Fully Atomistic Real-Time Simulations of Transient Absorption Spectroscopy

BONAFÉ, FRANCO P.; HERNÁNDEZ, FEDERICO J.; ARADI, BÁLINT; FRAUENHEIM, THOMAS; SÁNCHEZ, CRISTIÁN G.

Journal of Physical Chemistry Letters

American Chemical Society

Año: 2018 vol. 9 p. 4355 - 4359

We have implemented an electron-nuclear real-time propagation scheme for the calculation of transient absorption spectra. When this technique is applied to the study of ultrafast dynamics of Soret-excited zinc(II) tetraphenylporphyrin in the subpicosecond time scale, quantum beats in the transient absorption caused by impulsively excited molecular vibrations are observed. The launching mechanism of such vibrations can be regarded as a displacive excitation of the zinc-pyrrole and pyrrole C-C bonds.