Development of a total internal reflection ultrafast transient lens method for studying molecular dynamics on an interface

Analytical Chemistry
Tsuyoshi SugimotoTsuguo Sawada

Abstract

We have developed the total internal reflection ultrafast transient lens (TIR-UTL) method to detect nonradiative chemical processes at interfaces and surfaces with subpicosecond time resolution. In the TIR-UTL measurements, the evanescent field of a pump beam irradiated under the TIR condition generates a refractive index change. The refractive index change is attributed to changes of the molecular electronic state, of density by molecular orientation/structure change, and of temperature by vibrational relaxation processes. The refractive index change is detected as a change of the power intensity of the probe beam adjusted coaxially with the pump beam. At first, we discuss a theoretical principle of a coaxial configuration in the TIR-UTL measurement. This configuration has an advantage of versatility over the established TIR configuration. Then, we evaluate time resolution of TIR-UTL and obtain a value of less than 400 fs. We measure the ultrafast molecular dynamics of the cationic chromophore Auramine O (AuO) at a silica/water interface. Two slow time constants originating from AuO adsorbed on the silica surface are detected by TIR-UTL. These are attributed to AuO, whose twisting motion is strongly hindered by adsorption on a...Continue Reading

Citations

Nov 30, 2004·Analytical Sciences : the International Journal of the Japan Society for Analytical Chemistry·Hiroharu YuiTsuguo Sawada
Mar 2, 2005·Chemical Record : an Official Publication of the Chemical Society of Japan ... [et Al.]·Yasushi HiroseTsuguo Sawada

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