Giant spin-splitting and gap renormalization driven by trions in single-layer WS2/h-BN heterostructures

Katoch, Jyoti; Ulstrup, Soren; Koch, Roland J.; Moser, Simon; McCreary, Kathleen M.; Singh, Simranjeet; Xu, Jinsong; Jonker, Berend T.; Kawakami, Roland K.; Bostwick, Aaron; Rotenberg, Eli; Jozwiak, Chris

doi:10.1038/s41567-017-0033-4

Title: Giant spin-splitting and gap renormalization driven by trions in single-layer WS₂/h-BN heterostructures

Journal Article · Mon Jan 22 00:00:00 EST 2018 · Nature Physics

DOI:https://doi.org/10.1038/s41567-017-0033-4· OSTI ID:1462967

^[1];

^[2];

^[3];

^[4]; Singh, Simranjeet ^[1]; Xu, Jinsong ^[1];

^[4];

^[1]; Bostwick, Aaron ^[3];

^[3];

^[3]

The Ohio State Univ., Columbus, OH (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Aarhus Univ., Aarhus C (Denmark)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Naval Research Lab., Washington, D.C. (United States)

In two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs), new electronic phenomena such as tunable bandgaps and strongly bound excitons and trions emerge from strong many-body effects, beyond the spin and valley degrees of freedom induced by spin-orbit coupling and by lattice symmetry. Combining single-layer TMDs with other 2D materials in van der Waals heterostructures offers an intriguing means of controlling the electronic properties through these many-body effects, by means of engineered interlayer interactions. Here, we use micro-focused angle-resolved photoemission spectroscopy (microARPES) and in situ surface doping to manipulate the electronic structure of single-layer WS₂ on hexagonal boron nitride (WS₂/h-BN). Upon electron doping, we observe an unexpected giant renormalization of the spin-orbit splitting of the single-layer WS₂ valence band, from 430 meV to 660 meV, together with a bandgap reduction of at least 325 meV, attributed to the formation of trionic quasiparticles. Furthermore, these findings suggest that the electronic, spintronic and excitonic properties are widely tunable in 2D TMD/h-BN heterostructures, as these are intimately linked to the quasiparticle dynamics of the materials.

View Accepted Manuscript (DOE)

Cite

Export

Save

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

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1462967

Journal Information:: Nature Physics, Vol. 14, Issue 4; Related Information: © 2017 The Author(s).; ISSN 1745-2473

Publisher:: Nature Publishing Group (NPG)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 68 works

Citation information provided by
Web of Science

References (33)

Coupled Spin and Valley Physics in Monolayers of ${MoS}_{2}$ and Other Group-VI Dichalcogenides Xiao, Di; Liu, Gui-Bin; Feng, Wanxiang Physical Review Letters, Vol. 108, Issue 19 https://doi.org/10.1103/PhysRevLett.108.196802	journal	May 2012
Direct Measurement of the Thickness-Dependent Electronic Band Structure of ${MoS}_{2}$ Using Angle-Resolved Photoemission Spectroscopy Jin, Wencan; Yeh, Po-Chun; Zaki, Nader Physical Review Letters, Vol. 111, Issue 10 https://doi.org/10.1103/PhysRevLett.111.106801	journal	September 2013
Negative electronic compressibility and tunable spin splitting in WSe2 Riley, J. M.; Meevasana, W.; Bawden, L. Nature Nanotechnology, Vol. 10, Issue 12 https://doi.org/10.1038/nnano.2015.217	journal	September 2015
Direct observation of the transition from indirect to direct bandgap in atomically thin epitaxial MoSe2 Zhang, Yi; Chang, Tay-Rong; Zhou, Bo Nature Nanotechnology, Vol. 9, Issue 2 https://doi.org/10.1038/nnano.2013.277	journal	December 2013
Spatially Resolved Electronic Properties of Single-Layer WS ₂ on Transition Metal Oxides Ulstrup, Søren; Katoch, Jyoti; Koch, Roland J. ACS Nano, Vol. 10, Issue 11 https://doi.org/10.1021/acsnano.6b04914	journal	October 2016
Gaps induced by inversion symmetry breaking and second-generation Dirac cones in graphene/hexagonal boron nitride Wang, Eryin; Lu, Xiaobo; Ding, Shijie Nature Physics, Vol. 12, Issue 12 https://doi.org/10.1038/nphys3856	journal	August 2016
Van der Waals heterostructures Geim, A. K.; Grigorieva, I. V. Nature, Vol. 499, Issue 7459, p. 419-425 https://doi.org/10.1038/nature12385	journal	July 2013
Spin and pseudospins in layered transition metal dichalcogenides Xu, Xiaodong; Yao, Wang; Xiao, Di Nature Physics, Vol. 10, Issue 5 https://doi.org/10.1038/nphys2942	journal	April 2014
Electronic Structure, Surface Doping, and Optical Response in Epitaxial WSe ₂ Thin Films Zhang, Yi; Ugeda, Miguel M.; Jin, Chenhao Nano Letters, Vol. 16, Issue 4 https://doi.org/10.1021/acs.nanolett.6b00059	journal	March 2016
Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides Mak, Kin Fai; Shan, Jie Nature Photonics, Vol. 10, Issue 4 https://doi.org/10.1038/nphoton.2015.282	journal	March 2016
Exciton Binding Energy of Monolayer WS2 Zhu, Bairen; Chen, Xi; Cui, Xiaodong Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep09218	journal	March 2015
Population inversion and giant bandgap renormalization in atomically thin WS2 layers Chernikov, Alexey; Ruppert, Claudia; Hill, Heather M. Nature Photonics, Vol. 9, Issue 7 https://doi.org/10.1038/nphoton.2015.104	journal	June 2015
Corrigendum: k.p theory for two-dimensional transition metal dichalcogenide semiconductors (2015 2D Mater. 2 022001) Kormányos, Andor; Burkard, Guido; Gmitra, Martin 2D Materials, Vol. 2, Issue 4 https://doi.org/10.1088/2053-1583/2/4/049501	journal	November 2015
Universal Mechanism of Band-Gap Engineering in Transition-Metal Dichalcogenides Kang, Mingu; Kim, Beomyoung; Ryu, Sae Hee Nano Letters, Vol. 17, Issue 3 https://doi.org/10.1021/acs.nanolett.6b04775	journal	February 2017
Band Offset and Negative Compressibility in Graphene-MoS ₂ Heterostructures Larentis, Stefano; Tolsma, John R.; Fallahazad, Babak Nano Letters, Vol. 14, Issue 4 https://doi.org/10.1021/nl500212s	journal	March 2014
Electrical Tuning of Exciton Binding Energies in Monolayer ${WS}_{2}$ Chernikov, Alexey; van der Zande, Arend M.; Hill, Heather M. Physical Review Letters, Vol. 115, Issue 12 https://doi.org/10.1103/PhysRevLett.115.126802	journal	September 2015
Carrier Plasmon Induced Nonlinear Band Gap Renormalization in Two-Dimensional Semiconductors Liang, Yufeng; Yang, Li Physical Review Letters, Vol. 114, Issue 6 https://doi.org/10.1103/PhysRevLett.114.063001	journal	February 2015
One-Dimensional Electrical Contact to a Two-Dimensional Material Wang, L.; Meric, I.; Huang, P. Y. Science, Vol. 342, Issue 6158 https://doi.org/10.1126/science.1244358	journal	October 2013
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
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
Electronic Structure of Epitaxial Single-Layer ${MoS}_{2}$ Miwa, Jill A.; Ulstrup, Søren; Sørensen, Signe G. Physical Review Letters, Vol. 114, Issue 4 https://doi.org/10.1103/PhysRevLett.114.046802	journal	January 2015
Quasiparticle dynamics in graphene Bostwick, Aaron; Ohta, Taisuke; Seyller, Thomas Nature Physics, Vol. 3, Issue 1 https://doi.org/10.1038/nphys477	journal	December 2006
Effective tight-binding model for $M X_{2}$ under electric and magnetic fields Shanavas, K. V.; Satpathy, S. Physical Review B, Vol. 91, Issue 23 https://doi.org/10.1103/PhysRevB.91.235145	journal	June 2015
Growth and electronic structure of epitaxial single-layer ${WS}_{2}$ on Au(111) Dendzik, Maciej; Michiardi, Matteo; Sanders, Charlotte Physical Review B, Vol. 92, Issue 24 https://doi.org/10.1103/PhysRevB.92.245442	journal	December 2015
Boron nitride substrates for high-quality graphene electronics Dean, C. R.; Young, A. F.; Meric, I. Nature Nanotechnology, Vol. 5, Issue 10, p. 722-726 https://doi.org/10.1038/nnano.2010.172	journal	August 2010
Large conduction band and Fermi velocity spin splitting due to Coulomb interactions in single-layer ${MoS}_{2}$ Ferreiros, Yago; Cortijo, Alberto Physical Review B, Vol. 90, Issue 19 https://doi.org/10.1103/PhysRevB.90.195426	journal	November 2014
Large excitonic effects in monolayers of molybdenum and tungsten dichalcogenides Ramasubramaniam, Ashwin Physical Review B, Vol. 86, Issue 11 https://doi.org/10.1103/PhysRevB.86.115409	journal	September 2012
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
Zeeman-type spin splitting controlled by an electric field Yuan, Hongtao; Bahramy, Mohammad Saeed; Morimoto, Kazuhiro Nature Physics, Vol. 9, Issue 9 https://doi.org/10.1038/nphys2691	journal	July 2013
Isospin Pomeranchuk effect in twisted bilayer graphene Saito, Yu; Yang, Fangyuan; Ge, Jingyuan Nature, Vol. 592, Issue 7853 https://doi.org/10.1038/s41586-021-03409-2	journal	April 2021
Band offset and negative compressibility in graphene-MoS2 heterostructures Larentis, S.; Tolsma, J. R.; Fallahazad, B. arXiv https://doi.org/10.48550/arxiv.1402.1981	text	January 2014
Exciton Binding Energy of Monolayer WS2 Zhu, Bairen; Chen, Xi; Cui, Xiaodong arXiv https://doi.org/10.48550/arxiv.1403.5108	text	January 2014
Spatially Resolved Electronic Properties of Single-Layer WS$_2$ on Transition Metal Oxides Ulstrup, Søren; Katoch, Jyoti; Koch, Roland J. arXiv https://doi.org/10.48550/arxiv.1610.08480	text	January 2016

Cited By (24)

Uncovering the Conduction Behavior of van der Waals Ambipolar Semiconductors Wang, Feng; Tu, Bin; He, Peng Advanced Materials, Vol. 31, Issue 1 https://doi.org/10.1002/adma.201805317	journal	October 2018
Recent Advances in van der Waals Heterojunctions Based on Semiconducting Transition Metal Dichalcogenides Li, Ruiping; Li, Lain‐Jong; Cheng, Yingchun Advanced Electronic Materials, Vol. 4, Issue 11 https://doi.org/10.1002/aelm.201800270	journal	August 2018
Nanoscale mapping of quasiparticle band alignment Ulstrup, Søren; Giusca, Cristina E.; Miwa, Jill A. Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-11253-2	journal	July 2019
Dielectric disorder in two-dimensional materials Raja, Archana; Waldecker, Lutz; Zipfel, Jonas Nature Nanotechnology, Vol. 14, Issue 9 https://doi.org/10.1038/s41565-019-0520-0	journal	August 2019
Visualizing electrostatic gating effects in two-dimensional heterostructures Nguyen, Paul V.; Teutsch, Natalie C.; Wilson, Nathan P. Nature, Vol. 572, Issue 7768 https://doi.org/10.1038/s41586-019-1402-1	journal	July 2019
Demonstration of the key substrate-dependent charge transfer mechanisms between monolayer MoS2 and molecular dopants Park, Soohyung; Schultz, Thorsten; Xu, Xiaomin Communications Physics, Vol. 2, Issue 1 https://doi.org/10.1038/s42005-019-0212-y	journal	September 2019
Angle-resolved photoemission spectroscopy and its application to topological materials Lv, Baiqing; Qian, Tian; Ding, Hong Nature Reviews Physics, Vol. 1, Issue 10 https://doi.org/10.1038/s42254-019-0088-5	journal	August 2019
BX ₁ –BX ₂ (X ₁ , X ₂ = P, As, Sb) lateral heterostructure: novel and efficient two-dimensional photovoltaic materials with ultra-high carrier mobilities Wang, Qiang; Li, Jianwei; Liang, Yan Journal of Materials Chemistry A, Vol. 7, Issue 17 https://doi.org/10.1039/c9ta01451a	journal	January 2019
Imaging microscopic electronic contrasts at the interface of single-layer WS ₂ with oxide and boron nitride substrates Ulstrup, Søren; Koch, Roland J.; Schwarz, Daniel Applied Physics Letters, Vol. 114, Issue 15 https://doi.org/10.1063/1.5088968	journal	April 2019
Electronegativity, phase transition, and ferroelectricity of TeSe ₂ few-layers Debela, Tekalign Terfa; Liu, Shuyuan; Choi, Jin-Ho Journal of Physics: Condensed Matter, Vol. 32, Issue 4 https://doi.org/10.1088/1361-648x/ab4ac2	journal	October 2019
Multimodal spectromicroscopy of monolayer WS ₂ enabled by ultra-clean van der Waals epitaxy Kastl, C.; Chen, C. T.; Koch, R. J. 2D Materials, Vol. 5, Issue 4 https://doi.org/10.1088/2053-1583/aad21c	journal	July 2018
Production and processing of graphene and related materials Backes, Claudia; Abdelkader, Amr M.; Alonso, Concepción 2D Materials, Vol. 7, Issue 2 https://doi.org/10.1088/2053-1583/ab1e0a	journal	January 2020
Electronic band structure of Two-Dimensional ${WS}_{2}$ /Graphene van der Waals Heterostructures Henck, Hugo; Ben Aziza, Zeineb; Pierucci, Debora Physical Review B, Vol. 97, Issue 15 https://doi.org/10.1103/physrevb.97.155421	journal	April 2018
Nanospot angle-resolved photoemission study of Bernal-stacked bilayer graphene on hexagonal boron nitride: Band structure and local variation of lattice alignment Joucken, Frédéric; Quezada-López, Eberth A.; Avila, Jose Physical Review B, Vol. 99, Issue 16 https://doi.org/10.1103/physrevb.99.161406	journal	April 2019
Direct Determination of Band-Gap Renormalization in the Photoexcited Monolayer ${MoS}_{2}$ Liu, Fang; Ziffer, Mark E.; Hansen, Kameron R. Physical Review Letters, Vol. 122, Issue 24 https://doi.org/10.1103/physrevlett.122.246803	journal	June 2019
Rigid Band Shifts in Two-Dimensional Semiconductors through External Dielectric Screening Waldecker, Lutz; Raja, Archana; Rösner, Malte Physical Review Letters, Vol. 123, Issue 20 https://doi.org/10.1103/physrevlett.123.206403	journal	November 2019
Enhanced Electron-Phonon Interaction in Multivalley Materials Sohier, Thibault; Ponomarev, Evgeniy; Gibertini, Marco Physical Review X, Vol. 9, Issue 3 https://doi.org/10.1103/physrevx.9.031019	journal	August 2019
Giant gate-tunable bandgap renormalization and excitonic effects in a 2D semiconductor Qiu, Zhizhan; Trushin, Maxim; Fang, Hanyan Science Advances, Vol. 5, Issue 7 https://doi.org/10.1126/sciadv.aaw2347	journal	July 2019
A Perspective on the Application of Spatially Resolved ARPES for 2D Materials Cattelan, Mattia; Fox, Neil Nanomaterials, Vol. 8, Issue 5 https://doi.org/10.3390/nano8050284	journal	April 2018
Production and processing of graphene and related materials Backes, C.; Abdelkader, Am; Alonso, C. Apollo - University of Cambridge Repository https://doi.org/10.17863/cam.63418	text	January 2020
Production and processing of graphene and related materials Backes, Claudia; Abdelkader, Amr M.; Alonso, Concepción RWTH Aachen University https://doi.org/10.18154/rwth-2020-02443	text	January 2020
Imaging microscopic electronic contrasts at the interface of single-layer WS$_2$ with oxide and boron nitride substrates Ulstrup, Søren; Koch, Roland J.; Schwarz, Daniel arXiv https://doi.org/10.48550/arxiv.1903.10400	text	January 2019
Nanospot Angle-Resolved Photoemission Study of Bernal-Stacked Bilayer Graphene on Hexagonal Boron Nitride: Band Structure and Local Variation of Lattice Alignment Joucken, Frédéric; Quezada-López, Eberth A.; Avila, Jose arXiv https://doi.org/10.48550/arxiv.1904.11080	text	January 2019
Angle-resolved photoemission spectroscopy and its application to topological materials Lv, Baiqing; Qian, Tian; Ding, Hong arXiv https://doi.org/10.48550/arxiv.2106.09797	text	January 2021

Figures / Tables (4)

Similar Records

Revealing the biexciton and trion-exciton complexes in BN encapsulated WSe₂

Journal Article · Thu Sep 13 00:00:00 EDT 2018 · Nature Communications · OSTI ID:1462967

Li, Zhipeng; Wang, Tianmeng; Lu, Zhengguang; +9 more

Observation of two distinct negative trions in tungsten disulfide monolayers

Journal Article · Fri Sep 25 00:00:00 EDT 2015 · Physical Review. B, Condensed Matter and Materials Physics · OSTI ID:1462967

Boulesbaa, Abdelaziz; Huang, Bing; Wang, Kai; +8 more

Negative electronic compressibility and tunable spin splitting in WSe₂

Journal Article · Mon Sep 21 00:00:00 EDT 2015 · Nature Nanotechnology · OSTI ID:1462967

Riley, J. M.; Meevasana, W.; Bawden, L.; +10 more

Related Subjects

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

Title: Giant spin-splitting and gap renormalization driven by trions in single-layer WS2/h-BN heterostructures

Citation Formats