I will present a rapid-scanning approach to fluorescence-detected two-dimensional electronic spectroscopy that combines acousto-optic phase-modulation with digital lock-in detection. The approach shifts the signal detection window to suppress 1/f laser noise and enables interferometric tracking of the time delays to allow for correction of spectral phase distortions and accurate phasing of the data. This use of digital lock-in detection enables acquisition of linear and nonlinear signals of interest in a single measurement, with dramatically reduced acquisition times enabled by rapid scanning. We demonstrate the method on a laser dye, extracting both linear fluorescence excitation spectra as well as rephasing, non-rephasing and absorptive fluorescence-detected two-dimensional spectra.

Phase modulated rapid scanning fluorescence detected two dimensional electronic spectroscopy

ACS Fall 2021

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