Quantum chemical study of the effect of precursor stereochemistry on dissociative chemisorption and surface redox reactions during the atomic layer deposition of the transition metal copper

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dc.contributor.author Dey, Gangotri
dc.contributor.author Elliott, Simon D.
dc.date.accessioned 2015-09-28T12:41:26Z
dc.date.available 2015-09-28T12:41:26Z
dc.date.issued 2015-03-11
dc.identifier.citation DEY, G. & ELLIOTT, S. D. 2015. Quantum Chemical Study of the Effect of Precursor Stereochemistry on Dissociative Chemisorption and Surface Redox Reactions During the Atomic Layer Deposition of the Transition Metal Copper. The Journal of Physical Chemistry C, 119, 5914-5927. DOI: http://dx.doi.org/10.1021/jp509334u en
dc.identifier.volume 119 en
dc.identifier.issued 11 en
dc.identifier.startpage 5914 en
dc.identifier.endpage 5927 en
dc.identifier.issn 1932-7447
dc.identifier.uri http://hdl.handle.net/10468/1990
dc.identifier.doi 10.1021/jp509334u
dc.description.abstract Using quantum chemical calculations, we investigate surface reactions of copper precursors and diethylzinc as the reducing agent for effective Atomic Layer Deposition (ALD) of Cu. The adsorption of various commonly used Cu(II) precursors is explored. The precursors vary in the electronegativity and conjugation of the ligands and flexibility of the whole molecule. Our study shows that the overall stereochemistry of the precursor governs the adsorption onto its surface. Formation of different Cu(II)/Cu(I)/Cu(0) intermediate complexes from the respective Cu(II) compounds on the surface is also explored. The surface model is a (111) facet of a Cu55 cluster. Cu(I) compounds are found to cover the surface after the precursor pulse, irrespective of the precursor chosen. We provide new information about the surface chemistry of Cu(II) versus Cu(I) compounds. A pair of CuEt intermediates or the dimer Cu2Et2 reacts in order to deposit a new Cu atom and release gaseous butane. In this reaction, two electrons from the Et anions are donated to copper for reduction to metallic form. This indicates that a ligand exchange between the Cu and Zn is important for the success of this transmetalation reaction. The effect of the ligands in the precursor on the electron density before and after adsorption onto the surface has also been computed through population analysis. In the Cu(I) intermediate, charge is delocalized between the Cu precursor and the bare copper surface, indicating metallic bonding as the precursor densifies to the surface. en
dc.description.sponsorship ALDesign project en
dc.format.mimetype application/pdf en
dc.language.iso en en
dc.publisher American Chemical Society en
dc.relation.uri http://pubs.acs.org/doi/suppl/10.1021/jp509334u
dc.rights This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Journal of Physical Chemistry C, copyright © American Chemical Society after peer review. en
dc.subject Atomic layer deposition (ALD) en
dc.title Quantum chemical study of the effect of precursor stereochemistry on dissociative chemisorption and surface redox reactions during the atomic layer deposition of the transition metal copper en
dc.type Article (peer-reviewed) en
dc.internal.authorcontactother Simon Elliott, Tyndall Theory Modelling & Design Centre, University College Cork, Cork, Ireland. +353-21-490-3000 Email: simon.elliott@tyndall.ie en
dc.internal.availability Full text available en
dc.date.updated 2015-04-13T14:27:31Z
dc.description.version Submitted Version en
dc.internal.rssid 297892844
dc.description.status Peer reviewed en
dc.identifier.journaltitle Journal of Physical Chemistry C en
dc.internal.copyrightchecked Yes 12 month embargo. !!CORA!! Embargo required on accepted version only. Submitted version uploaded. en
dc.internal.licenseacceptance Yes en
dc.internal.IRISemailaddress simon.elliott@tyndall.ie en

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