Abstract: Two-dimensional (2-D) metal–halide perovskites containing first-row transition metals and long-chain organic cations have been explored for thermal energy storage and, recently, for solid-state barocaloric cooling. While manipulating the thermal transport properties of these materials is crucial to realizing their full potential in thermal energy applications, only a few studies have measured the thermal conductivity of 2-D perovskites. Most importantly, much remains to be understood about the chemical and structural factors that influence thermal transport at a molecular level. Here, we report systematic investigations into the thermal conductivity of 2-D perovskites, with a focus on understanding how chemical tuning of the organic–organic interface influences thermal transport. Specifically, variable temperature frequency-domain thermoreflectance measurements were performed on a library of 2-D Mn–Cl perovskites whose organic bilayers feature an array of chain flexibilities, interlayer interactions, and hydrogen-bond networks. The measurements were carried out across their order–disorder phase transitions to evaluate the effects of structural disorder and interface chemistry on thermal conductivity. Furthermore, nanomechanical measurements across this temperature range provide additional insight into the role of acoustic phonons in thermal transport.

Understanding thermal conductivity in two-dimensional metal–halide perovskites

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