Detection of thermodynamic "valley noise" in monolayer semiconductors: access to intrinsic valley relaxation timescales
Abstract
Together with charge and spin, many novel two-dimensional materials also permit information to be encoded in an electron’s valley degree of freedom—that is, in particular momentum states in the material’s Brillouin zone. With a view toward valley-based (opto)electronic technologies, the intrinsic time scales of valley scattering are therefore of fundamental interest. Here, we demonstrate an entirely noise-based approach for exploring valley dynamics in monolayer transition-metal dichalcogenide semiconductors. Exploiting their valley-specific optical selection rules, we use optical Faraday rotation to passively detect the thermodynamic fluctuations of valley polarization in a Fermi sea of resident carriers. This spontaneous “valley noise” reveals narrow Lorentzian line shapes and, therefore, long exponentially-decaying intrinsic valley relaxation. Moreover, the noise signatures validate both the relaxation times and the spectral dependence of conventional (perturbative) pump-probe measurements. These results provide a viable route toward quantitative measurements of intrinsic valley dynamics, free from any external perturbation, pumping, or excitation.
- Authors:
-
[1];
[1];
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Univ. of Washington, Seattle, WA (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1501810
- Report Number(s):
- LA-UR-18-27841
Journal ID: ISSN 2375-2548
- Grant/Contract Number:
- 89233218CNA000001
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Science Advances
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 3; Journal ID: ISSN 2375-2548
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; High Magnetic Field Science
Citation Formats
Goryca, Mateusz Marek, Crooker, Scott A., Xu, Xiaodong, Wilson, Nathan, and Dey, Prasenjit. Detection of thermodynamic "valley noise" in monolayer semiconductors: access to intrinsic valley relaxation timescales. United States: N. p., 2019.
Web. doi:10.1126/sciadv.aau4899.
Goryca, Mateusz Marek, Crooker, Scott A., Xu, Xiaodong, Wilson, Nathan, & Dey, Prasenjit. Detection of thermodynamic "valley noise" in monolayer semiconductors: access to intrinsic valley relaxation timescales. United States. https://doi.org/10.1126/sciadv.aau4899
Goryca, Mateusz Marek, Crooker, Scott A., Xu, Xiaodong, Wilson, Nathan, and Dey, Prasenjit. Fri .
"Detection of thermodynamic "valley noise" in monolayer semiconductors: access to intrinsic valley relaxation timescales". United States. https://doi.org/10.1126/sciadv.aau4899. https://www.osti.gov/servlets/purl/1501810.
@article{osti_1501810,
title = {Detection of thermodynamic "valley noise" in monolayer semiconductors: access to intrinsic valley relaxation timescales},
author = {Goryca, Mateusz Marek and Crooker, Scott A. and Xu, Xiaodong and Wilson, Nathan and Dey, Prasenjit},
abstractNote = {Together with charge and spin, many novel two-dimensional materials also permit information to be encoded in an electron’s valley degree of freedom—that is, in particular momentum states in the material’s Brillouin zone. With a view toward valley-based (opto)electronic technologies, the intrinsic time scales of valley scattering are therefore of fundamental interest. Here, we demonstrate an entirely noise-based approach for exploring valley dynamics in monolayer transition-metal dichalcogenide semiconductors. Exploiting their valley-specific optical selection rules, we use optical Faraday rotation to passively detect the thermodynamic fluctuations of valley polarization in a Fermi sea of resident carriers. This spontaneous “valley noise” reveals narrow Lorentzian line shapes and, therefore, long exponentially-decaying intrinsic valley relaxation. Moreover, the noise signatures validate both the relaxation times and the spectral dependence of conventional (perturbative) pump-probe measurements. These results provide a viable route toward quantitative measurements of intrinsic valley dynamics, free from any external perturbation, pumping, or excitation.},
doi = {10.1126/sciadv.aau4899},
journal = {Science Advances},
number = 3,
volume = 5,
place = {United States},
year = {Fri Mar 01 00:00:00 EST 2019},
month = {Fri Mar 01 00:00:00 EST 2019}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 14 works
Citation information provided by
Web of Science
Web of Science
Figures / Tables:
Fig. 1. : Sample, experimental setup, and valley noise spectrum of resident holes in monolayer WSe2. (A) Sample: A single WSe2 monolayer is sandwiched between hBN layers and electrically gated. (B) Band structure and σ± optical transitions of hole-doped monolayer WSe2. Even in thermal equilibrium, resident holes spontaneously scatter between K and K′ valleys, giving a randomly fluctuating valley polarization noise. (C) To detect valley noise, a CW probe laser is linearly polarized and focused through the sample. Thermodynamic valley fluctuations impart FR fluctuationsmore »
All figures and tables
(5 total)
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
Probing dark excitons in atomically thin semiconductors via near-field coupling to surface plasmon polaritons
journal, June 2017
- Zhou, You; Scuri, Giovanni; Wild, Dominik S.
- Nature Nanotechnology, Vol. 12, Issue 9
Many-Body Effects in Valleytronics: Direct Measurement of Valley Lifetimes in Single-Layer MoS 2
journal, December 2013
- Mai, Cong; Barrette, Andrew; Yu, Yifei
- Nano Letters, Vol. 14, Issue 1
Valley dynamics probed through charged and neutral exciton emission in monolayer
journal, August 2014
- Wang, G.; Bouet, L.; Lagarde, D.
- Physical Review B, Vol. 90, Issue 7
Optically initialized robust valley-polarized holes in monolayer WSe2
journal, November 2015
- Hsu, Wei-Ting; Chen, Yen-Lun; Chen, Chang-Hsiao
- Nature Communications, Vol. 6, Issue 1
Valley filter and valley valve in graphene
journal, February 2007
- Rycerz, A.; Tworzydło, J.; Beenakker, C. W. J.
- Nature Physics, Vol. 3, Issue 3, p. 172-175
Valley and spin dynamics in MoSe 2 two-dimensional crystals
journal, January 2014
- Kumar, Nardeep; He, Jiaqi; He, Dawei
- Nanoscale, Vol. 6, Issue 21
Transport Theory of Monolayer Transition-Metal Dichalcogenides through Symmetry
journal, July 2013
- Song, Yang; Dery, Hanan
- Physical Review Letters, Vol. 111, Issue 2
Magnetic brightening and control of dark excitons in monolayer WSe2
journal, June 2017
- Zhang, Xiao-Xiao; Cao, Ting; Lu, Zhengguang
- Nature Nanotechnology, Vol. 12, Issue 9
Spin and pseudospins in layered transition metal dichalcogenides
journal, April 2014
- Xu, Xiaodong; Yao, Wang; Xiao, Di
- Nature Physics, Vol. 10, Issue 5
Spin-noise spectroscopy: from proof of principle to applications
journal, January 2013
- Zapasskii, Valerii S.
- Advances in Optics and Photonics, Vol. 5, Issue 2
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
In-Plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules
journal, July 2017
- Wang, G.; Robert, C.; Glazov, M. M.
- Physical Review Letters, Vol. 119, Issue 4
Valley Splitting of AlAs Two-Dimensional Electrons in a Perpendicular Magnetic Field
journal, November 2002
- Shkolnikov, Y. P.; De Poortere, E. P.; Tutuc, E.
- Physical Review Letters, Vol. 89, Issue 22
k · p theory for two-dimensional transition metal dichalcogenide semiconductors
journal, April 2015
- Kormányos, Andor; Burkard, Guido; Gmitra, Martin
- 2D Materials, Vol. 2, Issue 2
Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide
journal, September 2016
- Plechinger, Gerd; Nagler, Philipp; Arora, Ashish
- Nature Communications, Vol. 7, Issue 1
Valley Susceptibility of an Interacting Two-Dimensional Electron System
journal, November 2006
- Gunawan, O.; Shkolnikov, Y. P.; Vakili, K.
- Physical Review Letters, Vol. 97, Issue 18
Intervalley dark trion states with spin lifetimes of 150 ns in
journal, June 2017
- Volmer, F.; Pissinger, S.; Ersfeld, M.
- Physical Review B, Vol. 95, Issue 23
Valley-dependent optoelectronics from inversion symmetry breaking
journal, June 2008
- Yao, Wang; Xiao, Di; Niu, Qian
- Physical Review B, Vol. 77, Issue 23
Valley-Contrasting Physics in Graphene: Magnetic Moment and Topological Transport
journal, December 2007
- Xiao, Di; Yao, Wang; Niu, Qian
- Physical Review Letters, Vol. 99, Issue 23
Long valley relaxation time of free carriers in monolayer
journal, June 2017
- Yan, Tengfei; Yang, Siyuan; Li, Dian
- Physical Review B, Vol. 95, Issue 24
Spectroscopy of spontaneous spin noise as a probe of spin dynamics and magnetic resonance
journal, September 2004
- Crooker, S. A.; Rickel, D. G.; Balatsky, A. V.
- Nature, Vol. 431, Issue 7004
Long-Lived Hole Spin/Valley Polarization Probed by Kerr Rotation in Monolayer WSe 2
journal, July 2016
- Song, Xinlin; Xie, Saien; Kang, Kibum
- Nano Letters, Vol. 16, Issue 8
Long-lived nanosecond spin relaxation and spin coherence of electrons in monolayer MoS2 and WS2
journal, August 2015
- Yang, Luyi; Sinitsyn, Nikolai A.; Chen, Weibing
- Nature Physics, Vol. 11, Issue 10
Valley Carrier Dynamics in Monolayer Molybdenum Disulfide from Helicity-Resolved Ultrafast Pump–Probe Spectroscopy
journal, November 2013
- Wang, Qinsheng; Ge, Shaofeng; Li, Xiao
- ACS Nano, Vol. 7, Issue 12
Gate-Controlled Spin-Valley Locking of Resident Carriers in Monolayers
journal, September 2017
- Dey, P.; Yang, Luyi; Robert, C.
- Physical Review Letters, Vol. 119, Issue 13
Imaging spin dynamics in monolayer WS 2 by time-resolved Kerr rotation microscopy
journal, November 2017
- McCormick, Elizabeth J.; Newburger, Michael J.; Luo, Yunqiu Kelly
- 2D Materials, Vol. 5, Issue 1
Valley-selective circular dichroism of monolayer molybdenum disulphide
journal, January 2012
- Cao, Ting; Wang, Gang; Han, Wenpeng
- Nature Communications, Vol. 3, Issue 1
Valleytronics in 2D materials
journal, August 2016
- Schaibley, John R.; Yu, Hongyi; Clark, Genevieve
- Nature Reviews Materials, Vol. 1, Issue 11
Spin-valley relaxation and quantum transport regimes in two-dimensional transition-metal dichalcogenides
journal, December 2014
- Ochoa, Hector; Finocchiaro, Francesca; Guinea, Francisco
- Physical Review B, Vol. 90, Issue 23
Observation of ultralong valley lifetime in WSe 2 /MoS 2 heterostructures
journal, July 2017
- Kim, Jonghwan; Jin, Chenhao; Chen, Bin
- Science Advances, Vol. 3, Issue 7
Spin noise of conduction electrons in -type bulk GaAs
journal, January 2009
- Crooker, Scott A.; Cheng, Lili; Smith, Darryl L.
- Physical Review B, Vol. 79, Issue 3
The fluctuation-dissipation theorem
journal, January 1966
- Kubo, R.
- Reports on Progress in Physics, Vol. 29, Issue 1
Field-induced polarization of Dirac valleys in bismuth
journal, October 2011
- Zhu, Zengwei; Collaudin, Aurélie; Fauqué, Benoît
- Nature Physics, Vol. 8, Issue 1
Generation, transport and detection of valley-polarized electrons in diamond
journal, July 2013
- Isberg, Jan; Gabrysch, Markus; Hammersberg, Johan
- Nature Materials, Vol. 12, Issue 8
Control of valley polarization in monolayer MoS2 by optical helicity
journal, June 2012
- Mak, Kin Fai; He, Keliang; Shan, Jie
- Nature Nanotechnology, Vol. 7, Issue 8
Valley depolarization due to intervalley and intravalley electron-hole exchange interactions in monolayer
journal, May 2014
- Yu, T.; Wu, M. W.
- Physical Review B, Vol. 89, Issue 20
Twist-tailoring Coulomb correlations in van der Waals homobilayers
text, January 2020
- Merkl, Philipp; Mooshammer, Fabian; Brem, Samuel
- Universität Regensburg
Spin noise spectroscopy in GaAs
other, January 2005
- Oestreich, Michael; Römer, M.; Haug, Rolf J.
- College Park, MD : American Physical Society
Valley Dependent Optoelectronics from Inversion Symmetry Breaking
text, January 2007
- Yao, Wang; Xiao, Di; Niu, Qian
- arXiv
Valley contrasting physics in graphene: magnetic moment and topological transport
text, January 2007
- Xiao, Di; Yao, Wang; Niu, Qian
- arXiv
Valley-based noise-resistant quantum computation using Si quantum dots
text, January 2011
- Culcer, Dimitrie; Saraiva, A. L.; Koiller, Belita
- arXiv
Valley Carrier Dynamics in Monolayer Molybdenum Disulphide from Helicity Resolved Ultrafast Pump-probe Spectroscopy
text, January 2013
- Wang, Qinsheng; Ge, Shaofeng; Li, Xiao
- arXiv
k.p theory for two-dimensional transition metal dichalcogenide semiconductors
text, January 2014
- Kormányos, Andor; Burkard, Guido; Gmitra, Martin
- arXiv
Long-lived nanosecond spin relaxation and spin coherence of electrons in monolayer MoS_2 and WS_2
text, January 2015
- Yang, Luyi; Sinitsyn, Nikolai A.; Chen, Weibing
- arXiv
Imaging Spin Dynamics in Monolayer WS2 by Time-Resolved Kerr Rotation Microscopy
text, January 2016
- Bushong, Elizabeth J.; Newburger, Michael; McCreary, Kathleen M.
- arXiv
Magnetic brightening and control of dark excitons in monolayer WSe2
text, January 2016
- Zhang, Xiao-Xiao; Cao, Ting; Lu, Zhengguang
- arXiv
In-plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules
text, January 2017
- Wang, G.; Robert, C.; Glazov, M. M.
- arXiv
Valley splitting of AlAs two-dimensional electrons in a perpendicular magnetic field
text, January 2002
- Shkolnikov, Y. P.; De Poortere, E. P.; Tutuc, E.
- arXiv
Valley susceptibility of an interacting two-dimensional electron system
text, January 2006
- Gunawan, O.; Shkolnikov, Y. P.; Vakili, K.
- arXiv
Valley filter and valley valve in graphene
text, January 2006
- Rycerz, A.; Tworzydlo, J.; Beenakker, C. W. J.
- arXiv
Long-Lived Hole Spin/Valley Polarization Probed by Kerr Rotation in Monolayer WSe 2
journal, July 2016
- Song, Xinlin; Xie, Saien; Kang, Kibum
- Nano Letters, Vol. 16, Issue 8
Many-Body Effects in Valleytronics: Direct Measurement of Valley Lifetimes in Single-Layer MoS 2
journal, December 2013
- Mai, Cong; Barrette, Andrew; Yu, Yifei
- Nano Letters, Vol. 14, Issue 1
Valley-selective circular dichroism of monolayer molybdenum disulphide
journal, January 2012
- Cao, Ting; Wang, Gang; Han, Wenpeng
- Nature Communications, Vol. 3, Issue 1
Optically initialized robust valley-polarized holes in monolayer WSe2
journal, November 2015
- Hsu, Wei-Ting; Chen, Yen-Lun; Chen, Chang-Hsiao
- Nature Communications, Vol. 6, Issue 1
Generation, transport and detection of valley-polarized electrons in diamond
journal, July 2013
- Isberg, Jan; Gabrysch, Markus; Hammersberg, Johan
- Nature Materials, Vol. 12, Issue 8
Valley-Based Noise-Resistant Quantum Computation Using Si Quantum Dots
journal, March 2012
- Culcer, Dimitrie; Saraiva, A. L.; Koiller, Belita
- Physical Review Letters, Vol. 108, Issue 12
Optical Spectroscopy of Spin Noise
journal, April 2013
- Zapasskii, V. S.; Greilich, A.; Crooker, S. A.
- Physical Review Letters, Vol. 110, Issue 17
Long-Lived Valley Polarization of Intravalley Trions in Monolayer
journal, December 2016
- Singh, Akshay; Tran, Kha; Kolarczik, Mirco
- Physical Review Letters, Vol. 117, Issue 25
Spin Noise Spectroscopy in GaAs
journal, November 2005
- Oestreich, M.; Römer, M.; Haug, R. J.
- Physical Review Letters, Vol. 95, Issue 21
"Listening" to the spin noise of conduction electrons in bulk n:GaAs
text, January 2009
- Crooker, S. A.; Cheng, L.; Smith, D. L.
- arXiv
Spin noise spectroscopy: From proof of the principle to applications
preprint, January 2013
- Zapasskii, Valerii S.
- arXiv
Valley Carrier Dynamics in Monolayer Molybdenum Disulphide from Helicity Resolved Ultrafast Pump-probe Spectroscopy
text, January 2013
- Wang, Qinsheng; Ge, Shaofeng; Li, Xiao
- arXiv
Brightening of dark excitons in monolayers of semiconducting transition metal dichalcogenides
text, January 2016
- Molas, M. R.; Faugeras, C.; Slobodeniuk, A. O.
- arXiv
Inter-valley dark trion states with spin lifetimes of 150 ns in WSe$_2$
text, January 2017
- Volmer, F.; Pissinger, S.; Ersfeld, M.
- arXiv
Valley splitting of AlAs two-dimensional electrons in a perpendicular magnetic field
text, January 2002
- Shkolnikov, Y. P.; De Poortere, E. P.; Tutuc, E.
- arXiv
Works referencing / citing this record:
Detection and amplification of spin noise using scattered laser light in a quantum-dot microcavity
journal, January 2020
- Kamenskii, A. N.; Petrov, M. Yu.; Kozlov, G. G.
- Physical Review B, Vol. 101, Issue 4
Detection and amplification of spin noise using scattered laser light in a quantum-dot microcavity
text, January 2019
- Kamenskii, A. N.; Petrov, M. Yu.; Kozlov, G. G.
- arXiv
Figures / Tables found in this record:
Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.