Hostname: page-component-76fb5796d-vvkck Total loading time: 0 Render date: 2024-04-26T01:13:31.104Z Has data issue: false hasContentIssue false
  • English
  • Français

Semiempirical Self-Consistent Field Modeling of the Ce+3 4f AND 5d Energy Levels in Solid State Luminescent Materials

Published online by Cambridge University Press:  15 February 2011

Philip D. Rack ,
Paul H. Holloway ,
Ted A O'Brien  and
Michael C. Zerner
Philip D. Rack
Affiliation:
Department of Microelectronic Engineering, Rochester Institute of Technology, Rochester, NY 14623-5604
Paul H. Holloway
Affiliation:
Department of Materials Science and Engineering, University of Florida, Gainesville, FL 32611-6400
Ted A O'Brien
Affiliation:
Quantum Theory Project, PO Box 118435, University of Florida, Gainesville, FL 32611-8435
Michael C. Zerner
Affiliation:
Quantum Theory Project, PO Box 118435, University of Florida, Gainesville, FL 32611-8435
Get access

Abstract

Rare earth doped semiconductors are known to be efficient luminescent materials. In particular, SrS and SrxS and SrxGa2S4 doped with Ce+3 have recently been explored as efficient blue cathodoluminsecent and electroluminescent materials for flat panel display applications. The blue emission in these materials is due to Ce+3 5d-4f transitions, and the transition energies are sensitive to the local chemistry of the Ce+3 ion. To understand the effect that the local chemistry has on the Ce+3 4f–5d emission spectrum, we used a self-consistent-field configuration interaction (SCF/CI) model to calculate the electronic spectrum of the Ce−3 ion embedded in a cluster representation of the semiconductor lattice. The effects of changing nearest neighbor anions and cations have been modeled and are in excellent agreement with the experimental spectroscopy. While vibronic transitions are not calculated in this model, the calculated line transitions were fit to Gaussian peaks to generate absorption and emission spectra. Calculated and experimental Ce3+ 4f–5d emission spectra are compared for different materials, and the observed spectral changes are correlated to an analysis of the magnitude of the ligand field splitting and the nephelauxetic effect in various host lattices. Computed atomic orbital electron populations support these arguments.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 579: Symposium B – The Optical Properties of Materials , 1999 , 221
Copyright
Copyright © Materials Research Society 2000

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

1. O'Brien, T. A., Rack, P. D., Holloway, P. H., and Zemer, M. C., Journal of Luminescence 78, 245 (1998).Google Scholar
2. Pople, J.A., Beveridge, D.L., Approximate Molecular Orbital Theory, (McGraw-Hill, New York, 1970).Google Scholar
3. Sadlej, J., Semiempirical Methods of Quantum Chemistry, (Wiley, New York, 1985.)Google Scholar
4. Cotton, F. A., ChemicalApplications of Group Theory, 3rd ed. (John Wiley & Sons, New York, 1990).Google Scholar
5. Yamashita, N., Michitsuji, Y., and Asano, S., Journal of the Electrochemical Society 134, 2932 (1987).Google Scholar
6. Harris, D. C. and Bertolucci, M. D., Symmetry and Spectroscopy (Oxford University Press, New York, 1978).Google Scholar
7. Kotzian, M., Rosch, N., Schröder, H., and Zerner, M. C., Journal of the American Chemical Society 111, 7687 (1989).Google Scholar
8. Rack, P.D., Holloway, P.H., Sun, S.-S., Journal of the Society for Information Display 4 (4), 281 (1996).Google Scholar
9. Rack, P. D., Holloway, P. H., O'Brien, T. A., and Zerner, M. C., Journal of Applied Physics, 86 (5), 2377 (1999).Google Scholar