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, Jennifer P. Ogilvie
Source abstract
Pulse shapers are widely utilized in two-dimensional (2D) spectroscopy to generate 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 molecular response. Here, we illustrate the potential sources of nonlinearity 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.
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