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Title: Electronic d-band properties of gold nanoclusters grown on amorphous carbon

Abstract

The electronic d-band properties are important factors for the emerging catalytic activity of Au nanoclusters of sub-5-nm size. We analyzed the d-band properties of Au nanoclusters grown on amorphous carbon supports by photoelectron spectroscopy using synchrotron-radiation light coupled with high-resolution ion scattering spectrometry which enables us to estimate the size and shape of Au nanoclusters. The d-band width (W{sub d}), d-band center position (E{sub d}), and apparent 5d{sub 3/2}-d{sub 5/2} spin-orbit splitting (E{sub SO}) were determined as a function of a number of Au atoms per cluster (n{sub A}) and an average coordination number (n{sub C}) in a wide range (11<n{sub A}<1600). The W{sub d} and E{sub SO} values decrease steeply with decreasing n{sub A} below {approx}150 owing to band narrowing which is caused by hybridization of fewer wave functions of the valence electrons. However, E{sub d} shifts to the higher binding energy side with decreasing cluster size. The rapid movement of E{sub d} is attributed to the dynamic final-state effect, which results in higher binding energy shifts of core and valence states due to a positive hole created after photoelectron emission. We have estimated the contribution from the final-state effect and derived the approximated initial-state spectra. Modified data, however,more » still show a slight movement of the d-band center away from the Fermi level (E{sub F}) although the E{sub d} values for Au nanoclusters are closer to E{sub F} compared to the bulk value. This behavior is ascribed to the contraction of average Au-Au bond length with decreasing cluster size.« less

Authors:
; ; ; ;  [1];  [2]
  1. Department of Physics, Ritsumeikan University, Kusatsu, Shiga 525-8577 (Japan)
  2. Advanced Industrial Science and Technology (AIST) Kansai Center, Ikeda, Osaka 563-8577 (Japan)
Publication Date:
OSTI Identifier:
21538293
Resource Type:
Journal Article
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 83; Journal Issue: 16; Other Information: DOI: 10.1103/PhysRevB.83.165428; (c) 2011 American Institute of Physics; Journal ID: ISSN 1098-0121
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; ATOMIC CLUSTERS; ATOMS; BINDING ENERGY; BOND LENGTHS; CARBON; COORDINATION NUMBER; EMISSION; FERMI LEVEL; GOLD; IONS; NANOSTRUCTURES; ORBITS; PHOTOELECTRON SPECTROSCOPY; RESOLUTION; SCATTERING; SPECTRA; SPIN; SYNCHROTRON RADIATION; WAVE FUNCTIONS; ANGULAR MOMENTUM; BREMSSTRAHLUNG; CHARGED PARTICLES; DIMENSIONS; ELECTROMAGNETIC RADIATION; ELECTRON SPECTROSCOPY; ELEMENTS; ENERGY; ENERGY LEVELS; FUNCTIONS; LENGTH; METALS; NONMETALS; PARTICLE PROPERTIES; RADIATIONS; SPECTROSCOPY; TRANSITION ELEMENTS

Citation Formats

Visikovskiy, Anton, Matsumoto, Hisashi, Mitsuhara, Kei, Nakada, Toshitaka, Kido, Yoshiaki, and Akita, Tomoki. Electronic d-band properties of gold nanoclusters grown on amorphous carbon. United States: N. p., 2011. Web. doi:10.1103/PHYSREVB.83.165428.
Visikovskiy, Anton, Matsumoto, Hisashi, Mitsuhara, Kei, Nakada, Toshitaka, Kido, Yoshiaki, & Akita, Tomoki. Electronic d-band properties of gold nanoclusters grown on amorphous carbon. United States. https://doi.org/10.1103/PHYSREVB.83.165428
Visikovskiy, Anton, Matsumoto, Hisashi, Mitsuhara, Kei, Nakada, Toshitaka, Kido, Yoshiaki, and Akita, Tomoki. 2011. "Electronic d-band properties of gold nanoclusters grown on amorphous carbon". United States. https://doi.org/10.1103/PHYSREVB.83.165428.
@article{osti_21538293,
title = {Electronic d-band properties of gold nanoclusters grown on amorphous carbon},
author = {Visikovskiy, Anton and Matsumoto, Hisashi and Mitsuhara, Kei and Nakada, Toshitaka and Kido, Yoshiaki and Akita, Tomoki},
abstractNote = {The electronic d-band properties are important factors for the emerging catalytic activity of Au nanoclusters of sub-5-nm size. We analyzed the d-band properties of Au nanoclusters grown on amorphous carbon supports by photoelectron spectroscopy using synchrotron-radiation light coupled with high-resolution ion scattering spectrometry which enables us to estimate the size and shape of Au nanoclusters. The d-band width (W{sub d}), d-band center position (E{sub d}), and apparent 5d{sub 3/2}-d{sub 5/2} spin-orbit splitting (E{sub SO}) were determined as a function of a number of Au atoms per cluster (n{sub A}) and an average coordination number (n{sub C}) in a wide range (11<n{sub A}<1600). The W{sub d} and E{sub SO} values decrease steeply with decreasing n{sub A} below {approx}150 owing to band narrowing which is caused by hybridization of fewer wave functions of the valence electrons. However, E{sub d} shifts to the higher binding energy side with decreasing cluster size. The rapid movement of E{sub d} is attributed to the dynamic final-state effect, which results in higher binding energy shifts of core and valence states due to a positive hole created after photoelectron emission. We have estimated the contribution from the final-state effect and derived the approximated initial-state spectra. Modified data, however, still show a slight movement of the d-band center away from the Fermi level (E{sub F}) although the E{sub d} values for Au nanoclusters are closer to E{sub F} compared to the bulk value. This behavior is ascribed to the contraction of average Au-Au bond length with decreasing cluster size.},
doi = {10.1103/PHYSREVB.83.165428},
url = {https://www.osti.gov/biblio/21538293}, journal = {Physical Review. B, Condensed Matter and Materials Physics},
issn = {1098-0121},
number = 16,
volume = 83,
place = {United States},
year = {Fri Apr 15 00:00:00 EDT 2011},
month = {Fri Apr 15 00:00:00 EDT 2011}
}