Perturbative Theoretical Model of Electronic Transient Circular Dichroism Spectroscopy of Molecular Aggregates
A chiral analog of transient absorption spectroscopy, transient circular dichroism (TCD) spectroscopy is an emerging time-resolved method. Both spectroscopic methods can probe the electronic transitions of a sample, and TCD is additionally sensitive to the dynamic aspects of chirality, such as those induced by molecular excitons. Here, we develop a theoretical description of TCD for electronic multi-level models in which the pump pulse is linearly polarized and probe pulse is alternately left- and right-circularly polarized. We derive effective response functions analogous to those often used to describe other four-wave mixing methods and then simulate and analyze TCD spectra for three representative multi-level electronic model systems. We elaborate on the presence and detection of the spectral signatures of electronic coherences.
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Arpin, Paul C. and Turner, Daniel B.. (2022). "Perturbative Theoretical Model of Electronic Transient Circular Dichroism Spectroscopy of Molecular Aggregates". The Journal of Chemical Physics, 157(15), 154101. https://doi.org/10.1063/5.0119626