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

Sungnam Park, Jeongho Kim, Andrew M. Moran, Norbert F. Scherer

Research output: Contribution to journalArticlepeer-review

11 Citations (Scopus)

Abstract

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 CH3CN and CHCl3, 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 CHCl3 were also found to be coupled to the electronic excitation of C153.

Original languageEnglish
Pages (from-to)214-223
Number of pages10
JournalPhysical Chemistry Chemical Physics
Volume13
Issue number1
DOIs
Publication statusPublished - 2011 Jan 7

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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