Observation of Excitonic Rydberg States in Monolayer MoS2 and WS2 by Photoluminescence Excitation Spectroscopy

Hill, Heather M.; Rigosi, Albert F.; Roquelet, Cyrielle; Chernikov, Alexey; Berkelbach, Timothy C.; Reichman, David R.; Hybertsen, Mark S.; Brus, Louis E.; Heinz, Tony F.

doi:10.1021/nl504868p

Title: Observation of Excitonic Rydberg States in Monolayer MoS₂ and WS₂ by Photoluminescence Excitation Spectroscopy

Abstract

Here, we have identified excited exciton states in monolayers of MoS₂ and WS₂ supported on fused silica by means of photoluminescence excitation spectroscopy. In monolayer WS₂, the positions of the excited A exciton states imply an exciton binding energy of 0.32 eV. In monolayer MoS₂, excited exciton transitions are observed at energies of 2.24 and 2.34 eV. Assigning these states to the B exciton Rydberg series yields an exciton binding energy of 0.44 eV.

Authors:

Hill, Heather M. ^[1]; Rigosi, Albert F. ^[1]; Roquelet, Cyrielle ^[1]; Chernikov, Alexey ^[1]; Berkelbach, Timothy C. ^[1]; Reichman, David R. ^[1]; Hybertsen, Mark S. ^[2]; Brus, Louis E. ^[1]; Heinz, Tony F. ^[1]

Columbia Univ., New York, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)

Publication Date:: Fri Mar 27 00:00:00 EDT 2015

Research Org.:: Energy Frontier Research Centers (EFRC) (United States). Re-Defining Photovoltaic Efficiency Through Molecule Scale Control (RPEMSC)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF); Keck Foundation; Alexander von Humboldt Foundation; Feodor Lynen Research Fellowship

OSTI Identifier:: 1370381

Grant/Contract Number:: SC0001085; DMR-1122594; DGE-1069240; AC02-98CH10886; AC05-06OR23100

Resource Type:: Accepted Manuscript

Journal Name:: Nano Letters

Additional Journal Information:: Journal Volume: 15; Journal Issue: 5; Related Information: RPEMSC partners with Columbia University (lead); Brookhaven National Laboratory; Purdue University; Journal ID: ISSN 1530-6984

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; transition metal dichalcogenides; molybdenum disulfide; tungsten disulfide; 2D materials; binding energy; excitons; monolayers; energy; phase transitions

Citation Formats


                    Hill, Heather M., Rigosi, Albert F., Roquelet, Cyrielle, Chernikov, Alexey, Berkelbach, Timothy C., Reichman, David R., Hybertsen, Mark S., Brus, Louis E., and Heinz, Tony F. Observation of Excitonic Rydberg States in Monolayer MoS2 and WS2 by Photoluminescence Excitation Spectroscopy.  United States: N. p., 2015. 
Web.  doi:10.1021/nl504868p.

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                    Hill, Heather M., Rigosi, Albert F., Roquelet, Cyrielle, Chernikov, Alexey, Berkelbach, Timothy C., Reichman, David R., Hybertsen, Mark S., Brus, Louis E., & Heinz, Tony F. Observation of Excitonic Rydberg States in Monolayer MoS2 and WS2 by Photoluminescence Excitation Spectroscopy.  United States.  https://doi.org/10.1021/nl504868p

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                    Hill, Heather M., Rigosi, Albert F., Roquelet, Cyrielle, Chernikov, Alexey, Berkelbach, Timothy C., Reichman, David R., Hybertsen, Mark S., Brus, Louis E., and Heinz, Tony F. Fri .  
"Observation of Excitonic Rydberg States in Monolayer MoS2 and WS2 by Photoluminescence Excitation Spectroscopy".  United States.  https://doi.org/10.1021/nl504868p.  https://www.osti.gov/servlets/purl/1370381.

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@article{osti_1370381,

  title        = {Observation of Excitonic Rydberg States in Monolayer MoS2 and WS2 by Photoluminescence Excitation Spectroscopy},

  author       = {Hill, Heather M. and Rigosi, Albert F. and Roquelet, Cyrielle and Chernikov, Alexey and Berkelbach, Timothy C. and Reichman, David R. and Hybertsen, Mark S. and Brus, Louis E. and Heinz, Tony F.},

  abstractNote = {Here, we have identified excited exciton states in monolayers of MoS2 and WS2 supported on fused silica by means of photoluminescence excitation spectroscopy. In monolayer WS2, the positions of the excited A exciton states imply an exciton binding energy of 0.32 eV. In monolayer MoS2, excited exciton transitions are observed at energies of 2.24 and 2.34 eV. Assigning these states to the B exciton Rydberg series yields an exciton binding energy of 0.44 eV.},

  doi          = {10.1021/nl504868p},

  journal      = {Nano Letters},

  number       = 5,

  volume       = 15,

  place        = {United States},

  year         = {Fri Mar 27 00:00:00 EDT 2015},

  month        = {Fri Mar 27 00:00:00 EDT 2015}

}

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Stier, A. V.; Wilson, N. P.; Velizhanin, K. A.
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Tian, Xiangling; Wei, Rongfei; Guo, Qianyi
Advanced Materials, Vol. 30, Issue 28
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Widely tunable Bi ₂ Se ₃ /transition metal dichalcogenide 2D heterostructures for write-read-erase-reuse applications
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Hennighausen, Zachariah; Bilgin, Ismail; Casey, Colin
2D Materials, Vol. 6, Issue 4
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Gerber, Iann C.; Courtade, Emmanuel; Shree, Shivangi
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Exciton routing in the heterostructure of a transition metal dichalcogenide monolayer on a paraelectric substrate
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Shahnazaryan, V.; Kyriienko, O.; Rostami, H.
Physical Review B, Vol. 100, Issue 16
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Optical spectroscopy of excited exciton states in ${MoS}_{2}$ monolayers in van der Waals heterostructures
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Robert, C.; Semina, M. A.; Cadiz, F.
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Surface susceptibility and conductivity of ${MoS}_{2}$ and ${WSe}_{2}$ monolayers: A first-principles and ellipsometry characterization
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Elliott, Joshua D.; Xu, Zhemi; Umari, Paolo
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A tight-binding model for MoS ₂ monolayers
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Ridolfi, E.; Le, D.; Rahman, T. S.
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Brunetti, Matthew N.; Berman, Oleg L.; Kezerashvili, Roman Ya
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Multiple-peak resonance of optical second harmonic generation arising from band nesting in monolayer transition metal dichalcogenides $T X_{2}$ on $Si O_{2} / Si (001)$ substrates $(T = Mo, W; X = S, Se)$
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Kikuchi, Yuhei; Miyauchi, Yoshihiro; Takaoka, Ryosei
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Gonçalves, P. A. D.; Bertelsen, L. P.; Xiao, Sanshui
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Oxygen Passivation Mediated Tunability of Trion and Excitons in ${MoS}_{2}$
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Gogoi, Pranjal Kumar; Hu, Zhenliang; Wang, Qixing
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Stiehm, Torsten; Schneider, Robert; Kern, Johannes
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Mode-locked, 194-μm, all-fiberized laser using WS_2-based evanescent field interaction
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Jung, Minwan; Lee, Junsu; Park, June
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Ultrafast Laser Spectroscopy of Two-Dimensional Materials Beyond Graphene
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Koperski, Maciej; Molas, Maciej R.; Arora, Ashish
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Colloidal synthesis of monolayer-thick formamidinium lead bromide perovskite nanosheets with a lateral size of micrometers
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Theoretical investigation of electron-hole complexes in anisotropic two-dimensional materials
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A dielectric-defined lateral heterojunction in a monolayer semiconductor
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Utama, M. Iqbal Bakti; Kleemann, Hans; Zhao, Wenyu
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Bosonic interactions in a nonlocal theory in ( $2 + 1$ ) dimensions
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Direct determination of monolayer MoS ₂ and WSe ₂ exciton binding energies on insulating and metallic substrates
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Park, Soohyung; Mutz, Niklas; Schultz, Thorsten
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Onset of exciton-exciton annihilation in single-layer black phosphorus
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Surrente, A.; Mitioglu, A. A.; Galkowski, K.
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Ultrafast exciton dynamics in chemical heterogenous WSe ₂ monolayer
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Nan, Fan; Qiu, Yun-Hang; Zhou, Li
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Two-dimensional excitons in monolayer transition metal dichalcogenides from radial equation and variational calculations
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Improved luminescence properties of MoS ₂ monolayers grown via MOCVD: role of pre-treatment and growth parameters
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Andrzejewski, D.; Marx, M.; Grundmann, A.
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Orbital, spin and valley contributions to Zeeman splitting of excitonic resonances in MoSe ₂ , WSe ₂ and WS ₂ Monolayers
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Koperski, Maciej; Molas, Maciej R.; Arora, Ashish
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1s-intraexcitonic dynamics in monolayer MoS2 probed by ultrafast mid-infrared spectroscopy
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Noninvasive control of excitons in two-dimensional materials
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Large second harmonic generation in alloyed TMDs and boron nitride nanostructures
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Two-dimensional transition-metal dichalcogenide materials: Toward an age of atomic-scale photonics
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Modulation of New Excitons in Transition Metal Dichalcogenide‐Perovskite Oxide System
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Exciton broadening in ${WS}_{2}$ /graphene heterostructures
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Exciton broadening in WS2 /graphene heterostructures
text, January 2017

Hill, Heather M.; Rigosi, Albert F.; Raja, Archana
Universität Regensburg
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Binding energies of exciton complexes in transition metal dichalcogenides and effect of dielectric environment
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Kylänpää, Ilkka; Komsa, Hannu-Pekka
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Steinhoff, Alexander; Florian, Matthias; Rösner, Malte
arXiv
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Onset of exciton-exciton annihilation in single layer black phosphorus
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Surrente, A.; Mitioglu, A. A.; Galkowski, K.
arXiv
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text, January 2016

Thilagam, A.
arXiv
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Trushin, Maxim; Goerbig, Mark Oliver; Belzig, Wolfgang
arXiv
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Exciton Relaxation Cascade in Two-dimensional Transition-metal dichalcogenides
text, January 2017

Brem, Samuel; Berghaeuser, Gunnar; Selig, Malte
arXiv
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Orbital, spin and valley contributions to Zeeman splitting of excitonic resonances in MoSe$_2$, WSe$_2$ and WS$_2$ monolayers
preprint, January 2018

Koperski, M.; Molas, M. R.; Arora, A.
arXiv
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Defect-induced modification of low-lying excitons and valley selectivity in monolayer transition metal dichalcogenides
text, January 2018

Refaely-Abramson, Sivan; Qiu, Diana Y.; Louie, Steven G.
arXiv
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Fundamental exciton linewidth broadening in monolayer transition metal dichalcogenides
text, January 2019

Gupta, Garima; Majumdar, Kausik
arXiv
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Intrinsic Lifetime of Higher Excitonic States in Tungsten Diselenide Monolayers
text, January 2019

Brem, Samuel; Zipfel, Jonas; Selig, Malte
arXiv
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Hybrid MoS$_2$-gap-mode metasurfaces photodetectors
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Ni, Peinan; Bugallo, Andres De Luna; Yang, Xun
arXiv
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Colloquium : Excitons in atomically thin transition metal dichalcogenides
text, January 2018

Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M.
Universität Regensburg
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Modulation of New Excitons in Transition Metal Dichalcogenide‐Perovskite Oxide System
journal, April 2019

Yin, Xinmao; Yang, Ming; Tang, Chi Sin
Advanced Science, Vol. 6, Issue 12
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1s-intraexcitonic dynamics in monolayer MoS2 probed by ultrafast mid-infrared spectroscopy
journal, February 2016

Cha, Soonyoung; Sung, Ji Ho; Sim, Sangwan
Nature Communications, Vol. 7, Issue 1
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Cascaded exciton energy transfer in a monolayer semiconductor lateral heterostructure assisted by surface plasmon polariton
journal, June 2017

Shi, Jinwei; Lin, Meng-Hsien; Chen, I-Tung
Nature Communications, Vol. 8, Issue 1
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Scaling law for excitons in 2D perovskite quantum wells
journal, June 2018

Blancon, J. -C.; Stier, A. V.; Tsai, H.
Nature Communications, Vol. 9, Issue 1
DOI: 10.1038/s41467-018-04659-x

Exciton Relaxation Cascade in two-dimensional Transition Metal Dichalcogenides
journal, May 2018

Brem, Samuel; Selig, Malte; Berghaeuser, Gunnar
Scientific Reports, Vol. 8, Issue 1
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Large second harmonic generation in alloyed TMDs and boron nitride nanostructures
journal, July 2018

Lucking, Michael C.; Beach, Kory; Terrones, Humberto
Scientific Reports, Vol. 8, Issue 1
DOI: 10.1038/s41598-018-27702-9

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Title: Observation of Excitonic Rydberg States in Monolayer MoS2 and WS2 by Photoluminescence Excitation Spectroscopy

Abstract

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Temperature dependent photoluminescence from WS2 nanostructures journal, October 2018

Dielectric disorder in two-dimensional materials journal, August 2019

Binding energies of exciton complexes in transition metal dichalcogenide monolayers and effect of dielectric environment journal, November 2015

Optical nonlinearities of excitons in monolayer MoS 2 journal, April 2018

Engineering of optical and electronic band gaps in transition metal dichalcogenide monolayers through external dielectric screening journal, October 2017

Impact of substrate induced band tail states on the electronic and optical properties of MoS 2 journal, December 2019

Layer-modulated two-photon absorption in MoS 2 : probing the shift of the excitonic dark state and band-edge journal, January 2019

Title: Observation of Excitonic Rydberg States in Monolayer MoS₂ and WS₂ by Photoluminescence Excitation Spectroscopy

Atomically Thin ${MoS}_{2}$ A New Direct-Gap Semiconductor
journal, September 2010

Emerging Photoluminescence in Monolayer MoS₂
journal, April 2010

Evolution of Electronic Structure in Atomically Thin Sheets of WS ₂ and WSe ₂
journal, December 2012

Optical Properties and Band Gap of Single- and Few-Layer MoTe ₂ Crystals
journal, October 2014

Photoluminescence from Chemically Exfoliated MoS₂
journal, December 2011

Extraordinary Sunlight Absorption and One Nanometer Thick Photovoltaics Using Two-Dimensional Monolayer Materials
journal, July 2013

Strong Light-Matter Interactions in Heterostructures of Atomically Thin Films
journal, May 2013

Charge Dynamics and Electronic Structures of Monolayer MoS ₂ Films Grown by Chemical Vapor Deposition
journal, December 2013

Measurement of the optical dielectric function of monolayer transition-metal dichalcogenides: ${MoS}_{2}$ , $Mo S e_{2}$ , ${WS}_{2}$ , and $WS e_{2}$
journal, November 2014

Photoluminescence of freestanding single- and few-layer ${MoS}_{2}$
journal, March 2014

Investigation of the optical properties of MoS ₂ thin films using spectroscopic ellipsometry
journal, March 2014

Valley-selective circular dichroism of monolayer molybdenum disulphide
journal, January 2012

Control of valley polarization in monolayer MoS2 by optical helicity
journal, June 2012

Robust optical emission polarization in MoS $_{2}$ monolayers through selective valley excitation
journal, August 2012

Valley polarization in MoS2 monolayers by optical pumping
journal, June 2012

Coupled Spin and Valley Physics in Monolayers of ${MoS}_{2}$ and Other Group-VI Dichalcogenides
journal, May 2012

Optical generation of excitonic valley coherence in monolayer WSe2
journal, August 2013

Carrier and Polarization Dynamics in Monolayer ${MoS}_{2}$
journal, January 2014

The valley Hall effect in MoS2 transistors
journal, June 2014

Valley dynamics probed through charged and neutral exciton emission in monolayer ${WSe}_{2}$
journal, August 2014

Spin and pseudospins in layered transition metal dichalcogenides
journal, April 2014

Electronics and optoelectronics of two-dimensional transition metal dichalcogenides
journal, November 2012

Progress, Challenges, and Opportunities in Two-Dimensional Materials Beyond Graphene
journal, March 2013

Emerging Device Applications for Semiconducting Two-Dimensional Transition Metal Dichalcogenides
journal, January 2014

Synthesis of Large-Area MoS₂ Atomic Layers with Chemical Vapor Deposition
journal, March 2012

Extraordinary Room-Temperature Photoluminescence in Triangular WS ₂ Monolayers
journal, December 2012

Synthesis and Transfer of Single-Layer Transition Metal Disulfides on Diverse Surfaces
journal, March 2013

Vapour phase growth and grain boundary structure of molybdenum disulphide atomic layers
journal, June 2013

Grains and grain boundaries in highly crystalline monolayer molybdenum disulphide
journal, May 2013

Vertical and in-plane heterostructures from WS₂/MoS₂ monolayers
journal, September 2014

Chemical Vapor Deposition Growth of Crystalline Monolayer MoSe₂
journal, April 2014

Tightly bound trions in monolayer MoS2
journal, December 2012

Electrical control of neutral and charged excitons in a monolayer semiconductor
journal, February 2013

Quasiparticle band structure calculation of monolayer, bilayer, and bulk MoS $_{2}$
journal, May 2012

Strain-engineered artificial atom as a broad-spectrum solar energy funnel
journal, November 2012

Effects of confinement and environment on the electronic structure and exciton binding energy of MoS $_{2}$ from first principles
journal, December 2012

Large excitonic effects in monolayers of molybdenum and tungsten dichalcogenides
journal, September 2012

How dielectric screening in two-dimensional crystals affects the convergence of excited-state calculations: Monolayer MoS $_{2}$
journal, December 2013

Effect of spin-orbit interaction on the optical spectra of single-layer, double-layer, and bulk MoS $_{2}$
journal, July 2013

Optical Spectrum of ${MoS}_{2}$ : Many-Body Effects and Diversity of Exciton States
journal, November 2013

Quasiparticle band structures and optical properties of strained monolayer MoS $_{2}$ and WS $_{2}$
journal, April 2013

Analytical approach to excitonic properties of MoS $_{2}$
journal, March 2014

Influence of Excited Carriers on the Optical and Electronic Properties of MoS ₂
journal, June 2014

Exciton band structure of monolayer ${MoS}_{2}$
journal, February 2015

Tightly Bound Excitons in Monolayer ${WSe}_{2}$
journal, July 2014

Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer ${WS}_{2}$
journal, August 2014

Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
journal, August 2014

Probing excitonic dark states in single-layer tungsten disulphide
journal, August 2014

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

Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy
journal, October 2014

Band nesting and the optical response of two-dimensional semiconducting transition metal dichalcogenides
journal, September 2013

Observation of Rapid Exciton–Exciton Annihilation in Monolayer Molybdenum Disulfide
journal, September 2014

Measurement of the Optical Conductivity of Graphene
journal, November 2008

Photocarrier relaxation pathway in two-dimensional semiconducting transition metal dichalcogenides
journal, July 2014

Femtosecond THz studies of intra-excitonic transitions
journal, June 2008

Exciton Relaxation Cascade in two-dimensional Transition Metal Dichalcogenides
journal, May 2018

Defect-Induced Modification of Low-Lying Excitons and Valley Selectivity in Monolayer Transition Metal Dichalcogenides
journal, October 2018

Magnetophotoluminescence of exciton Rydberg states in monolayer $WS e_{2}$
journal, May 2019

Room temperature observation of biexcitons in exfoliated WS ₂ monolayers
journal, May 2017

Strain dependence of band gaps and exciton energies in pure and mixed transition-metal dichalcogenides
journal, October 2016

Interlayer screening effects in WS ₂ /WSe ₂ van der Waals hetero-bilayer
journal, August 2018

Photonics and optoelectronics of two-dimensional materials beyond graphene
journal, October 2016

Why all the fuss about 2D semiconductors?
journal, March 2016

Screening and many-body effects in two-dimensional crystals: Monolayer ${MoS}_{2}$
journal, June 2016

Optical absorption by Dirac excitons in single-layer transition-metal dichalcogenides
journal, July 2016

Biexcitons in monolayer transition metal dichalcogenides tuned by magnetic fields
journal, September 2018

Atomic-scale defects and electronic properties of a transferred synthesized MoS ₂ monolayer
journal, May 2018

Ultrafast formation and dynamics of interlayer exciton in a large-area CVD-grown WS ₂ /WSe ₂ heterostructure
journal, November 2018

Exciton states in monolayer MoSe ₂ : impact on interband transitions
journal, November 2015

Resonance Profiles of Valley Polarization in Single-Layer ${MoS}_{2}$ and ${MoSe}_{2}$
journal, October 2018

Temperature dependent photoluminescence from WS2 nanostructures
journal, October 2018

Dielectric disorder in two-dimensional materials
journal, August 2019

Binding energies of exciton complexes in transition metal dichalcogenide monolayers and effect of dielectric environment
journal, November 2015

Optical nonlinearities of excitons in monolayer ${MoS}_{2}$
journal, April 2018

Engineering of optical and electronic band gaps in transition metal dichalcogenide monolayers through external dielectric screening
journal, October 2017

Impact of substrate induced band tail states on the electronic and optical properties of MoS ₂
journal, December 2019

Layer-modulated two-photon absorption in MoS ₂ : probing the shift of the excitonic dark state and band-edge
journal, January 2019

Exciton formation assisted by longitudinal optical phonons in monolayer transition metal dichalcogenides
journal, September 2016

Ultrafast dynamics in van der Waals heterostructures
journal, November 2018