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Phase-referenced nonlinear spectroscopy of the α-quartz/water interface

Author

Listed:
  • Paul E. Ohno

    (Northwestern University)

  • Sarah A. Saslow

    (Northwestern University
    Present address: Earth Systems Science Division, Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, USA)

  • Hong-fei Wang

    (Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory)

  • Franz M. Geiger

    (Northwestern University)

  • Kenneth B. Eisenthal

    (Columbia University)

Abstract

Probing the polarization of water molecules at charged interfaces by second harmonic generation spectroscopy has been heretofore limited to isotropic materials. Here we report non-resonant nonlinear optical measurements at the interface of anisotropic z-cut α-quartz and water under conditions of dynamically changing ionic strength and bulk solution pH. We find that the product of the third-order susceptibility and the interfacial potential, χ(3) × Φ(0), is given by (χ1(3)−iχ2(3)) × Φ(0), and that the interference between this product and the second-order susceptibility of bulk quartz depends on the rotation angle of α-quartz around the z axis. Our experiments show that this newly identified term, iχ(3) × Φ(0), which is out of phase from the surface terms, is of bulk origin. The possibility of internally phase referencing the interfacial response for the interfacial orientation analysis of species or materials in contact with α-quartz is discussed along with the implications for conditions of resonance enhancement.

Suggested Citation

  • Paul E. Ohno & Sarah A. Saslow & Hong-fei Wang & Franz M. Geiger & Kenneth B. Eisenthal, 2016. "Phase-referenced nonlinear spectroscopy of the α-quartz/water interface," Nature Communications, Nature, vol. 7(1), pages 1-5, December.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms13587
    DOI: 10.1038/ncomms13587
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