Exciton-Scattering-Induced Dephasing in Two-Dimensional Semiconductors.

Phys Rev Lett

Institut für Theoretische Physik, Nichtlineare Optik und Quantenelektronik, Technische Universität Berlin, 10623 Berlin, Germany.

Published: June 2020

Enhanced Coulomb interactions in monolayer transition metal dichalcogenides cause tightly bound electron-hole pairs (excitons) that dominate their linear and nonlinear optical response. The latter includes bleaching, energy renormalizations, and higher-order Coulomb correlation effects like biexcitons and excitation-induced dephasing. While the first three are extensively studied, no theoretical footing for excitation-induced dephasing in exciton-dominated semiconductors is available so far. In this Letter, we present microscopic calculations based on excitonic Heisenberg equations of motion and identify the coupling of optically pumped excitons to exciton-exciton scattering continua as the leading mechanism responsible for an optical-power-dependent linewidth broadening (excitation-induced dephasing) and sideband formation. Performing time-, momentum-, and energy-resolved simulations, we quantitatively evaluate the exciton-induced dephasing for the most common monolayer transition metal dichalcogenides and find an excellent agreement with recent experiments.

Download full-text PDF

Source
http://dx.doi.org/10.1103/PhysRevLett.124.257402DOI Listing

Publication Analysis

Top Keywords

excitation-induced dephasing
12
monolayer transition
8
transition metal
8
metal dichalcogenides
8
exciton-scattering-induced dephasing
4
dephasing two-dimensional
4
two-dimensional semiconductors
4
semiconductors enhanced
4
enhanced coulomb
4
coulomb interactions
4

Similar Publications

We present femtosecond pump-probe measurements of neutral and charged exciton optical response in monolayer MoSe to resonant photoexcitation of a given exciton state in the presence of 2D electron gas. We show that creation of charged exciton (X) population in a given K, K valley requires the capture of available free carriers in the opposite valley and reduces the interaction of neutral exciton (X) with the electron Fermi sea. We also observe spectral broadening of the X transition line with the increasing X population caused by efficient scattering and excitation induced dephasing.

View Article and Find Full Text PDF

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

J Phys Chem C Nanomater Interfaces

November 2023

School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia, 30332, United States.

We present a study on the many-body exciton interactions in a Ruddlesden-Popper tin halide, namely, (PEA)SnI (PEA = phenylethylammonium), 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 dephasing time with increasing excitation density as compared to its lead counterpart (PEA)PbI, which we have previously reported in a separate publication [, 153, 164706].

View Article and Find Full Text PDF

We review our recent quantum stochastic model for spectroscopic lineshapes in the presence of a coevolving and nonstationary background population of excitations. Starting from a field theory description for interacting bosonic excitons, we derive a reduced model whereby optical excitons are coupled to an incoherent background via scattering as mediated by their screened Coulomb coupling. The Heisenberg equations of motion for the optical excitons are then driven by an auxiliary stochastic population variable, which we take to be the solution of an Ornstein-Uhlenbeck process.

View Article and Find Full Text PDF

Searching for ideal materials with strong effective optical nonlinear responses is a long-term task enabling remarkable breakthroughs in contemporary quantum and nonlinear optics. Polaritons, hybridized light-matter quasiparticles, are an appealing candidate to realize such nonlinearities. Here, we explore a class of peculiar polaritons, named plasmon-exciton polaritons (plexcitons), in a hybrid system composed of silver nanodisk arrays and monolayer tungsten-disulfide (WS), which shows giant room-temperature nonlinearity due to their deep-subwavelength localized nature.

View Article and Find Full Text PDF

Perovskite nanoplatelets possess extremely narrow absorption and emission line widths, which are crucial characteristics for many optical applications. However, their underlying intrinsic and extrinsic line-broadening mechanisms are poorly understood. Here, we apply multidimensional coherent spectroscopy to determine the homogeneous line broadening of colloidal perovskite nanoplatelet ensembles.

View Article and Find Full Text PDF

Want AI Summaries of new PubMed Abstracts delivered to your In-box?

Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!