Many-Exciton Quantum Dynamics in a Ruddlesden-Popper Tin Iodide

Abstract

We present a study on the many-body exciton interactions in a prototype Ruddlesden-Popper metal halide (RPMH), namely \ce{(PEA)2SnI4} (PEA = phenylethylammine), using coherent two-dimensional electronic spectroscopy. The optical dephasing times of the third-order polarization observed in these systems are determined by exciton many-body interactions and lattice fluctuations. We investigate the excitation-induced dephasing (EID) and observe a significant reduction of the contribution to the dephasing time with increasing excitation density as compared to its lead counterpart \ce{(PEA)2PbI4}, which we have previously reported [A.~R.~Srimath~Kandada~\textit{et~al.}, J.\ Chem.\ Phys.\ \textbf{153}, 164706 (2020)]. Surprisingly, we find that the EID interaction parameter is four orders of magnitude higher in \ce{(PEA)2SnI4} than that in \ce{(PEA)2PbI4}. This increase in the EID rate may be due to exciton localization arising from a more strongly statically disordered lattice in the tin derivative. This is supported by the observation of multiple closely spaced exciton states and the broadening of the linewidth with increasing population time (spectral diffusion), which suggests a static disordered structure relative to the highly dynamic lead-halide. Additionally, we find that the exciton nonlinear coherent lineshape shows evidence of a biexcitonic state with low binding energy ($<10$\,meV) not observed in the lead system. We model the lineshapes based on a stochastic scattering theory that accounts for the interaction with a non-stationary population of dark background excitations. Our study provides evidence of differences in the exciton quantum dynamics between tin- and lead-based RPMHs and links them to the exciton-exciton interaction strength and the static disorder aspect of the crystalline structure.

arXiv commentSubmitted for publication

References in corpus (18)

• Intrinsic Exciton Linewidth in Monolayer Transition Metal Dichalcogenides
• Phonon coherences reveal the polaronic character of excitons in two-dimensional lead-halide perovskites
• Two-Dimensional hybrid perovskites sustaining strong polariton interactions at room temperature
• Perspective: Exciton polarons in two-dimensional hybrid metal-halide perovskites
• Exciton-polaron spectral structures in two dimensional hybrid lead-halide perovskites
• Stable biexcitons in two-dimensional metal-halide perovskites with strong dynamic lattice disorder
• All-optical retrieval of the global phase for two-dimensional Fourier-transform spectroscopy
• Polarization dependence of semiconductor exciton and biexciton contributions to phase-resolved optical two-dimensional Fourier-transform spectra
• Photophysics of two-dimensional perovskites -- learning from metal halide substitution
• Observation of two thresholds leading to polariton condensation in 2D hybrid perovskites
• Photophysics of Two-Dimensional Semiconducting Organic-Inorganic Metal-Halide Perovskites
• Enhanced screening and spectral diversity in many-body elastic scattering of excitons in two-dimensional hybrid metal-halide perovskites
• Emergence of Rashba-/Dresselhaus Effects in Ruddlesden-Popper Halide Perovskites with Octahedral Rotations
• Stochastic scattering theory for excitation induced dephasing: Time-dependent nonlinear coherent exciton lineshapes
• Homogeneous optical linewidths in hybrid Ruddlesden-Popper metal halides can only be measured using nonlinear spectroscopy
• Stochastic scattering theory for excitation induced dephasing: Comparison to the Anderson-Kubo lineshape
• Coherent Contributions to Population Dynamics in a Semiconductor Microcavity
• Stochastic exciton-scattering theory of optical lineshapes: Renormalized many-body contributions

Cited by in corpus (4)

• Slow Dephasing of Coherent Optical Phonons in Two-dimensional Lead Organic Chalcogenides
• Resolving exciton and polariton multi-particle correlations in an optical microcavity in the strong coupling regime
• Unveiling multi-quantum excitonic correlations in push-pull polymer semiconductors
• Spectroscopic signatures of biexcitons: A case study in Ruddlesden-Popper lead-halides