Abstract
Multiple polytypes of MoTe2 with distinct structures and intriguing electronic properties can be accessed by various physical and chemical approaches. Here, we report electrochemical lithium (Li) intercalation into 1T′-MoTe2 nanoflakes, leading to the discovery of two previously unreported lithiated phases. Distinguished by their structural differences from the pristine 1T′ phase, these distinct phases were characterized using in situ polarization Raman spectroscopy and in situ single-crystal X-ray diffraction. The lithiated phases exhibit increasing resistivity with decreasing temperature, and their carrier densities are two to 4 orders of magnitude smaller than the metallic 1T′ phase, as probed through in situ Hall measurements. The discovery of these gapped phases in initially metallic 1T′-MoTe2 underscores electrochemical intercalation as a potent tool for tuning the phase stability and electron density in two-dimensional (2D) materials.
Original language | English |
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Pages (from-to) | 17349-17358 |
Number of pages | 10 |
Journal | ACS Nano |
Volume | 18 |
Issue number | 26 |
DOIs | |
State | Published - Jul 2 2024 |
Funding
S.X. and J.J.C. gratefully acknowledge support from the National Science Foundation (NSF CBET #2240944). S.L. and P.G. acknowledge the support from the Air Force Office of Scientific Research (Grant No. FA9550-22-1-0209). J.J.H. and A.S. acknowledge the support by the Center for Alkaline-based Energy Solutions, an Energy Frontier Research Center funded by DOE, Office of Science, BES under Award # DE-SC0019445. Device fabrication and characterization were partly carried out at the Yale West Campus Materials Characterization Core and the Yale West Campus Cleanroom. This work was also performed in part at the Cornell NanoScale Facility, a member of the National Nanotechnology Coordinated Infrastructure (NNCI), which is supported by NSF (Grant NNCI-2025233). The authors acknowledge the use of facilities and instrumentation supported by NSF through the Cornell University Materials Research Science and Engineering Center DMR-1719875. This research used beamline 4-ID of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. TEM research was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a U.S. DOE, Office of Science User Facility at Oak Ridge National Laboratory. Theory and calculations were supported by the U.S. DOE, Office of Science, Basic Energy Sciences under Early Career Award No. DE-SC0021965. D.Y.Q. acknowledges support by a 2021 Packard Fellowship for Science and Engineering from the David and Lucile Packard Foundation. Development of the BerkeleyGW code was supported by Center for Computational Study of Excited-State Phenomena in Energy Materials (C2SEPEM) at the Lawrence Berkeley National Laboratory, funded by the U.S. DOE, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-C02-05CH11231. The calculations used resources of the National Energy Research Scientific Computing (NERSC), a DOE Office of Science User Facility operated under contract no. DE-AC02-05CH11231; the Advanced Cyberinfrastructure Coordination Ecosystem: Services & Support (ACCESS), which is supported by National Science Foundation grant number ACI-1548562; and the Texas Advanced Computing Center (TACC) at The University of Texas at Austin.
Funders | Funder number |
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University of Texas at Austin | |
Oak Ridge National Laboratory | |
U.S. Department of Energy | |
Texas Advanced Computing Center | |
David and Lucile Packard Foundation | |
Office of Science | |
Basic Energy Sciences | NNCI-2025233, DE-SC0021965, DE-SC0019445 |
Basic Energy Sciences | |
Division of Materials Sciences and Engineering | DE-AC02-05CH11231, DE-C02-05CH11231, ACI-1548562 |
Division of Materials Sciences and Engineering | |
Cornell University Materials Research Science and Engineering Center | DMR-1719875 |
National Science Foundation | 2240944 |
National Science Foundation | |
Air Force Office of Scientific Research | FA9550-22-1-0209 |
Air Force Office of Scientific Research | |
Brookhaven National Laboratory | DE-SC0012704 |
Brookhaven National Laboratory |
Keywords
- electron doping
- in situ Raman characterization
- layered materials
- lithium intercalation
- molybdenum ditelluride
- phase transitions