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Dual-Hyperspectral Optical Pump-Probe Microscopy with Single-Nanosecond Time Resolution.
Bowen Li1,2, Joy Xu1,2, Conrad A Kocoj1,2
1Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520, United States.
Journal of the American Chemical Society
|January 12, 2024
Summary
We developed a dual-hyperspectral optical pump-probe microscopy (PPM) technique with nanosecond to millisecond time windows. This advanced PPM method enables detailed imaging of slow electronic and thermal processes in semiconductors like perovskites.
Area of Science:
- Materials Science
- Condensed Matter Physics
- Spectroscopy
Background:
- Optical pump-probe microscopy (PPM) is crucial for imaging electronic excitations and charge transport.
- Current PPM methods face limitations in time window (nanoseconds) and spectral resolution, restricting the study of slow processes.
Purpose of the Study:
- To introduce a novel dual-hyperspectral PPM setup with an extended time window (nanoseconds to milliseconds) and single-nanosecond resolution.
- To overcome limitations of existing PPM techniques for studying slow dynamic processes in materials.
Main Methods:
- Developed a dual-hyperspectral PPM system with a wide-field probe (370-1000 nm) and broad pump (330 nm to 16 μm).
- Applied the technique to study two-dimensional metal-halide perovskites (2D-MHPs) using both electronic and vibrational pump excitations.
- Achieved single-nanosecond temporal resolution for imaging transient responses.
Main Results:
- Spatially and temporally resolved images revealed insights into heat dissipation, film uniformity, impurity phases, and interfaces in 2D-MHPs.
- Demonstrated imaging of in-plane strain wave propagation in 2D-MHP single crystals.
- The method provides extensive spectral tunability and improved time resolution.
Conclusions:
- The enhanced dual-hyperspectral PPM technique significantly advances the study of slow dynamic processes in semiconductors.
- Opens new avenues for imaging charge carriers, heat transport, and phase transformations in materials with complex properties.
- Facilitates detailed analysis of materials with spatially varying composition, strain, and interfaces.

