Title :

Environmental Effects with Frozen-Density Embedding in the Real-Time Time-Dependent Dirac-Kohn-Sham framework

Author(s) :

De Santis, Matteo [Orateur]
Physico-Chimie Moléculaire Théorique [PCMT]
Vallet, Valérie [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Severo Pereira Gomes, Andre [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Belpassi, Leonardo [Auteur]
Istituto di Scienze e Tecnologie Chimiche “Giulio Natta” [SCITEC]
Storchi, Loriano [Auteur]
Istituto di Scienze e Tecnologie Chimiche “Giulio Natta” [SCITEC]

Conference title :

REHE – 2020/2022 13th International Conference on Relativistic Effects in Heavy-Element Chemistry and Physics

City :

Assisi

Country :

Italie

Start date of the conference :

2022-09-26

Publication date :

2022-09-26

HAL domain(s) :

Chimie/Chimie théorique et/ou physique
Physique [physics]/Physique [physics]/Chimie-Physique [physics.chem-ph]

English abstract : [en]

Frozen Density Embedding (FDE)^[1,2] represents a versatile embedding scheme which allows to model complex molecular systems by partitioning the total system into sub-units: the environmental effects onto a given ...
Show more >Frozen Density Embedding (FDE)^[1,2] represents a versatile embedding scheme which allows to model complex molecular systems by partitioning the total system into sub-units: the environmental effects onto a given subsystem is described by accounting quantum mechanically for the surrounding subsystems through their electron density.<br>The accurate modeling of properties of matter when heavy elements are involved requires the inclusion of relativistic corrections. The Dirac-Kohn-Sham (DKS) method allows one to treat electron correlation and relativistic effects on the same footing.<br>The response of electrons in atoms and molecules to an applied external electro-magnetic field can be efficiently treated employing Time-Dependent Density Functional Theory (TDDFT) in the real-time domain (RT-TDDFT)^[3].<br>We extend the full 4-component relativistic RT-TDDKS^[4] method, as implemented in the BERTHA code, to include environmental and confinement effects with the FDE scheme (RT-TDDKS-in-DFT FDE)^[5].<br>Moreover, we demonstrate that the implementation of rather complex numerical algorithms can be enormously facilitated by BERTHA’s python API (PyBERTHA) which, besides all the well-known Python advantages, eases the interoperability with other FDE implementations available through the PyADF framework.<br><b>References:</b>1. Wesolowski, T. A.; Warshel, A. Frozen density functional approach for ab initio calculations of solvated molecules. J. Chem. Phys. 1993, 97, 8050–8053. <br>2. Höfener, S.; Gomes, A. S. P.; Visscher, L. Molecular properties via a subsystem density functional theory formulation: a common framework for electronic embedding. J. Chem Phys, 2012, 136(4), 044104.<br>3. Lopata, K.; Govind, N. Modeling Fast Electron Dynamics with Real-Time Time-Dependent Density Functional Theory: Application to Small Molecules and Chromophores. J. Chem. Theory Comput. 2011, 7, 1344–1355<br>4. De Santis, M.; Storchi, L.; Belpassi, L.; Quiney, H. M.; Tarantelli, F. PyBERTHART: A Relativistic Real-Time Four-Component TDDFT Implementation Using Prototyping Techniques Based on Python. J. Chem. Theory Comput. 2020, 16, 2410–2429. <br>5. De Santis, M.; Sorbelli, D.; Vallet, V.; Gomes, A. S. P.; Storchi, L.; Belpassi, L. Frozen-Density Embedding for including environmental effects in the Dirac-Kohn-Sham theory: an implementation based on density fitting and prototyping techniques. https://doi.org/10.48550/arXiv.2205.05523Show less >

Language :

Anglais

Peer reviewed article :

Oui

Audience :

Internationale

Popular science :

Non

ANR Project :

Physiques et Chimie de l'Environnement Atmosphérique
ULNE
Calcul de la diffusion inélastique résonante de rayons X pour toute la classification périodique

Collections :

• Laboratoire de Physique des Lasers, Atomes et Molécules (PhLAM) - UMR 8523

Source :

Harvested from HAL