Energy Transfer and Vibrationally Mediated Photodissociation in Liquids

Abstract

Vibrational energy is a central aspect of chemical reactivity. Because a few vibrationally energized molecules are the ones that actually overcome the barriers to reaction to form products, the means by which molecules acquire and lose energy is at the heart of chemistry. Thus, vibrationally excited molecules are important in an enormous variety of environments, ranging from the conventional, such as solutions, to the exotic, such as plasmas. The authors have extended their previous studies of the energy transfer and photodissociation dynamics of isolated molecules into the more complex environment of liquids with the goal of understanding the role that solvents play in the behavior of vibrationally excited molecules. In these experiments, a 100-fs pulse of near or mid-infrared light excites a high frequency stretching vibration of a solute molecule and another short pulse of ultraviolet light monitors the energy content of a subset of the vibrations by transient absorption. The measurements have revealed the influence that vibrational state structure and solvent interactions have on the flow of energy within the vibrationally excited molecule and into the surrounding solvent. (4 figures, 28 refs.)

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Document Details

Document Type
Technical Report
Publication Date
Mar 01, 2004
Accession Number
ADA424020

Entities

People

  • F. F. Crim

Tags

DTIC Thesaurus Topics

  • Absorption
  • Chemical Reactions
  • Chemistry
  • Difference Frequency
  • Dissociation
  • Dynamics
  • Energy Transfer
  • Environment
  • Frequency
  • Frequency Conversion
  • Lasers
  • Measurement
  • Molecules
  • Photodissociation
  • Reactivities
  • Vibration
  • Vibrational Relaxation

Fields of Study

  • Chemistry

Readers

  • Molecular Photonics/Laser Physics
  • Systems Analysis and Design