Optical nonlinearities of excitons in monolayer
Abstract
We calculate linear and nonlinear optical susceptibilities arising from the excitonic states of monolayer MoS2 for in-plane light polarizations, using second-quantized bound and unbound exciton operators. Optical selection rules are critical for obtaining the susceptibilities. We derive the valley-chirality rule for the second-order harmonic generation in monolayer MoS2 and find that the third-order harmonic process is efficient only for linearly polarized input light while the third-order two-photon process (optical Kerr effect) is efficient for circularly polarized light using a higher order exciton state. The absence of linear absorption due to the band gap and the unusually strong two-photon third-order nonlinearity make the monolayer MoS2 excitonic structure a promising resource for coherent nonlinear photonics.
- Authors:
-
[1];
- Stanford Univ., CA (United States). Edward L. Ginzton Lab.; Sandia National Lab. (SNL-CA), Livermore, CA (United States)
- Stanford Univ., CA (United States). Edward L. Ginzton Lab.
- Publication Date:
- Research Org.:
- Stanford Univ., CA (United States); Sandia National Lab. (SNL-CA), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1431585
- Alternate Identifier(s):
- OSTI ID: 1432104
- Grant/Contract Number:
- NA0003525
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 97; Journal Issue: 16; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Optical nonlinearity; TMD
Citation Formats
Soh, Daniel B. S., Rogers, Christopher, Gray, Dodd J., Chatterjee, Eric, and Mabuchi, Hideo. Optical nonlinearities of excitons in monolayer MoS2. United States: N. p., 2018.
Web. doi:10.1103/PhysRevB.97.165111.
Soh, Daniel B. S., Rogers, Christopher, Gray, Dodd J., Chatterjee, Eric, & Mabuchi, Hideo. Optical nonlinearities of excitons in monolayer MoS2. United States. https://doi.org/10.1103/PhysRevB.97.165111
Soh, Daniel B. S., Rogers, Christopher, Gray, Dodd J., Chatterjee, Eric, and Mabuchi, Hideo. Fri .
"Optical nonlinearities of excitons in monolayer MoS2". United States. https://doi.org/10.1103/PhysRevB.97.165111. https://www.osti.gov/servlets/purl/1431585.
@article{osti_1431585,
title = {Optical nonlinearities of excitons in monolayer MoS2},
author = {Soh, Daniel B. S. and Rogers, Christopher and Gray, Dodd J. and Chatterjee, Eric and Mabuchi, Hideo},
abstractNote = {We calculate linear and nonlinear optical susceptibilities arising from the excitonic states of monolayer MoS2 for in-plane light polarizations, using second-quantized bound and unbound exciton operators. Optical selection rules are critical for obtaining the susceptibilities. We derive the valley-chirality rule for the second-order harmonic generation in monolayer MoS2 and find that the third-order harmonic process is efficient only for linearly polarized input light while the third-order two-photon process (optical Kerr effect) is efficient for circularly polarized light using a higher order exciton state. The absence of linear absorption due to the band gap and the unusually strong two-photon third-order nonlinearity make the monolayer MoS2 excitonic structure a promising resource for coherent nonlinear photonics.},
doi = {10.1103/PhysRevB.97.165111},
journal = {Physical Review B},
number = 16,
volume = 97,
place = {United States},
year = {Fri Apr 06 00:00:00 EDT 2018},
month = {Fri Apr 06 00:00:00 EDT 2018}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 18 works
Citation information provided by
Web of Science
Web of Science
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:
Quantum Theory of the Optical and Electronic Properties of Semiconductors
book, January 2009
- Haug, Hartmut; Koch, Stephan W.
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
Comprehensive analysis of the optical Kerr coefficient of graphene
journal, August 2016
- Soh, Daniel B. S.; Hamerly, Ryan; Mabuchi, Hideo
- Physical Review A, Vol. 94, Issue 2
Mid-infrared optical parametric amplifier using silicon nanophotonic waveguides
journal, May 2010
- Liu, Xiaoping; Osgood, Richard M.; Vlasov, Yurii A.
- Nature Photonics, Vol. 4, Issue 8
An integrated diamond nanophotonics platform for quantum-optical networks
journal, October 2016
- Sipahigil, A.; Evans, R. E.; Sukachev, D. D.
- Science, Vol. 354, Issue 6314
Supercontinuum generation in silicon photonic wires
journal, January 2007
- Hsieh, I-Wei; Chen, Xiaogang; Liu, Xiaoping
- Optics Express, Vol. 15, Issue 23
Assembly of hybrid photonic architectures from nanophotonic constituents
journal, December 2011
- Benson, Oliver
- Nature, Vol. 480, Issue 7376
Fast exciton annihilation by capture of electrons or holes by defects via Auger scattering in monolayer metal dichalcogenides
journal, April 2015
- Wang, Haining; Strait, Jared H.; Zhang, Changjian
- Physical Review B, Vol. 91, Issue 16
Observation of Excitonic Rydberg States in Monolayer MoS 2 and WS 2 by Photoluminescence Excitation Spectroscopy
journal, April 2015
- Hill, Heather M.; Rigosi, Albert F.; Roquelet, Cyrielle
- Nano Letters, Vol. 15, Issue 5
Strong optical nonlinearity of CVD-grown monolayer as probed by wavelength-dependent second-harmonic generation
journal, September 2014
- Clark, D. J.; Senthilkumar, V.; Le, C. T.
- Physical Review B, Vol. 90, Issue 12
Dielectric screening in two-dimensional insulators: Implications for excitonic and impurity states in graphane
journal, August 2011
- Cudazzo, Pierluigi; Tokatly, Ilya V.; Rubio, Angel
- Physical Review B, Vol. 84, Issue 8
Nonlinear optical selection rule based on valley-exciton locking in monolayer ws2
journal, December 2015
- Xiao, Jun; Ye, Ziliang; Wang, Ying
- Light: Science & Applications, Vol. 4, Issue 12
Optical frequency comb generation from a monolithic microresonator
journal, December 2007
- Del’Haye, P.; Schliesser, A.; Arcizet, O.
- Nature, Vol. 450, Issue 7173
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
Radiative lifetimes of excitons and trions in monolayers of the metal dichalcogenide
journal, January 2016
- Wang, Haining; Zhang, Changjian; Chan, Weimin
- Physical Review B, Vol. 93, Issue 4
Direct Imaging of Band Profile in Single Layer MoS 2 on Graphite: Quasiparticle Energy Gap, Metallic Edge States, and Edge Band Bending
journal, April 2014
- Zhang, Chendong; Johnson, Amber; Hsu, Chang-Lung
- Nano Letters, Vol. 14, Issue 5
Large optical nonlinearity of indium tin oxide in its epsilon-near-zero region
journal, April 2016
- Alam, M. Z.; De Leon, I.; Boyd, R. W.
- Science, Vol. 352, Issue 6287
Absorption of light by excitons and trions in monolayers of metal dichalcogenide : Experiments and theory
journal, May 2014
- Zhang, Changjian; Wang, Haining; Chan, Weimin
- Physical Review B, Vol. 89, Issue 20
Optical Spectrum of : Many-Body Effects and Diversity of Exciton States
journal, November 2013
- Qiu, Diana Y.; da Jornada, Felipe H.; Louie, Steven G.
- Physical Review Letters, Vol. 111, Issue 21
A photon–photon quantum gate based on a single atom in an optical resonator
journal, July 2016
- Hacker, Bastian; Welte, Stephan; Rempe, Gerhard
- Nature, Vol. 536, Issue 7615
Determination of band alignment in the single-layer MoS2/WSe2 heterojunction
journal, July 2015
- Chiu, Ming-Hui; Zhang, Chendong; Shiu, Hung-Wei
- Nature Communications, Vol. 6, Issue 1
Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides
journal, September 2015
- Moody, Galan; Kavir Dass, Chandriker; Hao, Kai
- Nature Communications, Vol. 6, Issue 1
Generation of multiphoton entangled quantum states by means of integrated frequency combs
journal, March 2016
- Reimer, Christian; Kues, Michael; Roztocki, Piotr
- Science, Vol. 351, Issue 6278
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
Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy
journal, October 2014
- Klots, A. R.; Newaz, A. K. M.; Wang, Bin
- Scientific Reports, Vol. 4, Issue 1
Second harmonic microscopy of monolayer MoS
journal, April 2013
- Kumar, Nardeep; Najmaei, Sina; Cui, Qiannan
- Physical Review B, Vol. 87, Issue 16
Large excitonic effects in monolayers of molybdenum and tungsten dichalcogenides
journal, September 2012
- Ramasubramaniam, Ashwin
- Physical Review B, Vol. 86, Issue 11
Valley-selective circular dichroism of monolayer molybdenum disulphide
journal, January 2012
- Cao, Ting; Wang, Gang; Han, Wenpeng
- Nature Communications, Vol. 3, Issue 1
Erratum: Robust optical emission polarization in MoS monolayers through selective valley excitation [Phys. Rev. B 86 , 081301(R) (2012)]
journal, February 2014
- Sallen, G.; Bouet, L.; Marie, X.
- Physical Review B, Vol. 89, Issue 7
Effect of spin-orbit interaction on the optical spectra of single-layer, double-layer, and bulk MoS
journal, July 2013
- Molina-Sánchez, Alejandro; Sangalli, Davide; Hummer, Kerstin
- Physical Review B, Vol. 88, Issue 4
Photonic chip-based optical frequency comb using soliton Cherenkov radiation
journal, December 2015
- Brasch, V.; Geiselmann, M.; Herr, T.
- Science, Vol. 351, Issue 6271
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
Monolayer MoS : Trigonal warping, the valley, and spin-orbit coupling effects
journal, July 2013
- Kormányos, Andor; Zólyomi, Viktor; Drummond, Neil D.
- Physical Review B, Vol. 88, Issue 4
Second-Harmonic Light Generation in Crystals with Natural Optical Activity
journal, July 1968
- Simon, H. J.; Bloembergen, N.
- Physical Review, Vol. 171, Issue 3
Observation of intense second harmonic generation from MoS atomic crystals
journal, May 2013
- Malard, Leandro M.; Alencar, Thonimar V.; Barboza, Ana Paula M.
- Physical Review B, Vol. 87, Issue 20
Second harmonic generation in -BN and MoS monolayers: Role of electron-hole interaction
journal, February 2014
- Grüning, M.; Attaccalite, C.
- Physical Review B, Vol. 89, Issue 8
A tight-binding model for MoS 2 monolayers
journal, August 2015
- Ridolfi, E.; Le, D.; Rahman, T. S.
- Journal of Physics: Condensed Matter, Vol. 27, Issue 36
Photonic-Chip Supercontinuum with Tailored Spectra for Counting Optical Frequencies
journal, July 2017
- Carlson, David R.; Hickstein, Daniel D.; Lind, Alex
- Physical Review Applied, Vol. 8, Issue 1
On-Chip Strong Coupling and Efficient Frequency Conversion between Telecom and Visible Optical Modes
journal, September 2016
- Guo, Xiang; Zou, Chang-Ling; Jung, Hojoong
- Physical Review Letters, Vol. 117, Issue 12
Robust optical emission polarization in MoS monolayers through selective valley excitation
journal, August 2012
- Sallen, G.; Bouet, L.; Marie, X.
- Physical Review B, Vol. 86, Issue 8
Intraband effects in excitonic second-harmonic generation
journal, December 2015
- Pedersen, Thomas Garm
- Physical Review B, Vol. 92, Issue 23
Binding energies of exciton complexes in transition metal dichalcogenide monolayers and effect of dielectric environment
journal, November 2015
- Kylänpää, Ilkka; Komsa, Hannu-Pekka
- Physical Review B, Vol. 92, Issue 20
Electronics and optoelectronics of two-dimensional transition metal dichalcogenides
journal, November 2012
- Wang, Qing Hua; Kalantar-Zadeh, Kourosh; Kis, Andras
- Nature Nanotechnology, Vol. 7, Issue 11, p. 699-712
Experimental Demonstration of Continuous Electronic Structure Tuning via Strain in Atomically Thin MoS 2
journal, May 2013
- He, Keliang; Poole, Charles; Mak, Kin Fai
- Nano Letters, Vol. 13, Issue 6
Exciton band structure of monolayer
journal, February 2015
- Wu, Fengcheng; Qu, Fanyao; MacDonald, A. H.
- Physical Review B, Vol. 91, Issue 7
Deterministic quantum nonlinear optics with single atoms and virtual photons
journal, June 2017
- Kockum, Anton Frisk; Miranowicz, Adam; Macrì, Vincenzo
- Physical Review A, Vol. 95, Issue 6
Electrical control of second-harmonic generation in a WSe2 monolayer transistor
journal, April 2015
- Seyler, Kyle L.; Schaibley, John R.; Gong, Pu
- Nature Nanotechnology, Vol. 10, Issue 5
Optical spectroscopy of excited exciton states in monolayers in van der Waals heterostructures
journal, January 2018
- Robert, C.; Semina, M. A.; Cadiz, F.
- Physical Review Materials, Vol. 2, Issue 1
Characterization of the second- and third-order nonlinear optical susceptibilities of monolayer MoS 2 using multiphoton microscopy
journal, November 2016
- Woodward, R. I.; Murray, R. T.; Phelan, C. F.
- 2D Materials, Vol. 4, Issue 1
Two-dimensional van der Waals materials
journal, September 2016
- Ajayan, Pulickel; Kim, Philip; Banerjee, Kaustav
- Physics Today, Vol. 69, Issue 9
Nonlinear optical response of a two-dimensional atomic crystal
journal, December 2015
- Merano, Michele
- Optics Letters, Vol. 41, Issue 1
Effective mass approximation for excitons
journal, September 1956
- Dresselhaus, G.
- Journal of Physics and Chemistry of Solids, Vol. 1, Issue 1-2
Computational 2D Materials Database: Electronic Structure of Transition-Metal Dichalcogenides and Oxides
journal, June 2015
- Rasmussen, Filip A.; Thygesen, Kristian S.
- The Journal of Physical Chemistry C, Vol. 119, Issue 23
Theory of excitonic second-harmonic generation in monolayer
journal, June 2014
- Trolle, Mads L.; Seifert, Gotthard; Pedersen, Thomas G.
- Physical Review B, Vol. 89, Issue 23
Qubit limit of cavity nonlinear optics
journal, January 2012
- Mabuchi, Hideo
- Physical Review A, Vol. 85, Issue 1
Intensity of Optical Absorption by Excitons
journal, December 1957
- Elliott, R. J.
- Physical Review, Vol. 108, Issue 6
Ab initio tight-binding Hamiltonian for transition metal dichalcogenides
journal, November 2015
- Fang, Shiang; Kuate Defo, Rodrick; Shirodkar, Sharmila N.
- Physical Review B, Vol. 92, Issue 20
Single-layer MoS2 transistors
journal, January 2011
- Radisavljevic, B.; Radenovic, A.; Brivio, J.
- Nature Nanotechnology, Vol. 6, Issue 3, p. 147-150
Theory of neutral and charged excitons in monolayer transition metal dichalcogenides
journal, July 2013
- Berkelbach, Timothy C.; Hybertsen, Mark S.; Reichman, David R.
- Physical Review B, Vol. 88, Issue 4
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
Quasiparticle band structure calculation of monolayer, bilayer, and bulk MoS
journal, May 2012
- Cheiwchanchamnangij, Tawinan; Lambrecht, Walter R. L.
- Physical Review B, Vol. 85, Issue 20
Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides
conference, February 2017
- Selig, Malte; Berghäuser, Gunnar; Raja, Archana
- SPIE OPTO, SPIE Proceedings
Nonlinear optical response of a two-dimensional atomic crystal
conference, January 2016
- Merano, Michele
- Frontiers in Optics 2016
Generation of multiphoton entangled quantum states by means of integrated frequency combs
other, January 2016
- Reimer, Christian; Kues, Michael; Roztocki, Piotr
- Washington D.C. : American Association for the Advancement of Science
Twist-tailoring Coulomb correlations in van der Waals homobilayers
text, January 2020
- Merkl, Philipp; Mooshammer, Fabian; Brem, Samuel
- Universität Regensburg
Photonic Chip Based Optical Frequency Comb Using Soliton Induced Cherenkov Radiation
conference, January 2015
- Brasch, Victor; Geiselmann, Michael; Herr, Tobias
- CLEO: Science and Innovations, CLEO: 2015
Mid-infrared optical parametric amplifier using silicon nanophotonic waveguides
text, January 2010
- Liu, Xiaoping; Osgood, Richard M.; Vlasov, Yurii A.
- arXiv
Theory of Neutral and Charged Excitons in Monolayer Transition Metal Dichalcogenides
text, January 2013
- Berkelbach, Timothy C.; Hybertsen, Mark S.; Reichman, David R.
- arXiv
Direct imaging of the band profile in single layer ${\small MoS_2}$ on graphite: quasiparticle energy gap, metallic edge states and edge band bending
text, January 2014
- Zhang, Chendong; Johnson, Amber; Hsu, Chang-Lung
- arXiv
Fast Exciton Annihilation by Capture of Electrons or Holes by Defects via Auger Scattering in Monolayer Metal Dichalcogenides
text, January 2014
- Wang, Haining; Strait, Jared H.; Zhang, Changjian
- arXiv
k.p theory for two-dimensional transition metal dichalcogenide semiconductors
text, January 2014
- Kormányos, Andor; Burkard, Guido; Gmitra, Martin
- arXiv
Computational 2D Materials Database: Electronic Structure of Transition-Metal Dichalcogenides and Oxides
text, January 2015
- Rasmussen, Filip Anselm; Thygesen, Kristian Sommer
- arXiv
\textit{Ab-initio} Tight-Binding Hamiltonian for Transition Metal Dichalcogenides
text, January 2015
- Fang, Shiang; Defo, Rodrick Kuate; Shirodkar, Sharmila N.
- arXiv
Binding energies of exciton complexes in transition metal dichalcogenides and effect of dielectric environment
text, January 2015
- Kylänpää, Ilkka; Komsa, Hannu-Pekka
- arXiv
Comprehensive analysis of the optical Kerr coefficient of graphene
text, January 2016
- Soh, Daniel B. S.; Hamerly, Ryan; Mabuchi, Hideo
- arXiv
A photon-photon quantum gate based on a single atom in an optical resonator
text, January 2016
- Hacker, Bastian; Welte, Stephan; Rempe, Gerhard
- arXiv
Deterministic quantum nonlinear optics with single atoms and virtual photons
text, January 2017
- Kockum, Anton Frisk; Miranowicz, Adam; Macrì, Vincenzo
- arXiv
Works referencing / citing this record:
Two-dimensional nonlinear optical materials predicted by network visualization
journal, January 2019
- Yang, Guoyu; Wu, Kechen
- Molecular Systems Design & Engineering, Vol. 4, Issue 3
Intraband divergences in third order optical response of 2D systems
journal, March 2019
- Cheng, J. L.; Sipe, J. E.; Wu, S. W.
- APL Photonics, Vol. 4, Issue 3
Supercontinuum second harmonic generation spectroscopy of atomically thin semiconductors
journal, August 2019
- Stiehm, Torsten; Schneider, Robert; Kern, Johannes
- Review of Scientific Instruments, Vol. 90, Issue 8
Twist-angle modulation of exciton absorption in MoS 2 /graphene heterojunctions
journal, October 2019
- Zhang, Xiangzhe; Yang, Hang; Hou, Weiwei
- Applied Physics Letters, Vol. 115, Issue 18
Quantum-enhanced tunable spin-valley dependent excitonic second harmonic generation in molybdenum disulfide quantum dots
journal, November 2019
- Fouladi-Oskouei, J.; Shojaei, S.
- Materials Research Express, Vol. 6, Issue 12
Adiabatic Fock-state-generation scheme using Kerr nonlinearity
journal, September 2019
- Yanagimoto, Ryotatsu; Ng, Edwin; Onodera, Tatsuhiro
- Physical Review A, Vol. 100, Issue 3
Theory of second-order excitonic nonlinearities in transition metal dichalcogenides
journal, September 2019
- Mkrtchian, Garnik F.; Knorr, Andreas; Selig, Malte
- Physical Review B, Vol. 100, Issue 12
Triple sum frequency pump-probe spectroscopy of transition metal dichalcogenides
journal, December 2019
- Morrow, Darien J.; Kohler, Daniel D.; Zhao, Yuzhou
- Physical Review B, Vol. 100, Issue 23
Coherent feedback control of two-dimensional excitons
journal, January 2020
- Rogers, Christopher; Gray, Dodd; Bogdanowicz, Nathan
- Physical Review Research, Vol. 2, Issue 1
Enhanced four-wave mixing process near the excitonic resonances of bulk MoS 2
journal, January 2019
- Ko, Brian A.; Sokolov, Alexei V.; Scully, Marlan O.
- Photonics Research, Vol. 7, Issue 3
Adiabatic Fock State Generation Scheme Using Kerr Nonlinearity
conference, January 2018
- Yanagimoto, Ryotatsu; Onodera, Tatsuhiro; Ng, Edwin
- CLEO: QELS_Fundamental Science, Conference on Lasers and Electro-Optics