Stable biexcitons in two-dimensional metal-halide perovskites with strong dynamic lattice disorder

Abstract

With strongly bound and stable excitons at room temperature, single-layer, two-dimensional organic-inorganic hybrid perovskites are viable semiconductors for light-emitting quantum optoelectronics applications. In such a technological context, it is imperative to comprehensively explore all the factors --- chemical, electronic and structural --- that govern strong multi-exciton correlations. Here, by means of two-dimensional coherent spectroscopy, we examine excitonic many-body effects in pure, single-layer (PEA)${}_2$PbI${}_4$ (PEA = phenylethylammonium). We determine the binding energy of biexcitons --- correlated two-electron, two-hole quasiparticles --- to be $44\pm 5$\,meV at room temperature. The extraordinarily high values are similar to those reported in other strongly excitonic two-dimensional materials such as transition-metal dichalchogenides. Importantly, we show that this binding energy increases by $\sim 25$\% upon cooling to 5\,K. Our work highlights the importance of multi-exciton correlations in this class of technologically promising, solution-processable materials, in spite of the strong effects of lattice fluctuations and dynamic disorder.

arXiv comment37 pages including 4 figures and supplemental information

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• Photophysics of Two-Dimensional Semiconducting Organic-Inorganic Metal-Halide Perovskites
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• Coherent Spin Dynamics of Electrons in Two-Dimensional (PEA)${}_2$PbI${}_4$ Perovskites
• Simulations of Trions and Biexcitons in Layered Hybrid Organic-Inorganic Lead Halide Perovskites
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• Influence of Organic Spacer Cation on Dark Excitons in 2D Perovskites
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• The Optical Signatures of Stochastic Processes in Many-Body Exciton Scattering
• Temporally-decoherent and spatially-coherent vibrations in metal halide perovskite
• Machine Learning Enabled Lineshape Analysis in Optical Two-Dimensional Coherent Spectroscopy
• Many-Exciton Quantum Dynamics in a Ruddlesden-Popper Tin Iodide
• Measurement principles for quantum spectroscopy of molecular materials with entangled photons
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• Stochastic scattering theory for excitation induced dephasing: Comparison to the Anderson-Kubo lineshape
• Broadband Optical Two-Dimensional Coherent Spectroscopy of a Rubidium Atomic Vapor
• Pairing of electro-magnetic bosons under spin-orbit coupling
• Resolving exciton and polariton multi-particle correlations in an optical microcavity in the strong coupling regime
• Lattice vibrations and dynamic disorder in two-dimensional hybrid lead-halide perovskites
• Spectroscopic signatures of biexcitons: A case study in Ruddlesden-Popper lead-halides
• Material gain and eight-band k.p description for selected perovskites
• Controllable fusion of electromagnetic bosons in two-dimensional semiconductors
• Thickness dependent dark exciton emission in (PEA)2PbI4 nanoflake and its brightening by in-plane magnetic field
• Room-temperature polariton condensate in a two-dimensional hybrid perovskite
• Variational and field-theoretical approach to exciton-exciton interactions and biexcitons in semiconductors
• Excitonic-trion population in two-dimensional halide perovskites