embedding Theory 24.06.2018 Polanica Zdroj, Poland Wesolowski Tomasz;
Departamental talk: KIT, Karlsruhe, April 16, 2018 Individual talk Frozen-Density Embedding Theory: from the general formulation to practical simulations 16.04.2018 Karlsruhe, Germany Wesolowski Tomasz; Chalaye Emilie; Banafsheh Mojdeh; Gimbal-Zofka Yann;
Molecules in Extreme Environments Meeting, Oslo, January 15-17, 2018 Talk given at a conference Recent developments in Frozen-Density Embedding Theory and its applications in multi-scale modelling 15.01.2018 Oslo, Norway Wesolowski Tomasz;
Deppartamental talk, Technical University of Munich, Dec. 4, 2017 Individual talk Embedding theory for electronic structure of molecules in condensed phase 04.12.2017 Munich, Germany Wesolowski Tomasz;
DFT-2017 : Development and Application of Density Functional Theory. A meeting in honor of Prof. emeritus Henry Chermette 10 Nov 2017 Lyon-Villeurbanne (France) Talk given at a conference Unexpected and expected features of the Lembarki-Chermette approximation for the density functional for the kinetic energy 10.11.2017 Lyon, France Wesolowski Tomasz;
Modelling Interactions in Biomolecules'17, Pilsen, Czech Republic, Sept. 3-8, 2017 Talk given at a conference Additional insight into biomolecular systems from simulating UV/Vis absorption spectra using Frozen-Density Embedding Theor 03.09.2017 Pilsen, Czech Republic Gimbal-Zofka Yann; Macchi Piero; Chalaye Emilie; Banafsheh Mojdeh; Fu Mingxue;


Knowledge transfer events



Self-organised

Title Date Place
2019 Spring Meeting of Swiss Association of Computational Chemists 14.02.2019 Geneve, Switzerland

Associated projects

Number Title Start Funding scheme
134791 Computer simulations studies of the electronic structure of chemical species in their realistic condensed-phase environment 01.04.2011 Project funding (Div. I-III)
177033 A dual wavelength X-ray single crystal diffractometer for accurate investigations at extreme conditions 01.08.2018 R'EQUIP
152779 Computer simulations studies of the electronic structure of chemical species in their realistic condensed-phase environment 01.04.2014 Project funding (Div. I-III)

Abstract

The key feature of Frozen-Density Embedding Theory (FDET) is the embedding potential, which is uniquely determined by charge densities in the embedded chemical species and in its environment. Since the charge density is a well-defined quantity in both micro- and macro scales, FDET is, therefore, a formal basis for multi-level simulations. The variational principle origin of this potential assures numerical stability of the results and self-consistency between the energy and embedded wavefunction which makes it particularly suitable for studying the effect of environment on electronic structure of embedded species.The FDET based multi-level simulations methods, the interest in which is systematically growing in the recent years, apply approximations concerning: the embedding potential, the quantum mechanical descriptor for the embedded species, and the method to generate the electron density of the environment. Our past efforts focused on theoretical foundations of FDET, development of approximations for the needed density functionals, development of numerical implementations, and applications. As a result, we developed and tested FDET based methods to model chemical species which are non-covalently bound to the environment. The principal goal of the planned research is to exploit to the full the potential of FDET based methodologies in studies of host-guest complexes, chromophres in biological environments, chromophores in porous materials, optically active impurities in solids, solvated molecules, etc. Several sub-projects aimed at interpretation of experimental data and conducted in collaborative research with our experimental partners are planned. The other objective of this proposal is to extend the range of applicability of the existing FDET computational methods developed so far. This will be achieved through, i) improvements in numerical implementation of the currently developed FDET technology in order to enable to studies of even larger systems and to evaluate efficiently and accurately also other observables besides electronic excitations, ii) development of a robust FDET technology for embedded interacting wavefunction, to be used for cases where the methods using embedded non-interacting reference system are known not to be reliable, iii) improvements of approximations to the density bi-functionals used in approximate methods based on FDET. Further extension of methods going beyond FDET are also planned.
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