skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Valley Polarized Holes Induced Exciton Polaron Valley Splitting
Monolayer transition metal dichalcogenide semiconductors are promising valleytronic materials. Among various quasi-particle excitations hosted by the system, the valley polarized holes are particularly interesting due to their long valley lifetime preserved by the large spin–orbit splitting and spin–valley locking in the valence band. Here we report that in the absence of any magnetic field a surprising valley splitting of exciton polarons can be induced by such valley polarized holes in monolayer WSe2. The size of the splitting is comparable to that of the Zeeman effect in a magnetic field as high as 7 T and offers a quantitative approach to extract the hole density imbalance between the two valleys. We find that the density difference can easily achieve more than 1011 per cm2, and it is tunable by gate voltage as well as optical excitation power. Our study highlights the response of exciton polarons to optical pumping and advances understanding of valley dependent phenomena in monolayer transition metal dichalcogenide.  more » « less
Award ID(s):
2004474
PAR ID:
10525144
Author(s) / Creator(s):
; ; ;
Publisher / Repository:
American Chemical Society
Date Published:
Journal Name:
ACS Nano
Volume:
17
Issue:
16
ISSN:
1936-0851
Page Range / eLocation ID:
15641 to 15647
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Monolayer molybdenum di-selenide (1L-MoSe 2 ) stands out in the transition metal dichalcogenide family of materials as an outlier where optical generation of valley polarization is inefficient. Here we show that using charge doping in conjunction with an external magnetic field, the valley polarization of 1L-MoSe 2 can be controlled effectively. Most remarkably, the valley polarization can be tuned to negative values, where the higher energy Zeeman mode emission is more intense than the lower energy one. Our experimental observations are interpreted with valley-selective exciton-charge dressing that manifests when gate induced doping populates predominantly one valley in the presence of Zeeman splitting. 
    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 Nonreciprocity and nonreciprocal optical devices play a vital role in modern photonic technologies by enforcing one-way propagation of light. Here, we demonstrate an all-optical approach to nonreciprocity based on valley-selective response in transition metal dichalcogenides (TMDs). This approach overcomes the limitations of magnetic materials and it does not require an external magnetic field. We provide experimental evidence of photoinduced nonreciprocity in a monolayer WS2pumped by circularly polarized (CP) light. Nonreciprocity stems from valley-selective exciton population, giving rise to nonlinear circular dichroism controlled by CP pump fields. Our experimental results reveal a significant effect even at room temperature, despite considerable intervalley-scattering, showing promising potential for practical applications in magnetic-free nonreciprocal platforms. As an example, here we propose a device scheme to realize an optical isolator based on a pass-through silicon nitride (SiN) ring resonator integrating the optically biased TMD monolayer. 
    more » « less
  4. 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
  5. Coupling between exciton states across the Brillouin zone in monolayer transition metal dichalcogenides can lead to ultrafast valley depolarization. Using time- and angle-resolved photoemission, we present momentum- and energy-resolved measurements of exciton coupling in monolayer WS2. By comparing full 4D (kx,ky,E,t) data sets after both linearly and circularly polarized excitation, we are able to disentangle intervalley and intravalley exciton coupling dynamics. Recording in the exciton binding energy basis instead of excitation energy, we observe strong mixing between the B1s exciton and An>1 states. The photoelectron energy and momentum distributions observed from excitons populated via intervalley coupling (e.g. K− → K+) indicate that the dominant valley depolarization mechanism conserves the exciton binding energy and center-of-mass momentum, consistent with intervalley Coulomb exchange. On longer timescales, exciton relaxation is accompanied by contraction of the momentum space distribution. 
    more » « less