Many-body effects in nonlinear optical responses of 2D layered semiconductors

Aivazian, Grant; Yu, Hongyi; Wu, Sanfeng; Yan, Jiaqiang; Mandrus, David G.; Cobden, David; Yao, Wang; Xu, Xiaodong

doi:10.1088/2053-1583/aa56f1

Title: Many-body effects in nonlinear optical responses of 2D layered semiconductors

Journal Article · Thu Jan 05 00:00:00 EST 2017 · 2D Materials

DOI:https://doi.org/10.1088/2053-1583/aa56f1· OSTI ID:1376528

Aivazian, Grant ^[1]; Yu, Hongyi ^[2]; Wu, Sanfeng ^[1]; Yan, Jiaqiang ^[3]; Mandrus, David G. ^[3]; Cobden, David ^[1]; Yao, Wang ^[2]; Xu, Xiaodong ^[1]

Univ. of Washington, Seattle, WA (United States)
Univ. of Hong Kong (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

We performed ultrafast degenerate pump-probe spectroscopy on monolayer WSe2 near its exciton resonance. The observed differential reflectance signals exhibit signatures of strong many-body interactions including the exciton-exciton interaction and free carrier induced band gap renormalization. The exciton-exciton interaction results in a resonance blue shift which lasts for the exciton lifetime (several ps), while the band gap renormalization manifests as a resonance red shift with several tens ps lifetime. Our model based on the many-body interactions for the nonlinear optical susceptibility ts well the experimental observations. The power dependence of the spectra shows that with the increase of pump power, the exciton population increases linearly and then saturates, while the free carrier density increases superlinearly, implying that exciton Auger recombination could be the origin of these free carriers. Our model demonstrates a simple but efficient method for quantitatively analyzing the spectra, and indicates the important role of Coulomb interactions in nonlinear optical responses of such 2D materials.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1376528

Journal Information:: 2D Materials, Vol. 4, Issue 2; ISSN 2053-1583

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 33 works

Citation information provided by
Web of Science

References (64)

Atomically Thin ${MoS}_{2}$ A New Direct-Gap Semiconductor Mak, Kin Fai; Lee, Changgu; Hone, James Physical Review Letters, Vol. 105, Issue 13, Article No.136805 https://doi.org/10.1103/PhysRevLett.105.136805	journal	September 2010
Emerging Photoluminescence in Monolayer MoS₂ Splendiani, Andrea; Sun, Liang; Zhang, Yuanbo Nano Letters, Vol. 10, Issue 4, p. 1271-1275 https://doi.org/10.1021/nl903868w	journal	April 2010
Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer ${WS}_{2}$ Chernikov, Alexey; Berkelbach, Timothy C.; Hill, Heather M. Physical Review Letters, Vol. 113, Issue 7 https://doi.org/10.1103/PhysRevLett.113.076802	journal	August 2014
Tightly Bound Excitons in Monolayer ${WSe}_{2}$ He, Keliang; Kumar, Nardeep; Zhao, Liang Physical Review Letters, Vol. 113, Issue 2 https://doi.org/10.1103/PhysRevLett.113.026803	journal	July 2014
Direct Imaging of Band Profile in Single Layer MoS ₂ on Graphite: Quasiparticle Energy Gap, Metallic Edge States, and Edge Band Bending Zhang, Chendong; Johnson, Amber; Hsu, Chang-Lung Nano Letters, Vol. 14, Issue 5 https://doi.org/10.1021/nl501133c	journal	April 2014
Probing excitonic dark states in single-layer tungsten disulphide Ye, Ziliang; Cao, Ting; O’Brien, Kevin Nature, Vol. 513, Issue 7517 https://doi.org/10.1038/nature13734	journal	August 2014
Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor Ugeda, Miguel M.; Bradley, Aaron J.; Shi, Su-Fei Nature Materials, Vol. 13, Issue 12 https://doi.org/10.1038/nmat4061	journal	August 2014
Measurement of high exciton binding energy in the monolayer transition-metal dichalcogenides WS2 and WSe2 Hanbicki, A. T.; Currie, M.; Kioseoglou, G. Solid State Communications, Vol. 203 https://doi.org/10.1016/j.ssc.2014.11.005	journal	February 2015
Giant Enhancement of the Optical Second-Harmonic Emission of ${WSe}_{2}$ Monolayers by Laser Excitation at Exciton Resonances Wang, G.; Marie, X.; Gerber, I. Physical Review Letters, Vol. 114, Issue 9 https://doi.org/10.1103/PhysRevLett.114.097403	journal	March 2015
Exciton Binding Energy of Monolayer WS2 Zhu, Bairen; Chen, Xi; Cui, Xiaodong Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep09218	journal	March 2015
Tightly bound trions in monolayer MoS2 Mak, Kin Fai; He, Keliang; Lee, Changgu Nature Materials, Vol. 12, Issue 3 https://doi.org/10.1038/nmat3505	journal	December 2012
Electrical control of neutral and charged excitons in a monolayer semiconductor Ross, Jason S.; Wu, Sanfeng; Yu, Hongyi Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms2498	journal	February 2013
Optical generation of excitonic valley coherence in monolayer WSe2 Jones, Aaron M.; Yu, Hongyi; Ghimire, Nirmal J. Nature Nanotechnology, Vol. 8, Issue 9 https://doi.org/10.1038/nnano.2013.151	journal	August 2013
Coupled Spin and Valley Physics in Monolayers of ${MoS}_{2}$ and Other Group-VI Dichalcogenides Xiao, Di; Liu, Gui-Bin; Feng, Wanxiang Physical Review Letters, Vol. 108, Issue 19 https://doi.org/10.1103/PhysRevLett.108.196802	journal	May 2012
Spin and pseudospins in layered transition metal dichalcogenides Xu, Xiaodong; Yao, Wang; Xiao, Di Nature Physics, Vol. 10, Issue 5 https://doi.org/10.1038/nphys2942	journal	April 2014
Valley-selective circular dichroism of monolayer molybdenum disulphide Cao, Ting; Wang, Gang; Han, Wenpeng Nature Communications, Vol. 3, Issue 1 https://doi.org/10.1038/ncomms1882	journal	January 2012
Valley polarization in MoS2 monolayers by optical pumping Zeng, Hualing; Dai, Junfeng; Yao, Wang Nature Nanotechnology, Vol. 7, Issue 8 https://doi.org/10.1038/nnano.2012.95	journal	June 2012
Control of valley polarization in monolayer MoS2 by optical helicity Mak, Kin Fai; He, Keliang; Shan, Jie Nature Nanotechnology, Vol. 7, Issue 8 https://doi.org/10.1038/nnano.2012.96	journal	June 2012
Excitonic luminescence upconversion in a two-dimensional semiconductor Jones, Aaron M.; Yu, Hongyi; Schaibley, John R. Nature Physics, Vol. 12, Issue 4 https://doi.org/10.1038/nphys3604	journal	December 2015
Electrical Tuning of Exciton Binding Energies in Monolayer ${WS}_{2}$ Chernikov, Alexey; van der Zande, Arend M.; Hill, Heather M. Physical Review Letters, Vol. 115, Issue 12 https://doi.org/10.1103/PhysRevLett.115.126802	journal	September 2015
Population inversion and giant bandgap renormalization in atomically thin WS2 layers Chernikov, Alexey; Ruppert, Claudia; Hill, Heather M. Nature Photonics, Vol. 9, Issue 7 https://doi.org/10.1038/nphoton.2015.104	journal	June 2015
Photo-Induced Bandgap Renormalization Governs the Ultrafast Response of Single-Layer MoS ₂ Pogna, Eva A. A.; Marsili, Margherita; De Fazio, Domenico ACS Nano, Vol. 10, Issue 1 https://doi.org/10.1021/acsnano.5b06488	journal	December 2015
Exciton dynamics in atomically thin MoS $_{2}$ : Interexcitonic interaction and broadening kinetics Sim, Sangwan; Park, Jusang; Song, Jeong-Gyu Physical Review B, Vol. 88, Issue 7 https://doi.org/10.1103/PhysRevB.88.075434	journal	August 2013
Exciton Dynamics in Suspended Monolayer and Few-Layer MoS ₂ 2D Crystals Shi, Hongyan; Yan, Rusen; Bertolazzi, Simone ACS Nano, Vol. 7, Issue 2 https://doi.org/10.1021/nn303973r	journal	January 2013
Many-Body Effects in Valleytronics: Direct Measurement of Valley Lifetimes in Single-Layer MoS ₂ Mai, Cong; Barrette, Andrew; Yu, Yifei Nano Letters, Vol. 14, Issue 1 https://doi.org/10.1021/nl403742j	journal	December 2013
Valley Carrier Dynamics in Monolayer Molybdenum Disulfide from Helicity-Resolved Ultrafast Pump–Probe Spectroscopy Wang, Qinsheng; Ge, Shaofeng; Li, Xiao ACS Nano, Vol. 7, Issue 12 https://doi.org/10.1021/nn405419h	journal	November 2013
Ultrafast valley relaxation dynamics in monolayer ${MoS}_{2}$ probed by nonequilibrium optical techniques Dal Conte, S.; Bottegoni, F.; Pogna, E. A. A. Physical Review B, Vol. 92, Issue 23 https://doi.org/10.1103/PhysRevB.92.235425	journal	December 2015
Population Pulsation Resonances of Excitons in Monolayer ${MoSe}_{2}$ with Sub- $1 μ eV$ Linewidths Schaibley, John R.; Karin, Todd; Yu, Hongyi Physical Review Letters, Vol. 114, Issue 13 https://doi.org/10.1103/PhysRevLett.114.137402	journal	April 2015
Basic mechanisms of the optical nonlinearities of semiconductors near the band edge Haug, H.; Schmitt-Rink, S. Journal of the Optical Society of America B, Vol. 2, Issue 7 https://doi.org/10.1364/JOSAB.2.001135	journal	January 1985
Experimental Evidence for Dark Excitons in Monolayer ${WSe}_{2}$ Zhang, Xiao-Xiao; You, Yumeng; Zhao, Shu Yang Frank Physical Review Letters, Vol. 115, Issue 25 https://doi.org/10.1103/PhysRevLett.115.257403	journal	December 2015
Many-body effects in $n$ -type Si inversion layers. I. Effects in the lowest subband Vinter, B. Physical Review B, Vol. 13, Issue 10 https://doi.org/10.1103/PhysRevB.13.4447	journal	May 1976
Dirac cones and Dirac saddle points of bright excitons in monolayer transition metal dichalcogenides Yu, Hongyi; Liu, Gui-Bin; Gong, Pu Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4876	journal	May 2014
Coherent Electronic Coupling in Atomically Thin ${MoSe}_{2}$ Singh, Akshay; Moody, Galan; Wu, Sanfeng Physical Review Letters, Vol. 112, Issue 21 https://doi.org/10.1103/PhysRevLett.112.216804	journal	May 2014
Exciton band structure in layered MoSe ₂ : from a monolayer to the bulk limit Arora, Ashish; Nogajewski, Karol; Molas, Maciej Nanoscale, Vol. 7, Issue 48 https://doi.org/10.1039/C5NR06782K	journal	January 2015
Exciton radiative lifetime in transition metal dichalcogenide monolayers Robert, C.; Lagarde, D.; Cadiz, F. Physical Review B, Vol. 93, Issue 20 https://doi.org/10.1103/PhysRevB.93.205423	journal	May 2016
Auger recombination of dark excitons in WS ₂ and WSe ₂ monolayers Danovich, Mark; Zólyomi, Viktor; Fal’ko, Vladimir I. 2D Materials, Vol. 3, Issue 3 https://doi.org/10.1088/2053-1583/3/3/035011	journal	August 2016
Direct measurement of exciton valley coherence in monolayer WSe2 Hao, Kai; Moody, Galan; Wu, Fengcheng Nature Physics, Vol. 12, Issue 7 https://doi.org/10.1038/nphys3674	journal	February 2016
Exciton-exciton annihilation in MoSe $_{2}$ monolayers Kumar, Nardeep; Cui, Qiannan; Ceballos, Frank Physical Review B, Vol. 89, Issue 12 https://doi.org/10.1103/PhysRevB.89.125427	journal	March 2014
Observation of Rapid Exciton–Exciton Annihilation in Monolayer Molybdenum Disulfide Sun, Dezheng; Rao, Yi; Reider, Georg A. Nano Letters, Vol. 14, Issue 10 https://doi.org/10.1021/nl5021975	journal	September 2014
Nonlinear photoluminescence in atomically thin layered ${WSe}_{2}$ arising from diffusion-assisted exciton-exciton annihilation Mouri, Shinichiro; Miyauchi, Yuhei; Toh, Minglin Physical Review B, Vol. 90, Issue 15 https://doi.org/10.1103/PhysRevB.90.155449	journal	October 2014
Fundamental limits of exciton-exciton annihilation for light emission in transition metal dichalcogenide monolayers Yu, Yiling; Yu, Yifei; Xu, Chao Physical Review B, Vol. 93, Issue 20 https://doi.org/10.1103/PhysRevB.93.201111	journal	May 2016
Resonant internal quantum transitions and femtosecond radiative decay of excitons in monolayer WSe2 Poellmann, C.; Steinleitner, P.; Leierseder, U. Nature Materials, Vol. 14, Issue 9 https://doi.org/10.1038/nmat4356	journal	July 2015
Biexciton, single carrier, and trion generation dynamics in single-walled carbon nanotubes Yuma, B.; Berciaud, S.; Besbas, J. Physical Review B, Vol. 87, Issue 20 https://doi.org/10.1103/PhysRevB.87.205412	journal	May 2013
Optical Spectrum of ${MoS}_{2}$ : Many-Body Effects and Diversity of Exciton States Qiu, Diana Y.; da Jornada, Felipe H.; Louie, Steven G. Physical Review Letters, Vol. 111, Issue 21 https://doi.org/10.1103/PhysRevLett.111.216805	journal	November 2013
Excitonic Bloch equations for a two-dimensional system of interacting excitons Rochat, G.; Ciuti, C.; Savona, V. Physical Review B, Vol. 61, Issue 20 https://doi.org/10.1103/PhysRevB.61.13856	journal	May 2000
Charge Photogeneration in Few-Layer MoS ₂ Borzda, Tetiana; Gadermaier, Christoph; Vujicic, Natasa Advanced Functional Materials, Vol. 25, Issue 22 https://doi.org/10.1002/adfm.201500709	journal	April 2015
Low-temperature photocarrier dynamics in monolayer MoS ₂ Korn, T.; Heydrich, S.; Hirmer, M. Applied Physics Letters, Vol. 99, Issue 10 https://doi.org/10.1063/1.3636402	journal	September 2011
Carrier and Polarization Dynamics in Monolayer ${MoS}_{2}$ Lagarde, D.; Bouet, L.; Marie, X. Physical Review Letters, Vol. 112, Issue 4 https://doi.org/10.1103/PhysRevLett.112.047401	journal	January 2014
Valley dynamics probed through charged and neutral exciton emission in monolayer ${WSe}_{2}$ Wang, G.; Bouet, L.; Lagarde, D. Physical Review B, Vol. 90, Issue 7 https://doi.org/10.1103/PhysRevB.90.075413	journal	August 2014
Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides Moody, Galan; Kavir Dass, Chandriker; Hao, Kai Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9315	journal	September 2015
Theory of Trion Spectra in Semiconductor Nanostructures Esser, A.; Zimmermann, R.; Runge, E. physica status solidi (b), Vol. 227, Issue 2 https://doi.org/10.1002/1521-3951(200110)227:2<317::aid-pssb317>3.0.co;2-s	journal	October 2001
Photo-Induced Bandgap Renormalization Governs the Ultrafast Response of Single-Layer MoS2. Pogna, Eva AA; Marsili, Margherita; De Fazio, Domenico American Chemical Society (ACS) https://doi.org/10.17863/cam.26736	journalarticle	January 2016
Low-temperature photocarrier dynamics in monolayer MoS2 Korn, Tobias; Heydrich, Stefanie; Hirmer, Michael Universität Regensburg https://doi.org/10.5283/epub.26514	text	January 2011
Resonant internal Quantum transitions and femtosecond radiative decay of excitons in monolayer WSe2 Pöllmann, Christoph; Steinleitner, Philipp; Leierseder, Ursula Universität Regensburg https://doi.org/10.5283/epub.32244	text	January 2015
Biexciton, single carrier, and trion generation dynamics in single-walled carbon nanotubes Yuma, Bertrand; Berciaud, Stéphane; Besbas, Jean arXiv https://doi.org/10.48550/arxiv.1302.1590	text	January 2013
Optical Generation of Excitonic Valley Coherence in Monolayer WSe2 Jones, Aaron Mitchell; Yu, Hongyi; Ghimire, Nirmal arXiv https://doi.org/10.48550/arxiv.1303.5318	text	January 2013
Valley Carrier Dynamics in Monolayer Molybdenum Disulphide from Helicity Resolved Ultrafast Pump-probe Spectroscopy Wang, Qinsheng; Ge, Shaofeng; Li, Xiao arXiv https://doi.org/10.48550/arxiv.1311.3388	text	January 2013
Direct imaging of the band profile in single layer ${\small MoS_2}$ on graphite: quasiparticle energy gap, metallic edge states and edge band bending Zhang, Chendong; Johnson, Amber; Hsu, Chang-Lung arXiv https://doi.org/10.48550/arxiv.1401.5100	text	January 2014
Exciton Binding Energy of Monolayer WS2 Zhu, Bairen; Chen, Xi; Cui, Xiaodong arXiv https://doi.org/10.48550/arxiv.1403.5108	text	January 2014
Probing Excitonic Dark States in Single-layer Tungsten Disulfide Ye, Ziliang; Cao, Ting; O'Brien, Kevin arXiv https://doi.org/10.48550/arxiv.1403.5568	text	January 2014
Charge photogeneration in few-layer MoS2 Borzda, Tetiana; Gadermaier, Christoph; Vujicic, Natasa arXiv https://doi.org/10.48550/arxiv.1412.5338	preprint	January 2014
Exciton band structure in layered MoSe2: from a monolayer to the bulk limit Arora, Ashish; Nogajewski, Karol; Molas, Maciej R. arXiv https://doi.org/10.48550/arxiv.1509.06439	text	January 2015
Exciton Radiative Lifetime in Transition Metal Dichalcogenide Monolayers Robert, C.; Lagarde, D.; Cadiz, F. arXiv https://doi.org/10.48550/arxiv.1603.00277	text	January 2016
Photo-Induced Bandgap Renormalization Governs the Ultrafast Response of Single-Layer MoS2 Pogna, Eva A. A.; Marsili, Margherita; De Fazio, Domenico arXiv https://doi.org/10.48550/arxiv.1704.06372	text	January 2017

Cited By (6)

Dissociation of two-dimensional excitons in monolayer WSe2 Massicotte, Mathieu; Vialla, Fabien; Schmidt, Peter Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-03864-y	journal	April 2018
Upconverted electroluminescence via Auger scattering of interlayer excitons in van der Waals heterostructures Binder, J.; Howarth, J.; Withers, F. Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-10323-9	journal	May 2019
2D semiconductor nonlinear plasmonic modulators Klein, Matthew; Badada, Bekele H.; Binder, Rolf Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-11186-w	journal	July 2019
Probing the exciton k-space dynamics in monolayer tungsten diselenides Yan, Tengfei; Yu, Hongyi; Xiao, Ke 2D Materials, Vol. 6, Issue 2 https://doi.org/10.1088/2053-1583/ab0a4e	journal	March 2019
Ultrafast nonequilibrium dynamics of strongly coupled resonances in the intrinsic cavity of $W S_{2}$ nanotubes Višić, Bojana; Yadgarov, Lena; Pogna, Eva A. A. Physical Review Research, Vol. 1, Issue 3 https://doi.org/10.1103/physrevresearch.1.033046	journal	October 2019
Moiré excitons: From programmable quantum emitter arrays to spin-orbit–coupled artificial lattices Yu, Hongyi; Liu, Gui-Bin; Tang, Jianju Science Advances, Vol. 3, Issue 11 https://doi.org/10.1126/sciadv.1701696	journal	November 2017

Similar Records

Ultrafast exciton many-body interactions and hot-phonon bottleneck in colloidal cesium lead halide perovskite nanocrystals

Journal Article · Mon Sep 10 00:00:00 EDT 2018 · Physical Review B · OSTI ID:1376528

Mondal, Anirban; Aneesh, J.; Kumar Ravi, Vikash; +5 more

Atomlike interaction and optically tunable giant band-gap renormalization in large-area atomically thin MoS2

Journal Article · Thu Nov 11 00:00:00 EST 2021 · Physical Review B · OSTI ID:1376528

Bera, Santu K.; Shrivastava, Meghanns; Bramhachari, Khamari; +7 more

Measuring Photoexcited Free Charge Carriers in Mono- to Few-Layer Transition-Metal Dichalcogenides with Steady-State Microwave Conductivity

Journal Article · Mon Dec 02 00:00:00 EST 2019 · Journal of Physical Chemistry Letters · OSTI ID:1376528

Blackburn, Jeffrey L.; Zhang, Hanyu; Myers, Alexis R.; +10 more

Related Subjects

36 MATERIALS SCIENCE

Title: Many-body effects in nonlinear optical responses of 2D layered semiconductors

Citation Formats

References (64)

Cited By (6)

Similar Records

Related Subjects