Stochastic time-dependent DFT with optimally tuned range-separated hybrids: Application to excitonic effects in large phosphorene sheets

Vojtěch Vlček; Roi Baer; Daniel Neuhauser

doi:10.1063/1.5093707

Stochastic time-dependent DFT with optimally tuned range-separated hybrids: Application to excitonic effects in large phosphorene sheets

Vojtěch Vlček, Roi Baer, Daniel Neuhauser

Institute of Chemistry

Research output: Contribution to journal › Article › peer-review

5 Scopus citations

Abstract

We develop a stochastic approach to time-dependent density functional theory with optimally tuned range-separated hybrids containing nonlocal exchange, for calculating optical spectra. The attractive electron-hole interaction, which leads to the formation of excitons, is included through a time-dependent linear-response technique with a nonlocal exchange interaction which is computed very efficiently through a stochastic scheme. The method is inexpensive and scales quadratically with the number of electrons, at almost the same (low) cost of time dependent Kohn-Sham with local functionals. Our results are in excellent agreement with experimental data, and the efficiency of the approach is demonstrated on large finite phosphorene sheets containing up to 1958 valence electrons.

Original language	American English
Article number	184118
Journal	Journal of Chemical Physics
Volume	150
Issue number	18
DOIs	https://doi.org/10.1063/1.5093707
State	Published - 14 May 2019

Bibliographical note

Funding Information:
D.N. acknowledges support from NSF Grant No. CHE-1763176. R.B. acknowledges the U.S.-Israel Binational Fund (Grant No. BSF2015687). The authors would like to acknowledge helpful discussions with Eran Rabani. The calculations were performed as part of the XSEDE57 computational Project No. TG-CHE180051.

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© 2019 Author(s).

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10.1063/1.5093707

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title = "Stochastic time-dependent DFT with optimally tuned range-separated hybrids: Application to excitonic effects in large phosphorene sheets",

abstract = "We develop a stochastic approach to time-dependent density functional theory with optimally tuned range-separated hybrids containing nonlocal exchange, for calculating optical spectra. The attractive electron-hole interaction, which leads to the formation of excitons, is included through a time-dependent linear-response technique with a nonlocal exchange interaction which is computed very efficiently through a stochastic scheme. The method is inexpensive and scales quadratically with the number of electrons, at almost the same (low) cost of time dependent Kohn-Sham with local functionals. Our results are in excellent agreement with experimental data, and the efficiency of the approach is demonstrated on large finite phosphorene sheets containing up to 1958 valence electrons.",

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AU - Neuhauser, Daniel

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Stochastic time-dependent DFT with optimally tuned range-separated hybrids: Application to excitonic effects in large phosphorene sheets

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