Solvent structural relaxation dynamics in dipolar solvation studied by resonant pump polarizability response spectroscopy

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Resonant pump polarizability response spectroscopy (RP-PORS) was used to study the isotropic and anisotropic solvent structural relaxation in solvation. RP-PORS is the optical heterodyne detected transient grating (OHD-TG) spectroscopy with an additional resonant pump pulse. A resonant pump excites the solute-solvent system and the subsequent relaxation of the solute-solvent system is monitored by the OHD-TG spectroscopy. This experimental method allows measuring the dispersive and absorptive parts of the signal as well as fully controlling the beam polarizations of incident pulses and signal. The experimental details of RP-PORS were described. By performing RP-PORS with Coumarin 153(C153) in CH(3)CN and CHCl(3), we have successfully measured the isotropic and anisotropic solvation polarizability spectra following electronic excitation of C153. The isotropic solvation polarizability responses result from the isotropic solvent structural relaxation of the solvent around the solute whereas the anisotropic solvation polarizability responses come from the anisotropic translational relaxation and orientational relaxation. The solvation polarizability responses were found to be solvent-specific. The intramolecular vibrations of CHCl(3) were also found to be coupled to the electronic excitation of C153.
Publisher
ROYAL SOC CHEMISTRY
Issue Date
2011
Language
English
Article Type
Article
Keywords

STIMULATED RAMAN-SPECTROSCOPY; TRANSIENT-GRATING SPECTROSCOPY; OPTICAL HETERODYNE-DETECTION; DIFFRACTIVE OPTICS; INTERMOLECULAR DYNAMICS; VIBRATIONAL DYNAMICS; PROBE SPECTROSCOPY; POLAR-SOLVENTS; EXCITED-STATE; BETA-CAROTENE

Citation

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, v.13, no.1, pp.214 - 223

ISSN
1463-9076
DOI
10.1039/c0cp01252a
URI
http://hdl.handle.net/10203/94581
Appears in Collection
RIMS Journal Papers
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