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Title: Magnetism in semiconducting molybdenum dichalcogenides

Abstract

Transition metal dichalcogenides (TMDs) are interesting for understanding the fundamental physics of two-dimensional (2D) materials as well as for applications to many emerging technologies, including spin electronics. Here, we report the discovery of long-range magnetic order belowTM = 40 and 100 K in bulk semiconducting TMDs 2H-MoTe2and 2H-MoSe2, respectively, by means of muon spin rotation (μSR), scanning tunneling microscopy (STM), and density functional theory (DFT) calculations. The μSR measurements show the presence of large and homogeneous internal magnetic fields at low temperatures in both compounds indicative of long-range magnetic order. DFT calculations show that this magnetism is promoted by the presence of defects in the crystal. The STM measurements show that the vast majority of defects in these materials are metal vacancies and chalcogen-metal antisites, which are randomly distributed in the lattice at the subpercent level. DFT indicates that the antisite defects are magnetic with a magnetic moment in the range of 0.9 to 2.8 μB. Further, we find that the magnetic order stabilized in 2H-MoTe2and 2H-MoSe2is highly sensitive to hydrostatic pressure. These observations establish 2H-MoTe2and 2H-MoSe2as a new class of magnetic semiconductors and open a path to studying the interplay of 2D physics and magnetism in these interesting semiconductors.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [2];  [2];  [3]; ORCiD logo [4];  [4];  [4];  [2];  [5];  [5];  [6]; ORCiD logo [5];  [5]; ORCiD logo [5]; ORCiD logo [2]; ORCiD logo [5]; ORCiD logo [7];  [4]; ORCiD logo [2] more »;  [2] « less
  1. Columbia Univ., New York, NY (United States); Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  2. Columbia Univ., New York, NY (United States)
  3. Univ. of Zurich (Switzerland)
  4. Queen's Univ., Belfast, Northern Ireland (United Kingdom)
  5. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  6. Tbilisi State Univ. (Georgia)
  7. Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Swiss National Science Foundation (SNSF); National Science Foundation (NSF); US Department of the Navy, Office of Naval Research (ONR); US Air Force Office of Scientific Research (AFOSR); SCOPES; Engineering and Physical Sciences Resource Council (EPSRC); Queen’s Univ. Belfast; Northern Ireland Department for the Economy
OSTI Identifier:
1625993
Grant/Contract Number:  
SC0012704; SC00112704; P2ZHP2-161980; P300P2-177832; PZ00P2-174015; DMR-1610110; DMR-1436095; DMR-1610633; DMR-1420634; TG-DMR120049; TG-DMR150017; N00014-14-1-0501; FA9550-11-1-0010; IZ74Z0-160484; EP/K013564/1; EP/P020194/1; M8407MPH; A5047TSL; USI-097
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 4; Journal Issue: 12; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Guguchia, Z., Kerelsky, A., Edelberg, D., Banerjee, S., von Rohr, F., Scullion, D., Augustin, M., Scully, M., Rhodes, D. A., Shermadini, Z., Luetkens, H., Shengelaya, A., Baines, C., Morenzoni, E., Amato, A., Hone, J. C., Khasanov, R., Billinge, S. J. L., Santos, E., Pasupathy, A. N., and Uemura, Y. J. Magnetism in semiconducting molybdenum dichalcogenides. United States: N. p., 2018. Web. doi:10.1126/sciadv.aat3672.
Guguchia, Z., Kerelsky, A., Edelberg, D., Banerjee, S., von Rohr, F., Scullion, D., Augustin, M., Scully, M., Rhodes, D. A., Shermadini, Z., Luetkens, H., Shengelaya, A., Baines, C., Morenzoni, E., Amato, A., Hone, J. C., Khasanov, R., Billinge, S. J. L., Santos, E., Pasupathy, A. N., & Uemura, Y. J. Magnetism in semiconducting molybdenum dichalcogenides. United States. https://doi.org/10.1126/sciadv.aat3672
Guguchia, Z., Kerelsky, A., Edelberg, D., Banerjee, S., von Rohr, F., Scullion, D., Augustin, M., Scully, M., Rhodes, D. A., Shermadini, Z., Luetkens, H., Shengelaya, A., Baines, C., Morenzoni, E., Amato, A., Hone, J. C., Khasanov, R., Billinge, S. J. L., Santos, E., Pasupathy, A. N., and Uemura, Y. J. Fri . "Magnetism in semiconducting molybdenum dichalcogenides". United States. https://doi.org/10.1126/sciadv.aat3672. https://www.osti.gov/servlets/purl/1625993.
@article{osti_1625993,
title = {Magnetism in semiconducting molybdenum dichalcogenides},
author = {Guguchia, Z. and Kerelsky, A. and Edelberg, D. and Banerjee, S. and von Rohr, F. and Scullion, D. and Augustin, M. and Scully, M. and Rhodes, D. A. and Shermadini, Z. and Luetkens, H. and Shengelaya, A. and Baines, C. and Morenzoni, E. and Amato, A. and Hone, J. C. and Khasanov, R. and Billinge, S. J. L. and Santos, E. and Pasupathy, A. N. and Uemura, Y. J.},
abstractNote = {Transition metal dichalcogenides (TMDs) are interesting for understanding the fundamental physics of two-dimensional (2D) materials as well as for applications to many emerging technologies, including spin electronics. Here, we report the discovery of long-range magnetic order belowTM = 40 and 100 K in bulk semiconducting TMDs 2H-MoTe2and 2H-MoSe2, respectively, by means of muon spin rotation (μSR), scanning tunneling microscopy (STM), and density functional theory (DFT) calculations. The μSR measurements show the presence of large and homogeneous internal magnetic fields at low temperatures in both compounds indicative of long-range magnetic order. DFT calculations show that this magnetism is promoted by the presence of defects in the crystal. The STM measurements show that the vast majority of defects in these materials are metal vacancies and chalcogen-metal antisites, which are randomly distributed in the lattice at the subpercent level. DFT indicates that the antisite defects are magnetic with a magnetic moment in the range of 0.9 to 2.8 μB. Further, we find that the magnetic order stabilized in 2H-MoTe2and 2H-MoSe2is highly sensitive to hydrostatic pressure. These observations establish 2H-MoTe2and 2H-MoSe2as a new class of magnetic semiconductors and open a path to studying the interplay of 2D physics and magnetism in these interesting semiconductors.},
doi = {10.1126/sciadv.aat3672},
journal = {Science Advances},
number = 12,
volume = 4,
place = {United States},
year = {Fri Dec 21 00:00:00 EST 2018},
month = {Fri Dec 21 00:00:00 EST 2018}
}

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