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

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.

doi:10.1038/srep06608

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

Journal Article · Thu Oct 16 00:00:00 EDT 2014 · Scientific Reports

DOI:https://doi.org/10.1038/srep06608· OSTI ID:1259492

Klots, A. R. ^[1]; Newaz, A. K. M. ^[1]; Wang, Bin ^[1]; Prasai, D. ^[1]; Krzyzanowska, H. ^[1]; Lin, Junhao ^[2]; Caudel, D. ^[1]; Ghimire, N. J. ^[3]; Yan, J. ^[4]; Ivanov, B. L. ^[1]; Velizhanin, K. A. ^[5]; Burger, A. ^[6]; Mandrus, D. G. ^[3]; Tolk, N. H. ^[1]; Pantelides, S. T. ^[2]; Bolotin, K. I. ^[1]

Vanderbilt Univ., Nashville, TN (United States)
Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Fisk Univ., Nashville, TN (United States)

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, E_bind ≥ 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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

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

OSTI ID:: 1259492

Alternate ID(s):: OSTI ID: 1265274

Journal Information:: Scientific Reports, Vol. 4; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 330 works

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Two-dimensional excitons in monolayer transition metal dichalcogenides from radial equation and variational calculations Zhang, J-Z; Ma, J-Z Journal of Physics: Condensed Matter, Vol. 31, Issue 10 https://doi.org/10.1088/1361-648x/aaf8c5	journal	January 2019
k · p theory for two-dimensional transition metal dichalcogenide semiconductors Kormányos, Andor; Burkard, Guido; Gmitra, Martin 2D Materials, Vol. 2, Issue 2 https://doi.org/10.1088/2053-1583/2/2/022001	journal	April 2015
Exciton states in monolayer MoSe ₂ : impact on interband transitions Wang, G.; Gerber, I. C.; Bouet, L. 2D Materials, Vol. 2, Issue 4 https://doi.org/10.1088/2053-1583/2/4/045005	journal	November 2015
Brightening of dark excitons in monolayers of semiconducting transition metal dichalcogenides Molas, M. R.; Faugeras, C.; Slobodeniuk, A. O. 2D Materials, Vol. 4, Issue 2 https://doi.org/10.1088/2053-1583/aa5521	journal	January 2017
Ultrasensitive tunability of the direct bandgap of 2D InSe flakes via strain engineering Li, Yang; Wang, Tianmeng; Wu, Meng 2D Materials, Vol. 5, Issue 2 https://doi.org/10.1088/2053-1583/aaa6eb	journal	January 2018
The Computational 2D Materials Database: high-throughput modeling and discovery of atomically thin crystals Haastrup, Sten; Strange, Mikkel; Pandey, Mohnish 2D Materials, Vol. 5, Issue 4 https://doi.org/10.1088/2053-1583/aacfc1	journal	September 2018
Roadmap on finding chiral valleys: screening 2D materials for valleytronics Bussolotti, Fabio; Kawai, Hiroyo; Ooi, Zi En Nano Futures, Vol. 2, Issue 3 https://doi.org/10.1088/2399-1984/aac9d7	journal	June 2018
Exciton broadening in ${WS}_{2}$ /graphene heterostructures Hill, Heather M.; Rigosi, Albert F.; Raja, Archana Physical Review B, Vol. 96, Issue 20 https://doi.org/10.1103/physrevb.96.205401	journal	November 2017
Optical nonlinearities of excitons in monolayer ${MoS}_{2}$ Soh, Daniel B. S.; Rogers, Christopher; Gray, Dodd J. Physical Review B, Vol. 97, Issue 16 https://doi.org/10.1103/physrevb.97.165111	journal	April 2018
Dependence of Raman and absorption spectra of stacked bilayer MoS_2 on the stacking orientation Park, Seki; Kim, Hyun; Kim, Min Su Optics Express, Vol. 24, Issue 19 https://doi.org/10.1364/oe.24.021551	journal	January 2016
Localized plasmonic fields of nanoantennas enhance second harmonic generation from two-dimensional molybdenum disulfide Forcherio, Gregory T.; Bonacina, Luigi; Wolf, Jean-Pierre MRS Communications, Vol. 8, Issue 03 https://doi.org/10.1557/mrc.2018.133	journal	July 2018
Two-dimensional transition-metal dichalcogenide materials: Toward an age of atomic-scale photonics Cao, Linyou MRS Bulletin, Vol. 40, Issue 7 https://doi.org/10.1557/mrs.2015.144	journal	July 2015
Thickness-Dependent Differential Reflectance Spectra of Monolayer and Few-Layer MoS2, MoSe2, WS2 and WSe2 Niu, Yue; Gonzalez-Abad, Sergio; Frisenda, Riccardo Nanomaterials, Vol. 8, Issue 9 https://doi.org/10.3390/nano8090725	journal	September 2018
Direct Observation of Monolayer MoS2 Prepared by CVD Using In-Situ Differential Reflectance Spectroscopy Wang, Yina; Zhang, Lei; Su, Chenhui Nanomaterials, Vol. 9, Issue 11 https://doi.org/10.3390/nano9111640	journal	November 2019
Fast and Highly Sensitive Ionic-Polymer-Gated WS ₂ -Graphene Photodetectors Mehew, Jake D.; Unal, Selim; Torres Alonso, Elias Advanced Materials, Vol. 29, Issue 23 https://doi.org/10.1002/adma.201700222	journal	April 2017
Many-Body Complexes in 2D Semiconductors Pei, Jiajie; Yang, Jiong; Yildirim, Tanju Advanced Materials, Vol. 31, Issue 2 https://doi.org/10.1002/adma.201706945	journal	August 2018
Observation of Novel Multifunctionalities in Monolayer CdO Ekuma, Chinedu E. Advanced Theory and Simulations, Vol. 1, Issue 12 https://doi.org/10.1002/adts.201800107	journal	September 2018
Electrically tunable organic–inorganic hybrid polaritons with monolayer WS2 Flatten, Lucas C.; Coles, David M.; He, Zhengyu Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14097	journal	January 2017
Dichroic spin–valley photocurrent in monolayer molybdenum disulphide Eginligil, Mustafa; Cao, Bingchen; Wang, Zilong Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8636	journal	July 2015
Band structure characterization of WS2 grown by chemical vapor deposition Tanabe, Iori; Gomez, Michael; Coley, William C. Applied Physics Letters, Vol. 108, Issue 25 https://doi.org/10.1063/1.4954278	journal	June 2016
Direct and indirect optical transitions in bulk and atomically thin MoS ₂ studied by photoreflectance and photoacoustic spectroscopy Kopaczek, J.; Zelewski, S. J.; Polak, M. P. Journal of Applied Physics, Vol. 125, Issue 13 https://doi.org/10.1063/1.5080300	journal	April 2019
Investigation on nonlinear optical properties of MoS 2 nanoflakes grown on silicon and quartz substrates Bayesteh, Samaneh; Mortazavi, Seyedeh Zahra; Reyhani, Ali Journal of Physics D: Applied Physics, Vol. 51, Issue 19 https://doi.org/10.1088/1361-6463/aab808	journal	April 2018
Calculating excitons, plasmons, and quasiparticles in 2D materials and van der Waals heterostructures Thygesen, Kristian Sommer 2D Materials, Vol. 4, Issue 2 https://doi.org/10.1088/2053-1583/aa6432	journal	June 2017
Band structure engineering in van der Waals heterostructures via dielectric screening: the GΔW method Winther, Kirsten T.; Thygesen, Kristian S. 2D Materials, Vol. 4, Issue 2 https://doi.org/10.1088/2053-1583/aa6531	journal	March 2017
Semiconductor channel-mediated photodoping in h-BN encapsulated monolayer MoSe ₂ phototransistors Quereda, Jorge; Ghiasi, Talieh S.; van der Wal, Caspar H. 2D Materials, Vol. 6, Issue 2 https://doi.org/10.1088/2053-1583/ab0c2d	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 Nikpay, Maryam Alsadat; Mortazavi, Seyedeh Zahra; Reyhani, Ali Materials Research Express, Vol. 6, Issue 8 https://doi.org/10.1088/2053-1591/ab23c5	journal	May 2019
Theoretical investigations of the anisotropic optical properties of distorted $1 T {ReS}_{2}$ and ${ReSe}_{2}$ monolayers, bilayers, and in the bulk limit Echeverry, J. P.; Gerber, I. C. Physical Review B, Vol. 97, Issue 7 https://doi.org/10.1103/physrevb.97.075123	journal	February 2018
Large-Area Growth of Uniform Single-Layer MoS2 Thin Films by Chemical Vapor Deposition Baek, Seung Hyun; Choi, Yura; Choi, Woong Nanoscale Research Letters, Vol. 10, Issue 1 https://doi.org/10.1186/s11671-015-1094-x	journal	October 2015
Effect of Doping on Hydrogen Evolution Reaction of Vanadium Disulfide Monolayer Qu, Yuanju; Pan, Hui; Kwok, Chi Tat Nanoscale Research Letters, Vol. 10, Issue 1 https://doi.org/10.1186/s11671-015-1182-y	journal	December 2015
Schottky-barrier modulation at germanium/monolayer MoS ₂ heterojunction interface: the roles of passivation and interfacial layer Ma, Xiaolei; Jiang, Xiangwei; Li, Yuan Applied Physics Express, Vol. 13, Issue 2 https://doi.org/10.35848/1882-0786/ab6f2a	journal	February 2020
Exciton broadening in WS2 /graphene heterostructures Hill, Heather M.; Rigosi, Albert F.; Raja, Archana Universität Regensburg https://doi.org/10.5283/epub.40515	text	January 2017
Effect of Processing Parameters on Monolayer MoS2 Prepared by APCVD in a Quasiclosed Crucible Yang, Yong; Pu, Hongbin; Li, Lianbi Journal of Electronic Materials, Vol. 48, Issue 8 https://doi.org/10.1007/s11664-019-07297-1	journal	May 2019
Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide Plechinger, Gerd; Nagler, Philipp; Arora, Ashish Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms12715	journal	September 2016
Strong interlayer hybridization in the aligned SnS2/WSe2 hetero-bilayer structure Zribi, Jihene; Khalil, Lama; Zheng, Biyuan npj 2D Materials and Applications, Vol. 3, Issue 1 https://doi.org/10.1038/s41699-019-0109-3	journal	July 2019
Transport properties of unrestricted carriers in bridge-channel MoS ₂ field-effect transistors Qiu, Dongri; Lee, Dong Uk; Park, Chang Soo Nanoscale, Vol. 7, Issue 41 https://doi.org/10.1039/c5nr04397b	journal	January 2015
Magneto-optics in transition metal diselenide monolayers Wang, G.; Bouet, L.; Glazov, M. M. 2D Materials, Vol. 2, Issue 3 https://doi.org/10.1088/2053-1583/2/3/034002	journal	June 2015
Interlayer exciton dynamics in a dichalcogenide monolayer heterostructure Nagler, Philipp; Plechinger, Gerd; Ballottin, Mariana V. 2D Materials, Vol. 4, Issue 2 https://doi.org/10.1088/2053-1583/aa7352	journal	June 2017
Direct versus indirect band gap emission and exciton-exciton annihilation in atomically thin molybdenum ditelluride $({MoTe}_{2})$ Froehlicher, Guillaume; Lorchat, Etienne; Berciaud, Stéphane Physical Review B, Vol. 94, Issue 8 https://doi.org/10.1103/physrevb.94.085429	journal	August 2016
Determination of band offsets, hybridization, and exciton binding in 2D semiconductor heterostructures Wilson, Neil R.; Nguyen, Paul V.; Seyler, Kyle Science Advances, Vol. 3, Issue 2 https://doi.org/10.1126/sciadv.1601832	journal	February 2017
k.p theory for two-dimensional transition metal dichalcogenide semiconductors Kormányos, Andor; Burkard, Guido; Gmitra, Martin arXiv https://doi.org/10.48550/arxiv.1410.6666	text	January 2014
Polarization and time-resolved photoluminescence spectroscopy of excitons in MoSe2 monolayers Wang, G.; Palleau, E.; Amand, T. arXiv https://doi.org/10.48550/arxiv.1502.03591	text	January 2015
Fast and Highly Sensitive Ionic Polymer Gated WS$_2$-Graphene Photodetectors Mehew, Jake D.; Unal, Selim; Alonso, Elias Torres arXiv https://doi.org/10.48550/arxiv.1704.07642	text	January 2017
Simple vertex correction improves GW band energies of bulk and two-dimensional crystals Schmidt, Per S.; Patrick, Christopher E.; Thygesen, Kristian S. arXiv https://doi.org/10.48550/arxiv.1711.02922	text	January 2017
Symmetry regimes for circular photocurrents in monolayer MoSe2 Quereda, Jorge; Ghiasi, Talieh S.; You, Jhih-Shih arXiv https://doi.org/10.48550/arxiv.1803.08289	text	January 2018
Thickness-Dependent Differential Reflectance Spectra of Monolayer and Few-Layer MoS2, MoSe2, WS2 and WSe2 Niu, Yue; Gonzalez-Abad, Sergio; Frisenda, Riccardo arXiv https://doi.org/10.48550/arxiv.1810.04745	text	January 2018
Colloquium : Excitons in atomically thin transition metal dichalcogenides Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M. Universität Regensburg https://doi.org/10.5283/epub.40518	text	January 2018
Ionic gate spectroscopy of 2D semiconductors Gutiérrez-Lezama, Ignacio; Ubrig, Nicolas; Ponomarev, Evgeniy Nature Reviews Physics, Vol. 3, Issue 7 https://doi.org/10.1038/s42254-021-00317-2	journal	May 2021
An anomalous interlayer exciton in MoS2 Azhikodan, Dilna; Nautiyal, Tashi; Shallcross, Sam Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep37075	journal	November 2016
Exciton-dominated Dielectric Function of Atomically Thin MoS2 Films Yu, Yiling; Yu, Yifei; Cai, Yongqing arXiv https://doi.org/10.48550/arxiv.1510.03121	preprint	January 2015
Band parameters and hybridization in 2D semiconductor heterostructures from photoemission spectroscopy Wilson, Neil R.; Nguyen, Paul V.; Seyler, Kyle L. arXiv https://doi.org/10.48550/arxiv.1601.05865	preprint	January 2016
Efficient ionization of two dimensional excitons by intense single cycle terahertz pulses Kamban, Høgni C.; Pedersen, Thomas G. arXiv https://doi.org/10.48550/arxiv.2103.12463	text	January 2021

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