Commercial hot carrier devices have not yet been realized, in part due to poor understanding of how operational device conditions impact hot carrier dynamics.  Single monolayer transition metal dichalcogenides (2D TMDs) are promising active materials for hot carrier devices due to their broad and large visible light absorption, optimal thin geometry, and slow hot carrier cooling.  To push hot carrier devices towards being a disruptive technology, one must understand the tuning parameters available in the devices and how to predict behaviors of the 2D TMDs.  In this talk, I will describe efforts in combining theory with experiment to characterize and describe hot carrier dynamics in a monolayer MoS<sub>2</sub>-based electrochemical cell.  Results from in operando spectroscopy, including steady-state photocurrent spectroscopy and transient absorption spectroscopy, will be presented.  We observe extraction of hot carriers occurs within 50 fs and high photocurrent yields in our device that exceed photocurrent yields observed in bulk MoS<sub>2</sub>.  In addition, the experiments are interpreted within a theoretical framework that allows for: 1. the origin of the experimental observations to be described and 2. A streamlined modelling approach taken to describe many-body effects that are observed in the experiments.

Observing hot carrier dynamics in TMD-based electrochemical cells through the lenses of nonlinear spectroscopy & theory

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