Electrically driven photon emission from individual atomic defects in monolayer WS 2
Abstract
Quantum dot–like single-photon sources in transition metal dichalcogenides (TMDs) exhibit appealing quantum optical properties but lack a well-defined atomic structure and are subject to large spectral variability. Here, we demonstrate electrically stimulated photon emission from individual atomic defects in monolayer WS 2 and directly correlate the emission with the local atomic and electronic structure. Radiative transitions are locally excited by sequential inelastic electron tunneling from a metallic tip into selected discrete defect states in the WS 2 bandgap. Coupling to the optical far field is mediated by tip plasmons, which transduce the excess energy into a single photon. The applied tip-sample voltage determines the transition energy. Atomically resolved emission maps of individual point defects closely resemble electronic defect orbitals, the final states of the optical transitions. Inelastic charge carrier injection into localized defect states of two-dimensional materials provides a powerful platform for electrically driven, broadly tunable, atomic-scale single-photon sources.
- Authors:
-
[1];
[1];
[2];
[1];
[3];
[1];
[1];
[1]
- Molecular Foundry, Lawrence Berkeley National Laboratory, CA 94720, USA.
- Molecular Foundry, Lawrence Berkeley National Laboratory, CA 94720, USA., Walter-Schottky-Institut and Physik-Department, Technical University of Munich, Garching 85748, Germany.
- Molecular Foundry, Lawrence Berkeley National Laboratory, CA 94720, USA., Department of Physics, Montana State University, Bozeman, MT 59717, USA.
- ICFO-Institut de Ciències Fotòniques, The Barcelona Institute of Science and Technology, 08860 Castelldefels, Barcelona, Spain., ICREA-Institució Catalana de Recerca i Estudis Avançats, 08010 Barcelona, Spain.
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); Swiss National Science Foundation (SNSF); Ministry of Economic Affairs and Digital Transformation of Spain (MINECO); European Research Council (ERC)
- OSTI Identifier:
- 1664431
- Alternate Identifier(s):
- OSTI ID: 1706663
- Grant/Contract Number:
- AC02-05CH11231; Early Career Award; P2SKP2171770; MAT2017-88492-R; SEV2015-0522; 789104-eNANO
- Resource Type:
- Published Article
- Journal Name:
- Science Advances
- Additional Journal Information:
- Journal Name: Science Advances Journal Volume: 6 Journal Issue: 38; Journal ID: ISSN 2375-2548
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS
Citation Formats
Schuler, Bruno, Cochrane, Katherine A., Kastl, Christoph, Barnard, Edward S., Wong, Edward, Borys, Nicholas J., Schwartzberg, Adam M., Ogletree, D. Frank, de Abajo, F. Javier García, and Weber-Bargioni, Alexander. Electrically driven photon emission from individual atomic defects in monolayer WS 2. United States: N. p., 2020.
Web. doi:10.1126/sciadv.abb5988.
Schuler, Bruno, Cochrane, Katherine A., Kastl, Christoph, Barnard, Edward S., Wong, Edward, Borys, Nicholas J., Schwartzberg, Adam M., Ogletree, D. Frank, de Abajo, F. Javier García, & Weber-Bargioni, Alexander. Electrically driven photon emission from individual atomic defects in monolayer WS 2. United States. https://doi.org/10.1126/sciadv.abb5988
Schuler, Bruno, Cochrane, Katherine A., Kastl, Christoph, Barnard, Edward S., Wong, Edward, Borys, Nicholas J., Schwartzberg, Adam M., Ogletree, D. Frank, de Abajo, F. Javier García, and Weber-Bargioni, Alexander. Wed .
"Electrically driven photon emission from individual atomic defects in monolayer WS 2". United States. https://doi.org/10.1126/sciadv.abb5988.
@article{osti_1664431,
title = {Electrically driven photon emission from individual atomic defects in monolayer WS 2},
author = {Schuler, Bruno and Cochrane, Katherine A. and Kastl, Christoph and Barnard, Edward S. and Wong, Edward and Borys, Nicholas J. and Schwartzberg, Adam M. and Ogletree, D. Frank and de Abajo, F. Javier García and Weber-Bargioni, Alexander},
abstractNote = {Quantum dot–like single-photon sources in transition metal dichalcogenides (TMDs) exhibit appealing quantum optical properties but lack a well-defined atomic structure and are subject to large spectral variability. Here, we demonstrate electrically stimulated photon emission from individual atomic defects in monolayer WS 2 and directly correlate the emission with the local atomic and electronic structure. Radiative transitions are locally excited by sequential inelastic electron tunneling from a metallic tip into selected discrete defect states in the WS 2 bandgap. Coupling to the optical far field is mediated by tip plasmons, which transduce the excess energy into a single photon. The applied tip-sample voltage determines the transition energy. Atomically resolved emission maps of individual point defects closely resemble electronic defect orbitals, the final states of the optical transitions. Inelastic charge carrier injection into localized defect states of two-dimensional materials provides a powerful platform for electrically driven, broadly tunable, atomic-scale single-photon sources.},
doi = {10.1126/sciadv.abb5988},
journal = {Science Advances},
number = 38,
volume = 6,
place = {United States},
year = {2020},
month = {9}
}
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Works referenced in this record:
Single Charge and Exciton Dynamics Probed by Molecular-Scale-Induced Electroluminescence
journal, May 2018
- Rosławska, Anna; Merino, Pablo; Große, Christoph
- Nano Letters, Vol. 18, Issue 6
Solid-state single-photon emitters
journal, September 2016
- Aharonovich, Igor; Englund, Dirk; Toth, Milos
- Nature Photonics, Vol. 10, Issue 10
Room-Temperature Quantum Bit Memory Exceeding One Second
journal, June 2012
- Maurer, P. C.; Kucsko, G.; Latta, C.
- Science, Vol. 336, Issue 6086
Theory of photon emission in electron tunneling to metallic particles
journal, May 1992
- Persson, B. N. J.; Baratoff, A.
- Physical Review Letters, Vol. 68, Issue 21
Resonance Absorption by Nuclear Magnetic Moments in a Solid
journal, January 1946
- Purcell, E. M.; Torrey, H. C.; Pound, R. V.
- Physical Review, Vol. 69, Issue 1-2, p. 37-38
Strain-Induced Spatial and Spectral Isolation of Quantum Emitters in Mono- and Bilayer WSe 2
journal, October 2015
- Kumar, S.; Kaczmarczyk, A.; Gerardot, B. D.
- Nano Letters, Vol. 15, Issue 11
Single-photon emission from localized excitons in an atomically thin semiconductor
journal, January 2015
- Tonndorf, Philipp; Schmidt, Robert; Schneider, Robert
- Optica, Vol. 2, Issue 4
Light Emission from Inelastic Electron Tunneling
journal, October 1976
- Lambe, John; McCarthy, S. L.
- Physical Review Letters, Vol. 37, Issue 14
Enhanced Light Emission from Large-Area Monolayer MoS 2 Using Plasmonic Nanodisc Arrays
journal, March 2015
- Butun, Serkan; Tongay, Sefaattin; Aydin, Koray
- Nano Letters, Vol. 15, Issue 4
Probing the Photonic Local Density of States with Electron Energy Loss Spectroscopy
journal, March 2008
- García de Abajo, F. J.; Kociak, M.
- Physical Review Letters, Vol. 100, Issue 10
How Substitutional Point Defects in Two-Dimensional WS 2 Induce Charge Localization, Spin–Orbit Splitting, and Strain
journal, August 2019
- Schuler, Bruno; Lee, Jun-Ho; Kastl, Christoph
- ACS Nano, Vol. 13, Issue 9
Selective triplet exciton formation in a single molecule
journal, June 2019
- Kimura, Kensuke; Miwa, Kuniyuki; Imada, Hiroshi
- Nature, Vol. 570, Issue 7760
Electroluminescence from graphene excited by electron tunneling
journal, January 2014
- Beams, Ryan; Bharadwaj, Palash; Novotny, Lukas
- Nanotechnology, Vol. 25, Issue 5
Vibronic Spectroscopy with Submolecular Resolution from STM-Induced Electroluminescence
journal, March 2017
- Doppagne, Benjamin; Chong, Michael C.; Lorchat, Etienne
- Physical Review Letters, Vol. 118, Issue 12
Nonlocal Effects in the Plasmons of Strongly Interacting Nanoparticles, Dimers, and Waveguides
journal, October 2008
- García de Abajo, F. Javier
- The Journal of Physical Chemistry C, Vol. 112, Issue 46
Atomic-Scale Imaging and Spectroscopy of Electroluminescence at Molecular Interfaces
journal, February 2017
- Kuhnke, Klaus; Große, Christoph; Merino, Pablo
- Chemical Reviews, Vol. 117, Issue 7
Theory of the scanning tunneling microscope
journal, January 1985
- Tersoff, J.; Hamann, D. R.
- Physical Review B, Vol. 31, Issue 2
Spontaneous light emission in complex nanostructures
journal, May 2004
- Blanco, L. A.; García de Abajo, F. J.
- Physical Review B, Vol. 69, Issue 20
2D materials and van der Waals heterostructures
journal, July 2016
- Novoselov, K. S.; Mishchenko, A.; Carvalho, A.
- Science, Vol. 353, Issue 6298
Intramolecular photon emission from a single molecule in a scanning tunneling microscope
journal, May 2008
- Wu, S. W.; Nazin, G. V.; Ho, W.
- Physical Review B, Vol. 77, Issue 20
Photon emission with the scanning tunneling microscope
journal, December 1988
- Gimzewski, J. K.; Reihl, B.; Coombs, J. H.
- Zeitschrift f�r Physik B Condensed Matter, Vol. 72, Issue 4
A silicon carbide room-temperature single-photon source
journal, November 2013
- Castelletto, S.; Johnson, B. C.; Ivády, V.
- Nature Materials, Vol. 13, Issue 2
Fundamental Limits to the Coupling between Light and 2D Polaritons by Small Scatterers
journal, March 2019
- Dias, Eduardo J. C.; García de Abajo, F. Javier
- ACS Nano, Vol. 13, Issue 5
Bimodal exciton-plasmon light sources controlled by local charge carrier injection
journal, May 2018
- Merino, Pablo; Rosławska, Anna; Große, Christoph
- Science Advances, Vol. 4, Issue 5
Tip influence on plasmon excitations in single gold particles in an STM
journal, March 2002
- Nilius, N.; Ernst, N.; Freund, H. -J.
- Physical Review B, Vol. 65, Issue 11
Designing defect spins for wafer-scale quantum technologies
journal, November 2015
- Koehl, William F.; Seo, Hosung; Galli, Giulia
- MRS Bulletin, Vol. 40, Issue 12
Single photon emitters in exfoliated WSe2 structures
journal, May 2015
- Koperski, M.; Nogajewski, K.; Arora, A.
- Nature Nanotechnology, Vol. 10, Issue 6
Site-selectively generated photon emitters in monolayer MoS2 via local helium ion irradiation
journal, June 2019
- Klein, J.; Lorke, M.; Florian, M.
- Nature Communications, Vol. 10, Issue 1
Electronic Structure and Luminescence of Quasi-Freestanding MoS 2 Nanopatches on Au(111)
journal, July 2016
- Krane, Nils; Lotze, Christian; Läger, Julia M.
- Nano Letters, Vol. 16, Issue 8
Large Spin-Orbit Splitting of Deep In-Gap Defect States of Engineered Sulfur Vacancies in Monolayer
journal, August 2019
- Schuler, Bruno; Qiu, Diana Y.; Refaely-Abramson, Sivan
- Physical Review Letters, Vol. 123, Issue 7
Optically active quantum dots in monolayer WSe2
journal, May 2015
- Srivastava, Ajit; Sidler, Meinrad; Allain, Adrien V.
- Nature Nanotechnology, Vol. 10, Issue 6
Origin of multiple peaks in the light emission spectra of a Au(111) surface induced by the scanning tunneling microscope
journal, April 2002
- Meguro, Kazuyuki; Sakamoto, Kenji; Arafune, Ryuichi
- Physical Review B, Vol. 65, Issue 16
Molecular Orbital Gates for Plasmon Excitation
journal, May 2013
- Lutz, Theresa; Große, Christoph; Dette, Christian
- Nano Letters, Vol. 13, Issue 6
Localized emission from defects in MoSe_2 layers
journal, January 2016
- Chakraborty, Chitraleema; Goodfellow, Kenneth M.; Nick Vamivakas, A.
- Optical Materials Express, Vol. 6, Issue 6
Multimodal spectromicroscopy of monolayer WS 2 enabled by ultra-clean van der Waals epitaxy
journal, July 2018
- Kastl, C.; Chen, C. T.; Koch, R. J.
- 2D Materials, Vol. 5, Issue 4
Visualization of Nanoplasmonic Coupling to Molecular Orbital in Light Emission Induced by Tunneling Electrons
journal, April 2018
- Yu, Arthur; Li, Shaowei; Wang, Hui
- Nano Letters, Vol. 18, Issue 5
Scanning Confocal Optical Microscopy and Magnetic Resonance on Single Defect Centers
journal, June 1997
- Gruber, A.
- Science, Vol. 276, Issue 5321
Scanning Tunneling Microscope-Induced Excitonic Luminescence of a Two-Dimensional Semiconductor
journal, July 2019
- Pommier, Delphine; Bretel, Rémi; López, Luis E. Parra
- Physical Review Letters, Vol. 123, Issue 2
Influence of tip geometry in light emission from the scanning tunnelling microscope
journal, June 2001
- Hoffmann, G.; Aizpurua, J.; Apell, P.
- Surface Science, Vol. 482-485
Voltage-controlled quantum light from an atomically thin semiconductor
journal, May 2015
- Chakraborty, Chitraleema; Kinnischtzke, Laura; Goodfellow, Kenneth M.
- Nature Nanotechnology, Vol. 10, Issue 6
Beyond Graphene: Progress in Novel Two-Dimensional Materials and van der Waals Solids
journal, July 2015
- Das, Saptarshi; Robinson, Joshua A.; Dubey, Madan
- Annual Review of Materials Research, Vol. 45, Issue 1
Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides
journal, March 2016
- Mak, Kin Fai; Shan, Jie
- Nature Photonics, Vol. 10, Issue 4
Light Concentration at the Nanometer Scale
journal, July 2010
- Alvarez-Puebla, Ramón; Liz-Marzán, Luis M.; García de Abajo, F. Javier
- The Journal of Physical Chemistry Letters, Vol. 1, Issue 16, p. 2428-2434
Single quantum emitters in monolayer semiconductors
journal, May 2015
- He, Yu-Ming; Clark, Genevieve; Schaibley, John R.
- Nature Nanotechnology, Vol. 10, Issue 6
Different tips for high-resolution atomic force microscopy and scanning tunneling microscopy of single molecules
journal, February 2013
- Mohn, Fabian; Schuler, Bruno; Gross, Leo
- Applied Physics Letters, Vol. 102, Issue 7
Identifying substitutional oxygen as a prolific point defect in monolayer transition metal dichalcogenides
journal, July 2019
- Barja, Sara; Refaely-Abramson, Sivan; Schuler, Bruno
- Nature Communications, Vol. 10, Issue 1
Single Photon Emission from a Plasmonic Light Source Driven by a Local Field-Induced Coulomb Blockade
journal, March 2020
- Leon, Christopher C.; Gunnarsson, Olle; de Oteyza, Dimas G.
- ACS Nano, Vol. 14, Issue 4
High-speed force sensor for force microscopy and profilometry utilizing a quartz tuning fork
journal, December 1998
- Giessibl, Franz J.
- Applied Physics Letters, Vol. 73, Issue 26
Electrofluorochromism at the single-molecule level
journal, July 2018
- Doppagne, Benjamin; Chong, Michael C.; Bulou, Hervé
- Science, Vol. 361, Issue 6399
Light emission from a scanning tunneling microscope: Fully retarded calculation
journal, October 1998
- Johansson, Peter
- Physical Review B, Vol. 58, Issue 16
Tunnelling from a Many-Particle Point of View
journal, January 1961
- Bardeen, J.
- Physical Review Letters, Vol. 6, Issue 2
Optical excitations in electron microscopy
journal, February 2010
- García de Abajo, F. J.
- Reviews of Modern Physics, Vol. 82, Issue 1
Role of tip shape in light emission from the scanning tunneling microscope
journal, July 2000
- Aizpurua, J.; Apell, S. P.; Berndt, R.
- Physical Review B, Vol. 62, Issue 3
Towards wafer-size graphene layers by atmospheric pressure graphitization of silicon carbide
journal, February 2009
- Emtsev, Konstantin V.; Bostwick, Aaron; Horn, Karsten
- Nature Materials, Vol. 8, Issue 3
Monolayer semiconductor nanocavity lasers with ultralow thresholds
journal, March 2015
- Wu, Sanfeng; Buckley, Sonia; Schaibley, John R.
- Nature, Vol. 520, Issue 7545
Exciton dynamics of C60-based single-photon emitters explored by Hanbury Brown–Twiss scanning tunnelling microscopy
journal, September 2015
- Merino, P.; Große, C.; Rosławska, A.
- Nature Communications, Vol. 6, Issue 1
Inelastic tunneling excitation of tip-induced plasmon modes on noble-metal surfaces
journal, December 1991
- Berndt, Richard; Gimzewski, James K.; Johansson, Peter
- Physical Review Letters, Vol. 67, Issue 27