Stimulated Emission from Stable Multiexciton-Polaron States in Fully Inorganic Perovskite Quantum Wells
Pieter Geiregat a, Isabella Wagner b, Kai Chen c, Shalini Singh d, Justin Hodgkiss b, Zeger Hens a
a Physics and Chemistry of Nanostructures, Department of Chemistry, Ghent University, Ghent, Belgium
b School of Chemical and Physical Sciences, Victoria University of Wellington, Wellington, New Zealand, PO Box 600, Wellington, New Zealand
c Robinson Research Institute, Victoria University of Wellington, Wellington, New Zealand, PO Box 600, Wellington, New Zealand
d Bernal Institute, University of Limerick, V94 T9PX, Limerick, Ireland
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Spring Meeting 2022 (NSM22)
#PhotoPero22. Photophysics of Halide Perovskites and Related Materials - from Bulk to Nano
Online, Spain, 2022 March 7th - 11th
Organizers: Sascha Feldmann, Annamaria Petrozza and Ajay Ram Srimath Kandada
Contributed talk, Pieter Geiregat, presentation 064
DOI: https://doi.org/10.29363/nanoge.nsm.2022.064
Publication date: 7th February 2022

Solution processable semiconducting perovskites hold great promise for demanding applications involving light emission, such as printable lasers or quantum light sources. A case example is that of fully inorganic CsPbBr3 quantum wells (CQWs) which display high quantum yield at room temperature. Less studied than their organic-inorganic counterparts, these CQWs sustain high single exciton binding energies and luminescence quantum yields, yet little is known on the nature of the exciton and multi-excitons states required for advanced applications. Here, we show that charge carriers in fully inorganic 2D perovskites exist as stable exciton - polarons, a complex between a charge neutral exciton and a lattice deformation. Next, we show that these unique species can fuse together to form a hereto unexplored bi-exciton polaron state, i.e. a two-particle complex bound by attractive Coulomb attraction whilst simultaneously being strongly coupled to the lattice. Finally, we show that net stimulated emission occurs through radiative recombination from this unique bi-exciton polaron state to a single free exciton polaron, showing the stability of the newly found species. Consequences of the polaronic character are identified as a low threshold for stimulated emission but with limited optical gain coefficients, both of which we can fully reproduce using a thermodynamic gain model. As such, our results provide a general framework to understand and predict the behavior of not only single, but also multi-exciton polaron states in perovskite materials.

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