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Poster De Conférence Année : 2022

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

Résumé

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.
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.
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].
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].
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.
References: 1. Wesolowski, T. A.; Warshel, A. Frozen density functional approach for ab initio calculations of solvated molecules. J. Chem. Phys. 1993, 97, 8050–8053.
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.
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
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.
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.2205.05523
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Dates et versions

hal-03826007 , version 1 (23-10-2022)

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  • HAL Id : hal-03826007 , version 1

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Matteo de Santis, Valérie Vallet, André Severo Pereira Gomes, Leonardo Belpassi, Loriano Storchi. Environmental Effects with Frozen-Density Embedding in the Real-Time Time-Dependent Dirac-Kohn-Sham framework. Workshop of the GDR quantum gases, Oct 2022, Lille, France. , 2022. ⟨hal-03826007⟩
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