DOI: https://doi.org/10.29363/nanoge.almips.2021.001
Publication date: 23rd September 2021
Temperature dependent optical linewidths are widely employed in the context of metal halide perovskites and their derivatives to estimate electron-phonon coupling parameters. However, due to comparable contributions from homogeneous and inhomogeneous mechanisms to the spectral broadening, linear spectroscopies like photoluminescence are incapable of isolating the pure dephasing rate and thus are not representative of the system-bath interactions. In these circumstances, nonlinear coherent optical spectroscopy offers insights into the nature of many-body interactions that are entirely inaccessible to temperature-dependent linear spectroscopies. When applied to Ruddlesden-Popper metal halides, these techniques have indeed enabled us to quantify the elastic scattering effects on the exciton dephasing rates. Here, we will discuss the mechanistic nature of exciton-phonon[1], exciton-exciton[2] and phonon-phonon[3] interactions in prototypical Ruddlesden Popper metal halides based on such experimental observations. We will discuss our perspective on how the coherent lineshapes of Ruddlesden-Popper metal halides can be effectively rationalized within an exciton polaron framework. We will also discuss the critical role of the metal cation in the observed coherent exciton dynamics.
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