A real-time time-dependent density functional tight-binding implementation for semiclassical excited state electron-nuclear dynamics and pump-probe spectroscopy simulations
Bonafé, Franco P. and Aradi, Bálint and Hourahine, Ben and Medrano, Carlos R. and Hernández, Federico J. and Frauenheim, Thomas and Sánchez, Cristián G. (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). pp. 4454-4469. ISSN 1549-9618 (https://doi.org/10.1021/acs.jctc.9b01217)
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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.
ORCID iDs
Bonafé, Franco P., Aradi, Bálint, Hourahine, Ben ORCID: https://orcid.org/0000-0002-7667-7101, Medrano, Carlos R., Hernández, Federico J., Frauenheim, Thomas and Sánchez, Cristián G.;-
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Item type: Article ID code: 72639 Dates: DateEvent14 July 2020Published8 June 2020Published Online6 December 2019AcceptedNotes: Manuscript includes supplementary information. Subjects: Science > Physics > Solid state physics. Nanoscience Department: Faculty of Science > Physics
Strategic Research Themes > Measurement Science and Enabling TechnologiesDepositing user: Pure Administrator Date deposited: 09 Jun 2020 13:48 Last modified: 27 Nov 2024 03:45 URI: https://strathprints.strath.ac.uk/id/eprint/72639