TY - DATA T1 - Black-Box, Real-Time Simulations of Transient Absorption Spectroscopy PY - 2016/04/28 AU - Triet S. Nguyen AU - Joong Hoon Koh AU - Susan Lefelhocz AU - John Parkhill UR - https://acs.figshare.com/articles/media/Black_Box_Real_Time_Simulations_of_Transient_Absorption_Spectroscopy/3205171 DO - 10.1021/acs.jpclett.6b00421.ls01 L4 - https://ndownloader.figshare.com/files/5030281 KW - ultrafast spectroscopic experiments KW - adiabatic TDDFT KW - Transient Absorption Spectroscopy KW - absorption KW - method KW - OSCF 2 KW - structure code KW - dissipative extension KW - TA spectra N2 - 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. ER -