Ultrafast Multi-Dimensional Infrared Spectroscopy of Gases at Low and High Pressures

Abstract

Infrared pump-probe experiments were used to study vibrational relaxation of polyatomic molecules in supercritical fluids and the gas phase. IR pump-probe experiments and theory were used to investigate hydrogen bond dynamics in oligomers of alcohols. Vibrational echo correlation spectroscopy (VECS) was developed and experiments were performed on molecules in liquids and gases. VECS is an ultrafast multidimensional approach that is in many respects the vibrational equivalent of multidimensional NMR. VECS experiments have been performed on molecules in liquids and gases. The OD hydroxyl stretch of HOD in water was studied and the results were compared to theoretical simulation models of water. The time evolution of the vibrational echo correlation spectrum reflects the structural evolution of the hydrogen bond networks in water. The experiments and theory provide detailed tests of water models. A gas cell for performing ultrafast infrared experiments was developed and the first vibrational echo correlation spectroscopy experiments were performed in the gas phase. VECS was also been demonstrated as a new type of analytical tool that can aid in sorting out congested vibrational spectra.

Open PDF

Document Details

Document Type
Technical Report
Publication Date
May 11, 2005
Accession Number
ADA433247

Entities

People

  • Michael D. Fayer

Organizations

  • Stanford University

Tags

Communities of Interest

  • Energy and Power Technologies

DTIC Thesaurus Topics

  • Carbonyl Complexes
  • Chemistry
  • Dynamics
  • Gas Cells
  • High Pressure
  • Hydrogen Bonds
  • Infrared Spectroscopy
  • Molecular Dynamics
  • Molecules
  • Oligomers
  • Physical Chemistry
  • Polyatomic Molecules
  • Simulations
  • Spectra
  • Spectroscopy
  • Vibrational Relaxation
  • Vibrational Spectra

Readers

  • Molecular Photonics/Laser Physics