Environmental effects with Frozen Density ...
Type de document :
Compte-rendu et recension critique d'ouvrage
DOI :
Titre :
Environmental effects with Frozen Density Embedding in Real-Time Time-Dependent Density Functional Theory using localized basis functions
Auteur(s) :
De Santis, Matteo [Auteur correspondant]
Università degli Studi di Perugia = University of Perugia [UNIPG]
Istituto di Scienze e Tecnologie Chimiche “Giulio Natta” [SCITEC]
Belpassi, Leonardo [Auteur]
Istituto di Scienze e Tecnologie Chimiche “Giulio Natta” [SCITEC]
Jacob, Christoph R. [Auteur]
Severo Pereira Gomes, Andre [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Tarantelli, Francesco [Auteur]
Università degli Studi di Perugia = University of Perugia [UNIPG]
Visscher, Lucas [Auteur]
Storchi, Loriano [Auteur]
Università degli studi "G. d'Annunzio" Chieti-Pescara [Chieti-Pescara] [Ud'A]
Istituto di Scienze e Tecnologie Chimiche “Giulio Natta” [SCITEC]
Università degli Studi di Perugia = University of Perugia [UNIPG]
Istituto di Scienze e Tecnologie Chimiche “Giulio Natta” [SCITEC]
Belpassi, Leonardo [Auteur]
Istituto di Scienze e Tecnologie Chimiche “Giulio Natta” [SCITEC]
Jacob, Christoph R. [Auteur]
Severo Pereira Gomes, Andre [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Tarantelli, Francesco [Auteur]
Università degli Studi di Perugia = University of Perugia [UNIPG]
Visscher, Lucas [Auteur]
Storchi, Loriano [Auteur]
Università degli studi "G. d'Annunzio" Chieti-Pescara [Chieti-Pescara] [Ud'A]
Istituto di Scienze e Tecnologie Chimiche “Giulio Natta” [SCITEC]
Titre de la revue :
Journal of Chemical Theory and Computation
Pagination :
5695-5711
Éditeur :
American Chemical Society
Date de publication :
2020-09-08
ISSN :
1549-9618
Discipline(s) HAL :
Chimie/Chimie théorique et/ou physique
Résumé en anglais : [en]
Frozen Density Embedding (FDE) represents a versatile embedding scheme to describe the environmental effect on the electron dynamics in molecular systems. The extension of the general theory of FDE to the real-time ...
Lire la suite >Frozen Density Embedding (FDE) represents a versatile embedding scheme to describe the environmental effect on the electron dynamics in molecular systems. The extension of the general theory of FDE to the real-time time-dependent Kohn-Sham method has previously been presented and implemented in plane-waves and periodic boundary conditions (Pavanello et al. J. Chem. Phys. 142, 154116, 2015). In the current paper, we extend our recent formulation of real-time time-dependent Kohn-Sham method based on localized basis set functions and developed within the Psi4NumPy framework (De Santis et al. J. Chem. Theory Comput. 2020, 16, 2410) to the FDE scheme. The latter has been implemented in its "uncoupled" flavor (in which the time evolution is only carried out for the active subsystem, while the environment subsystems remain at their ground state), using and adapting the FDE implementation already available in the PyEmbed module of the scripting framework PyADF. The implementation was facilitated by the fact that both Psi4NumPy and PyADF, being native Python API, provided an ideal framework of development using the Python advantages in terms of code readability and reusability. We demonstrate that the inclusion of the FDE potential does not introduce any numerical instability in time propagation of the density matrix of the active subsystem and in the limit of weak external field, the numerical results for low-lying transition energies are consistent with those obtained using the reference FDE calculations based on the linear response TDDFT. The method is found to give stable numerical results also in the presence of strong external field inducing non-linear effects.Lire moins >
Lire la suite >Frozen Density Embedding (FDE) represents a versatile embedding scheme to describe the environmental effect on the electron dynamics in molecular systems. The extension of the general theory of FDE to the real-time time-dependent Kohn-Sham method has previously been presented and implemented in plane-waves and periodic boundary conditions (Pavanello et al. J. Chem. Phys. 142, 154116, 2015). In the current paper, we extend our recent formulation of real-time time-dependent Kohn-Sham method based on localized basis set functions and developed within the Psi4NumPy framework (De Santis et al. J. Chem. Theory Comput. 2020, 16, 2410) to the FDE scheme. The latter has been implemented in its "uncoupled" flavor (in which the time evolution is only carried out for the active subsystem, while the environment subsystems remain at their ground state), using and adapting the FDE implementation already available in the PyEmbed module of the scripting framework PyADF. The implementation was facilitated by the fact that both Psi4NumPy and PyADF, being native Python API, provided an ideal framework of development using the Python advantages in terms of code readability and reusability. We demonstrate that the inclusion of the FDE potential does not introduce any numerical instability in time propagation of the density matrix of the active subsystem and in the limit of weak external field, the numerical results for low-lying transition energies are consistent with those obtained using the reference FDE calculations based on the linear response TDDFT. The method is found to give stable numerical results also in the presence of strong external field inducing non-linear effects.Lire moins >
Langue :
Anglais
Vulgarisation :
Non
Projet ANR :
Source :
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