Coherent multidimensional spectroscopy: the role and dynamics of vibrations from a quantum-optical perspective

Coherent multidimensional spectroscopy represents an insightful tool for investigating the interplay of nuclear and electronic dynamics, which plays an important role in a variety of photophysical processes. In this Colloquium, after introducing the relevant concepts, I will focus on the vibrational wave packets resulting from nonlinear interactions with the electric field (sequences of laser pulses). Under physical assumptions underlying widely used models, these wave packets are shown to coincide with squeezed coherent states, whose analytical expressions are derived for systems with N electronic levels and M vibrational modes, along with those of the response functions. Besides representing a practical tool for the simulation of observed multidimensional spectra, these solutions provide a clear connection between the observed spectra and the underlying vibrational dynamics. Finally, connections with atomistic modeling and quantum computing will be discussed.

References:
Journal of Chemical Physics 157, 034107 (2022); ibid. 158, 054110 (2023); ibid. 159, 084111 (2023).

Seminar realized in the framework of the co-funded project:
-Multiphoton Microscopy and Ultrafast Spectroscopy: Imaging meets Quantum (MUSIQ) - Grant Agreement No. 812992