Title: Imaging Valley Excitons in a 2D Semiconductor with Scanning Tunneling Microscope-Induced Luminescence

Journal Article · · ACS Nano

Valley excitons dominate the optoelectronic response of transition-metal dichalcogenides and are drastically affected by structural and environmental inhomogeneities localized in these materials. Critical to understanding and controlling these nanoscale excitonic changes is the ability to correlate the imaging of excitonic states with crystalline structures on the atomic scale. Here, in this study, we apply scanning tunneling microscope-induced luminescence microscopy to image valley excitons in a semiconducting transition-metal dichalcogenide monolayer decoupled by a 10 nanometer-thick hexagonal-boron-nitride flake incorporated in a lateral homojunction on an Au electrode surface. This design enables the observation of chiral excitonic emission arising from neutral and charged valley excitons of the monolayer semiconductor at ambipolar voltages with a quantum efficiency up to similar to ~10-5 photon/electron. The measured light helicity demonstrates considerable circular polarization dependent on the sample voltage, reaching as much as 40%. The real-space luminescence imaging maps$$-$$at subnanometer resolution$$-$$of the valley excitons reveal striking spatial variations associated with localized inhomogeneities, including surface impurities and possibly nanoscale dielectric and/or potential disorders in the monolayer. Our study introduces a promising format for 2D materials to explore and tailor their optoelectronic processes at the atomic scale.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
Department of Human Resources and Social Security of Anhui Province; National Science Foundation of China (NSFC); USDOE
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
2520468
Journal Information:
ACS Nano, Journal Name: ACS Nano Journal Issue: 12 Vol. 18; ISSN 1936-0851
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (59)

Nanoscale Positioning of Single-Photon Emitters in Atomically Thin WSe 2 journal June 2016
Electroluminescent Devices Based on 2D Semiconducting Transition Metal Dichalcogenides journal August 2018
Observation of Single-Electron Transport and Charging on Individual Point Defects in Atomically Thin WSe2 journal June 2021
Universal Fermi-Level Pinning in Transition-Metal Dichalcogenides journal February 2019
Strain-Induced Spatial and Spectral Isolation of Quantum Emitters in Mono- and Bilayer WSe 2 journal October 2015
Electrically Tunable Valley-Light Emitting Diode (vLED) Based on CVD-Grown Monolayer WS 2 journal February 2016
Electronic Structure, Surface Doping, and Optical Response in Epitaxial WSe 2 Thin Films journal March 2016
Electronic Structure and Luminescence of Quasi-Freestanding MoS 2 Nanopatches on Au(111) journal July 2016
Many-Body State Description of Single-Molecule Electroluminescence Driven by a Scanning Tunneling Microscope journal January 2019
Charge Carrier Injection Electroluminescence with CO-Functionalized Tips on Single Molecular Emitters journal November 2019
Tunable Control over the Ionization State of Single Mn Acceptors in GaAs with Defect-Induced Band Bending journal May 2011
Valleytronics in 2D materials journal August 2016
Visualizing coherent intermolecular dipole–dipole coupling in real space journal March 2016
Real-space investigation of energy transfer in heterogeneous molecular dimers journal October 2016
Cascaded emission of single photons from the biexciton in monolayered WSe2 journal November 2016
Deterministic strain-induced arrays of quantum emitters in a two-dimensional semiconductor journal May 2017
Light-emitting diodes by band-structure engineering in van der Waals heterostructures journal February 2015
Optical generation of excitonic valley coherence in monolayer WSe2 journal August 2013
Electrically tunable excitonic light-emitting diodes based on monolayer WSe2 p–n junctions journal March 2014
Optically active quantum dots in monolayer WSe2 journal May 2015
Single photon emitters in exfoliated WSe2 structures journal May 2015
Single quantum emitters in monolayer semiconductors journal May 2015
Electrical generation and control of the valley carriers in a monolayer transition metal dichalcogenide journal April 2016
Generation of molecular hot electroluminescence by resonant nanocavity plasmons journal December 2009
Evidence for moiré intralayer excitons in twisted WSe2/WSe2 homobilayer superlattices journal June 2022
Charge-tuneable biexciton complexes in monolayer WSe2 journal September 2018
Valley phonons and exciton complexes in a monolayer semiconductor journal January 2020
Intrinsic donor-bound excitons in ultraclean monolayer semiconductors journal February 2021
Excitons in a reconstructed moiré potential in twisted WSe2/WSe2 homobilayers journal January 2021
Tip-induced excitonic luminescence nanoscopy of an atomically resolved van der Waals heterostructure journal March 2023
Radiative control of dark excitons at room temperature by nano-optical antenna-tip Purcell effect journal November 2017
Dielectric disorder in two-dimensional materials journal August 2019
Imaging strain-localized excitons in nanoscale bubbles of monolayer WSe2 at room temperature journal July 2020
Dynamics and efficient conversion of excitons to trions in non-uniformly strained monolayer WS2 journal February 2020
Sub-nanometre resolution in single-molecule photoluminescence imaging journal August 2020
2D materials for quantum information science journal August 2019
Signatures of moiré-trapped valley excitons in MoSe2/WSe2 heterobilayers journal February 2019
Evidence for moiré excitons in van der Waals heterostructures journal February 2019
Observation of moiré excitons in WSe2/WS2 heterostructure superlattices journal February 2019
Tunneling-current-induced local excitonic luminescence in p-doped WSe2monolayers journal January 2020
Plasmon-mediated circularly polarized luminescence of GaAs in a scanning tunneling microscope journal December 2015
Valley excitons in two-dimensional semiconductors journal December 2014
Tip-geometry effects in circularly polarized light emission from a scanning tunneling microscope journal February 1999
Tip-induced band bending by scanning tunneling spectroscopy of the states of the tip-induced quantum dot on InAs(110) journal March 1999
Binding energies of exciton complexes in transition metal dichalcogenide monolayers and effect of dielectric environment journal November 2015
Controlled Charge Switching on a Single Donor with a Scanning Tunneling Microscope journal August 2008
Viewing the Interior of a Single Molecule: Vibronically Resolved Photon Imaging at Submolecular Resolution journal November 2010
Nonlinear Valley and Spin Currents from Fermi Pocket Anisotropy in 2D Crystals journal October 2014
Defect Structure of Localized Excitons in a WSe 2 Monolayer journal July 2017
In-Plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules journal July 2017
Scanning Tunneling Microscope-Induced Excitonic Luminescence of a Two-Dimensional Semiconductor journal July 2019
Probing and Manipulating Valley Coherence of Dark Excitons in Monolayer WSe 2 journal August 2019
Valley-selective chiral phonon replicas of dark excitons and trions in monolayer WS e 2 journal October 2019
Bimodal exciton-plasmon light sources controlled by local charge carrier injection journal May 2018
Electrically driven photon emission from individual atomic defects in monolayer WS 2 journal September 2020
Electrically Switchable Chiral Light-Emitting Transistor journal April 2014
Electrofluorochromism at the single-molecule level journal July 2018
Electrically tunable valley polarization and valley coherence in monolayer WSe 2 embedded in a van der Waals heterostructure journal February 2019
Substrate engineering for high-quality emission of free and localized excitons from atomic monolayers in hybrid architectures journal January 2017