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

Journal Article · · Nano Letters
DOI:https://doi.org/10.1021/nl504868p· OSTI ID:1370381

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.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Re-Defining Photovoltaic Efficiency Through Molecule Scale Control (RPEMSC)
Sponsoring Organization:
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
Grant/Contract Number:
SC0001085; DMR-1122594; DGE-1069240; AC02-98CH10886; AC05-06OR23100
OSTI ID:
1370381
Journal Information:
Nano Letters, Vol. 15, Issue 5; Related Information: RPEMSC partners with Columbia University (lead); Brookhaven National Laboratory; Purdue University; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 280 works
Citation information provided by
Web of Science

References (55)

Atomically Thin MoS2 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

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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
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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
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Excitonic properties of semiconducting monolayer and bilayer MoT e 2 journal October 2016
Observation of Novel Multifunctionalities in Monolayer CdO journal September 2018
Model Prediction of Self-Rotating Excitons in Two-Dimensional Transition-Metal Dichalcogenides journal May 2018
Excitonic Properties of Chemically Synthesized 2D Organic-Inorganic Hybrid Perovskite Nanosheets journal March 2018
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Nonequilibrium Carrier Dynamics in Transition Metal Dichalcogenide Semiconductors text January 2016
Onset of exciton-exciton annihilation in single layer black phosphorus text January 2016
Exciton formation assisted by longitudinal optical phonons in monolayer transition metal dichalcogenides text January 2016
Model Prediction of Self-Rotating Excitons in Two-Dimensional Transition-Metal Dichalcogenides text January 2017
Exciton Relaxation Cascade in Two-dimensional Transition-metal dichalcogenides text January 2017
Orbital, spin and valley contributions to Zeeman splitting of excitonic resonances in MoSe$_2$, WSe$_2$ and WS$_2$ monolayers preprint January 2018
Defect-induced modification of low-lying excitons and valley selectivity in monolayer transition metal dichalcogenides text January 2018
Fundamental exciton linewidth broadening in monolayer transition metal dichalcogenides text January 2019
Intrinsic Lifetime of Higher Excitonic States in Tungsten Diselenide Monolayers text January 2019
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Colloquium : Excitons in atomically thin transition metal dichalcogenides text January 2018
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