Controlling the Thermal Stability and Volatility of Organogold(I) Compounds for Vapor Deposition with Complementary Ligand Design

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dc.creator Griffiths, Matthew B. E.
dc.creator Dubrawski, Zachary S.
dc.creator Bačić, Goran
dc.creator Japahuge, Achini
dc.creator Masuda, Jason D.
dc.creator Zeng, Tao
dc.creator Barry, Seán T.
dc.date.accessioned 2021-11-09T16:55:45Z
dc.date.available 2021-11-09T16:55:45Z
dc.date.issued 2019-12-15
dc.identifier.issn 1434-1948
dc.identifier.uri http://library2.smu.ca/xmlui/handle/01/29970
dc.description Submitted Version en_CA
dc.description.abstract Atomic layer deposition (ALD) of gold is being studied by multiple research groups, but to date no process using non-energetic co-reactants has been demonstrated. In order to access milder co-reactants, precursors with higher thermal stability are required. We set out to uncover how structure and bonding affect the stability and volatility of a family of twelve organogold(I) compounds using a combination of techniques: X-ray diffraction (XRD), thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), and density functional theory (DFT). Small, unsubstituted phosphonium ylide ligands bind more strongly to Au(I) than their silyl-substituted analogues, but the utility of both these ligands suffers due to their poor volatility and substantial thermal decomposition. Pentafluorophenyl (C6F5) is introduced as a new, very electronegative ligand for gold vapor deposition precursors, and it was found that the disadvantage to volatility due to π-stacking and other intermolecular interactions in the solid state was overshadowed by dramatic improvements to kinetic and thermodynamic stability. We introduce a new figure of merit to compare and rank the suitability of these and other complexes as precursors for vapor deposition. Finally, DFT calculations on four compounds that have high figures of merit show a linear correlation between the gold-coordinative ligand bond dissociation energies and the observed decomposition temperatures, highlighting and justifying this design strategy. en_CA
dc.description.provenance Submitted by Sherry Briere (sherry.briere@smu.ca) on 2021-11-09T16:55:45Z No. of bitstreams: 2 Masuda_Jason_D_article_2019.pdf: 2158016 bytes, checksum: 25d87fe475634f6933444ccb1b74b38e (MD5) Masuda_Jason_D_article_2019_orginial.pdf: 1392294 bytes, checksum: ef8d56d28044cc9abec5af32d213dd1e (MD5) en
dc.description.provenance Made available in DSpace on 2021-11-09T16:55:45Z (GMT). No. of bitstreams: 2 Masuda_Jason_D_article_2019.pdf: 2158016 bytes, checksum: 25d87fe475634f6933444ccb1b74b38e (MD5) Masuda_Jason_D_article_2019_orginial.pdf: 1392294 bytes, checksum: ef8d56d28044cc9abec5af32d213dd1e (MD5) Previous issue date: 2019-12-15 en
dc.language.iso en en_CA
dc.publisher John Wiley & Sons, Inc. en_CA
dc.relation.uri https://doi.org/10.1002/ejic.201901087
dc.rights This is the pre-peer reviewed version of the following article: [Griffiths, M.B.E., Dubrawski, Z.S., Bačić, G., Japahuge, A., Masuda, J.D., Zeng, T., and Barry, S.T. (2019). Controlling Thermal Stability and Volatility of Organogold(I) Compounds for Vapor Deposition with Complementary Ligand Design. European Journal of Inorganic Chemistry, Volume 2019, Issue 46, which has been published in final form at 10.1002/ejic.201901087. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions.
dc.title Controlling the Thermal Stability and Volatility of Organogold(I) Compounds for Vapor Deposition with Complementary Ligand Design en_CA
dc.type Text en_CA
dcterms.bibliographicCitation European Journal of Inorganic Chemistry 2019(46): 4927-4938. (2019) en_CA
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This is the pre-peer reviewed version of the following article: [Griffiths, M.B.E., Dubrawski, Z.S., Bačić, G., Japahuge, A., Masuda, J.D., Zeng, T., and Barry, S.T. (2019). Controlling Thermal Stability and Volatility of Organogold(I) Compounds for Vapor Deposition with Complementary Ligand Design. European Journal of Inorganic Chemistry, Volume 2019, Issue 46, which has been published in final form at 10.1002/ejic.201901087. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions.
 
Published Version: https://doi.org/10.1002/ejic.201901087
 
 

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