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Title: Negative electronic compressibility and tunable spin splitting in WSe2

Journal Article · · Nature Nanotechnology
 [1];  [2];  [3];  [4];  [5];  [2];  [6];  [6]; ORCiD logo [7];  [5];  [4];  [8]; ORCiD logo [3]
  1. Univ. of St. Andrews, Scotland (United Kingdom); Diamond Light Source, Harwell Campus, Didcot (United Kingdom)
  2. Suranaree University of Technology, Nakhon Ratchasima (Thailand)
  3. Univ. of St. Andrews, Scotland (United Kingdom)
  4. Tokyo Institute of Technology, Kanagawa (Japan)
  5. Univ. of Tokyo (Japan); Max Planck Institute for Solid State Research, Stuttgart (Germany)
  6. Diamond Light Source, Harwell Campus, Didcot (United Kingdom)
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  8. Univ. of Tokyo (Japan); RIKEN Center for Emergent Matter Science (CEMS), Wako (Japan)

We report that tunable bandgaps, extraordinarily large exciton-binding energies, strong light-matter coupling and a locking of the electron spin with layer and valley pseudospins have established transition-metal dichalcogenides (TMDs) as a unique class of two-dimensional (2D) semiconductors with wide-ranging practical applications. Using angle-resolved photoemission (ARPES), we show here that doping electrons at the surface of the prototypical strong spin-orbit TMD WSe2, akin to applying a gate voltage in a transistor-type device, induces a counterintuitive lowering of the surface chemical potential concomitant with the formation of a multivalley 2D electron gas (2DEG). These measurements provide a direct spectroscopic signature of negative electronic compressibility (NEC), a result of electron-electron interactions, which we find persists to carrier densities approximately three orders of magnitude higher than in typical semiconductor 2DEGs that exhibit this effect. An accompanying tunable spin splitting of the valence bands further reveals a complex interplay between single-particle band-structure evolution and many-body interactions in electrostatically doped TMDs. Lastly, understanding and exploiting this will open up new opportunities for advanced electronic and quantum-logic devices.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1530213
Journal Information:
Nature Nanotechnology, Vol. 10, Issue 12; ISSN 1748-3387
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 76 works
Citation information provided by
Web of Science

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Room‐Temperature Mesoscopic Fluctuations and Coulomb Drag in Multilayer WSe 2 journal March 2019
Spin–valley locking in the normal state of a transition-metal dichalcogenide superconductor journal May 2016
Large quantum-spin-Hall gap in single-layer 1T′ WSe2 journal May 2018
Holstein polaron in a valley-degenerate two-dimensional semiconductor journal May 2018
Giant spin-splitting and gap renormalization driven by trions in single-layer WS2/h-BN heterostructures journal January 2018
Visualizing electronic structures of quantum materials by angle-resolved photoemission spectroscopy journal August 2018
Visualizing electrostatic gating effects in two-dimensional heterostructures journal July 2019
Controlling the surface photovoltage on WSe 2 by surface chemical modification journal May 2018
Semiconductor-to-metal transition in the bulk of WSe 2 upon potassium intercalation journal March 2017
Negative electron compressibility in the Hubbard model journal December 2019
Two-dimensional hexagonal semiconductors beyond graphene journal September 2016
Quantum supercapacitors journal August 2019
Direct observation of hidden spin polarization in 2 H − MoT e 2 journal January 2020
Direct observation of strain-induced orbital valence band splitting in HfSe 2 by sodium intercalation journal May 2018
Band-Gap-Dependent Electronic Compressibility of Carbon Nanotubes in the Wigner Crystal Regime journal November 2019
A Perspective on the Application of Spatially Resolved ARPES for 2D Materials journal April 2018
Semiconductor-to-Metal Transition in the Bulk of WSe2 upon Potassium Intercalation text January 2017
Holstein polaron in a valley-degenerate two-dimensional semiconductor text January 2018
Negative electron compressibility in the Hubbard Model text January 2019
Large quantum-spin-Hall gap in single-layer 1T′ WSe2 journal May 2018
Interplay of negative electronic compressibility and capacitance enhancement in lightly-doped metal oxide Bi0.95La0.05FeO3 by quantum capacitance model journal March 2020
Determination of the band parameters of bulk 2H-MX2 (M = Mo, W; X = S, Se) by angle-resolved photoemission spectroscopy journal November 2016
Angle-resolved photoemission spectroscopy for the study of two-dimensional materials journal March 2017