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Title: Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy

Abstract

The optical response of semiconducting monolayer transition-metal dichalcogenides (TMDCs) is dominated by strongly bound excitons that are stable even at room temperature. Nonetheless, substrate-related effects such as screening and disorder in currently available specimens mask many anticipated physical phenomena and limit device applications of TMDCs. Here, we demonstrate that that these undesirable effects are strongly suppressed in suspended devices. Extremely robust (photogain > 1,000) and fast (response time < 1 ms) photoresponse allow us to study, for the first time, the formation, binding energies, and dissociation mechanisms of excitons in TMDCs through photocurrent spectroscopy. By analyzing the spectral positions of peaks in the photocurrent and by comparing them with first-principles calculations, we obtain binding energies, band gaps and spin-orbit splitting in monolayer TMDCs. For monolayer MoS2, in particular, we obtain an extremely large binding energy for band-edge excitons, Ebind ≥ 570 meV. Along with band-edge excitons, we observe excitons associated with a van Hove singularity of rather unique nature. In conclusion, the analysis of the source-drain voltage dependence of photocurrent spectra reveals exciton dissociation and photoconversion mechanisms in TMDCs.

Authors:
 [1];  [1];  [1];  [1];  [1];  [2];  [1];  [3];  [4];  [1];  [5];  [6];  [3];  [1];  [2];  [1]
+ Show Author Affiliations
  1. Vanderbilt Univ., Nashville, TN (United States)
  2. Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  5. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  6. Fisk Univ., Nashville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1259492
Alternate Identifier(s):
OSTI ID: 1265274
Grant/Contract Number:  
FGO2-99ER45781; W911NF-07-R-0003-02; NSF ARI-R2 DMR-0963361; NSF EPS1004083; ONR- N000141310299; NSF CAREER DMR-1056859; HDTRA1-10-0047; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 4; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Electronic properties and materials; Nanoscience and technology; Nanosensors; Two-dimensional materials

Citation Formats

Klots, A. R., Newaz, A. K. M., Wang, Bin, Prasai, D., Krzyzanowska, H., Lin, Junhao, Caudel, D., Ghimire, N. J., Yan, J., Ivanov, B. L., Velizhanin, K. A., Burger, A., Mandrus, D. G., Tolk, N. H., Pantelides, S. T., and Bolotin, K. I. Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy. United States: N. p., 2014. Web. doi:10.1038/srep06608.
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Klots, A. R., Newaz, A. K. M., Wang, Bin, Prasai, D., Krzyzanowska, H., Lin, Junhao, Caudel, D., Ghimire, N. J., Yan, J., Ivanov, B. L., Velizhanin, K. A., Burger, A., Mandrus, D. G., Tolk, N. H., Pantelides, S. T., & Bolotin, K. I. Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy. United States. https://doi.org/10.1038/srep06608
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Klots, A. R., Newaz, A. K. M., Wang, Bin, Prasai, D., Krzyzanowska, H., Lin, Junhao, Caudel, D., Ghimire, N. J., Yan, J., Ivanov, B. L., Velizhanin, K. A., Burger, A., Mandrus, D. G., Tolk, N. H., Pantelides, S. T., and Bolotin, K. I. Thu . "Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy". United States. https://doi.org/10.1038/srep06608. https://www.osti.gov/servlets/purl/1259492.
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@article{osti_1259492,
title = {Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy},
author = {Klots, A. R. and Newaz, A. K. M. and Wang, Bin and Prasai, D. and Krzyzanowska, H. and Lin, Junhao and Caudel, D. and Ghimire, N. J. and Yan, J. and Ivanov, B. L. and Velizhanin, K. A. and Burger, A. and Mandrus, D. G. and Tolk, N. H. and Pantelides, S. T. and Bolotin, K. I.},
abstractNote = {The optical response of semiconducting monolayer transition-metal dichalcogenides (TMDCs) is dominated by strongly bound excitons that are stable even at room temperature. Nonetheless, substrate-related effects such as screening and disorder in currently available specimens mask many anticipated physical phenomena and limit device applications of TMDCs. Here, we demonstrate that that these undesirable effects are strongly suppressed in suspended devices. Extremely robust (photogain > 1,000) and fast (response time < 1 ms) photoresponse allow us to study, for the first time, the formation, binding energies, and dissociation mechanisms of excitons in TMDCs through photocurrent spectroscopy. By analyzing the spectral positions of peaks in the photocurrent and by comparing them with first-principles calculations, we obtain binding energies, band gaps and spin-orbit splitting in monolayer TMDCs. For monolayer MoS2, in particular, we obtain an extremely large binding energy for band-edge excitons, Ebind ≥ 570 meV. Along with band-edge excitons, we observe excitons associated with a van Hove singularity of rather unique nature. In conclusion, the analysis of the source-drain voltage dependence of photocurrent spectra reveals exciton dissociation and photoconversion mechanisms in TMDCs.},
doi = {10.1038/srep06608},
journal = {Scientific Reports},
number = ,
volume = 4,
place = {United States},
year = {Thu Oct 16 00:00:00 EDT 2014},
month = {Thu Oct 16 00:00:00 EDT 2014}
}
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    • DOI: 10.1039/c4cs00265b

    Influence of interlayer interactions on the relaxation dynamics of excitons in ultrathin MoS 2
    journal, January 2019

    • Lu, Dongxiao; Zhou, Qiang; Li, Fangfei
    • Nanoscale Advances, Vol. 1, Issue 3
    • DOI: 10.1039/c8na00086g

    Copper( i ) sulfide: a two-dimensional semiconductor with superior oxidation resistance and high carrier mobility
    journal, January 2019

    • Guo, Yu; Wu, Qisheng; Li, Yunhai
    • Nanoscale Horizons, Vol. 4, Issue 1
    • DOI: 10.1039/c8nh00216a

    Study on photoelectric characteristics of monolayer WS 2 films
    journal, January 2019

    • Wang, Lin; Wang, Wenyan; Wang, Quan
    • RSC Advances, Vol. 9, Issue 64
    • DOI: 10.1039/c9ra07924f

    Polarization and time-resolved photoluminescence spectroscopy of excitons in MoSe 2 monolayers
    journal, March 2015

    • Wang, G.; Palleau, E.; Amand, T.
    • Applied Physics Letters, Vol. 106, Issue 11
    • DOI: 10.1063/1.4916089

    DFT study of structural and electronic properties of MoS 2(1−x) Se 2x alloy (x = 0.25)
    journal, April 2018

    • Gusakova, Julia; Gusakov, Vasilii; Tay, Beng Kang
    • Journal of Applied Physics, Vol. 123, Issue 16
    • DOI: 10.1063/1.5011326

    Large-area MoS 2 -MoO x heterojunction thin-film photodetectors with wide spectral range and enhanced photoresponse
    journal, June 2019

    • Im, Healin; Liu, Na; Bala, Arindam
    • APL Materials, Vol. 7, Issue 6
    • DOI: 10.1063/1.5094586

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

    • Klein, J.; Kerelsky, A.; Lorke, M.
    • Applied Physics Letters, Vol. 115, Issue 26
    • DOI: 10.1063/1.5131270

    Electrical control of spatial resolution in mixed-dimensional heterostructured photodetectors
    journal, March 2019

    • Zhang, Ke; Wei, Yang; Zhang, Jin
    • Proceedings of the National Academy of Sciences, Vol. 116, Issue 14
    • DOI: 10.1073/pnas.1817229116

    Highly sensitive visible to infrared MoTe 2 photodetectors enhanced by the photogating effect
    journal, September 2016

    Micro-reflectance and transmittance spectroscopy: a versatile and powerful tool to characterize 2D materials
    journal, January 2017

    • Frisenda, Riccardo; Niu, Yue; Gant, Patricia
    • Journal of Physics D: Applied Physics, Vol. 50, Issue 7
    • DOI: 10.1088/1361-6463/aa5256

    Optical absorption by indirect excitons in a transition metal dichalcogenide/hexagonal boron nitride heterostructure
    journal, May 2018

    • Brunetti, Matthew N.; Berman, Oleg L.; Kezerashvili, Roman Ya
    • Journal of Physics: Condensed Matter, Vol. 30, Issue 22
    • DOI: 10.1088/1361-648x/aabe53

    Two-dimensional excitons in monolayer transition metal dichalcogenides from radial equation and variational calculations
    journal, January 2019

    k · p theory for two-dimensional transition metal dichalcogenide semiconductors
    journal, April 2015

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

    Brightening of dark excitons in monolayers of semiconducting transition metal dichalcogenides
    journal, January 2017

    Ultrasensitive tunability of the direct bandgap of 2D InSe flakes via strain engineering
    journal, January 2018

    The Computational 2D Materials Database: high-throughput modeling and discovery of atomically thin crystals
    journal, September 2018

    Roadmap on finding chiral valleys: screening 2D materials for valleytronics
    journal, June 2018

    Exciton broadening in WS 2 /graphene heterostructures
    journal, November 2017

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

    Dependence of Raman and absorption spectra of stacked bilayer MoS_2 on the stacking orientation
    journal, January 2016

    Localized plasmonic fields of nanoantennas enhance second harmonic generation from two-dimensional molybdenum disulfide
    journal, July 2018

    • Forcherio, Gregory T.; Bonacina, Luigi; Wolf, Jean-Pierre
    • MRS Communications, Vol. 8, Issue 03
    • DOI: 10.1557/mrc.2018.133

    Thickness-Dependent Differential Reflectance Spectra of Monolayer and Few-Layer MoS2, MoSe2, WS2 and WSe2
    journal, September 2018

    • Niu, Yue; Gonzalez-Abad, Sergio; Frisenda, Riccardo
    • Nanomaterials, Vol. 8, Issue 9
    • DOI: 10.3390/nano8090725

    Direct Observation of Monolayer MoS2 Prepared by CVD Using In-Situ Differential Reflectance Spectroscopy
    journal, November 2019

    Fast and Highly Sensitive Ionic-Polymer-Gated WS 2 -Graphene Photodetectors
    journal, April 2017

    • Mehew, Jake D.; Unal, Selim; Torres Alonso, Elias
    • Advanced Materials, Vol. 29, Issue 23
    • DOI: 10.1002/adma.201700222

    Many-Body Complexes in 2D Semiconductors
    journal, August 2018

    Observation of Novel Multifunctionalities in Monolayer CdO
    journal, September 2018

    Electrically tunable organic–inorganic hybrid polaritons with monolayer WS2
    journal, January 2017

    • Flatten, Lucas C.; Coles, David M.; He, Zhengyu
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms14097

    Dichroic spin–valley photocurrent in monolayer molybdenum disulphide
    journal, July 2015

    • Eginligil, Mustafa; Cao, Bingchen; Wang, Zilong
    • Nature Communications, Vol. 6, Issue 1
    • DOI: 10.1038/ncomms8636

    Band structure characterization of WS2 grown by chemical vapor deposition
    journal, June 2016

    • Tanabe, Iori; Gomez, Michael; Coley, William C.
    • Applied Physics Letters, Vol. 108, Issue 25
    • DOI: 10.1063/1.4954278

    Direct and indirect optical transitions in bulk and atomically thin MoS 2 studied by photoreflectance and photoacoustic spectroscopy
    journal, April 2019

    • Kopaczek, J.; Zelewski, S. J.; Polak, M. P.
    • Journal of Applied Physics, Vol. 125, Issue 13
    • DOI: 10.1063/1.5080300

    Investigation on nonlinear optical properties of MoS 2 nanoflakes grown on silicon and quartz substrates
    journal, April 2018

    • Bayesteh, Samaneh; Mortazavi, Seyedeh Zahra; Reyhani, Ali
    • Journal of Physics D: Applied Physics, Vol. 51, Issue 19
    • DOI: 10.1088/1361-6463/aab808

    Calculating excitons, plasmons, and quasiparticles in 2D materials and van der Waals heterostructures
    journal, June 2017

    Band structure engineering in van der Waals heterostructures via dielectric screening: the GΔW method
    journal, March 2017

    Semiconductor channel-mediated photodoping in h-BN encapsulated monolayer MoSe 2 phototransistors
    journal, March 2019

    Growth of MoS 2 nanoflakes near/far from tubular furnace axis and their impact on the efficiency enhancement of the Si solar cells
    journal, May 2019

    • Nikpay, Maryam Alsadat; Mortazavi, Seyedeh Zahra; Reyhani, Ali
    • Materials Research Express, Vol. 6, Issue 8
    • DOI: 10.1088/2053-1591/ab23c5

    Large-Area Growth of Uniform Single-Layer MoS2 Thin Films by Chemical Vapor Deposition
    journal, October 2015

    Effect of Doping on Hydrogen Evolution Reaction of Vanadium Disulfide Monolayer
    journal, December 2015

    Schottky-barrier modulation at germanium/monolayer MoS 2 heterojunction interface: the roles of passivation and interfacial layer
    journal, February 2020

    Exciton broadening in WS2 /graphene heterostructures
    text, January 2017

    • Hill, Heather M.; Rigosi, Albert F.; Raja, Archana
    • Universität Regensburg
    • DOI: 10.5283/epub.40515

    Effect of Processing Parameters on Monolayer MoS2 Prepared by APCVD in a Quasiclosed Crucible
    journal, May 2019

    Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide
    journal, September 2016

    • Plechinger, Gerd; Nagler, Philipp; Arora, Ashish
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms12715

    Strong interlayer hybridization in the aligned SnS2/WSe2 hetero-bilayer structure
    journal, July 2019

    • Zribi, Jihene; Khalil, Lama; Zheng, Biyuan
    • npj 2D Materials and Applications, Vol. 3, Issue 1
    • DOI: 10.1038/s41699-019-0109-3

    Transport properties of unrestricted carriers in bridge-channel MoS 2 field-effect transistors
    journal, January 2015

    • Qiu, Dongri; Lee, Dong Uk; Park, Chang Soo
    • Nanoscale, Vol. 7, Issue 41
    • DOI: 10.1039/c5nr04397b

    Magneto-optics in transition metal diselenide monolayers
    journal, June 2015

    Interlayer exciton dynamics in a dichalcogenide monolayer heterostructure
    journal, June 2017

    Direct versus indirect band gap emission and exciton-exciton annihilation in atomically thin molybdenum ditelluride ( MoTe 2 )
    journal, August 2016

    • Froehlicher, Guillaume; Lorchat, Etienne; Berciaud, Stéphane
    • Physical Review B, Vol. 94, Issue 8
    • DOI: 10.1103/physrevb.94.085429

    Determination of band offsets, hybridization, and exciton binding in 2D semiconductor heterostructures
    journal, February 2017

    • Wilson, Neil R.; Nguyen, Paul V.; Seyler, Kyle
    • Science Advances, Vol. 3, Issue 2
    • DOI: 10.1126/sciadv.1601832

    k.p theory for two-dimensional transition metal dichalcogenide semiconductors
    text, January 2014

    Fast and Highly Sensitive Ionic Polymer Gated WS$_2$-Graphene Photodetectors
    text, January 2017

    Simple vertex correction improves GW band energies of bulk and two-dimensional crystals
    text, January 2017

    Symmetry regimes for circular photocurrents in monolayer MoSe2
    text, January 2018

    Colloquium : Excitons in atomically thin transition metal dichalcogenides
    text, January 2018

    • Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M.
    • Universität Regensburg
    • DOI: 10.5283/epub.40518

    Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide
    journal, September 2016

    • Plechinger, Gerd; Nagler, Philipp; Arora, Ashish
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms12715

    Symmetry regimes for circular photocurrents in monolayer MoSe2
    journal, August 2018

    Ionic gate spectroscopy of 2D semiconductors
    journal, May 2021

    • Gutiérrez-Lezama, Ignacio; Ubrig, Nicolas; Ponomarev, Evgeniy
    • Nature Reviews Physics, Vol. 3, Issue 7
    • DOI: 10.1038/s42254-021-00317-2

    Effect of interlayer interactions on exciton luminescence in atomic-layered MoS2 crystals
    journal, July 2016

    • Kim, Jung Gon; Yun, Won Seok; Jo, Sunghwan
    • Scientific Reports, Vol. 6, Issue 1
    • DOI: 10.1038/srep29813

    An anomalous interlayer exciton in MoS2
    journal, November 2016

    • Azhikodan, Dilna; Nautiyal, Tashi; Shallcross, Sam
    • Scientific Reports, Vol. 6, Issue 1
    • DOI: 10.1038/srep37075

    Electrical control of spatial resolution in mixed-dimensional heterostructured photodetectors
    journal, March 2019

    • Zhang, Ke; Wei, Yang; Zhang, Jin
    • Proceedings of the National Academy of Sciences, Vol. 116, Issue 14
    • DOI: 10.1073/pnas.1817229116

    Exciton-dominated Dielectric Function of Atomically Thin MoS2 Films
    preprint, January 2015

    Band parameters and hybridization in 2D semiconductor heterostructures from photoemission spectroscopy
    preprint, January 2016

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