Dynamic imaging of molecules using high order harmonic generation

Phys Chem Chem Phys. 2008 Jan 7;10(1):35-48. doi: 10.1039/b714126m. Epub 2007 Nov 14.

Abstract

We review recent progress towards imaging the electronic wavefunctions and nuclear dynamics of small molecules using the high order harmonics emitted when a molecule experiences an intense laser field. We illustrate that the essence of high harmonic emission is contained in the recombination amplitude between the continuum portion of the electronic wavefunction, that is formed through field ionization and which is accelerated and driven back to recollide in the laser field, and the bound electronic state. We review for the non-specialist some recent experimental and theoretical work dealing with high harmonic generation (HHG) in molecules. Particular attention is paid to two types of experiment recently performed in our group. The first of these types of experiment is the measurement of signatures of molecular electronic structure using HHG from molecules with a fixed orientation in space. The second is the use of HHG to track extremely fast proton rearrangement following ionization in light molecules, using the intrinsic temporal variation of the recolliding electron energy to extract these dynamics from measurements of the high harmonics.

Publication types

  • Research Support, Non-U.S. Gov't
  • Review

MeSH terms

  • Computer Simulation*
  • Electrons
  • Infrared Rays
  • Lasers
  • Models, Chemical*
  • Nonlinear Dynamics
  • Quantum Theory
  • Scattering, Radiation
  • Spectrophotometry, Ultraviolet / instrumentation*
  • Spectrophotometry, Ultraviolet / methods*
  • Time Factors