"Simulating electronic spectroscopy and interfacial processes in condensed-phase systems"
Spectroscopic and electrochemical experiments provide important insights into the fundamental molecular processes of excited-state energy transfer and interfacial reactivity. Theoretical methods can offer additional understanding by connecting the nuclear and electronic structure and dynamics to macroscopic experimental observables. I will present my work developing accurate and efficient quantum dynamics and machine learning methods to simulate two-dimensional electronic spectroscopy (2DES) at the atomistic level. First, I will describe an efficient strategy for simulating 2DES spectra using a machine-learning accelerated approach and show how this can be used to reproduce and explain the experimental 2DES spectra of Nile Blue in ethanol. Then I will introduce a set of Ehrenfest-based approaches that account for the coherence initial conditions in the response functions used to calculate 2DES spectra.