Di-tert-butyl disulfide as a replacement for hydrogen sulfide in the atomic layer deposition of two-dimensional molybdenum disulfide

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dc.check.date2026-02-11en
dc.check.infoAccess to this article is restricted until 12 months after publication by request of the publisheren
dc.contributor.authorCampbell, Ian E.en
dc.contributor.authorGupta, Aashien
dc.contributor.authorMetaxa, Pavlinaen
dc.contributor.authorArifutzzaman, A.en
dc.contributor.authorMa, Taoen
dc.contributor.authorArellano, Paulaen
dc.contributor.authorDuffy, Rayen
dc.contributor.authorBol, Ageeth A.en
dc.contributor.funderScience Foundation Irelanden
dc.contributor.funderNederlandse Organisatie voor Wetenschappelijk Onderzoeken
dc.contributor.funderHorizon 2020en
dc.date.accessioned2025-02-18T12:46:33Z
dc.date.available2025-02-18T12:46:33Z
dc.date.issued2025-02-11en
dc.description.abstractAtomic layer deposition (ALD), with its precise process control and conformality, has recently gained interest for synthesizing transition metal sulfides like MoS2, which have varied applications in low-dimensional electronics and electrocatalysts. Hydrogen sulfide (H2S) has been used in many sulfide ALD processes; however, H2S is a toxic gas that requires expensive containment and abatement measures for shipping, installation, and storage. Herein, we report a PEALD process capable of synthesizing MoS2 without H2S. This process utilizes a Mo precursor commonly used in ALD, hydrogen plasma, and di-tert-butyl disulfide (TBDS), which is a liquid that is significantly less hazardous and expensive than H2S. It was found that the TBDS-based PEALD process results in layered, stoichiometric MoS2 with limited contamination. The TBDS-based PEALD process was also analyzed via mass spectrometry to determine the mechanistic roles of each reactant. Apparently, H2 plasma removes ligands from the chemisorbed Mo precursor, which allows TBDS to sulfurize the top layer, producing H2S and isobutene as byproducts. MoS2 films deposited via the TBDS-based process possessed fewer yet taller out-of-plane growths and similar crystal grain diameter (∼10 nm) and electrical resistivity (13.6–15.5 Ω·cm for 3 nm thick films) compared to films made with H2S. Thus, the TBDS-based process is a suitable and safer alternative to the H2S-based process for large-area synthesis of layered MoS2.en
dc.description.statusPeer revieweden
dc.description.versionAccepted Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationCampbell, I. E., Gupta, A., Metaxa, P., Arifutzzaman, A., Ma, T., Arellano, P., Duffy, R. and Bol, A. A. (2025) 'Di-tert-butyl disulfide as a replacement for hydrogen sulfide in the atomic layer deposition of two-dimensional molybdenum disulfide', Chemistry of Materials. https://doi.org/10.1021/acs.chemmater.4c02561en
dc.identifier.doihttps://doi.org/10.1021/acs.chemmater.4c02561en
dc.identifier.eissn1520-5002en
dc.identifier.issn0897-4756en
dc.identifier.journaltitleChemistry of Materialsen
dc.identifier.urihttps://hdl.handle.net/10468/17062
dc.language.isoenen
dc.publisherAmerican Chemical Societyen
dc.relation.ispartofChemistry of Materialsen
dc.relation.projectinfo:eu-repo/grantAgreement/NWO//17846/NL/Defects, a curse or a blessing: tailoring defects in two-dimensional transition metal dichalcogenides by atomic layer deposition/en
dc.relation.projectinfo:eu-repo/grantAgreement/EC/H2020::RIA/871130/EU/Access to European Infrastructure for Nanoelectronics/ASCENTPlusen
dc.relation.projectinfo:eu-repo/grantAgreement/SFI/SFI Frontiers for the Future::Awards/21/FFP-A/9897/IE/Pulsed laser annealing of low temperature 2D semiconductors for large area applications in electronics using flexible substrates/en
dc.rights© 2025, American Chemical Society. This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials after technical editing by the publisher. To access the final edited and published work see: https://doi.org/10.1021/acs.chemmater.4c02561en
dc.subjectAtomic layer depositionen
dc.subjectDepositionen
dc.subjectPlasmaen
dc.subjectPrecursorsen
dc.subjectThicknessen
dc.titleDi-tert-butyl disulfide as a replacement for hydrogen sulfide in the atomic layer deposition of two-dimensional molybdenum disulfideen
dc.typeArticle (peer-reviewed)en
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