Coordination-resolved spectrometrics of local bonding and electronic dynamics of Au atomic clusters, solid skins, and oxidized foils
By using combination of bond-order–length–strength (BOLS) correlation, the tight-binding (TB) approach, and zone-selective photoelectron spectroscopy (ZPS), we were able to resolve local bond relaxation and the associated 4f7/2 core-level shift of Au atomic clusters, Au(100, 110, 111) skins, and Au...
| Main Authors: | , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2015
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/103744 http://hdl.handle.net/10220/25920 |
| _version_ | 1826113606285000704 |
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| author | Yu, Wang Bo, Maolin Huang, Yongli Wang, Yan Li, Can Sun, Chang Qing |
| author2 | School of Electrical and Electronic Engineering |
| author_facet | School of Electrical and Electronic Engineering Yu, Wang Bo, Maolin Huang, Yongli Wang, Yan Li, Can Sun, Chang Qing |
| author_sort | Yu, Wang |
| collection | NTU |
| description | By using combination of bond-order–length–strength (BOLS) correlation, the tight-binding (TB) approach, and zone-selective photoelectron spectroscopy (ZPS), we were able to resolve local bond relaxation and the associated 4f7/2 core-level shift of Au atomic clusters, Au(100, 110, 111) skins, and Au foils exposed to ozone for different lengths of time. In addition to quantitative information, such as local bond length, bond energy, binding-energy density, and atomic cohesive energy, the results confirm our predictions that bond-order deficiency shortens and stiffens the bond between undercoordinated atoms, which results in local densification and quantum entrapment of bonding electrons. The entrapment perturbs the Hamiltonian, and hence, shifts the core-level energy accordingly. ZPS also confirms that oxidation enhances the effect of atomic undercoordination on the positive 4f7/2 energy shift, with the associated valence electron polarization contributing to the catalytic ability of undercoordinated Au atoms. |
| first_indexed | 2024-10-01T03:25:58Z |
| format | Journal Article |
| id | ntu-10356/103744 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T03:25:58Z |
| publishDate | 2015 |
| record_format | dspace |
| spelling | ntu-10356/1037442020-03-07T13:57:28Z Coordination-resolved spectrometrics of local bonding and electronic dynamics of Au atomic clusters, solid skins, and oxidized foils Yu, Wang Bo, Maolin Huang, Yongli Wang, Yan Li, Can Sun, Chang Qing School of Electrical and Electronic Engineering DRNTU::Science::Chemistry::Organic chemistry::Oxidation By using combination of bond-order–length–strength (BOLS) correlation, the tight-binding (TB) approach, and zone-selective photoelectron spectroscopy (ZPS), we were able to resolve local bond relaxation and the associated 4f7/2 core-level shift of Au atomic clusters, Au(100, 110, 111) skins, and Au foils exposed to ozone for different lengths of time. In addition to quantitative information, such as local bond length, bond energy, binding-energy density, and atomic cohesive energy, the results confirm our predictions that bond-order deficiency shortens and stiffens the bond between undercoordinated atoms, which results in local densification and quantum entrapment of bonding electrons. The entrapment perturbs the Hamiltonian, and hence, shifts the core-level energy accordingly. ZPS also confirms that oxidation enhances the effect of atomic undercoordination on the positive 4f7/2 energy shift, with the associated valence electron polarization contributing to the catalytic ability of undercoordinated Au atoms. 2015-06-16T10:24:24Z 2019-12-06T21:19:15Z 2015-06-16T10:24:24Z 2019-12-06T21:19:15Z 2015 2015 Journal Article Yu, W., Bo, M., Huang, Y., Wang, Y., Li, C., & Sun, C. Q. (2015). Coordination-resolved spectrometrics of local bonding and electronic dynamics of Au atomic clusters, solid skins, and oxidized foils. ChemPhysChem, 16(10), 2159-2164. 1439-4235 https://hdl.handle.net/10356/103744 http://hdl.handle.net/10220/25920 10.1002/cphc.201500171 en ChemPhysChem © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. |
| spellingShingle | DRNTU::Science::Chemistry::Organic chemistry::Oxidation Yu, Wang Bo, Maolin Huang, Yongli Wang, Yan Li, Can Sun, Chang Qing Coordination-resolved spectrometrics of local bonding and electronic dynamics of Au atomic clusters, solid skins, and oxidized foils |
| title | Coordination-resolved spectrometrics of local bonding and electronic dynamics of Au atomic clusters, solid skins, and oxidized foils |
| title_full | Coordination-resolved spectrometrics of local bonding and electronic dynamics of Au atomic clusters, solid skins, and oxidized foils |
| title_fullStr | Coordination-resolved spectrometrics of local bonding and electronic dynamics of Au atomic clusters, solid skins, and oxidized foils |
| title_full_unstemmed | Coordination-resolved spectrometrics of local bonding and electronic dynamics of Au atomic clusters, solid skins, and oxidized foils |
| title_short | Coordination-resolved spectrometrics of local bonding and electronic dynamics of Au atomic clusters, solid skins, and oxidized foils |
| title_sort | coordination resolved spectrometrics of local bonding and electronic dynamics of au atomic clusters solid skins and oxidized foils |
| topic | DRNTU::Science::Chemistry::Organic chemistry::Oxidation |
| url | https://hdl.handle.net/10356/103744 http://hdl.handle.net/10220/25920 |
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