Accurate determination of complex χ (2) spectrum of the air/water interface

Satoshi Nihonyanagi, Ryoji Kusaka, Ken Ichi Inoue, Aniruddha Adhikari, Shoichi Yamaguchi, Tahei Tahara

Research output: Contribution to journalArticlepeer-review

145 Citations (Scopus)


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.

Original languageEnglish
Article number124707
JournalJournal of Chemical Physics
Issue number12
Publication statusPublished - 2015 Sept 28


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