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We report charged exciton (trion) formation dynamics in doped monolayer transition metal dichalcogenides, specifically molybdenum diselenide (MoSe2), using resonant two-color pump-probe spectroscopy. When resonantly pumping the exciton transition, trions are generated on a picosecond time scale through excitonelectron interaction. As the pump energy is tuned from the high energy to low energy side of the inhomogeneously broadened exciton resonance, the trion formation time increases by ~50%. This feature can be explained by the existence of both localized and delocalized excitons in a disordered potential and suggests the existence of an exciton mobility edge in transition metal dichalcogenides. [ABSTRACT FROM AUTHOR]

We report the first direct spectroscopic evidence for coherent electronic coupling between excitons and trions in atomically thin transition metal dichalcogenides, specifically monolayer MoSe2. Signatures of coupling appear as isolated cross-peaks in two-color pump-probe spectra, and the line shape of the peaks reveals that the coherent coupling originates from many-body interactions. Excellent agreement between the experiment and density matrix calculations suggests that coherent exciton-trion coupling leads to the formation of a correlated state with a remarkably large binding energy. [ABSTRACT FROM AUTHOR]

We study an asymmetric double InGaAs quantum well using optical two-dimensional coherent spectroscopy. The collection of zero-quantum, one-quantum, and two-quantum two-dimensional spectra provides a unique and comprehensive picture of the double well coherent optical response. Coherent and incoherent contributions to the coupling between the two quantum well excitons are clearly separated. An excellent agreement with density matrix calculations reveals that coherent interwell coupling originates from many-body interactions. [ABSTRACT FROM AUTHOR]

In atomically thin two-dimensional semiconductors such as transition metal dichalcogenides (TMDs), controlling the density and type of defects promises to be an effective approach for engineering light-matter interactions. We demonstrate that electron-beam irradiation is a simple tool for selectively introducing defect-bound exciton states associated with chalcogen vacancies in TMDs. Our first-principles calculations and time-resolved spectroscopy measurements of monolayer WSe2 reveal that these defect-bound excitons exhibit exceptional optical properties including a recombination lifetime approaching 200 ns and a valley lifetime longer than 1 μs. The ability to engineer the crystal lattice through electron irradiation provides a new approach for tailoring the optical response of TMDs for photonics, quantum optics, and valleytronics applications. [ABSTRACT FROM AUTHOR]

Exciton transport in nanomaterials is sensitive to fluctuations in the confinement potential that are intrinsic to heterogeneous solid-state systems. Redistribution of exciton population manifests as spectral diffusion in which the exciton energy shifts. It is generally assumed that increase or decrease in the exciton energy are equally probable. We show that this assumption is not necessarily valid using two-dimensional coherent spectroscopy on a disordered GaAs quantum well. High-energy excitons relax into lower-energy localized states over a time scale of tens of picoseconds at low sample temperatures (~5K). A transition to uniform spectral diffusion of excitons is observed as the temperature is increased to ~20K. Numerical simulations reveal the contribution of exciton-phonon interactions to spectral diffusion of excitons. These results provide a perspective on the process of dynamic localization and the effect of the correlation length of disorder on spectral diffusion of excitons. [ABSTRACT FROM AUTHOR]

The homogeneous and inhomogeneous linewidths of the heavy-hole exciton resonance in a (110)-oriented GaAs multiple-quantum-well sample are measured using optical two-dimensional Fourier transform spectroscopy. By probing the optical nonlinear response for polarization along the in-plane crystal axes [110] and [110], we measure different homogeneous linewidths for the two orthogonal directions. This difference is found to be due to anisotropic excitation-induced dephasing, caused by a crystal-axis-dependent absorption coefficient. The extrapolated zero-excitation density homogeneous linewidth exhibits an activation-like temperature dependence. We find that the homogeneous linewidth extrapolated to zero excitation density and temperature is ∼34 μeV, while the inhomogeneous linewidth is 1.9 meV for both polarizations. [ABSTRACT FROM AUTHOR]

In van der Waals (vdW) heterostructures formed by stacking two monolayers of transition metal dichalcogenides, multiple exciton resonances with highly tunable properties are formed and subject to both vertical and lateral confinement. We investigate how a unique control knob, the twist angle between the two monolayers, can be used to control the exciton dynamics. We observe that the interlayer exciton lifetimes in MoSe2/WSe2 twisted bilayers (TBLs) change by one order of magnitude when the twist angle is varied from 1° to 3.5°. Using a low-energy continuum model, we theoretically separate two leading mechanisms that influence interlayer exciton radiative lifetimes. The shift to indirect transitions in the momentum space with an increasing twist angle and the energy modulation from the moiré potential both have a significant impact on interlayer exciton lifetimes. We further predict distinct temperature dependence of interlayer exciton lifetimes in TBLs with different twist angles, which is partially validated by experiments. While many recent studies have highlighted how the twist angle in a vdW TBL can be used to engineer the ground states and quantum phases due to many-body interaction, our studies explore its role in controlling the dynamics of optically excited states, thus, expanding the conceptual applications of "twistronics". [ABSTRACT FROM AUTHOR]

The exciton coherent signal decay rate in GaAs quantum wells, as measured in four-wave mixing experiments, depends on the polarization of the excitation pulses. Using polarization-dependent two-dimensional coherent spectroscopy, we show that this behavior is due to the bosonic character of excitons. Interference between two different quantum mechanical pathways results in a smaller decay rate for cocircular and colinear polarization of the optical excitation pulses. This interference does not exist for cross-linearly polarized excitation pulses resulting in a larger decay rate. Our result shows that the bosonic nature of excitons must be considered when interpreting ultrafast spectroscopic studies of exciton dephasing in semiconductors. This behavior should be considered while interpreting results of ultrafast spectroscopy experiments involving bosonlike excitations. [ABSTRACT FROM AUTHOR]

Studies have shown that many-body interactions among semiconductor excitons can produce distinct features in two-dimensional optical spectra. However, to the best of our knowledge, the dynamics of many-body interactions have not been measured in two-dimensional (2D) spectroscopy studies. Here we measure 2D spectra of GaAs quantum wells at many different "waiting" times and study the time dependence of the spectral features. Characteristic signatures of exciton polarization correlations manifest in the diagonal peaks decay at the exciton dephasing rate, consistent with theoretical predictions. Other many-body interactions manifest in off-diagonal features decay much more slowly. These persistent off-diagonal features must be due to many-body interactions involving exciton populations, and their persistence cannot be predicted by theoretical descriptions restricted to the coherent limit. [ABSTRACT FROM AUTHOR]

In van der Waals (vdW) heterostructures formed by stacking two monolayers of transition metal dichalcogenides, multiple exciton resonances with highly tunable properties are formed and subject to both vertical and lateral confinement. We investigate how a unique control knob, the twist angle between the two monolayers, can be used to control the exciton dynamics. We observe that the interlayer exciton lifetimes in MoSe_{2}/WSe_{2} twisted bilayers (TBLs) change by one order of magnitude when the twist angle is varied from 1° to 3.5°. Using a low-energy continuum model, we theoretically separate two leading mechanisms that influence interlayer exciton radiative lifetimes. The shift to indirect transitions in the momentum space with an increasing twist angle and the energy modulation from the moiré potential both have a significant impact on interlayer exciton lifetimes. We further predict distinct temperature dependence of interlayer exciton lifetimes in TBLs with different twist angles, which is partially validated by experiments. While many recent studies have highlighted how the twist angle in a vdW TBL can be used to engineer the ground states and quantum phases due to many-body interaction, our studies explore its role in controlling the dynamics of optically excited states, thus, expanding the conceptual applications of "twistronics".

In atomically thin two-dimensional semiconductors such as transition metal dichalcogenides (TMDs), controlling the density and type of defects promises to be an effective approach for engineering light-matter interactions. We demonstrate that electron-beam irradiation is a simple tool for selectively introducing defect-bound exciton states associated with chalcogen vacancies in TMDs. Our first-principles calculations and time-resolved spectroscopy measurements of monolayer WSe_{2} reveal that these defect-bound excitons exhibit exceptional optical properties including a recombination lifetime approaching 200 ns and a valley lifetime longer than 1  μs. The ability to engineer the crystal lattice through electron irradiation provides a new approach for tailoring the optical response of TMDs for photonics, quantum optics, and valleytronics applications.