Proton Order toward the Surface of Ice Ih Revealed by Heterodyne-Detected Sum Frequency Generation Spectroscopy
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Department of Applied Chemistry, Graduate School of Science and Engineering, Saitama University, 255 Shimo-Okubo, Sakura, Saitama 338-8570, Japan
*E-mail: [email protected]
Abstract
Using heterodyne-detected sum frequency generation (HD-SFG) spectroscopy, we investigated surface proton order at the basal, primary prism, and secondary prism faces of single-crystalline ice Ih at ca. 130 K. The complex phase of the obtained spectra clearly indicates that second-order nonlinear polarization from which the HD-SFG signal arises is generated exclusively at the surfaces. This suggests surface proton ordering along the normal, whereas the bulk remains proton-disordered, as is well known for ice Ih. A strong positive peak observed in the HD-SFG spectra enables us to determine the “direction” of the surface proton order as “H-up”, that is, the hydrogen atom of the OH group pointing away from the bulk, irrespective of the ice faces. Reliable HD-SFG measurements carried out in the present study have greatly advanced our understanding of surface structure of ice Ih.
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