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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.

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