Publication date: 15th May 2025
Ultrafast microscopies provide unique insight into spatially varying material properties, carrier dynamics, and heat transfer of nanoscale materials. These properties can vary dramatically when nanomaterials are deposited into thin films. Recently, we demonstrated the influence of interfacial reflections present in thin films on photothermal heterodyne imaging (PHI), which uses an infrared pump and visible probe to track chemical bonding. Using time-resolved data, the origin of signal and three-dimensional dispersion information could be extracted. However, these results are not exclusive to PHI, and the same features are also relevant for transient absorption techniques, particularly regarding interfacial reflectance and resonant cavity engineering. This offers new potential to enhance sensitivity and extract additional time-dependent information with other ultrafast microscopy techniques.
Here, we use ultrafast PHI and circularly polarized transient absorption microscopy to track heat transfer and spin evolution in a variety of inorganic materials. A novel integrated multiphysics model provides insight into the mechanism of thermal evolution and signal generation, which can extract additional information about vertical heat transfer in these nanomaterials and their distribution. Our results provide a computational and theoretical framework for the informed optimization of transient absorption microscopy, demonstrating that through interface engineering, cavity formation, and sample engineering we can significantly enhance the signal of these techniques. This provides a new avenue for ultrafast investigation of inorganic nanoparticles, nanocrystals, and thin films with high spatial and spectral resolution as well as the extraction of important thermal and spin figures of merit.
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