We investigate the nonlinear optical response of alpha-quartz with phase-sensitive vibrational sum frequency generation (SFG) spectroscopy. Phase and amplitude of the generated sum frequency signal are determined by a complex interplay between signal contributions from the surface and the bulk of the crystal with the experimental geometry, in particular, the quartz azimuth. By combining anisotropy measurements with spectral- and phase resolution in our SFG experiment, we study this interplay and show that we can quantitatively isolate and characterize the contributions from the surface and bulk of the crystal. The obtained optical constants in combination with the presented mathematical framework fully describe the nonlinear response and allow for a precise determination of the phase of the overall SFG signal of quartz for any experimental geometry. This knowledge is of particular relevance because quartz is commonly used as a reference in phase sensitive SFG experiments. In such studies, the surface contribution is typically neglected and a constant value for the phase of the sum frequency response is assumed. Our study shows that this assumption is not generally accurate by revealing the considerable impact that the surface contribution can have on the overall response of the crystal.
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Quantitative determination of the nonlinear bulk and surface response from alpha-quartz using phase sensitive SFG spectroscopy
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14 August 2019
Research Article|
August 09 2019
Quantitative determination of the nonlinear bulk and surface response from alpha-quartz using phase sensitive SFG spectroscopy

Martin Thämer
;
Martin Thämer
a)
Fritz Haber Institute of the Max Planck Society
, 4-6 Faradayweg, 14195 Berlin, Germany
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Tobias Garling;
Tobias Garling
Fritz Haber Institute of the Max Planck Society
, 4-6 Faradayweg, 14195 Berlin, Germany
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R. Kramer Campen
;
R. Kramer Campen
Fritz Haber Institute of the Max Planck Society
, 4-6 Faradayweg, 14195 Berlin, Germany
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Martin Wolf
Martin Wolf
Fritz Haber Institute of the Max Planck Society
, 4-6 Faradayweg, 14195 Berlin, Germany
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a)
Electronic mail: [email protected]
J. Chem. Phys. 151, 064707 (2019)
Article history
Received:
May 13 2019
Accepted:
July 09 2019
Connected Content
A companion article has been published:
Measurements indicate alpha-quartz’s surface signal should not be neglected in spectroscopy calibration
Citation
Martin Thämer, Tobias Garling, R. Kramer Campen, Martin Wolf; Quantitative determination of the nonlinear bulk and surface response from alpha-quartz using phase sensitive SFG spectroscopy. J. Chem. Phys. 14 August 2019; 151 (6): 064707. https://doi.org/10.1063/1.5109868
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