Phase-referenced nonlinear spectroscopy of the α-quartz/water interface
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. Lastly, 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.
- Authors:
-
[1];
[2];
[3];
- Northwestern Univ., Evanston, IL (United States)
- Northwestern Univ., Evanston, IL (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Columbia Univ., New York, NY (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1339853
- Report Number(s):
- PNNL-SA-119274
Journal ID: ISSN 2041-1723
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 7; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS; optical spectroscopy; surface spectroscopy
Citation Formats
Ohno, Paul E., Saslow, Sarah A., Wang, Hong-fei, Geiger, Franz M., and Eisenthal, Kenneth B. Phase-referenced nonlinear spectroscopy of the α-quartz/water interface. United States: N. p., 2016.
Web. doi:10.1038/ncomms13587.
Ohno, Paul E., Saslow, Sarah A., Wang, Hong-fei, Geiger, Franz M., & Eisenthal, Kenneth B. Phase-referenced nonlinear spectroscopy of the α-quartz/water interface. United States. https://doi.org/10.1038/ncomms13587
Ohno, Paul E., Saslow, Sarah A., Wang, Hong-fei, Geiger, Franz M., and Eisenthal, Kenneth B. Tue .
"Phase-referenced nonlinear spectroscopy of the α-quartz/water interface". United States. https://doi.org/10.1038/ncomms13587. https://www.osti.gov/servlets/purl/1339853.
@article{osti_1339853,
title = {Phase-referenced nonlinear spectroscopy of the α-quartz/water interface},
author = {Ohno, Paul E. and Saslow, Sarah A. and Wang, Hong-fei and Geiger, Franz M. and Eisenthal, Kenneth B.},
abstractNote = {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. Lastly, 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.},
doi = {10.1038/ncomms13587},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Tue Dec 13 00:00:00 EST 2016},
month = {Tue Dec 13 00:00:00 EST 2016}
}
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