Black-Box, Real-Time Simulations of Transient Absorption
Spectroscopy
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Abstract
We introduce an atomistic, all-electron,
black-box electronic structure
code to simulate transient absorption (TA) spectra and apply it to
simulate pyrazole and a GFP-chromophore derivative. The method is
an application of OSCF2, our dissipative extension of time-dependent
density functional theory. We compare our simulated spectra directly
with recent ultrafast spectroscopic experiments. We identify features
in the TA spectra to Pauli-blocking, which may be missed without a
first-principles model. An important ingredient in this method is
the stationary-TDDFT correction scheme recently put forward by Fischer,
Govind, and Cramer that allows us to overcome a limitation of adiabatic
TDDFT. We demonstrate that OSCF2 is able to reproduce the energies
of bleaches and induced absorptions as well as the decay of the transient
spectrum with only the molecular structure as input