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X-ray pump optical probe cross-correlation study of GaAs

Nature Photonics volume 6, pages 111–114 (2012)Cite this article

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Abstract

Ultrafast dynamics in atomic, molecular and condensed-matter systems are increasingly being studied using optical-pump, X-ray probe techniques where subpicosecond laser pulses excite the system and X-rays detect changes in absorption spectra and local atomic structure1,2,3. New opportunities are appearing as a result of improved synchrotron capabilities and the advent of X-ray free-electron lasers4,5. These source improvements also allow for the reverse measurement: X-ray pump followed by optical probe. We describe here how an X-ray pump beam transforms a thin GaAs specimen from a strong absorber into a nearly transparent window in less than 100 ps, for laser photon energies just above the bandgap. We find the opposite effect—X-ray induced optical opacity—for photon energies just below the bandgap. This raises interesting questions about the ultrafast many-body response of semiconductors to X-ray absorption, and provides a new approach for an X-ray/optical cross-correlator for synchrotron and X-ray free-electron laser applications.

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Figure 1: Transmission at 860 nm versus time after X-ray pump pulse.
Figure 2: Model for X-ray-induced transmission and absorption.
Figure 3: Absorption factor (μ(λ)L = −ln(T)) versus time delay.
Figure 4: Transmission at 890 nm from 1 × 10−11 to 1 × 10−4 s.

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Acknowledgements

This research was supported by the US Department of Energy, Office of Basic Energy Science (award no. DE-SC0004078). Use of the Advanced Photon Source was supported by the US Department of Energy, Basic Energy Sciences, Office of Science (contract no. DE-AC02-06CH11357). Use of the BioCARS Sector 14 was supported by the National Institutes of Health, National Center for Research Resources (grant no. RR007707). The time-resolved set-up at Sector 14 was funded in part through a collaboration with Philip Anfinrud (NIH/NIDDK).

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Authors and Affiliations

  1. Department of Physics, Purdue University, West Lafayette, 47907, Indiana, USA

    S. M. Durbin & T. Clevenger

  2. The Center for Advanced Radiation Sources, University of Chicago, Chicago, 60637, Illinois, USA

    T. Graber & R. Henning

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  1. S. M. Durbin
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  2. T. Clevenger
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All four authors were substantially involved with acquiring the data. S.M.D. analysed the results and wrote the manuscript, with assistance from T.G.

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Correspondence to S. M. Durbin.

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Durbin, S., Clevenger, T., Graber, T. et al. X-ray pump optical probe cross-correlation study of GaAs. Nature Photon 6, 111–114 (2012). https://doi.org/10.1038/nphoton.2011.327

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