Excited state absorption is an important nonlinear optical process. Studying this process with quantum chemical methods is fairly complex, as methods beyond linear response TD-DFT are needed. With some approximations though, linear response can be used to calculate the excited state absorption intensities. How crude are these approximations? In this collaboration with Prof. Denis Jacquemin and Prof. Boris Le Guennic, we systematically address the shortcomings of the linear response approximation, determine its range of applicability, and propose simple corrections.
Širůček, J.; Le Guennic, B.; Cupellini, L. & Jacquemin, D.
Shortcomings of Linear-Response TD-DFT for ESA Oscillator Strength Calculations
J. Chem. Theory Comput. (2026)
Read the full paper here: https://pubs.acs.org/doi/10.1021/acs.jctc.5c01770
