May 15, 2017
Time-resolved Raman spectroscopy has proven useful for studying the formation of polarons in conjugated polymers, verifying the presence of reactive intermediates in photochemical reactions, investigating nonradiative transitions in the short lifetime of the photoexcited species, and resolving electron−phonon coupling strengths and exciton dissociation in crystalline materials.
We extended the recently published transient vibrational analysis to develop an excited state transient Raman analysis protocol combining ab initio direct molecular dynamics, transient excited state Hessian, and excited state nonresonant Raman activities evaluations. This protocol is capable of capturing the time evolution of transient phenomena and providing an interpretation for transient Raman spectroscopic signals in terms of the evolution of molecular degrees of freedom. This work is published in the Journal of Physical Chemistry A and can be found here.