Adsorption Processes during Electrochemical Atomic Layer Deposition of Gold

Wasalathanthri, Ruwani N.; Gong, Yukun; Biener, Monika M.; Ivanovskaya, Anna N.; Dudukovic, Nikola A.; Akolkar, Rohan

doi:10.1149/1945-7111/ac3310

Adsorption Processes during Electrochemical Atomic Layer Deposition of Gold

Journal Article · Mon Nov 08 04:00:00 EST 2021 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/1945-7111/ac3310· OSTI ID:1837812

Wasalathanthri, Ruwani N. ^[1]; ^[1]; Biener, Monika M. ^[2]; Ivanovskaya, Anna N. ^[2]; Dudukovic, Nikola A. ^[2]; ^[1]

Case Western Reserve Univ., Cleveland, OH (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Electrochemical atomic layer deposition (e-ALD) technique offers a simple and effective "wet chemistry" approach enabling high-precision monolayer-by-monolayer deposition of metal films. The process of e-ALD of Au involves lead underpotential deposition (PbUPD) followed by its redox replacement by a Au monolayer. The time evolution of the deposit mass during "one-pot" Au e-ALD is known to exhibit a unique three-stage response that is presently not well understood. In this work, we probe this response using voltammetry, electrochemical quartz crystal microgravimetry (e-QCM), and chronoamperometry to unravel the underlying mechanistic events during Au e-ALD. Furthermore, the presence of adsorbed Au⁺³-ligand complex(es) (Au-L) on the Au surface is established. In stage I of e-ALD, this Au-L adsorbed layer is reduced to Au while a Pb_UPD adlayer is formed. In stage II, the Pb_UPD adlayer undergoes spontaneous surface-limited redox replacement by nobler Au under open-circuit conditions. Finally, in stage III, re-adsorption of the Au-L occurs on the newly deposited Au. Quantitative analysis of the deposit mass transients obtained under a variety of conditions provides an estimate of the Au-L mass and its molecular weight.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1837812

Report Number(s):: LLNL-JRNL--825881; 1040200

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 11 Vol. 168; ISSN 0013-4651

Publisher:: IOP Publishing - The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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