Ultrafast vibrational dynamics at aqueous interfaces studied by 2D heterodyne-detected vibrational sum frequency generation spectroscopy

Kenichi Inoue, Satoshi Nihonyanagi, Tahei Tahara

Research output: Chapter in Book/Report/Conference proceedingChapter

Abstract

In this article, we review our recent studies on the ultrafast vibrational dynamics at aqueous interfaces carried out with two-dimensional (2D) heterodyne-detected vibrational sum frequency generation (HD-VSFG) spectroscopy. Compared to the wealth of knowledge about bulk water, molecular-level understanding of interfacial water is still poor due to the technical difficulty in selectively observing molecules at the interfaces. HD-VSFG spectroscopy is based on the second-order optical process and thus intrinsically interface-selective. 2D HD-VSFG spectroscopy is its extension to the time-resolved measurement, and it is an interfacial analog of 2D IR spectroscopy which has been extensively utilized for bulk studies. This novel interface-selective ultrafast spectroscopy has enabled us to investigate ultrafast vibrational dynamics at aqueous interfaces at the high level equivalent to the bulk studies. We describe the principle and instrumentation of 2D HD-VSFG spectroscopy as well as several selected examples of 2D HD-VSFG studies that provided new insights into aqueous interfaces. At the air/neat water interface, 2D HD-VSFG indicated high similarity of hydrogen-bonded OH of interfacial water to that of bulk water while unique non-hydrogen bonded OH is present at the interface. At the charged surfactant/water interfaces, 2D HD-VSFG enabled us to clearly observe ultrafast spectral diffusion in the OH stretch band and demonstrated the importance of isotopic dilution for unambiguous observation of vibrational dynamics. At model membrane lipid/water interfaces, it was found that the hydrogen-bonded dynamics is greatly affected by the interaction between the interfacial water and the head group of the lipids and that the effects of coexisting head groups cannot simply be summed up but they are highly cooperative.

Original languageEnglish
Title of host publicationSpringer Series in Optical Sciences
PublisherSpringer-Verlag
Pages215-236
Number of pages22
DOIs
Publication statusPublished - 2019 Jan 1

Publication series

NameSpringer Series in Optical Sciences
Volume226
ISSN (Print)0342-4111
ISSN (Electronic)1556-1534

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials

Fingerprint Dive into the research topics of 'Ultrafast vibrational dynamics at aqueous interfaces studied by 2D heterodyne-detected vibrational sum frequency generation spectroscopy'. Together they form a unique fingerprint.

  • Cite this

    Inoue, K., Nihonyanagi, S., & Tahara, T. (2019). Ultrafast vibrational dynamics at aqueous interfaces studied by 2D heterodyne-detected vibrational sum frequency generation spectroscopy. In Springer Series in Optical Sciences (pp. 215-236). (Springer Series in Optical Sciences; Vol. 226). Springer-Verlag. https://doi.org/10.1007/978-981-13-9753-0_10