Structure and Dynamics of Water Interfaces Revealed by Novel Interface-Selective Nonlinear Spectroscopy

Tahei Tahara (RIKEN, Japan)
Event Date and Time: 
Tue, 2013-11-05 16:00 - 17:00
Chem D-215
Local Contact: 
Taka Momose
Intended Audience: 

Second-order nonlinear spectroscopy provides interface-selective spectral information, and it is an indispensable tool to study interfaces. Recently, we developed multiplex phase-sensitive heterodyne-detected electronic and vibrational sum-frequency generation (HD-ESFG [1] and HD-VSFG [2]) spectroscopies, which enable us to directly measure the imaginary and real parts of the electronically and vibrationally resonant second-order susceptibility (c(2)). The heterodyne detection is advantageous over the traditional homodyne detection in essential respects: The imaginary c(2) (Im c(2)) spectra at the interface obtained with heterodyne detection can be directly compared to bulk absorption spectra that correspond to Im c(1), and the sign of Im c(2) includes information about the absolute orientation of the interfacial molecules. We have studied the steady-state and dynamical properties of water interfaces using HD-ESFG and HD-VSFG, and clarified fundamental phenomena at the interface [3-7]. Furthermore, by combining femtosecond photoexcitation with HD-VSFG, we have realized time-resolved HD-VSFG (TR-HD-VSFG) that allows us to examine femtosecond vibrational dynamics at liquid interfaces [8]. Very recently, we have extended TR-HD-VSFG to 2D spectroscopy (2D HD-VSFG) and have succeeded in observing the hole burning and the following spectral diffusion in the OH stretch region at a water interface [9]. With development of these new interface-selective nonlinear spectroscopic methods, we are now able to study steady-state and dynamical properties of interfacial molecules as we study molecules in solution by steady-state and time-resolved absorption spectroscopy [10-11].


In this talk, I discuss recent results obtained with these new interface-selective nonlinear spectroscopy developed in my laboratory.


[1]   S. Yamaguchi and T. Tahara, J. Chem. Phys. 129, 101102 (2008).

[2]   S. Nihonyanagi, S. Yamaguchi, T. Tahara, J. Chem. Phys. 130, 204704 (2009).

[3]   S. Yamaguchi, H. Watanabe, S. Mondal, A. Kundu, T. Tahara, J. Chem. Phys. 135, 194705 (2011).

[4]   S. Nihonyanagi, S. Yamaguchi, T. Tahara, J. Am. Chem. Soc. 132, 6867 (2010).

[5]        S. Nihonyanagi, T. Ishiyama, T-K. Lee, S. Yamaguchi, M. Bonn, A. Morita, T. Tahara, J. Am. Chem.

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