Oxidation State Discrimination in the Atomic Layer Deposition of Vanadium Oxides

Weimer, Matthew S.; Kim, In Soo; Guo, Peijun; Schaller, Richard D.; Martinson, Alex B.  F.; Hock, Adam S.

doi:10.1021/acs.chemmater.7b01130

Title: Oxidation State Discrimination in the Atomic Layer Deposition of Vanadium Oxides

Journal Article · Fri Jun 02 00:00:00 EDT 2017 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.7b01130· OSTI ID:1393545

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Illinois Inst. of Technology, Chicago, IL (United States). Dept. of Chemistry; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Div.
Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Div.
Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering and Dept. of Chemistry
Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
Illinois Inst. of Technology, Chicago, IL (United States). Dept. of Chemistry; Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Div.

We describe the use of a vanadium 3+ precursor for atomic layer deposition (ALD) of thin films that span the common oxidation states of vanadium oxides. Self-limiting surface synthesis of V₂O₃, VO₂, and V₂O₅ are realized via four distinct reaction mechanisms accessed via judicious choice of oxygen ALD partners. In situ quartz crystal microbalance and quadrupole mass spectrometry were used to study the reaction mechanism of the vanadium precursor with O₃, H₂O₂, H₂O/O₂, and H₂O₂/H₂. A clear distinction between non-oxidative protic ligand exchange and metal oxidation is demonstrated through sequential surface reactions with different non-metal precursors. This synergistic effect, provides greater control of the resultant metal species in the film, as well as reactive surface species during growth. In an extension of this approach, we introduce oxidation state control through reducing equivalents of H₂ gas. When H₂ is dosed after H₂O₂ during growth, amorphous films of VO₂ are deposited that are readily crystallized with a low temperature anneal. These VO₂ films show a temperature dependent Raman spectroscopy response in the expected range and consistent with the well-known phase-change behavior of VO₂.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1393545

Journal Information:: Chemistry of Materials, Vol. 29, Issue 15; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 14 works

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