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Title: Visualizing nanoscale excitonic relaxation properties of disordered edges and grain boundaries in monolayer molybdenum disulfide

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms8993· OSTI ID:1256037
 [1];  [2];  [3];  [3];  [3];  [2];  [1];  [2];  [2];  [2];  [2];  [1];  [4];  [2];  [2];  [1];  [1];  [2]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Univ. of California, Berkeley, CA (United States)
  4. Univ. of California, Berkeley, CA (United States); Arizona State Univ., Tempe, AZ (United States)

Two-dimensional monolayer transition metal dichalcogenide semiconductors are ideal building blocks for atomically thin, flexible optoelectronic and catalytic devices. Although challenging for two-dimensional systems, sub-diffraction optical microscopy provides a nanoscale material understanding that is vital for optimizing their optoelectronic properties. Here we use the 'Campanile' nano-optical probe to spectroscopically image exciton recombination within monolayer MoS < inf > 2 < /inf > with sub-wavelength resolution (60 nm), at the length scale relevant to many critical optoelectronic processes. Synthetic monolayer MoS < inf > 2 < /inf > is found to be composed of two distinct optoelectronic regions: an interior, locally ordered but mesoscopically heterogeneous two-dimensional quantum well and an unexpected ~300-nm wide, energetically disordered edge region. Further, grain boundaries are imaged with sufficient resolution to quantify local exciton-quenching phenomena, and complimentary nano-Auger microscopy reveals that the optically defective grain boundary and edge regions are sulfur deficient. The nanoscale structure-property relationships established here are critical for the interpretation of edge- and boundary-related phenomena and the development of next-generation two-dimensional optoelectronic devices.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231; DMR-1055938
OSTI ID:
1256037
Alternate ID(s):
OSTI ID: 1407380
Journal Information:
Nature Communications, Vol. 6; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 190 works
Citation information provided by
Web of Science

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Cited By (45)

Nanoassembly Growth Model for Subdomain and Grain Boundary Formation in 1T′ Layered ReS 2 journal September 2019
Microstructure and Elastic Constants of Transition Metal Dichalcogenide Monolayers from Friction and Shear Force Microscopy journal August 2018
Scanning Probe Lithography Patterning of Monolayer Semiconductors and Application in Quantifying Edge Recombination journal September 2019
Boosting the Photoluminescence of Monolayer MoS 2 on High-Density Nanodimer Arrays with Sub-10 nm Gap journal December 2017
Direct Vapor Growth of 2D Vertical Heterostructures with Tunable Band Alignments and Interfacial Charge Transfer Behaviors journal February 2019
Nanoimaging of Electronic Heterogeneity in Bi 2 Se 3 and Sb 2 Te 3 Nanocrystals journal December 2017
Refractive Index Dispersion of Hexagonal Boron Nitride in the Visible and Near‐Infrared journal October 2018
CVD grown 2D MoS 2 layers: A photoluminescence and fluorescence lifetime imaging study journal September 2016
Imaging Nanoscale Inhomogeneities and Edge Delamination in As‐Grown MoS 2 Using Tip‐Enhanced Photoluminescence journal May 2019
A Versatile Scanning Photocurrent Mapping System to Characterize Optoelectronic Devices based on 2D Materials journal May 2017
Tip-enhanced Raman spectroscopy: principles, practice, and applications to nanospectroscopic imaging of 2D materials journal October 2018
Bandgap broadening at grain boundaries in single-layer MoS2 journal July 2018
Spectral focusing of broadband silver electroluminescence in nanoscopic FRET-LEDs journal April 2017
Charge density wave order in 1D mirror twin boundaries of single-layer MoSe2 journal April 2016
Nanoscale mapping of quasiparticle band alignment journal July 2019
Nanoscale investigation of materials, chemical reactions, and biological systems by tip enhanced Raman spectroscopy – a review journal January 2018
The role of a plasmonic substrate on the enhancement and spatial resolution of tip-enhanced Raman scattering journal January 2019
Photoluminescence enhancement of monolayer MoS 2 using plasmonic gallium nanoparticles journal January 2019
Physics of excitons and their transport in two dimensional transition metal dichalcogenide semiconductors journal January 2019
Note: Controlling the length of plasmonic tips obtained by pulsed electrochemical etching journal September 2018
Plasticity resulted from phase transformation for monolayer molybdenum disulfide film during nanoindentation simulations journal March 2017
Inhomogeneous photocarrier dynamics and transport in monolayer MoS 2 by ultrafast microscopy journal September 2019
2D materials advances: from large scale synthesis and controlled heterostructures to improved characterization techniques, defects and applications journal December 2016
The important role of water in growth of monolayer transition metal dichalcogenides journal March 2017
Multimodal spectromicroscopy of monolayer WS 2 enabled by ultra-clean van der Waals epitaxy journal July 2018
Probing the origin of lateral heterogeneities in synthetic monolayer molybdenum disulfide journal February 2019
Disentangling the effects of doping, strain and disorder in monolayer WS 2 by optical spectroscopy journal January 2020
Edge states in dichalcogenide nanoribbons and triangular quantum dots journal February 2016
Optical identification of sulfur vacancies: Bound excitons at the edges of monolayer tungsten disulfide journal April 2017
Strain tolerance of two-dimensional crystal growth on curved surfaces journal May 2019
Large range modification of exciton species in monolayer WS_2 journal January 2016
Reconfigurable Local Photoluminescence of Atomically-Thin Semiconductors via Ferroelectric-Assisted Effects journal November 2019
Tip-enhanced Raman Spectroscopy: Principles, Practice, and Applications to Nanospectroscopic Imaging of 2D Materials text January 2019
Spectral focusing of broadband silver electroluminescence in nanoscopic FRET-LEDs text January 2017
Large Range Manipulation of Exciton Species in Monolayer WS2 text January 2016
Spectral focusing of broadband silver electroluminescence in nanoscopic FRET-LEDs text January 2017
Virtual trions in the photoluminescence of monolayer transition-metal dichalcogenides text January 2018
Disentangling the effects of doping, strain and defects in monolayer WS2 by optical spectroscopy text January 2019
Imaging Nanoscale Inhomogeneities and Edge Delamination in As-Grown MoS2 Using Tip-Enhanced Photoluminescence text January 2019
Mapping Catalytically Relevant Edge Electronic States of MoS 2 journal February 2018
Virtual substrate method for nanomaterials characterization journal May 2017
Deconvoluting the Photonic and Electronic Response of 2D Materials: The Case of MoS2 journal December 2017
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Improving resolution in quantum subnanometre-gap tip-enhanced Raman nanoimaging journal May 2016
Manipulation of local optical properties and structures in molybdenum-disulfide monolayers using electric field-assisted near-field techniques journal April 2017

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