Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields

Goryca, Mateusz Marek; Li, Jing; Stier, Andreas V.; Taniguchi, Takashi; Watanabe, K.; Courtade, Emmanuel; Shree, S.; Robert, Cedric; Urbaszek, B.; Marie, X.; Crooker, Scott A.

doi:10.1038/s41467-019-12180-y

Title: Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields

Journal Article · 13 September 2019 · Nature Communications

DOI: https://doi.org/10.1038/s41467-019-12180-y · OSTI ID:1565907

^[1];

^[1]; Taniguchi, Takashi ^[2];

^[2]; Courtade, Emmanuel ^[3]; Shree, S. ^[3]; Robert, Cedric ^[3];

^[3]; Marie, X. ^[3];

^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
National Institute for Materials Science, Ibaraki (Japan)
Univ. de Toulouse, Toulouse (France)

In semiconductor physics, many essential optoelectronic material parameters can be experimentally revealed via optical spectroscopy in sufficiently large magnetic fields. For monolayer transition-metal dichalcogenide semiconductors, this field scale is substantial—tens of teslas or more—due to heavy carrier masses and huge exciton binding energies. Here we report absorption spectroscopy of monolayer MoS₂, MoSe₂, MoTe₂, and WS₂ in very high magnetic fields to 91 T. We follow the diamagnetic shifts and valley Zeeman splittings of not only the exciton’s 1s ground state but also its excited 2s,3s,…,ns Rydberg states. This provides a direct experimental measure of the effective (reduced) exciton masses and dielectric properties. Exciton binding energies, exciton radii, and free-particle bandgaps are also determined. The measured exciton masses are heavier than theoretically predicted, especially for Mo-based monolayers. These results provide essential and quantitative parameters for the rational design of opto-electronic van der Waals heterostructures incorporating 2D semiconductors.

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Research Organization:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: LDRD; USDOE

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1565907

Report Number(s):: LA-UR--19-23579

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 10; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Environmentally sensitive theory of electronic and optical transitions in atomically thin semiconductors Cho, Yeongsu; Berkelbach, Timothy C. Physical Review B, Vol. 97, Issue 4 https://doi.org/10.1103/PhysRevB.97.041409	journal	January 2018
Excitons, trions, and biexcitons in transition-metal dichalcogenides: Magnetic-field dependence Van der Donck, M.; Zarenia, M.; Peeters, F. M. Physical Review B, Vol. 97, Issue 19 https://doi.org/10.1103/PhysRevB.97.195408	journal	May 2018
Large effective mass and interaction-enhanced Zeeman splitting of K -valley electrons in MoSe 2 Larentis, Stefano; Movva, Hema C. P.; Fallahazad, Babak Physical Review B, Vol. 97, Issue 20 https://doi.org/10.1103/PhysRevB.97.201407	journal	May 2018
Observation of interlayer excitons in MoSe 2 single crystals Horng, Jason; Stroucken, Tineke; Zhang, Long Physical Review B, Vol. 97, Issue 24 https://doi.org/10.1103/PhysRevB.97.241404	journal	June 2018
Spatial extent of the excited exciton states in WS 2 monolayers from diamagnetic shifts Zipfel, Jonas; Holler, Johannes; Mitioglu, Anatolie A. Physical Review B, Vol. 98, Issue 7 https://doi.org/10.1103/PhysRevB.98.075438	journal	August 2018
Coulomb interaction in monolayer transition-metal dichalcogenides Van Tuan, Dinh; Yang, Min; Dery, Hanan Physical Review B, Vol. 98, Issue 12 https://doi.org/10.1103/PhysRevB.98.125308	journal	September 2018
Atomically Thin MoS2 A New Direct-Gap Semiconductor Mak, Kin Fai; Lee, Changgu; Hone, James Physical Review Letters, Vol. 105, Issue 13, Article No.136805 https://doi.org/10.1103/PhysRevLett.105.136805	journal	September 2010
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
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
Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS 2 Chernikov, Alexey; Berkelbach, Timothy C.; Hill, Heather M. Physical Review Letters, Vol. 113, Issue 7 https://doi.org/10.1103/PhysRevLett.113.076802	journal	August 2014
Valley Splitting and Polarization by the Zeeman Effect in Monolayer MoSe 2 Li, Yilei; Ludwig, Jonathan; Low, Tony Physical Review Letters, Vol. 113, Issue 26 https://doi.org/10.1103/PhysRevLett.113.266804	journal	December 2014
Breaking of Valley Degeneracy by Magnetic Field in Monolayer MoSe 2 MacNeill, David; Heikes, Colin; Mak, Kin Fai Physical Review Letters, Vol. 114, Issue 3 https://doi.org/10.1103/PhysRevLett.114.037401	journal	January 2015
In-Plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules Wang, G.; Robert, C.; Glazov, M. M. Physical Review Letters, Vol. 119, Issue 4 https://doi.org/10.1103/PhysRevLett.119.047401	journal	July 2017
Realization of an Electrically Tunable Narrow-Bandwidth Atomically Thin Mirror Using Monolayer MoSe 2 Back, Patrick; Zeytinoglu, Sina; Ijaz, Aroosa Physical Review Letters, Vol. 120, Issue 3 https://doi.org/10.1103/PhysRevLett.120.037401	journal	January 2018
Large Excitonic Reflectivity of Monolayer MoSe 2 Encapsulated in Hexagonal Boron Nitride Scuri, Giovanni; Zhou, You; High, Alexander A. Physical Review Letters, Vol. 120, Issue 3 https://doi.org/10.1103/PhysRevLett.120.037402	journal	January 2018
Magnetooptics of Exciton Rydberg States in a Monolayer Semiconductor Stier, A. V.; Wilson, N. P.; Velizhanin, K. A. Physical Review Letters, Vol. 120, Issue 5 https://doi.org/10.1103/PhysRevLett.120.057405	journal	February 2018
Interactions and Magnetotransport through Spin-Valley Coupled Landau Levels in Monolayer MoS 2 Pisoni, Riccardo; Kormányos, Andor; Brooks, Matthew Physical Review Letters, Vol. 121, Issue 24 https://doi.org/10.1103/PhysRevLett.121.247701	journal	December 2018
Energy Spectrum of Two-Dimensional Excitons in a Nonuniform Dielectric Medium Molas, M. R.; Slobodeniuk, A. O.; Nogajewski, K. Physical Review Letters, Vol. 123, Issue 13 https://doi.org/10.1103/PhysRevLett.123.136801	journal	September 2019
Optical spectroscopy of excited exciton states in MoS 2 monolayers in van der Waals heterostructures Robert, C.; Semina, M. A.; Cadiz, F. Physical Review Materials, Vol. 2, Issue 1 https://doi.org/10.1103/PhysRevMaterials.2.011001	journal	January 2018
Colloquium : Excitons in atomically thin transition metal dichalcogenides Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M. Reviews of Modern Physics, Vol. 90, Issue 2 https://doi.org/10.1103/RevModPhys.90.021001	journal	April 2018
Interband Optical Transitions in Extremely Anisotropic Semiconductors. II. Coexistence of Exciton and the Landau Levels Akimoto, Okikazu; Hasegawa, Hiroshi Journal of the Physical Society of Japan, Vol. 22, Issue 1 https://doi.org/10.1143/JPSJ.22.181	journal	January 1967
Realization of an Electrically Tunable Narrow-Bandwidth Atomically Thin Mirror Using Monolayer MoSe2 Back, Patrick; Zeytinoglu, Sina; Ijaz, Aroosa ETH Zurich https://doi.org/10.3929/ethz-b-000231337	text	January 2018
Interactions and Magnetotransport through Spin-Valley Coupled Landau Levels in Monolayer Pisoni, Riccardo; Kormányos, Andor; Brooks, Matthew ETH Zurich https://doi.org/10.3929/ethz-b-000311260	text	January 2018
Theory of Neutral and Charged Excitons in Monolayer Transition Metal Dichalcogenides Berkelbach, Timothy C.; Hybertsen, Mark S.; Reichman, David R. arXiv https://doi.org/10.48550/arxiv.1305.4972	text	January 2013
Magneto-optics in transition metal diselenide monolayers Wang, G.; Bouet, L.; Glazov, M. M. arXiv https://doi.org/10.48550/arxiv.1503.04105	text	January 2015
Binding energies of exciton complexes in transition metal dichalcogenides and effect of dielectric environment Kylänpää, Ilkka; Komsa, Hannu-Pekka arXiv https://doi.org/10.48550/arxiv.1508.06737	text	January 2015
Exciton Diamagnetic Shifts and Valley Zeeman Effects in Monolayer WS$_2$ and MoS$_2$ to 65 Tesla Stier, Andreas V.; McCreary, Kathleen M.; Jonker, Berend T. arXiv https://doi.org/10.48550/arxiv.1510.07022	text	January 2015
Probing the influence of dielectric environment on excitons in monolayer WSe2: Insight from high magnetic fields Stier, Andreas V.; Wilson, Nathan P.; Clark, Genevieve arXiv https://doi.org/10.48550/arxiv.1608.05093	text	January 2016
Excitonic valley effects in monolayer WS$_2$ under high magnetic fields Plechinger, Gerd; Nagler, Philipp; Arora, Ashish arXiv https://doi.org/10.48550/arxiv.1612.03004	text	January 2016
Magnetic brightening and control of dark excitons in monolayer WSe2 Zhang, Xiao-Xiao; Cao, Ting; Lu, Zhengguang arXiv https://doi.org/10.48550/arxiv.1612.03558	text	January 2016
In-plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules Wang, G.; Robert, C.; Glazov, M. M. arXiv https://doi.org/10.48550/arxiv.1704.05341	text	January 2017
Direct exciton emission from atomically thin transition metal dichalcogenide heterostructures near the lifetime limit Wierzbowski, Jakob; Klein, Julian; Sigger, Florian arXiv https://doi.org/10.48550/arxiv.1705.00348	text	January 2017
Environmentally-Sensitive Theory of Electronic and Optical Transitions in Atomically-Thin Semiconductors Cho, Yeongsu; Berkelbach, Timothy C. arXiv https://doi.org/10.48550/arxiv.1709.01094	text	January 2017
The dielectric impact of layer distances on exciton and trion binding energies in van der Waals heterostructures Florian, M.; Hartmann, M.; Steinhoff, A. arXiv https://doi.org/10.48550/arxiv.1712.05607	text	January 2017
Orbital, spin and valley contributions to Zeeman splitting of excitonic resonances in MoSe$_2$, WSe$_2$ and WS$_2$ monolayers Koperski, M.; Molas, M. R.; Arora, A. arXiv https://doi.org/10.48550/arxiv.1803.00376	preprint	January 2018
Luminescent emission of excited Rydberg excitons from monolayer WSe2 Chen, Shao-Yu; Lu, Zhengguang; Goldstein, Thomas arXiv https://doi.org/10.48550/arxiv.1903.07073	text	January 2019
Coulomb engineering of the bandgap and excitons in two-dimensional materials Chernikov, Alexey; Raja, Archana; Chaves, Andrey Universität Regensburg https://doi.org/10.5283/epub.35591	text	January 2017
Coulomb engineering of the bandgap and excitons in two-dimensional materials Raja, Archana; Chaves, Andrey; Yu, Jaeeun Universität Regensburg https://doi.org/10.5283/epub.40514	text	January 2017
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
Spatial extent of the excited exciton states in WS2 monolayers from diamagnetic shifts Zipfel, Jonas; Holler, Johannes; Mitioglu, Anatolie A. Universität Regensburg https://doi.org/10.5283/epub.40520	text	January 2018

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Rydberg series of dark excitons and the conduction band spin-orbit splitting in monolayer WSe2 Kapuściński, Piotr; Delhomme, Alex; Vaclavkova, Diana Communications Physics, Vol. 4, Issue 1 https://doi.org/10.1038/s42005-021-00692-3	journal	August 2021
Spontaneous Valley Polarization of Interacting Carriers in a Monolayer Semiconductor Li, J.; Goryca, M.; Wilson, N. P. Physical Review Letters, Vol. 125, Issue 14 https://doi.org/10.1103/physrevlett.125.147602	journal	October 2020
Coherent dynamics and mapping of excitons in single-layer MoSe$_2$ and WSe$_2$ at the homogeneous limit Boule, Caroline; Vaclavkova, Diana; Bartos, Miroslav arXiv https://doi.org/10.48550/arxiv.2002.01436	text	January 2020
Controlling exciton many-body states by the electric-field effect in monolayer MoS$_2$ Klein, Julian; Hötger, Alexander; Florian, Matthias arXiv https://doi.org/10.48550/arxiv.2007.14441	text	January 2020
Magnetoexcitons in transition-metal dichalcogenides monolayers, bilayers, and van der Waals heterostructures Kezerashvili, Roman Ya.; Spiridonova, Anastasia arXiv https://doi.org/10.48550/arxiv.2012.07125	text	January 2020
Tunable quantum confinement of neutral excitons using electric fields and exciton-charge interactions Thureja, Deepankur; Imamoglu, Atac; Smolenski, Tomasz arXiv https://doi.org/10.48550/arxiv.2102.08989	preprint	January 2021
Excitons in monolayer semiconductors in complex environments and under external fields Zipfel, Jonas Universität Regensburg https://doi.org/10.5283/epub.43395	text	January 2020
High optical quality of MoS ₂ monolayers grown by chemical vapor deposition Shree, Shivangi; George, Antony; Lehnert, Tibor 2D Materials, Vol. 7, Issue 1 https://doi.org/10.1088/2053-1583/ab4f1f	journal	November 2019
Energy Spectrum of Two-Dimensional Excitons in a Nonuniform Dielectric Medium Molas, M. R.; Slobodeniuk, A. O.; Nogajewski, K. Physical Review Letters, Vol. 123, Issue 13 https://doi.org/10.1103/physrevlett.123.136801	journal	September 2019

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