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

Zakhidov, Dante; Rehn, Daniel Adam; Reed, Evan J.; Salleo, Alberto

doi:10.1021/acsnano.9b07095

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

Journal Article · Tue Feb 11 00:00:00 EST 2020 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.9b07095· OSTI ID:1603986

^[1]; ^[2]; Reed, Evan J. ^[1]; Salleo, Alberto ^[1]

Stanford Univ., CA (United States)
Stanford Univ., CA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

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.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: National Science Foundation (SNSF); USDOE

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1603986

Report Number(s):: LA-UR--19-22684

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 3 Vol. 14; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (54)

Synthesis of High-Quality Large-Area Homogenous 1T′ MoTe ₂ from Chemical Vapor Deposition Zhou, Lin; Zubair, Ahmad; Wang, Ziqiang Advanced Materials, Vol. 28, Issue 43 https://doi.org/10.1002/adma.201602687	journal	September 2016
Electronic and Optical Properties of 2D Transition Metal Carbides and Nitrides (MXenes) Hantanasirisakul, Kanit; Gogotsi, Yury Advanced Materials, Vol. 30, Issue 52 https://doi.org/10.1002/adma.201804779	journal	November 2018
Large-Area 2D Layered MoTe ₂ by Physical Vapor Deposition and Solid-Phase Crystallization in a Tellurium-Free Atmosphere Huang, Jyun-Hong; Deng, Kuang-Ying; Liu, Pang-Shiuan Advanced Materials Interfaces, Vol. 4, Issue 17 https://doi.org/10.1002/admi.201700157	journal	April 2017
Raman andab initio study of the conformational isomerism in the 1-ethyl-3-methyl-imidazolium bis(trifluoromethanesulfonyl)imide ionic liquid Lassègues, J. C.; Grondin, J.; Holomb, R. Journal of Raman Spectroscopy, Vol. 38, Issue 5 https://doi.org/10.1002/jrs.1680	journal	January 2007
Über den Tellurwasserstoff Ernyei, Edmund Zeitschrift für anorganische Chemie, Vol. 25, Issue 1 https://doi.org/10.1002/zaac.19000250123	journal	November 1900
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
First principles phonon calculations in materials science Togo, Atsushi; Tanaka, Isao Scripta Materialia, Vol. 108 https://doi.org/10.1016/j.scriptamat.2015.07.021	journal	November 2015
Probing the Dynamics of the Metallic-to-Semiconducting Structural Phase Transformation in MoS ₂ Crystals Guo, Yinsheng; Sun, Dezheng; Ouyang, Bin Nano Letters, Vol. 15, Issue 8 https://doi.org/10.1021/acs.nanolett.5b01196	journal	July 2015
Li Intercalation in MoS ₂ : In Situ Observation of Its Dynamics and Tuning Optical and Electrical Properties Xiong, Feng; Wang, Haotian; Liu, Xiaoge Nano Letters, Vol. 15, Issue 10 https://doi.org/10.1021/acs.nanolett.5b02619	journal	September 2015
Room Temperature Semiconductor–Metal Transition of MoTe ₂ Thin Films Engineered by Strain Song, Seunghyun; Keum, Dong Hoon; Cho, Suyeon Nano Letters, Vol. 16, Issue 1 https://doi.org/10.1021/acs.nanolett.5b03481	journal	December 2015
Photoinduced Vacancy Ordering and Phase Transition in MoTe ₂ Si, Chen; Choe, Dukhyun; Xie, Weiyu Nano Letters, Vol. 19, Issue 6 https://doi.org/10.1021/acs.nanolett.9b00613	journal	April 2019
Nano-“Squeegee” for the Creation of Clean 2D Material Interfaces Rosenberger, Matthew R.; Chuang, Hsun-Jen; McCreary, Kathleen M. ACS Applied Materials & Interfaces, Vol. 10, Issue 12 https://doi.org/10.1021/acsami.8b01224	journal	March 2018
Environmental Changes in MoTe ₂ Excitonic Dynamics by Defects-Activated Molecular Interaction Chen, Bin; Sahin, Hasan; Suslu, Aslihan ACS Nano, Vol. 9, Issue 5 https://doi.org/10.1021/acsnano.5b00985	journal	April 2015
Phase-Engineered Synthesis of Centimeter-Scale 1T′- and 2H-Molybdenum Ditelluride Thin Films Park, Jin Cheol; Yun, Seok Joon; Kim, Hyun ACS Nano, Vol. 9, Issue 6 https://doi.org/10.1021/acsnano.5b02511	journal	May 2015
Structural Phase Transitions by Design in Monolayer Alloys Duerloo, Karel-Alexander N.; Reed, Evan J. ACS Nano, Vol. 10, Issue 1 https://doi.org/10.1021/acsnano.5b04359	journal	December 2015
Characterization of Few-Layer 1T′ MoTe ₂ by Polarization-Resolved Second Harmonic Generation and Raman Scattering Beams, Ryan; Cançado, Luiz Gustavo; Krylyuk, Sergiy ACS Nano, Vol. 10, Issue 10 https://doi.org/10.1021/acsnano.6b05127	journal	October 2016
Defects and Surface Structural Stability of MoTe 2 Under Vacuum Annealing Zhu, Hui; Wang, Qingxiao; Cheng, Lanxia ACS Nano, Vol. 11, Issue 11 https://doi.org/10.1021/acsnano.7b04984	journal	September 2017
Hydrogen Telluride and the Atomic Weight of Tellurium. Dennis, L. M.; Anderson, R. P. Journal of the American Chemical Society, Vol. 36, Issue 5 https://doi.org/10.1021/ja02182a012	journal	May 1914
The Role of Ionic Liquid Breakdown in the Electrochemical Metallization of VO ₂ : An NMR Study of Gating Mechanisms and VO ₂ Reduction Hope, Michael A.; Griffith, Kent J.; Cui, Bin Journal of the American Chemical Society, Vol. 140, Issue 48 https://doi.org/10.1021/jacs.8b09513	journal	November 2018
Optical Properties and Band Gap of Single- and Few-Layer MoTe ₂ Crystals Ruppert, Claudia; Aslan, Ozgur Burak; Heinz, Tony F. Nano Letters, Vol. 14, Issue 11 https://doi.org/10.1021/nl502557g	journal	October 2014
Indirect-to-Direct Band Gap Crossover in Few-Layer MoTe ₂ Lezama, Ignacio Gutiérrez; Arora, Ashish; Ubaldini, Alberto Nano Letters, Vol. 15, Issue 4 https://doi.org/10.1021/nl5045007	journal	March 2015
Raman Enhancement on Graphene: Adsorbed and Intercalated Molecular Species Jung, Naeyoung; Crowther, Andrew C.; Kim, Namdong ACS Nano, Vol. 4, Issue 11 https://doi.org/10.1021/nn102227u	journal	October 2010
2D metal carbides and nitrides (MXenes) for energy storage Anasori, Babak; Lukatskaya, Maria R.; Gogotsi, Yury Nature Reviews Materials, Vol. 2, Issue 2 https://doi.org/10.1038/natrevmats.2016.98	journal	January 2017
2D transition metal dichalcogenides Manzeli, Sajedeh; Ovchinnikov, Dmitry; Pasquier, Diego Nature Reviews Materials, Vol. 2, Issue 8 https://doi.org/10.1038/natrevmats.2017.33	journal	June 2017
Structural phase transition in monolayer MoTe2 driven by electrostatic doping Wang, Ying; Xiao, Jun; Zhu, Hanyu Nature, Vol. 550, Issue 7677 https://doi.org/10.1038/nature24043	journal	October 2017
The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets Chhowalla, Manish; Shin, Hyeon Suk; Eda, Goki Nature Chemistry, Vol. 5, Issue 4, p. 263-275 https://doi.org/10.1038/nchem.1589	journal	April 2013
Structural semiconductor-to-semimetal phase transition in two-dimensional materials induced by electrostatic gating Li, Yao; Duerloo, Karel-Alexander N.; Wauson, Kerry Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms10671	journal	February 2016
Structural phase transitions in two-dimensional Mo- and W-dichalcogenide monolayers Duerloo, Karel-Alexander N.; Li, Yao; Reed, Evan J. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5214	journal	July 2014
The rise of graphene Geim, A. K.; Novoselov, K. S. Nature Materials, Vol. 6, Issue 3, p. 183-191 https://doi.org/10.1038/nmat1849	journal	March 2007
Buckled two-dimensional Xene sheets Molle, Alessandro; Goldberger, Joshua; Houssa, Michel Nature Materials, Vol. 16, Issue 2 https://doi.org/10.1038/nmat4802	journal	January 2017
Bandgap opening in few-layered monoclinic MoTe2 Keum, Dong Hoon; Cho, Suyeon; Kim, Jung Ho Nature Physics, Vol. 11, Issue 6 https://doi.org/10.1038/nphys3314	journal	May 2015
Theoretical potential for low energy consumption phase change memory utilizing electrostatically-induced structural phase transitions in 2D materials Rehn, Daniel A.; Li, Yao; Pop, Eric npj Computational Materials, Vol. 4, Issue 1 https://doi.org/10.1038/s41524-017-0059-2	journal	January 2018
Electric-field induced structural transition in vertical MoTe2- and Mo1–xWxTe2-based resistive memories Zhang, Feng; Zhang, Huairuo; Krylyuk, Sergiy Nature Materials, Vol. 18, Issue 1 https://doi.org/10.1038/s41563-018-0234-y	journal	December 2018
Electrolyte-based ionic control of functional oxides Leighton, Chris Nature Materials, Vol. 18, Issue 1 https://doi.org/10.1038/s41563-018-0246-7	journal	December 2018
Strain-based room-temperature non-volatile MoTe2 ferroelectric phase change transistor Hou, Wenhui; Azizimanesh, Ahmad; Sewaket, Arfan Nature Nanotechnology, Vol. 14, Issue 7 https://doi.org/10.1038/s41565-019-0466-2	journal	June 2019
Fabrication of large-scale single-crystal bismuth telluride (Bi ₂ Te ₃ ) nanosheet arrays by a single-step electrolysis process Tsai, Hung-Wei; Wang, Tsang-Hsiu; Chan, Tsung-Cheng Nanoscale, Vol. 6, Issue 14 https://doi.org/10.1039/C4NR00184B	journal	January 2014
Electrochemical synthesis of ultrafast and gram-scale surfactant-free tellurium nanowires by gas–solid transformation and their applications as supercapacitor electrodes for p-doping of graphene transistors Tsai, Hung-Wei; Yaghoubi, Alireza; Chan, Tsung-Cheng Nanoscale, Vol. 7, Issue 17 https://doi.org/10.1039/C5NR00876J	journal	January 2015
Controlling the H to T′ structural phase transition via chalcogen substitution in MoTe ₂ monolayers Young, Joshua; Reinecke, Thomas L. Physical Chemistry Chemical Physics, Vol. 19, Issue 47 https://doi.org/10.1039/C7CP05634F	journal	January 2017
A possible high-mobility signal in bulk MoTe ₂ : Temperature independent weak phonon decay Li, Titao; Zhang, Zhaojun; Zheng, Wei AIP Advances, Vol. 6, Issue 11 https://doi.org/10.1063/1.4967351	journal	November 2016
The structural phases and vibrational properties of Mo _1−x W _x Te ₂ alloys Oliver, Sean M.; Beams, Ryan; Krylyuk, Sergiy 2D Materials, Vol. 4, Issue 4 https://doi.org/10.1088/2053-1583/aa7a32	journal	August 2017
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium Kresse, G.; Hafner, J. Physical Review B, Vol. 49, Issue 20, p. 14251-14269 https://doi.org/10.1103/PhysRevB.49.14251	journal	May 1994
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Interference effect on Raman spectrum of graphene on SiO 2 / Si Yoon, Duhee; Moon, Hyerim; Son, Young-Woo Physical Review B, Vol. 80, Issue 12 https://doi.org/10.1103/PhysRevB.80.125422	journal	September 2009
Double resonance Raman modes in monolayer and few-layer MoTe 2 Guo, Huaihong; Yang, Teng; Yamamoto, Mahito Physical Review B, Vol. 91, Issue 20 https://doi.org/10.1103/PhysRevB.91.205415	journal	May 2015
Phase transition and electronic structure evolution of MoTe 2 induced by W substitution Jin, Wencan; Schiros, Theanne; Lin, Yi Physical Review B, Vol. 98, Issue 14 https://doi.org/10.1103/PhysRevB.98.144114	journal	October 2018
Strongly Constrained and Appropriately Normed Semilocal Density Functional Sun, Jianwei; Ruzsinszky, Adrienn; Perdew, John P. Physical Review Letters, Vol. 115, Issue 3 https://doi.org/10.1103/PhysRevLett.115.036402	journal	July 2015
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Refrigeration in 2D: Electrostaticaloric effect in monolayer materials Rehn, Daniel A.; Li, Yao; Reed, Evan J. Physical Review Materials, Vol. 2, Issue 11 https://doi.org/10.1103/PhysRevMaterials.2.114004	journal	November 2018
Versatile van der Waals Density Functional Based on a Meta-Generalized Gradient Approximation Peng, Haowei; Yang, Zeng-Hui; Perdew, John P. Physical Review X, Vol. 6, Issue 4 https://doi.org/10.1103/PhysRevX.6.041005	journal	October 2016
Phase patterning for ohmic homojunction contact in MoTe2 Cho, S.; Kim, S.; Kim, J. H. Science, Vol. 349, Issue 6248 https://doi.org/10.1126/science.aab3175	journal	August 2015
Toward Single Atom Chains with Exfoliated Tellurium Churchill, Hugh O. H.; Salamo, Gregory J.; Yu, Shui-Qing Nanoscale Research Letters, Vol. 12, Issue 1 https://doi.org/10.1186/s11671-017-2255-x	journal	August 2017

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

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