Accurate Evaluation of Real-Time Density Functional Theory Providing Access to Challenging Electron Dynamics

Journal of Chemical Theory and Computation
Ingo Schelter, Stephan Kümmel

Abstract

We demonstrate that electronic excitations and their transition densities can be obtained from real-time density functional theory calculations with great accuracy by relating the data from numerical propagation to the analytical form of the electronic response after a boost excitation. The latter is derived in this article. This approach facilitates quantitatively obtaining oscillator strengths, identifying excitations that carry very small oscillator strengths, and assessing electronic couplings from transition densities based on comparatively short propagation times. These features are of interest in particular for studying light-harvesting systems. For demonstration purposes, we study the Q band excitations of bacteriochlorophyll a (BChl a) and calculate coupling strengths between two BChl a's to check the validity of the dipole-dipole and pure Coulomb coupling mechanisms. For further illustration, we investigate the paradigm test system Na4 and the coupling between two Na2 dimers.

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Citations

Oct 22, 2018·The Journal of Chemical Physics·Simon P Neville, Michael S Schuurman
May 17, 2019·The Journal of Chemical Physics·Simon P Neville, Michael S Schuurman
Mar 24, 2021·The Journal of Chemical Physics·Luke BhanKálmán Varga
May 28, 2021·Journal of Chemical Theory and Computation·Alberto Baiardi
Nov 9, 2018·Journal of Chemical Theory and Computation·Rajarshi Sinha-RoyHans-Christian Weissker
May 30, 2020·Journal of Chemical Theory and Computation·Min Chen, Kenneth Lopata
May 16, 2019·Journal of Chemical Theory and Computation·Joaquim Jornet-Somoza, Irina Lebedeva
Sep 9, 2021·The Journal of Physical Chemistry. a·Mohammed I SorourSpiridoula Matsika
Jan 14, 2022·Journal of Chemical Theory and Computation·Mengqi YangKenneth Lopata

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