Atomic-Scale Mechanisms of MoS2 Oxidation for Kinetic Control of MoS2/MoO3 Interfaces

Kate Reidy; Wouter Mortelmans; Seong Soon Jo; Aubrey N. Penn; Alexandre C. Foucher; Zhenjing Liu; Tao Cai; Baoming Wang; Frances M. Ross; R. Jaramillo

doi:10.1021/acs.nanolett.3c00303

Atomic-Scale Mechanisms of MoS₂ Oxidation for Kinetic Control of MoS₂/MoO₃ Interfaces

Kate Reidy, Wouter Mortelmans, Seong Soon Jo, Aubrey N. Penn, Alexandre C. Foucher, Zhenjing Liu, Tao Cai, Baoming Wang, Frances M. Ross, R. Jaramillo

Research output: Contribution to journal › Article › peer-review

11 Scopus citations

Abstract

Oxidation of transition metal dichalcogenides (TMDs) occurs readily under a variety of conditions. Therefore, understanding the oxidation processes is necessary for successful TMD handling and device fabrication. Here, we investigate atomic-scale oxidation mechanisms of the most widely studied TMD, MoS₂. We find that thermal oxidation results in α-phase crystalline MoO₃ with sharp interfaces, voids, and crystallographic alignment with the underlying MoS₂. Experiments with remote substrates prove that thermal oxidation proceeds via vapor-phase mass transport and redeposition, a challenge to forming thin, conformal films. Oxygen plasma accelerates the kinetics of oxidation relative to the kinetics of mass transport, forming smooth and conformal oxides. The resulting amorphous MoO₃ can be grown with subnanometer to several-nanometer thickness, and we calibrate the oxidation rate for different instruments and process parameters. Our results provide quantitative guidance for managing both the atomic scale structure and thin-film morphology of oxides in the design and processing of TMD devices.

Original language	English
Pages (from-to)	5894-5901
Number of pages	8
Journal	Nano Letters
Volume	23
Issue number	13
DOIs	https://doi.org/10.1021/acs.nanolett.3c00303
State	Published - Jul 12 2023
Externally published	Yes

Funding

This work was funded in part by Semiconductor Research Corporation (SRC) under contract no. 2021-NM-3027. This work was supported by the Office of Naval Research (ONR) MURI through Grant No. N00014-17-1-2661. This work was performed with the use of facilities and instrumentation supported by NSF through the Massachusetts Institute of Technology Materials Research Science and Engineering Center DMR-1419807. This work was performed in part through the use of MIT.nano’s facilities. This work was performed in part at the Harvard University Center for Nanoscale Systems (CNS). K.R. acknowledges funding and support from a MIT MathWorks Engineering Fellowship and ExxonMobil Research and Engineering Company through the MIT Energy Initiative. We thank Prof. Deji Akinwande (University of Texas at Austin) and Drs. Sudarat Lee, Kevin O’Brien, and Chelsey Dorow (Intel Corporation) for useful discussions. We thank Dr. Yifei Li and Jiahao Dong (MIT) and Dr. Austin Akey and Dr. Jules Gardener (Harvard University) for technical assistance.

Funders	Funder number
MIT Energy Initiative
MIT MathWorks Engineering Fellowship
Massachusetts Institute of Technology Materials Research Science and Engineering Center	DMR-1419807
National Science Foundation
Office of Naval Research
Semiconductor Research Corporation	2021-NM-3027
ExxonMobil Research and Engineering Company
Multidisciplinary University Research Initiative	N00014-17-1-2661

Keywords

kinetics
oxidation
oxide/semiconductor interface
thin film morphology
transition metal dichalcogenides (TMDs)

Access to Document

10.1021/acs.nanolett.3c00303

Cite this

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title = "Atomic-Scale Mechanisms of MoS2 Oxidation for Kinetic Control of MoS2/MoO3 Interfaces",

abstract = "Oxidation of transition metal dichalcogenides (TMDs) occurs readily under a variety of conditions. Therefore, understanding the oxidation processes is necessary for successful TMD handling and device fabrication. Here, we investigate atomic-scale oxidation mechanisms of the most widely studied TMD, MoS2. We find that thermal oxidation results in α-phase crystalline MoO3 with sharp interfaces, voids, and crystallographic alignment with the underlying MoS2. Experiments with remote substrates prove that thermal oxidation proceeds via vapor-phase mass transport and redeposition, a challenge to forming thin, conformal films. Oxygen plasma accelerates the kinetics of oxidation relative to the kinetics of mass transport, forming smooth and conformal oxides. The resulting amorphous MoO3 can be grown with subnanometer to several-nanometer thickness, and we calibrate the oxidation rate for different instruments and process parameters. Our results provide quantitative guidance for managing both the atomic scale structure and thin-film morphology of oxides in the design and processing of TMD devices.",

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author = "Kate Reidy and Wouter Mortelmans and Jo, {Seong Soon} and Penn, {Aubrey N.} and Foucher, {Alexandre C.} and Zhenjing Liu and Tao Cai and Baoming Wang and Ross, {Frances M.} and R. Jaramillo",

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AU - Mortelmans, Wouter

AU - Jo, Seong Soon

AU - Penn, Aubrey N.

AU - Foucher, Alexandre C.

AU - Liu, Zhenjing

AU - Cai, Tao

AU - Wang, Baoming

AU - Ross, Frances M.

AU - Jaramillo, R.

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N2 - Oxidation of transition metal dichalcogenides (TMDs) occurs readily under a variety of conditions. Therefore, understanding the oxidation processes is necessary for successful TMD handling and device fabrication. Here, we investigate atomic-scale oxidation mechanisms of the most widely studied TMD, MoS2. We find that thermal oxidation results in α-phase crystalline MoO3 with sharp interfaces, voids, and crystallographic alignment with the underlying MoS2. Experiments with remote substrates prove that thermal oxidation proceeds via vapor-phase mass transport and redeposition, a challenge to forming thin, conformal films. Oxygen plasma accelerates the kinetics of oxidation relative to the kinetics of mass transport, forming smooth and conformal oxides. The resulting amorphous MoO3 can be grown with subnanometer to several-nanometer thickness, and we calibrate the oxidation rate for different instruments and process parameters. Our results provide quantitative guidance for managing both the atomic scale structure and thin-film morphology of oxides in the design and processing of TMD devices.

AB - Oxidation of transition metal dichalcogenides (TMDs) occurs readily under a variety of conditions. Therefore, understanding the oxidation processes is necessary for successful TMD handling and device fabrication. Here, we investigate atomic-scale oxidation mechanisms of the most widely studied TMD, MoS2. We find that thermal oxidation results in α-phase crystalline MoO3 with sharp interfaces, voids, and crystallographic alignment with the underlying MoS2. Experiments with remote substrates prove that thermal oxidation proceeds via vapor-phase mass transport and redeposition, a challenge to forming thin, conformal films. Oxygen plasma accelerates the kinetics of oxidation relative to the kinetics of mass transport, forming smooth and conformal oxides. The resulting amorphous MoO3 can be grown with subnanometer to several-nanometer thickness, and we calibrate the oxidation rate for different instruments and process parameters. Our results provide quantitative guidance for managing both the atomic scale structure and thin-film morphology of oxides in the design and processing of TMD devices.

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