Multidimensional four-wave mixing signals offer tremendous insight into correlated electron dynamics. Such excited-state processes show how different electrons are coupled, yielding a rich picture of electronic mechanisms in molecules. Stimulated emission allows for an excited state electronic wavepacket to return down to the ground state. Multidimensional spectra can be challenging to obtain with time-dependent density functional theory (TDDFT), however, we show that it is possible to obtain the stimulated emission spectra using real-time (RT)-TDDFT via a two-step simulation protocol. To demonstrate the robustness of this method, we calculate the 2D stimulated emission spectra of nitrogen K-edge (core) excitations in glycine. From this we show how the emission profile is correlated to the core excited-state dynamics.

Calculating simulated emission by real time-time dependent density functional theory

ACS Spring 2022

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