Nihonyanagi Satoshi, Kusaka Ryoji, Inoue Ken-ichi, Adhikari Aniruddha, Yamaguchi Shoichi, Tahara Tahei
Molecular Spectroscopy Laboratory, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198, Japan.
J Chem Phys. 2015 Sep 28;143(12):124707. doi: 10.1063/1.4931485.
Discussion on the structure of the water surface relies on accurate determination of the χ(2) spectrum. For obtaining accurate χ(2) spectrum of the air/water interface in the OH stretch region, we performed heterodyne-detected vibrational sum-frequency generation measurements with a high phase accuracy, and also examined the validity of the phase and amplitude calibration using different non-resonant materials. In contrast to the previous reports, it was concluded that the imaginary part of the χ(2) spectrum of the air/water interface does not exhibit noticeable positive resonance in the low frequency region within the experimental error. This result urges us to reconsider the structure of the air/water interface based on the accurate χ(2) spectrum.
关于水面结构的讨论依赖于χ(2)光谱的精确测定。为了在OH伸缩区域获得空气/水界面的精确χ(2)光谱，我们进行了具有高相位精度的外差检测振动和频产生测量，并使用不同的非共振材料检验了相位和幅度校准的有效性。与之前的报道不同，得出的结论是，在实验误差范围内，空气/水界面χ(2)光谱的虚部在低频区域没有明显的正共振。这一结果促使我们基于精确的χ(2)光谱重新考虑空气/水界面的结构。
