Nonlinear-response properties in a simplified time-dependent density functional theory (sTD-DFT) framework: Evaluation of the first hyperpolarizability

The Journal of Chemical Physics
Marc de Wergifosse, Stefan Grimme

Abstract

Recent developments in nonlinear imaging microscopy show the need to implement new theoretical tools, which are able to characterize nonlinear optical properties in an efficient way. For second-harmonic imaging microscopy (SHIM), quantum chemistry could play an important role to design new exogenous dyes with enhanced first hyperpolarizabilities or to characterize the response origin in large endogenous biological systems. Such methods should be able to screen a large number of compounds while reproducing their trends and to treat large systems in reasonable computation times. To fulfill these requirements, we present a new simplified time-dependent density functional theory (sTD-DFT) implementation to evaluate the first hyperpolarizability where the Coulomb and exchange integrals are approximated by short-range damped Coulomb interactions of transition density monopoles. For an ultra-fast computation of the first hyperpolarizability, a tight-binding version (sTD-DFT-xTB) is also proposed. In our implementation, a sTD-DFT calculation is more than 600 time faster with respect to a regular TD-DFT treatment, while the xTB version speeds up the entire calculation further by at least two orders of magnitude. We challenge our impleme...Continue Reading

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Citations

Jan 24, 2020·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Barbara PatriziMario Siciliani de Cumis
Sep 3, 2020·The Journal of Chemical Physics·Marc de WergifosseStefan Grimme
Apr 20, 2021·Physical Chemistry Chemical Physics : PCCP·Alberto GuandaliniCarlo Andrea Rozzi
May 1, 2021·The Journal of Physical Chemistry. a·Marc de Wergifosse, Stefan Grimme
Mar 10, 2020·The Journal of Physical Chemistry. B·Jakob SeibertMarc de Wergifosse
Nov 18, 2020·Journal of Chemical Theory and Computation·Marc de Wergifosse, Stefan Grimme
Nov 20, 2018·The Journal of Physical Chemistry. a·T Q TeodoroL Visscher
Oct 1, 2021·The Journal of Physical Chemistry Letters·Pierre BeaujeanMarc de Wergifosse

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