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  A Real-Time Time-Dependent Density Functional Tight-Binding Implementation for Semiclassical Excited State Electron–Nuclear Dynamics and Pump–Probe Spectroscopy Simulations

Bonafé, F., Aradi, B., Hourahine, B., Medrano, C. R., Hernández, F. J., Frauenheim, T., et al. (2020). A Real-Time Time-Dependent Density Functional Tight-Binding Implementation for Semiclassical Excited State Electron–Nuclear Dynamics and Pump–Probe Spectroscopy Simulations. Journal of Chemical Theory and Computation, 16(7), 4454-4469. doi:10.1021/acs.jctc.9b01217.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0006-9A90-9 Version Permalink: http://hdl.handle.net/21.11116/0000-0006-B64E-6
Genre: Journal Article

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https://dx.doi.org/10.1021/acs.jctc.9b01217 (Publisher version)
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 Creators:
Bonafé, F.1, 2, 3, Author              
Aradi, B.4, Author
Hourahine, B.5, Author
Medrano, C. R.2, 3, Author
Hernández, F. J.2, 3, 6, Author
Frauenheim, T.4, Author
Sánchez, C. G.7, Author
Affiliations:
1Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
2Universidad Nacional de Córdoba, Facultad de Ciencias Químicas, Departamento de Química Teórica y Computacional, ou_persistent22              
3Instituto de Investigaciones en Fisico-química de Córdoba, INFIQC (CONICET - Universidad Nacional de Córdoba), ou_persistent22              
4Bremen Center for Computational Materials Science, Universität Bremen, ou_persistent22              
5SUPA, Department of Physics, John Anderson Building, The University of Strathclyde, ou_persistent22              
6Department of Physics, Universidad de Santiago de Chile, ou_persistent22              
7Computational Science Research Center (CSRC) Beijing and Computational Science and Applied Research (CSAR) Institute, ou_persistent22              

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 Abstract: 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.

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Language(s): eng - English
 Dates: 2019-12-062020-06-082020-07-14
 Publication Status: Published in print
 Pages: 16
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acs.jctc.9b01217
 Degree: -

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Title: Journal of Chemical Theory and Computation
  Other : J. Chem. Theory Comput.
Source Genre: Journal
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Publ. Info: Washington, D.C. : American Chemical Society
Pages: - Volume / Issue: 16 (7) Sequence Number: - Start / End Page: 4454 - 4469 Identifier: ISSN: 1549-9618
CoNE: https://pure.mpg.de/cone/journals/resource/111088195283832