Abstract

A multimodal method for correlating linear and nonlinear optical spectra with a spatial resolution is presented. Using a partially collinear pump-probe geometry and two-frame phase-cycling, ultrafast two-dimensional electronic spectroscopy (2DES) was performed with transverse-spatial and temporal resolutions of 17 μm and 80 fs, respectively. Time-resolved 2DES maps were spatially correlated with linear extinction spectra obtained in the same imaging platform, enabling the examination of state-resolved dynamics of spatially heterogeneous materials. Thin films of aggregated CdSe nanocrystals were studied to demonstrate the combined spectral, temporal, and imaging capabilities of this method.

© 2019 Optical Society of America

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