Molecular Limits to the Quantum Confinement Model in Diamond Clusters

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The electronic structure of monodisperse, hydrogen-passivated diamond clusters in the gas phase has been studied with x-ray absorption spectroscopy. The data show that the bulk-related unoccupied states do not exhibit any quantum confinement. Additionally, density of states below the bulk absorption edge appears, consisting of features correlated to CH and CH{sub 2} hydrogen surface termination, resulting in an effective red shift of the lowest unoccupied states. The results contradict the commonly used and very successful quantum confinement model for semiconductors which predicts increasing band edge blue shifts with decreasing particle size. Our findings indicate that in the ultimate size limit ... continued below

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6 p. (0.2 MB)

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Willey, T M; Bostedt, C; van Buuren, T; Dahl, J E; Liu, S E; Carlson, R K et al. April 7, 2005.

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The electronic structure of monodisperse, hydrogen-passivated diamond clusters in the gas phase has been studied with x-ray absorption spectroscopy. The data show that the bulk-related unoccupied states do not exhibit any quantum confinement. Additionally, density of states below the bulk absorption edge appears, consisting of features correlated to CH and CH{sub 2} hydrogen surface termination, resulting in an effective red shift of the lowest unoccupied states. The results contradict the commonly used and very successful quantum confinement model for semiconductors which predicts increasing band edge blue shifts with decreasing particle size. Our findings indicate that in the ultimate size limit for nanocrystals a more molecular description is necessary.

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6 p. (0.2 MB)

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PDF-file: 6 pages; size: 0.2 Mbytes

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  • Journal Name: Physical Review Letters; Journal Volume: 95; Journal Issue: 11

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  • Report No.: UCRL-JRNL-211271
  • Grant Number: W-7405-ENG-48
  • Office of Scientific & Technical Information Report Number: 875931
  • Archival Resource Key: ark:/67531/metadc876588

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Office of Scientific & Technical Information Technical Reports

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  • April 7, 2005

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  • Sept. 21, 2016, 2:29 a.m.

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  • April 17, 2017, 12:13 p.m.

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Willey, T M; Bostedt, C; van Buuren, T; Dahl, J E; Liu, S E; Carlson, R K et al. Molecular Limits to the Quantum Confinement Model in Diamond Clusters, article, April 7, 2005; Livermore, California. (digital.library.unt.edu/ark:/67531/metadc876588/: accessed October 15, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.