Exchange-driven intravalley mixing of excitons in monolayer transition metal dichalcogenides

Guo, Liang; Wu, Meng; Cao, Ting; Monahan, Daniele M.; Lee, Yi-Hsien; Louie, Steven G.; Fleming, Graham R.

doi:10.1038/s41567-018-0362-y

Exchange-driven intravalley mixing of excitons in monolayer transition metal dichalcogenides

Journal Article · Sun Dec 09 23:00:00 EST 2018 · Nature Physics

DOI:https://doi.org/10.1038/s41567-018-0362-y· OSTI ID:1581333

Guo, Liang; ; ; Monahan, Daniele M.; ; ; Fleming, Graham R.

Monolayer transition metal dichalcogenides (TMDCs) are promising two-dimensional (2D) semiconductors for application in optoelectronics. Their optical properties are dominated by two series of photo-excited exciton states—A (XA) and B (XB) 1,2 —that are derived from direct interband transitions near the band extrema. These exciton states have large binding energies and strong optical absorption 3–6 , and form an ideal system to investigate many-body effects in low dimensions. Because spin–orbit coupling causes a large splitting between bands of opposite spins, XA and XB are usually treated as spin-polarized Ising excitons, each arising from interactions within a specific set of states induced by interband transitions between pairs of either spin-up or spin-down bands (TA or TB). Here, by using monolayer MoS₂ as a prototypical system and solving the first-principles Bethe–Salpeter equations, we demonstrate a strong intravalley exchange interaction between TA and TB, indicating that XA and XB are mixed states instead of pure Ising excitons. Using 2D electronic spectroscopy, we observe that an optical excitation of the lower-energy TA induces a population of the higher-energy TB, manifesting the intravalley exchange interaction. This work elucidates the dynamics of exciton formation in monolayer TMDCs, and sheds light on many-body effects in 2D materials.

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

DOE Contract Number:: AC02-05CH11231

OSTI ID:: 1581333

Journal Information:: Nature Physics, Journal Name: Nature Physics Journal Issue: 3 Vol. 15; ISSN 1745-2473

Publisher:: Nature Publishing Group (NPG)

Country of Publication:: United States

Language:: English

References (45)

Coherent and Incoherent Coupling Dynamics between Neutral and Charged Excitons in Monolayer MoSe ₂ Hao, Kai; Xu, Lixiang; Nagler, Philipp Nano Letters, Vol. 16, Issue 8 https://doi.org/10.1021/acs.nanolett.6b02041	journal	July 2016
Exchange interaction and polariton effects in quantum-well excitons Andreani, Lucio Claudio; Bassani, Franco Physical Review B, Vol. 41, Issue 11 https://doi.org/10.1103/PhysRevB.41.7536	journal	April 1990
Two-Dimensional Electronic Spectroscopy Reveals the Dynamics of Phonon-Mediated Excitation Pathways in Semiconducting Single-Walled Carbon Nanotubes Graham, Matt W.; Calhoun, Tessa R.; Green, Alexander A. Nano Letters, Vol. 12, Issue 2 https://doi.org/10.1021/nl2038503	journal	January 2012
Exciton spin dynamics in quantum wells Maialle, M. Z.; de Andrada e. Silva, E. A.; Sham, L. J. Physical Review B, Vol. 47, Issue 23 https://doi.org/10.1103/PhysRevB.47.15776	journal	June 1993
Long-lived quantum coherence in photosynthetic complexes at physiological temperature Panitchayangkoon, G.; Hayes, D.; Fransted, K. A. Proceedings of the National Academy of Sciences, Vol. 107, Issue 29 https://doi.org/10.1073/pnas.1005484107	journal	July 2010
Nonuniform sampling schemes of the Brillouin zone for many-electron perturbation-theory calculations in reduced dimensionality da Jornada, Felipe H.; Qiu, Diana Y.; Louie, Steven G. Physical Review B, Vol. 95, Issue 3 https://doi.org/10.1103/PhysRevB.95.035109	journal	January 2017
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
Electron-hole excitations and optical spectra from first principles Rohlfing, Michael; Louie, Steven G. Physical Review B, Vol. 62, Issue 8 https://doi.org/10.1103/PhysRevB.62.4927	journal	August 2000
Two-dimensional spectroscopy of electronic couplings in photosynthesis Brixner, Tobias; Stenger, Jens; Vaswani, Harsha M. Nature, Vol. 434, Issue 7033 https://doi.org/10.1038/nature03429	journal	March 2005
BerkeleyGW: A massively parallel computer package for the calculation of the quasiparticle and optical properties of materials and nanostructures Deslippe, Jack; Samsonidze, Georgy; Strubbe, David A. Computer Physics Communications, Vol. 183, Issue 6 https://doi.org/10.1016/j.cpc.2011.12.006	journal	June 2012
Fine structure of quantum well excitons Rössler, U.; Jorda, S.; Broido, D. Solid State Communications, Vol. 73, Issue 3 https://doi.org/10.1016/0038-1098(90)90959-F	journal	January 1990
wannier90: A tool for obtaining maximally-localised Wannier functions Mostofi, Arash A.; Yates, Jonathan R.; Lee, Young-Su Computer Physics Communications, Vol. 178, Issue 9 https://doi.org/10.1016/j.cpc.2007.11.016	journal	May 2008
Room-Temperature Coherent Optical Phonon in 2D Electronic Spectra of CH ₃ NH ₃ PbI ₃ Perovskite as a Possible Cooling Bottleneck Monahan, Daniele M.; Guo, Liang; Lin, Jia The Journal of Physical Chemistry Letters, Vol. 8, Issue 14 https://doi.org/10.1021/acs.jpclett.7b01357	journal	June 2017
Exciton band structure of monolayer MoS 2 Wu, Fengcheng; Qu, Fanyao; MacDonald, A. H. Physical Review B, Vol. 91, Issue 7 https://doi.org/10.1103/PhysRevB.91.075310	journal	February 2015
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
Long-lived nanosecond spin relaxation and spin coherence of electrons in monolayer MoS2 and WS2 Yang, Luyi; Sinitsyn, Nikolai A.; Chen, Weibing Nature Physics, Vol. 11, Issue 10 https://doi.org/10.1038/nphys3419	journal	August 2015
Design, Modeling, and Fabrication of Chemical Vapor Deposition Grown MoS ₂ Circuits with E-Mode FETs for Large-Area Electronics Yu, Lili; El-Damak, Dina; Radhakrishna, Ujwal Nano Letters, Vol. 16, Issue 10 https://doi.org/10.1021/acs.nanolett.6b02739	journal	September 2016
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
Nonanalyticity, Valley Quantum Phases, and Lightlike Exciton Dispersion in Monolayer Transition Metal Dichalcogenides: Theory and First-Principles Calculations Qiu, Diana Y.; Cao, Ting; Louie, Steven G. Physical Review Letters, Vol. 115, Issue 17 https://doi.org/10.1103/PhysRevLett.115.176801	journal	October 2015
Exciton dynamics in GaAs quantum wells under resonant excitation Vinattieri, A.; Shah, Jagdeep; Damen, T. C. Physical Review B, Vol. 50, Issue 15 https://doi.org/10.1103/PhysRevB.50.10868	journal	October 1994
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
Coulomb-hole summations and energies for G W calculations with limited number of empty orbitals: A modified static remainder approach Deslippe, Jack; Samsonidze, Georgy; Jain, Manish Physical Review B, Vol. 87, Issue 16 https://doi.org/10.1103/PhysRevB.87.165124	journal	April 2013
Pulse-front matching of ultrabroadband near-infrared noncollinear optical parametric amplified pulses Isaienko, Oleksandr; Borguet, Eric Journal of the Optical Society of America B, Vol. 26, Issue 5 https://doi.org/10.1364/JOSAB.26.000965	journal	January 2009
Electron-Hole Excitations in Semiconductors and Insulators Rohlfing, Michael; Louie, Steven G. Physical Review Letters, Vol. 81, Issue 11 https://doi.org/10.1103/PhysRevLett.81.2312	journal	September 1998
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
Atomically Thin MoS2 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
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
Rapid and economical data acquisition in ultrafast frequency-resolved spectroscopy using choppers and a microcontroller Guo, Liang; Monahan, Daniele M.; Fleming, Graham Optics Express, Vol. 24, Issue 16 https://doi.org/10.1364/OE.24.018126	journal	January 2016
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502 https://doi.org/10.1088/0953-8984/21/39/395502	journal	September 2009
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
Pulse-front-matched optical parametric amplification for sub-10-fs pulse generation tunable in the visible and near infrared Shirakawa, Akira; Sakane, Isao; Kobayashi, Takayoshi Optics Letters, Vol. 23, Issue 16 https://doi.org/10.1364/OL.23.001292	journal	January 1998
Valley depolarization due to intervalley and intravalley electron-hole exchange interactions in monolayer MoS 2 Yu, T.; Wu, M. W. Physical Review B, Vol. 89, Issue 20 https://doi.org/10.1103/PhysRevB.89.205303	journal	May 2014
Many-Body Interactions in Semiconductors Probed by Optical Two-Dimensional Fourier Transform Spectroscopy Li, Xiaoqin; Zhang, Tianhao; Borca, Camelia N. Physical Review Letters, Vol. 96, Issue 5 https://doi.org/10.1103/PhysRevLett.96.057406	journal	February 2006
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 Ultrafast Excitonic Dynamics of Few-Layer MoS ₂ Using State-Selective Coherent Multidimensional Spectroscopy Czech, Kyle J.; Thompson, Blaise J.; Kain, Schuyler ACS Nano, Vol. 9, Issue 12 https://doi.org/10.1021/acsnano.5b05198	journal	October 2015
Subpicosecond spin relaxation dynamics of excitons and free carriers in GaAs quantum wells Damen, T. C.; Via, Luis; Cunningham, J. E. Physical Review Letters, Vol. 67, Issue 24 https://doi.org/10.1103/PhysRevLett.67.3432	journal	December 1991
Sub-8-fs pulses from an ultrabroadband optical parametric amplifier in the visible Cerullo, G.; Nisoli, M.; Stagira, S. Optics Letters, Vol. 23, Issue 16 https://doi.org/10.1364/OL.23.001283	journal	January 1998
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
Electron correlation in semiconductors and insulators: Band gaps and quasiparticle energies Hybertsen, Mark S.; Louie, Steven G. Physical Review B, Vol. 34, Issue 8, p. 5390-5413 https://doi.org/10.1103/PhysRevB.34.5390	journal	October 1986
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
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
Phase-stabilized two-dimensional electronic spectroscopy Brixner, Tobias; Mančal, Tomáš; Stiopkin, Igor V. The Journal of Chemical Physics, Vol. 121, Issue 9 https://doi.org/10.1063/1.1776112	journal	September 2004
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
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
From Bulk to Monolayer MoS2: Evolution of Raman Scattering Li, Hong; Zhang, Qing; Yap, Chin Chong Ray Advanced Functional Materials, Vol. 22, Issue 7 https://doi.org/10.1002/adfm.201102111	journal	January 2012

Similar Records

Exchange-driven intravalley mixing of excitons in monolayer transition metal dichalcogenides

Journal Article · Sun Dec 09 23:00:00 EST 2018 · Nature Physics · OSTI ID:1530822

Lineshape characterization of excitons in monolayer WS₂ by two-dimensional electronic spectroscopy

Journal Article · Tue Apr 21 00:00:00 EDT 2020 · Nanoscale Advances · OSTI ID:2470943

Exchange-driven intravalley mixing of excitons in monolayer transition metal dichalcogenides

Citation Formats

References (45)

Similar Records

Related Subjects