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Plasmonic Control of Near-Interface Exciton Dynamics in Defect-Rich ZnO Thin Films

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Abstract

Zinc oxide (ZnO) is an attractive material for many electro-optical applications, but the control of impurities remains an issue in device fabrication. For this paper, the dynamics of defect states produced by annealing ZnO thin films at temperatures of 400–800 °C were probed by band-edge pump-probe spectroscopy in differential reflection and transmission. The distinction between the differential reflection and transmission spectra allowed for the analysis of ultrafast near-interface dynamics, which cannot be separated from the bulk thin-film dynamics by traditional ultrafast spectroscopies. In particular, simultaneous differential reflection and transmission spectroscopy provided clear evidence that the band-edge recombination dynamics in samples annealed at 400 °C were absent near the ZnO/substrate interface. However, the Purcell enhancement observed in Ag/ZnO heterostructures resulted in the dramatic emergence of the band-edge recombination signal nearly two orders of magnitude greater in intensity than the defect differential reflectivity. This indicates that the spatial range of the Purcell effect is at least twice as large as inferred from previous photoluminescence studies.

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Acknowledgements

BJL and RFH acknowledge support of the ultrafast spectroscopy experiments at Vanderbilt by the US Department of Energy, Office of Science (DE-FG02-01ER45916). PL experiments and thin-film fabrication at Fisk University were supported by an NSF-CREST grant (HRD-0420516) and by a Department of Defense grant (W911NF-11-1-0156). BJL acknowledges additional support from an IC postdoctoral fellowship at Oak Ridge National Laboratory. The Oak Ridge National Laboratory is managed by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725 with the US Department of Energy.

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  1. B. J. Lawrie

    Present address: Computational Sciences and Engineering Division, Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, TN, 37831-6082, USA

Authors and Affiliations

  1. Interdisciplinary Materials Science Program, Vanderbilt University, Nashville, TN, 37234-0106, USA

    B. J. Lawrie

  2. Department of Physics, Fisk University, 1000 17th Ave. North, Nashville, TN, 37208, USA

    R. Mu

  3. Department of Physics and Astronomy, Vanderbilt University, 6301 Stevenson Center, Nashville, TN, 37235-1807, USA

    R. F. Haglund

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  1. B. J. Lawrie
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  2. R. Mu
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  3. R. F. Haglund
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Correspondence to B. J. Lawrie.

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Lawrie, B.J., Mu, R. & Haglund, R. Plasmonic Control of Near-Interface Exciton Dynamics in Defect-Rich ZnO Thin Films. Plasmonics 8, 693–697 (2013). https://doi.org/10.1007/s11468-012-9459-9

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  • DOI: https://doi.org/10.1007/s11468-012-9459-9

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