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Title: Reversible Electrochemical Phase Change in Monolayer to Bulk-like MoTe2 by Ionic Liquid Gating

Abstract

Transition-metal dichalcogenides (TMDs) exist in various crystal structures with semiconducting, semi-metallic, and metallic properties. The dynamic control of these phases is of immediate interest for next-generation electronics such as phase change memories. Of the binary Mo and W-based TMDs, MoTe2 is attractive for electronic applications because it has the lowest energy difference (40 meV) between the semiconducting (2H) and semi-metallic (1T') phases, allowing for MoTe2 phase change by electrostatic doping. Here, we report phase change between the 2H and 1T' polymorphs of MoTe2 in thicknesses ranging from the monolayer to bulk-like case (73 nm) using an ionic liquid electrolyte at room temperature and in air. We find consistent evidence of a partially reversible 2H-1T' transition using in situ Raman spectroscopy where the phase change occurs in the topmost layers of the MoTe2 flake. We find a thickness-dependent transition voltage where higher voltages are necessary to drive the phase change for thicker flakes. We also show evidence of electrochemical activity during the gating process by observation of Te metal formation. This finding suggests the formation of Te vacancies which have been reported to lower the energy difference between the 2H and 1T' phases, potentially aiding the phase change process. Furthermore, ourmore » discovery that the phase change can be achieved on the surface layer of bulk-like materials reveals that this electrochemical mechanism does not require isolation of a single layer and the effect may be more broadly applicable than previously thought.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [1];  [1]
  1. Stanford Univ., CA (United States)
  2. Stanford Univ., CA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE; National Science Foundation (SNSF)
OSTI Identifier:
1603986
Report Number(s):
LA-UR-19-22684
Journal ID: ISSN 1936-0851
Grant/Contract Number:  
89233218CNA000001; ECCS-1542152; ECCS-1436626; DMR-1455050; W911NF-15-1-0570; N00014-15-1-2697; W911NF-07-0027; DGE-1656518
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 14; Journal Issue: 3; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 2d materials; electrostatic gating; phase change; transition-metal dichalcogenides; MoTe2; ionic liquid gating; electrostatic; vacancies

Citation Formats

Zakhidov, Dante, Rehn, Daniel Adam, Reed, Evan J., and Salleo, Alberto. Reversible Electrochemical Phase Change in Monolayer to Bulk-like MoTe2 by Ionic Liquid Gating. United States: N. p., 2020. Web. doi:10.1021/acsnano.9b07095.
Zakhidov, Dante, Rehn, Daniel Adam, Reed, Evan J., & Salleo, Alberto. Reversible Electrochemical Phase Change in Monolayer to Bulk-like MoTe2 by Ionic Liquid Gating. United States. https://doi.org/10.1021/acsnano.9b07095
Zakhidov, Dante, Rehn, Daniel Adam, Reed, Evan J., and Salleo, Alberto. Tue . "Reversible Electrochemical Phase Change in Monolayer to Bulk-like MoTe2 by Ionic Liquid Gating". United States. https://doi.org/10.1021/acsnano.9b07095. https://www.osti.gov/servlets/purl/1603986.
@article{osti_1603986,
title = {Reversible Electrochemical Phase Change in Monolayer to Bulk-like MoTe2 by Ionic Liquid Gating},
author = {Zakhidov, Dante and Rehn, Daniel Adam and Reed, Evan J. and Salleo, Alberto},
abstractNote = {Transition-metal dichalcogenides (TMDs) exist in various crystal structures with semiconducting, semi-metallic, and metallic properties. The dynamic control of these phases is of immediate interest for next-generation electronics such as phase change memories. Of the binary Mo and W-based TMDs, MoTe2 is attractive for electronic applications because it has the lowest energy difference (40 meV) between the semiconducting (2H) and semi-metallic (1T') phases, allowing for MoTe2 phase change by electrostatic doping. Here, we report phase change between the 2H and 1T' polymorphs of MoTe2 in thicknesses ranging from the monolayer to bulk-like case (73 nm) using an ionic liquid electrolyte at room temperature and in air. We find consistent evidence of a partially reversible 2H-1T' transition using in situ Raman spectroscopy where the phase change occurs in the topmost layers of the MoTe2 flake. We find a thickness-dependent transition voltage where higher voltages are necessary to drive the phase change for thicker flakes. We also show evidence of electrochemical activity during the gating process by observation of Te metal formation. This finding suggests the formation of Te vacancies which have been reported to lower the energy difference between the 2H and 1T' phases, potentially aiding the phase change process. Furthermore, our discovery that the phase change can be achieved on the surface layer of bulk-like materials reveals that this electrochemical mechanism does not require isolation of a single layer and the effect may be more broadly applicable than previously thought.},
doi = {10.1021/acsnano.9b07095},
journal = {ACS Nano},
number = 3,
volume = 14,
place = {United States},
year = {Tue Feb 11 00:00:00 EST 2020},
month = {Tue Feb 11 00:00:00 EST 2020}
}

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