Excitons and Phonons in 2D perovskites
Paulina Plochocka a b, Michał Baranowski b
a Laboratoire National des Champs Magnétiques Intenses, CNRS (FR)
b Department of Experimental Physics, Faculty of Fundamental Problems of Technology, Wroclaw University of Science and Technology, Wroclaw, Poland
Proceedings of Applied Light-Matter Interactions in Perovskite Semiconductors 2021 (ALMIPS2021)
Online, Spain, 2021 October 5th - 7th
Organizers: Rafael Sánchez Sánchez and Miguel Anaya
Invited Speaker, Michał Baranowski, presentation 006
DOI: https://doi.org/10.29363/nanoge.almips.2021.006
Publication date: 23rd September 2021

High environmental stability and surprisingly high efficiency of solar cells based on 2D perovskites have renewed interest in these materials. These natural quantum wells consist of planes of metal-halide octahedra, separated by organic spacers.  Remarkably the organic spacers play crucial role in optoelectronic properties of these compounds. The characteristic for ionic crystal coupling of excitonic species to lattice vibration became particularly important in case of soft perovskite lattice. The nontrivial mutual dependencies between lattice dynamics, organic spacers and electronic excitation manifest in a complex absorption and emission spectrum which detailed origin is subject of ongoing controversy. First, I will discuss electronic properties of 2D perovskites with different thicknesses of the octahedral layers and two types of organic spacer.  I will demonstrate that the energy spacing of excitonic features depends on organic spacer but very weakly depends on octahedral layer thickness. This indicates the vibrionic progression scenario which is confirmed by high magnetic fields studies up to 67T. Furthermore, I will show that in 2D perovskites, the distortion imposed by the organic spacers governs the effective mass of the carriers.  As a result, and unlike in any other semiconductor, the effective mass in 2D perovskites can be easily tailored.  Finally,   I will discuss the exciton fine structure, which result from the exchange interaction between the electron and hole spins leading to a splitting of the bright and dark states.  This splitting can have catastrophic consequences for light emitters which rely on exciton recombination, since the lowest excitonic state is typically dark. I will demonstrate magnetic field induced brightening  of the dark exciton. I will show, that we observe non-Boltzmann distribution of the bright-dark exciton populations, which we attribute to the phonon bottle-neck, which results from the weak exciton-acoustic phonon coupling in soft 2D perovskites. Hot photoluminescence is responsible for the strong emission observed in these materials, despite the significant bright-dark exciton splitting.

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