Polariton hyperspectral imaging of two-dimensional semiconductor crystals
Abstract
Atomically thin crystals of transition metal dichalcogenides (TMDs) host excitons with strong binding energies and sizable light-matter interactions. Coupled to optical cavities, monolayer TMDs routinely reach the regime of strong light-matter coupling, where excitons and photons admix coherently to form polaritons up to room temperature. Here, we explore the two-dimensional nature of TMD polaritons with scanning-cavity hyperspectral imaging. We record a spatial map of polariton properties of extended WS2 monolayers coupled to a tunable micro cavity in the strong coupling regime, and correlate it with maps of exciton extinction and fluorescence taken from the same fake with the cavity. We find a high level of homogeneity, and show that polariton splitting variations are correlated with intrinsic exciton properties such as oscillator strength and linewidth. Moreover, we observe a deviation from thermal equilibrium in the resonant polariton population, which we ascribe to non-Markovian polariton-phonon coupling. Our measurements reveal a promisingly consistent polariton landscape, and highlight the importance of phonons for future polaritonic devices.
- Authors:
-
[1];
[6]
- Ludwig Maximilian Univ. of Munich, Munich (Germany). Faculty of Physics; Max Planck Inst. fuer Quantenoptik, Garching (Germany)
- Ludwig Maximilian Univ. of Munich, Munich (Germany). Faculty for Physics. Center for NanoScience (CeNS). Munich Quantum Center
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Materials Physics and Applications Division. Materials Synthesis and Integrated Devices
- Univ. of Bremen (Germany). Inst. for Theoretical Physics
- Ludwig Maximilian Univ. of Munich, Munich (Germany). Faculty of Physics; Max Planck Inst. fuer Quantenoptik, Garching (Germany)
- Karlsruhe Inst. of Technology (KIT) (Germany). Physikalisches Inst.
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1624493
- Grant/Contract Number:
- AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Scientific Reports
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2045-2322
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Science & Technology - Other Topics
Citation Formats
Gebhardt, Christian, Förg, Michael, Yamaguchi, Hisato, Bilgin, Ismail, Mohite, Aditya D., Gies, Christopher, Florian, Matthias, Hartmann, Malte, Hänsch, Theodor W., Högele, Alexander, and Hunger, David. Polariton hyperspectral imaging of two-dimensional semiconductor crystals. United States: N. p., 2019.
Web. doi:10.1038/s41598-019-50316-8.
Gebhardt, Christian, Förg, Michael, Yamaguchi, Hisato, Bilgin, Ismail, Mohite, Aditya D., Gies, Christopher, Florian, Matthias, Hartmann, Malte, Hänsch, Theodor W., Högele, Alexander, & Hunger, David. Polariton hyperspectral imaging of two-dimensional semiconductor crystals. United States. https://doi.org/10.1038/s41598-019-50316-8
Gebhardt, Christian, Förg, Michael, Yamaguchi, Hisato, Bilgin, Ismail, Mohite, Aditya D., Gies, Christopher, Florian, Matthias, Hartmann, Malte, Hänsch, Theodor W., Högele, Alexander, and Hunger, David. Tue .
"Polariton hyperspectral imaging of two-dimensional semiconductor crystals". United States. https://doi.org/10.1038/s41598-019-50316-8. https://www.osti.gov/servlets/purl/1624493.
@article{osti_1624493,
title = {Polariton hyperspectral imaging of two-dimensional semiconductor crystals},
author = {Gebhardt, Christian and Förg, Michael and Yamaguchi, Hisato and Bilgin, Ismail and Mohite, Aditya D. and Gies, Christopher and Florian, Matthias and Hartmann, Malte and Hänsch, Theodor W. and Högele, Alexander and Hunger, David},
abstractNote = {Atomically thin crystals of transition metal dichalcogenides (TMDs) host excitons with strong binding energies and sizable light-matter interactions. Coupled to optical cavities, monolayer TMDs routinely reach the regime of strong light-matter coupling, where excitons and photons admix coherently to form polaritons up to room temperature. Here, we explore the two-dimensional nature of TMD polaritons with scanning-cavity hyperspectral imaging. We record a spatial map of polariton properties of extended WS2 monolayers coupled to a tunable micro cavity in the strong coupling regime, and correlate it with maps of exciton extinction and fluorescence taken from the same fake with the cavity. We find a high level of homogeneity, and show that polariton splitting variations are correlated with intrinsic exciton properties such as oscillator strength and linewidth. Moreover, we observe a deviation from thermal equilibrium in the resonant polariton population, which we ascribe to non-Markovian polariton-phonon coupling. Our measurements reveal a promisingly consistent polariton landscape, and highlight the importance of phonons for future polaritonic devices.},
doi = {10.1038/s41598-019-50316-8},
journal = {Scientific Reports},
number = 1,
volume = 9,
place = {United States},
year = {Tue Sep 24 00:00:00 EDT 2019},
month = {Tue Sep 24 00:00:00 EDT 2019}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Coupled Spin and Valley Physics in Monolayers of and Other Group-VI Dichalcogenides
journal, May 2012
- Xiao, Di; Liu, Gui-Bin; Feng, Wanxiang
- Physical Review Letters, Vol. 108, Issue 19
Cavity-enhanced Raman microscopy of individual carbon nanotubes
journal, July 2016
- Hümmer, Thomas; Noe, Jonathan; Hofmann, Matthias S.
- Nature Communications, Vol. 7, Issue 1
Controlling the interactions between polaritons and molecular vibrations in strongly coupled organic semiconductor microcavities
journal, July 2008
- Chovan, J.; Perakis, I. E.; Ceccarelli, S.
- Physical Review B, Vol. 78, Issue 4
Fermi polaron-polaritons in charge-tunable atomically thin semiconductors
journal, October 2016
- Sidler, Meinrad; Back, Patrick; Cotlet, Ovidiu
- Nature Physics, Vol. 13, Issue 3
Emerging Photoluminescence in Monolayer MoS2
journal, April 2010
- Splendiani, Andrea; Sun, Liang; Zhang, Yuanbo
- Nano Letters, Vol. 10, Issue 4, p. 1271-1275
Imaging exciton–polariton transport in MoSe2 waveguides
journal, May 2017
- Hu, F.; Luan, Y.; Scott, M. E.
- Nature Photonics, Vol. 11, Issue 6
Cavity-enhanced Raman microscopy of individual carbon nanotubes
text, January 2016
- Hümmer, T.; Noe, J.; Hofmann, M. S.
- Karlsruhe
Room-temperature Tamm-plasmon exciton-polaritons with a WSe2 monolayer
journal, October 2016
- Lundt, Nils; Klembt, Sebastian; Cherotchenko, Evgeniia
- Nature Communications, Vol. 7, Issue 1
Brightening of dark excitons in monolayers of semiconducting transition metal dichalcogenides
journal, January 2017
- Molas, M. R.; Faugeras, C.; Slobodeniuk, A. O.
- 2D Materials, Vol. 4, Issue 2
Identification of excitons, trions and biexcitons in single-layer WS 2 : Identification of excitons, trions and biexcitons in single-layer WS
journal, July 2015
- Plechinger, Gerd; Nagler, Philipp; Kraus, Julia
- physica status solidi (RRL) - Rapid Research Letters, Vol. 9, Issue 8
Strain engineering in monolayer WS 2 , MoS 2 , and the WS 2 /MoS 2 heterostructure
journal, October 2016
- He, Xin; Li, Hai; Zhu, Zhiyong
- Applied Physics Letters, Vol. 109, Issue 17
Direct observation of strong light-exciton coupling in thin WS_2 flakes
journal, January 2016
- Wang, Qi; Sun, Liaoxin; Zhang, Bo
- Optics Express, Vol. 24, Issue 7
Quantum well excitons in semiconductor microcavities: Unified treatment of weak and strong coupling regimes
journal, March 1995
- Savona, V.; Andreani, L. C.; Schwendimann, P.
- Solid State Communications, Vol. 93, Issue 9
Atomically Thin A New Direct-Gap Semiconductor
journal, September 2010
- Mak, Kin Fai; Lee, Changgu; Hone, James
- Physical Review Letters, Vol. 105, Issue 13, Article No.136805
Room-temperature exciton-polaritons with two-dimensional WS2
journal, September 2016
- Flatten, L. C.; He, Z.; Coles, D. M.
- Scientific Reports, Vol. 6, Issue 1
Coulomb engineering of the bandgap and excitons in two-dimensional materials
journal, May 2017
- Raja, Archana; Chaves, Andrey; Yu, Jaeeun
- Nature Communications, Vol. 8, Issue 1
Bandgap Engineering of Strained Monolayer and Bilayer MoS2
journal, July 2013
- Conley, Hiram J.; Wang, Bin; Ziegler, Jed I.
- Nano Letters, Vol. 13, Issue 8, p. 3626-3630
Monolayer excitonic laser
journal, October 2015
- Ye, Yu; Wong, Zi Jing; Lu, Xiufang
- Nature Photonics, Vol. 9, Issue 11
Polariton quantum blockade in a photonic dot
journal, May 2006
- Verger, A.; Ciuti, C.; Carusotto, I.
- Physical Review B, Vol. 73, Issue 19
Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides
journal, November 2016
- Selig, Malte; Berghäuser, Gunnar; Raja, Archana
- Nature Communications, Vol. 7, Issue 1
Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
journal, August 2014
- Ugeda, Miguel M.; Bradley, Aaron J.; Shi, Su-Fei
- Nature Materials, Vol. 13, Issue 12
Opto-valleytronic imaging of atomically thin semiconductors
journal, January 2017
- Neumann, Andre; Lindlau, Jessica; Colombier, Léo
- Nature Nanotechnology, Vol. 12, Issue 4
Phonons in single-layer and few-layer MoS and WS
journal, October 2011
- Molina-Sánchez, A.; Wirtz, L.
- Physical Review B, Vol. 84, Issue 15
Physics and applications of exciton–polariton lasers
journal, September 2016
- Fraser, Michael D.; Höfling, Sven; Yamamoto, Yoshihisa
- Nature Materials, Vol. 15, Issue 10
Topological Polaritons
journal, July 2015
- Karzig, Torsten; Bardyn, Charles-Edouard; Lindner, Netanel H.
- Physical Review X, Vol. 5, Issue 3
Intrinsic transport properties of electrons and holes in monolayer transition-metal dichalcogenides
journal, July 2014
- Jin, Zhenghe; Li, Xiaodong; Mullen, Jeffrey T.
- Physical Review B, Vol. 90, Issue 4
Laser micro-fabrication of concave, low-roughness features in silica
journal, March 2012
- Hunger, D.; Deutsch, C.; Barbour, R. J.
- AIP Advances, Vol. 2, Issue 1
Efficient Excitonic Photoluminescence in Direct and Indirect Band Gap Monolayer MoS 2
journal, September 2015
- Steinhoff, A.; Kim, J. -H.; Jahnke, F.
- Nano Letters, Vol. 15, Issue 10
Quantum correlations of light and matter through environmental transitions
journal, January 2016
- Iles-Smith, Jake; Nazir, Ahsan
- Optica, Vol. 3, Issue 2
Coulomb engineering of the bandgap and excitons in two-dimensional materials
text, January 2017
- Raja, Archana; Chaves, Andrey; Yu, Jaeeun
- Universität Regensburg
Photonic Architectures for Equilibrium High-Temperature Bose-Einstein Condensation in Dichalcogenide Monolayers
journal, December 2014
- Jiang, Jian-Hua; John, Sajeev
- Scientific Reports, Vol. 4, Issue 1
Nano-optical imaging of waveguide modes revealing light-exciton interactions
journal, August 2016
- Fei, Z.; Scott, M. E.; Gosztola, D. J.
- Physical Review B, Vol. 94, Issue 8
Electrical Tuning of Exciton Binding Energies in Monolayer
journal, September 2015
- Chernikov, Alexey; van der Zande, Arend M.; Hill, Heather M.
- Physical Review Letters, Vol. 115, Issue 12
Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides
conference, February 2017
- Selig, Malte; Berghäuser, Gunnar; Raja, Archana
- SPIE OPTO, SPIE Proceedings
Exciton–polaritons in van der Waals heterostructures embedded in tunable microcavities
journal, October 2015
- Dufferwiel, S.; Schwarz, S.; Withers, F.
- Nature Communications, Vol. 6, Issue 1
A scanning cavity microscope
journal, June 2015
- Mader, Matthias; Reichel, Jakob; Hänsch, Theodor W.
- Nature Communications, Vol. 6, Issue 1
Stimulated Scattering and Lasing of Intersubband Cavity Polaritons
journal, March 2009
- De Liberato, Simone; Ciuti, Cristiano
- Physical Review Letters, Vol. 102, Issue 13
Strong light–matter coupling in two-dimensional atomic crystals
journal, December 2014
- Liu, Xiaoze; Galfsky, Tal; Sun, Zheng
- Nature Photonics, Vol. 9, Issue 1
The Dielectric Impact of Layer Distances on Exciton and Trion Binding Energies in van der Waals Heterostructures
journal, March 2018
- Florian, Matthias; Hartmann, Malte; Steinhoff, Alexander
- Nano Letters, Vol. 18, Issue 4
Coulomb engineering of the bandgap and excitons in two-dimensional materials
text, January 2017
- Chernikov, Alexey; Raja, Archana; Chaves, Andrey
- Universität Regensburg
Purcell-Enhanced Single-Photon Emission from Nitrogen-Vacancy Centers Coupled to a Tunable Microcavity
text, January 2016
- Kaupp, Hanno; Hümmer, Thomas; Mader, Matthias
- Karlsruhe
A fiber Fabry–Perot cavity with high finesse
journal, June 2010
- Hunger, D.; Steinmetz, T.; Colombe, Y.
- New Journal of Physics, Vol. 12, Issue 6
Excitonic luminescence upconversion in a two-dimensional semiconductor
journal, December 2015
- Jones, Aaron M.; Yu, Hongyi; Schaibley, John R.
- Nature Physics, Vol. 12, Issue 4
Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer
journal, August 2014
- Chernikov, Alexey; Berkelbach, Timothy C.; Hill, Heather M.
- Physical Review Letters, Vol. 113, Issue 7
Measurement of the optical dielectric function of monolayer transition-metal dichalcogenides: , , , and
journal, November 2014
- Li, Yilei; Chernikov, Alexey; Zhang, Xian
- Physical Review B, Vol. 90, Issue 20
Purcell-Enhanced Single-Photon Emission from Nitrogen-Vacancy Centers Coupled to a Tunable Microcavity
journal, November 2016
- Kaupp, Hanno; Hümmer, Thomas; Mader, Matthias
- Physical Review Applied, Vol. 6, Issue 5
Exciton-phonon scattering and photoexcitation dynamics in -aggregate microcavities
journal, January 2009
- Michetti, Paolo; La Rocca, Giuseppe C.
- Physical Review B, Vol. 79, Issue 3
Two-Dimensional Heterojunctions from Nonlocal Manipulations of the Interactions
journal, March 2016
- Rösner, M.; Steinke, C.; Lorke, M.
- Nano Letters, Vol. 16, Issue 4
Laser micro-fabrication of concave, low-roughness features in silica
preprint, January 2011
- Hunger, David; Deutsch, Christian; Barbour, Russell J.
- arXiv
Topological Polaritons
text, January 2014
- Karzig, Torsten; Bardyn, Charles-Edouard; Lindner, Netanel
- arXiv
A Scanning Cavity Microscope
text, January 2014
- Mader, Matthias; Reichel, Jakob; Hänsch, Theodor W.
- arXiv
Photonic Architectures for Equilibrium High-Temperature Bose-Einstein Condensation in Dichalcogenide Monolayers
text, January 2014
- Jiang, Jian-Hua; John, Sajeev
- arXiv
Quantum correlations of light and matter through environmental transitions
text, January 2014
- Iles-Smith, Jake; Nazir, Ahsan
- arXiv
Fermi polaron-polaritons in charge-tunable atomically thin semiconductors
text, January 2016
- Sidler, Meinrad; Back, Patrick; Cotlet, Ovidiu
- arXiv
The dielectric impact of layer distances on exciton and trion binding energies in van der Waals heterostructures
text, January 2017
- Florian, M.; Hartmann, M.; Steinhoff, A.
- arXiv
Polariton quantum blockade in a photonic dot
text, January 2005
- Verger, Arnaud; Ciuti, Cristiano; Carusotto, Iacopo
- arXiv