Accounting for pulse shaper nonlinearity in action-detected two-dimensional electronic spectroscopy

MUYI ZHANG, STEPHANIE E. SANDERS, JULIAN LÜTTIG, STEFAN MUELLER, ALASTAIR T. GARDINER, TOBIAS BRIXNER AND JENNIFER P. OGILVIE

Pulseshapers arewidely utilized in two-dimensional (2D) spectroscopy togenerate a pump pulse pair with variable time delay and relative carrier–envelope phase. Their use in action-detected 2D spectroscopy has recently garnered interest due to the compatibility with microscopy and potentially higher sensitivity down to the single-molecule level. However, under the conditions necessary for action-detected 2D spectroscopy experiments, pulse shapers are prone to exhibiting nonlinear responses, obscuring the molecularr esponse. Here, we illustrate the potential sources o fnonlinearity in an acousto optic programmable dispersive filter (AOPDF) and demonstrate methods to account for them in data collection and processing, enabling artifact-free action-detected 2D spectroscopy measurements.