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.
All Science Journal Classification (ASJC) codes
- Atomic and Molecular Physics, and Optics