Stochastic scattering theory for excitation induced dephasing: Time-dependent nonlinear coherent exciton lineshapes

Abstract

We develop a stochastic theory that treats time-dependent exciton-exciton s-wave scattering and that accounts for dynamic Coulomb screening, which we describe within a mean-field limit. With this theory, we model excitation-induced dephasing effects on time-resolved two-dimensional coherent optical lineshapes and we identify a number of features that can be attributed to the many-body dynamics occurring in the background of the exciton, including dynamic line narrowing, mixing of real and imaginary spectral components, and multi-quantum states. We test the model by means of multidimensional coherent spectroscopy on a two-dimensional metal-halide semiconductor that hosts tightly bound excitons and biexcitons that feature strong polaronic character. We find that the exciton nonlinear coherent lineshape reflects many-body correlations that give rise to excitation-induced dephasing. Furthermore, we observe that the exciton lineshape evolves with population time over time windows in which the population itself is static, in a manner that reveals the evolution of the multi-exciton many-body couplings. Specifically, the dephasing dynamics slow down with time, at a rate that is governed by the strength of exciton many-body interactions and on the dynamic Coulomb screening potential. The real part of the coherent optical lineshape displays strong dispersive character at zero time, which transforms to an absorptive lineshape on the dissipation timescale of excitation-induced dephasing effects, while the imaginary part displays converse behavior. Our microscopic theoretical approach is sufficiently flexible to allow for a wide exploration of how system-bath dynamics contribute to linear and non-linear time-resolved spectral behavior.

arXiv commentAccepted in The Journal of Chemical Physics, special issue on Excitons: Energetics and Spatio-temporal Dynamics

References in corpus (16)

• Intrinsic Exciton Linewidth in Monolayer Transition Metal Dichalcogenides
• Phonon coherences reveal the polaronic character of excitons in two-dimensional lead-halide perovskites
• Spin-Orbital Separation in the quasi 1D Mott-insulator Sr2CuO3
• Optical spectroscopy of two-dimensional layered $(C_6{H}_5{C}_2{H}_4-N{H}_3{)}_2-Pb{I}_4$ perovskite
• 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
• Many-body two-quantum coherences in semiconductor nanostructures
• Exciton-exciton interaction in transition metal dichalcogenide monolayers and van der Waals heterostructures
• Exciton-Scattering-Induced Dephasing in Two-Dimensional Semiconductors
• Coherent Excitonic Coupling in an Asymmetric Double InGaAs Quantum Well Arises from Many-Body Effects
• Electron-phonon couplings inherent in polarons drive exciton dynamics in two-dimensional metal-halide perovskites
• Optical conductivity of one-dimensional Mott insulators
• Encapsulation Narrows Excitonic Homogeneous Linewidth of Exfoliated MoSe${}_2$ Monolayer
• Enhanced screening and spectral diversity in many-body elastic scattering of excitons in two-dimensional hybrid metal-halide perovskites
• Stochastic scattering theory for excitation induced dephasing: Comparison to the Anderson-Kubo lineshape

Cited by in corpus (12)

• Exciton-exciton interaction in transition metal dichalcogenide monolayers and van der Waals heterostructures
• Homogeneous optical linewidths in hybrid Ruddlesden-Popper metal halides can only be measured using nonlinear spectroscopy
• The Optical Signatures of Stochastic Processes in Many-Body Exciton Scattering
• Measurement principles for quantum spectroscopy of molecular materials with entangled photons
• Many-Exciton Quantum Dynamics in a Ruddlesden-Popper Tin Iodide
• Stochastic scattering theory for excitation induced dephasing: Comparison to the Anderson-Kubo lineshape
• Resolving exciton and polariton multi-particle correlations in an optical microcavity in the strong coupling regime
• Stochastic exciton-scattering theory of optical lineshapes: Renormalized many-body contributions
• Spectroscopic signatures of biexcitons: A case study in Ruddlesden-Popper lead-halides
• Unveiling multi-quantum excitonic correlations in push-pull polymer semiconductors
• Exciton-photocarrier interference in mixed lead-halide-perovskite nanocrystals
• Excitons: Energetics and spatio-temporal dynamics