skip to main content


Title: Phonon-exciton Interactions in WSe2 under a quantizing magnetic field
Abstract

Strong many-body interaction in two-dimensional transitional metal dichalcogenides provides a unique platform to study the interplay between different quasiparticles, such as prominent phonon replica emission and modified valley-selection rules. A large out-of-plane magnetic field is expected to modify the exciton-phonon interactions by quantizing excitons into discrete Landau levels, which is largely unexplored. Here, we observe the Landau levels originating from phonon-exciton complexes and directly probe exciton-phonon interaction under a quantizing magnetic field. Phonon-exciton interaction lifts the inter-Landau-level transition selection rules for dark trions, manifested by a distinctively different Landau fan pattern compared to bright trions. This allows us to experimentally extract the effective mass of both holes and electrons. The onset of Landau quantization coincides with a significant increase of the valley-Zeeman shift, suggesting strong many-body effects on the phonon-exciton interaction. Our work demonstrates monolayer WSe2as an intriguing playground to study phonon-exciton interactions and their interplay with charge, spin, and valley.

 
more » « less
Award ID(s):
1933214 1904716 1838443 1945420 1806227
NSF-PAR ID:
10163456
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publisher / Repository:
Nature Publishing Group
Date Published:
Journal Name:
Nature Communications
Volume:
11
Issue:
1
ISSN:
2041-1723
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Selection rules are of vital importance in determining the basic optical properties of atoms, molecules and semiconductors. They provide general insights into the symmetry of the system and the nature of relevant electronic states. A two-dimensional electron gas in a magnetic field is a model system where optical transitions between Landau levels (LLs) are described by simple selection rules associated with the LL indexN. Here we examine the inter-LL optical transitions of high-quality bilayer graphene by photocurrent spectroscopy measurement. We observed valley-dependent optical transitions that violate the conventional selection rules Δ|N| = ± 1. Moreover, we can tune the relative oscillator strength by tuning the bilayer graphene bandgap. Our findings provide insights into the interplay between magnetic field, band structure and many-body interactions in tunable semiconductor systems, and the experimental technique can be generalized to study symmetry-broken states and low energy magneto-optical properties of other nano and quantum materials.

     
    more » « less
  2. Abstract

    The interactions between charges and excitons involve complex many-body interactions at high densities. The exciton-polaron model has been adopted to understand the Fermi sea screening of charged excitons in monolayer transition metal dichalcogenides. The results provide good agreement with absorption measurements, which are dominated by dilute bright exciton responses. Here we investigate the Fermi sea dressing of spin-forbidden dark excitons in monolayer WSe2. With a Zeeman field, the valley-polarized dark excitons show distinct p-doping dependence in photoluminescence when the carriers reach a critical density. This density can be interpreted as the onset of strongly modified Fermi sea interactions and shifts with increasing exciton density. Through valley-selective excitation and dynamics measurements, we also infer an intervalley coupling between the dark trions and exciton-polarons mediated by the many-body interactions. Our results reveal the evolution of Fermi sea screening with increasing exciton density and the impacts of polaron-polaron interactions, which lay the foundation for understanding electronic correlations and many-body interactions in 2D systems.

     
    more » « less
  3. Abstract

    Selective breaking of degenerate energy levels is a well-known tool for coherent manipulation of spin states. Though most simply achieved with magnetic fields, polarization-sensitive optical methods provide high-speed alternatives. Exploiting the optical selection rules of transition metal dichalcogenide monolayers, the optical Stark effect allows for ultrafast manipulation of valley-coherent excitons. Compared to excitons in these materials, microcavity exciton-polaritons offer a promising alternative for valley manipulation, with longer lifetimes, enhanced valley coherence, and operation across wider temperature ranges. Here, we show valley-selective control of polariton energies in WS2using the optical Stark effect, extending coherent valley manipulation to the hybrid light-matter regime. Ultrafast pump-probe measurements reveal polariton spectra with strong polarization contrast originating from valley-selective energy shifts. This demonstration of valley degeneracy breaking at picosecond timescales establishes a method for coherent control of valley phenomena in exciton-polaritons.

     
    more » « less
  4. We develop an ab initio nonadiabatic molecular dynamics (NAMD) method based on GW plus real-time Bethe-Salpeter equation ( GW + rtBSE-NAMD) for the spin-resolved exciton dynamics. From investigations on MoS 2 , we provide a comprehensive picture of spin-valley exciton dynamics where the electron-phonon (e-ph) scattering, spin-orbit interaction (SOI), and electron-hole (e-h) interactions come into play collectively. In particular, we provide a direct evidence that e-h exchange interaction plays a dominant role in the fast valley depolarization within a few picoseconds, which is in excellent agreement with experiments. Moreover, there are bright-to-dark exciton transitions induced by e-ph scattering and SOI. Our study proves that e-h many-body effects are essential to understand the spin-valley exciton dynamics in transition metal dichalcogenides and the newly developed GW + rtBSE-NAMD method provides a powerful tool for exciton dynamics in extended systems with time, space, momentum, energy, and spin resolution. 
    more » « less
  5. The polarized photoluminescence from atomically thin transition metal dichalcogenides is a frequently applied tool to scrutinize optical selection rules and valley physics, yet it is known to sensibly depend on a variety of internal and external material and sample properties. In this work, we apply combined angle- and polarization-resolved spectroscopy to explore the interplay of excitonic physics and phenomena arising from the commonly utilized encapsulation procedure on the optical properties of atomically thinMoSe2. We probe monolayers prepared in both suspended and encapsulated manners. We show that the hBN encapsulation significantly enhances the linear polarization of exciton photoluminescence emission at large emission angles. This degree of linear polarization of excitons can increase up to∼<#comment/>17%<#comment/>in the hBN encapsulated samples. As we confirm by finite-difference time-domain simulations, it can be directly connected to the optical anisotropy of the hBN layers. In comparison, the linear polarization at finite exciton momenta is significantly reduced in a suspendedMoSe2monolayer, and becomes notable only in cryogenic conditions. This phenomenon strongly suggests that the effect is rooted in the k-dependent anisotropic exchange coupling inherent in 2D excitons. Our results have strong implications on further studies on valley contrasting selection rules and valley coherence phenomena using standard suspended and encapsulated samples.

     
    more » « less