Publication date: 21st July 2025
The functionalities of photoactive materials ranging from optoelectronics, plasmonics, catalysis and phase-switching applications require not only control over the photoexcited charges but also heat generation, transport and dissipation. Controlling nanoscale thermal transport is fundamental to virtually all such applications, as they either inherently generate heat as a byproduct or deliberately harness it for operation. While pump–probe spectroscopy signals are typically attributed to electronic energy carriers (i.e., electrons, holes, excitons), there is increasing recognition that laser induced heating can also lead to transient spectral signals in semiconductor films. On one hand there is a need to better understand the contributions of heating to pump–probe measurements for accurate assignments, and at the same time this presents opportunities to investigate microscopic thermal transport and dissipation. Recent advances in thermoreflectance have enabled critical temporal and spatial thermophysical characterization to probe the mechanistic impact of nanoscale structuring on heat propagation. In this presentation I will describe how pump–probe optical measurements and modeling of thermal transport provide access to nanosecond dynamical information with local, sub-micron specificity. I will highlight examples including metallic nanocrystal superlattices,[1],[2] semiconductor nanocrystal films,[3] and insulator-to-metal phase transition thin films. We will touch on questions including: How do heterogeneous environments and interfaces impact microscopic energy transport? How can we access information about energy carriers that traditionally do not have clear spectroscopic signals? How can we control the directionality of energy carrier flow?
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