Artículo
A Real-Time Time-Dependent Density Functional Tight-Binding Implementation for Semiclassical Excited State Electron-Nuclear Dynamics and Pump-Probe Spectroscopy Simulations
Bonafé, Franco Paúl
; Aradi, Bálint; Hourahine, Ben; Medrano, Carlos Raúl
; Hernández, Federico Javier
; Frauenheim, Thomas; Sanchez, Cristian Gabriel
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Fecha de publicación:
07/2020
Editorial:
American Chemical Society
Revista:
Journal of Chemical Theory and Computation
ISSN:
1549-9618
Idioma:
Inglés
Tipo de recurso:
Artículo publicado
Clasificación temática:
Resumen
The increasing need to simulate the dynamics of photoexcited molecular systems and nanosystems in the subpicosecond regime demands new efficient tools able to describe the quantum nature of matter at a low computational cost. By combining the power of the approximate DFTB method with the semiclassical Ehrenfest method for nuclear-electron dynamics, we have achieved a real-time time-dependent DFTB (TD-DFTB) implementation that fits such requirements. In addition to enabling the study of nuclear motion effects in photoinduced charge transfer processes, our code adds novel features to the realm of static and time-resolved computational spectroscopies. In particular, the optical properties of periodic materials such as graphene nanoribbons or the use of corrections such as the "LDA+U"and "pseudo SIC"methods to improve the optical properties in some systems can now be handled at the TD-DFTB level. Moreover, the simulation of fully atomistic time-resolved transient absorption spectra and impulsive vibrational spectra can now be achieved within reasonable computing time, owing to the good performance of the implementation and a parallel simulation protocol. Its application to the study of UV/visible light-induced vibrational coherences in molecules is demonstrated and opens a new door into the mechanisms of nonequilibrium ultrafast phenomena in countless materials with relevant applications.
Palabras clave:
TD-DFTB
,
electron ion dynamics
,
simulation
,
pump probe spectroscopy
Archivos asociados
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Colecciones
Articulos(ICB)
Articulos de INSTITUTO INTERDISCIPLINARIO DE CIENCIAS BASICAS
Articulos de INSTITUTO INTERDISCIPLINARIO DE CIENCIAS BASICAS
Articulos(INFIQC)
Articulos de INST.DE INVESTIGACIONES EN FISICO- QUIMICA DE CORDOBA
Articulos de INST.DE INVESTIGACIONES EN FISICO- QUIMICA DE CORDOBA
Citación
Bonafé, Franco Paúl; Aradi, Bálint; Hourahine, Ben; Medrano, Carlos Raúl; Hernández, Federico Javier; et al.; A Real-Time Time-Dependent Density Functional Tight-Binding Implementation for Semiclassical Excited State Electron-Nuclear Dynamics and Pump-Probe Spectroscopy Simulations; American Chemical Society; Journal of Chemical Theory and Computation; 16; 7; 7-2020; 4454-4469
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