Atomic resolution mapping of the excited-state electronic structure of Cu2O with time-resolved x-ray absorption spectroscopy

P. W. Hillyard, S. V. N. T. Kuchibhatla, T. E. Glover, M. P. Hertlein, N. Huse, P. Nachimuthu, L. V. Saraf, S. Thevuthasan, and K. J. Gaffney
Phys. Rev. B 80, 125210 – Published 29 September 2009

Abstract

We have used time-resolved soft x-ray spectroscopy to investigate the electronic structure of optically excited cuprous oxide at the OK edge and the CuL3 edge. The 400 nm optical excitation shifts the Cu and O absorptions to lower energy, but does not change the integrated x-ray absorption significantly for either edge. The constant integrated x-ray absorption cross-section indicates that the conduction-band and valence-band edges have very similar Cu3d and O2p orbital contributions. The 2.1 eV optical band gap of Cu2O significantly exceeds the one eV shift in the CuL3- and OK-edges absorption edges induced by optical excitation, demonstrating the importance of core-hole excitonic effects and valence electron screening in the x-ray absorption process.

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  • Received 1 May 2009

DOI:https://doi.org/10.1103/PhysRevB.80.125210

©2009 American Physical Society

Authors & Affiliations

P. W. Hillyard1,2,*, S. V. N. T. Kuchibhatla3, T. E. Glover4, M. P. Hertlein4, N. Huse5, P. Nachimuthu3, L. V. Saraf3, S. Thevuthasan3, and K. J. Gaffney1,†

  • 1PULSE Institute for Ultrafast Energy Science, Stanford Linear Accelerator Center, Stanford University, Stanford, California 94305, USA
  • 2Department of Chemistry, Stanford University, Stanford, California 94305, USA
  • 3EMSL, Pacific Northwest National Laboratory, Richland, Washington 99352, USA
  • 4Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA
  • 5Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA

  • *Present address: Bay Area Environmental Research Institute, Sonoma, CA 95476.
  • Corresponding author; kgaffney@slac.stanford.edu

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Issue

Vol. 80, Iss. 12 — 15 September 2009

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