The Importance of Decarbonylation Mechanisms in the Atomic Layer Deposition of High-Quality Ru Films by Zero-Oxidation State Ru(DMBD)(CO)3

Schneider, Joel R.; Paula, Camila; Lewis, Jacqueline; Woodruff, Jacob; Raiford, James A.; Bent, Stacey F.

doi:10.1002/smll.202105513

Title: The Importance of Decarbonylation Mechanisms in the Atomic Layer Deposition of High-Quality Ru Films by Zero-Oxidation State Ru(DMBD)(CO)₃

Journal Article · 04 January 2022 · Small

DOI: https://doi.org/10.1002/smll.202105513 · OSTI ID:1840537

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Stanford Univ., CA (United States); Stanford University
Stanford Univ., CA (United States)
EMD Electronics, Haverhill, MA (United States)

Achieving facile nucleation of noble metal films through atomic layer deposition (ALD) is extremely challenging. To this end, η⁴-2,3-dimethylbutadiene ruthenium tricarbonyl (Ru(DMBD)(CO)₃), a zero-valent complex, has recently been reported to achieve good nucleation by ALD at relatively low temperatures and mild reaction conditions. Here, we study the growth mechanism of this precursor by in situ quartz-crystal microbalance and quadrupole mass spectrometry during Ru ALD, complemented by ex situ film characterization and kinetic modeling. These studies reveal that Ru(DMBD)(CO)₃ produces high-quality Ru films with excellent nucleation properties. This results in smooth, coalesced films even at low film thicknesses, all important traits for device applications. However, Ru deposition follows a kinetically limited decarbonylation reaction scheme, akin to typical CVD processes, with a strong dependence on both temperature and reaction timescale. The non-self-limiting nature of the kinetically driven mechanism presents both challenges for ALD implementation and opportunities for process tuning. By surveying reports of similar precursors, we suggest that the findings can be generalized to the broader class of zero-oxidation state carbonyl-based precursors used in thermal ALD, with insight into the design of effective saturation studies.

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Research Organization:: Stanford Univ., CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Science Foundation (NSF)

Grant/Contract Number:: SC0004782

OSTI ID:: 1840537

Journal Information:: Small, Journal Name: Small Journal Issue: 9 Vol. 18; ISSN 1613-6810

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: The Importance of Decarbonylation Mechanisms in the Atomic Layer Deposition of High-Quality Ru Films by Zero-Oxidation State Ru(DMBD)(CO)3

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References (80)

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Title: The Importance of Decarbonylation Mechanisms in the Atomic Layer Deposition of High-Quality Ru Films by Zero-Oxidation State Ru(DMBD)(CO)₃