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New Approaches to Liquid Interfaces through Changes in the Refractive Index and Nonlinear Susceptibility Utilizing Ultrashort Laser Pulses

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Abstract

Molecules in inhomogeneous liquid environments, such as air/liquid, liquid/liquid, solid/liquid interfaces interact with each other specifically, and sometimes form characteristic structures and emerge unique properties. Here, we introduce two newly developed spectroscopic techniques, the total-internal-reflection ultrafast transient lens method (TIR-UTL) and second harmonic generation-coherent vibrational spectroscopy (SHG-CVS), to investigate the characteristic behaviors of molecules in such inhomogeneous environments. TIR-UTL probes the refractive-index change with sub-picosecond resolution and provides information on ultrafast changes in the population, density, and thermal properties, such as temperature increase and energy transfer from the solute molecules to the surrounding solvent molecules. On the other hand, SHG-CVS probes nonlinear susceptibility changes at the interfacial areas, and is expected to provide spectroscopic information on the low-frequency vibrational modes that reflect the corrective motion of the molecules in such an inhomogeneous environment. These new approaches are based on pump-probe techniques utilizing (ultra) short laser pulses. They are expected to provide further information on inhomogeneous environments from the viewpoints of solute- solvent interactions, changes in the molecular orientation, and the corrective motion of molecules at liquid interfaces.

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Authors and Affiliations

  1. CREST, Japan Science and Technology Agency (JST), Nanoarchitectonics Research Center (NARC), National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba Central, 4-1-1 Higashi, Tsukuba, Ibaraki, 305-8562, Japan

    Hiroharu Yui & Tsuguo Sawada

  2. Department of Advanced Materials Science, Graduate School of Frontier Sciences, The University of Tokyo, 5-1-5-603, Kashiwanoha, Kashiwa, Chiba, 277-8561, Japan

    Hiroharu Yui, Yasushi Hirose & Tsuguo Sawada

Authors
  1. Hiroharu Yui
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  2. Yasushi Hirose
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  3. Tsuguo Sawada
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Correspondence to Hiroharu Yui.

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Yui, H., Hirose, Y. & Sawada, T. New Approaches to Liquid Interfaces through Changes in the Refractive Index and Nonlinear Susceptibility Utilizing Ultrashort Laser Pulses. ANAL. SCI. 20, 1493–1499 (2004). https://doi.org/10.2116/analsci.20.1493

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