Proceedings of Online International Conference on Hybrid and Organic Photovoltaics (OnlineHOPV20)
DOI: https://doi.org/10.29363/nanoge.onlinehopv.2020.015
Publication date: 22nd May 2020
Two-dimensional hybrid metal-halide perovskites are quantum-well like structures that exhibit large exciton binding energies (200 – 400 meV) and have garnered considerable attention for many emerging quantum opto-electronic applications. We investigated the peculiar spectroscopic signatures that make the excitons in these materials distinct from conventional 2D semiconductors. The most striking one of them is the spectral finestructure with an energetic spacing of about 35-40 meV that is ubiquitously present at the excitonic transition in their linear absorption spectra[1]. Via a combination of linear and coherent non-linear optical spectroscopies, we show that (a) there are at least four distinct excitonic states that are non-adiabatically coupled via phonon-driven fluctuations[1,2], (b) Each one of them is distinctly dressed by the lattice optical phonons[3], (c) they are subjected to diverse elastic exciton-exciton and exciton-phonon scattering processes[4] and (d) Stable biexcitons are present, yet they differ in the presence of both attractive and repulsive inter-excitonic interactions[5]. Given the direct consequences of phonon interactions in the finestructure characteristics and due to the fundamental polaronic nature of excitations in ionic metal-halide perovskite lattices, we propose that exciton-polarons are primary photo-excitations in these material architectures.
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