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Investigation of the nonlinear refractive index of single-crystalline thin gold films and plasmonic nanostructures

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Abstract

The nonlinear refractive index of plasmonic materials may be used to obtain nonlinear functionality, e.g., power-dependent switching. Here, we investigate the nonlinear refractive index of single-crystalline gold in thin layers and nanostructures on dielectric substrates. In a first step, we implement a z-scan setup to investigate ~100-µm-sized thin-film samples. We determine the nonlinear refractive index of fused silica, n 2(SiO2) = 2.9 × 10−20 m2/W, in agreement with literature values. Subsequent z-scan measurements of single-crystalline gold films reveal a damage threshold of 0.22 TW/cm2 and approximate upper limits of the real and imaginary parts of the nonlinear refractive index, |n 2′(Au)| < 1.2 × 10−16 m2/W and |n 2″(Au)| < 0.6 × 10−16 m2/W, respectively. To further determine possible effects of a nonlinear refractive index in plasmonic circuitry, interferometry is proposed as a phase-sensitive probe. In corresponding nanostructures, relative phase changes between two propagating near-field modes are converted to amplitude changes by mode interference. Power-dependent experiments using sub-10-fs near-infrared pulses and diffraction-limited resolution (NA = 1.4) reveal linear behavior up to the damage threshold (0.23 times relative to that of a solid single-crystalline gold film). An upper limit for the nonlinear power-dependent phase change between two propagating near-field modes is determined to Δφ < 0.07 rad.

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Acknowledgments

This work was supported by the German Science Foundation (DFG) within the Priority Program “Ultrafast Nanooptics” (SPP 1391).

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Author notes

  1. Monika Pawłowska

    Present address: Nencki Institute for Experimental Biology, Polish Academy of Sciences, 3 Pasteur Street, 02-093, Warsaw, Poland

Authors and Affiliations

  1. Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Am Hubland, 97074, Würzburg, Germany

    Sebastian Goetz, Christian Dreher, Matthias Wurdack, Monika Pawłowska & Tobias Brixner

  2. Nano-Optics and Biophotonics Group, Experimentelle Physik 5, Universität Würzburg, Am Hubland, 97074, Würzburg, Germany

    Gary Razinskas, Enno Krauss, Peter Geisler & Bert Hecht

  3. Röntgen Research Center for Complex Material Systems (RCCM), Universität Würzburg, Am Hubland, 97074, Würzburg, Germany

    Bert Hecht & Tobias Brixner

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  1. Sebastian Goetz
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Correspondence to Bert Hecht or Tobias Brixner.

Additional information

This article is part of the topical collection “Ultrafast Nanooptics” guest edited by Martin Aeschlimann and Walter Pfeiffer.

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Goetz, S., Razinskas, G., Krauss, E. et al. Investigation of the nonlinear refractive index of single-crystalline thin gold films and plasmonic nanostructures. Appl. Phys. B 122, 94 (2016). https://doi.org/10.1007/s00340-016-6370-7

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  • DOI: https://doi.org/10.1007/s00340-016-6370-7

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