Publication

SOLUTION DYNAMICS BY LINE-SHAPE ANALYSIS, RESONANCE LIGHT-SCATTERING AND FEMTOSECOND 4-WAVE-MIXING

NIBBERING, ETJ., DUPPEN, K. & WIERSMA, DA., 15-Jan-1992, In : Journal of photochemistry and photobiology a-Chemistry. 62, 3, p. 347-370 24 p.

Research output: Contribution to journalArticleAcademicpeer-review

  • ETJ NIBBERING
  • K DUPPEN
  • DA WIERSMA

The results of line shape analysis, resonance light scattering and femtosecond four-wave mixing measurements are reported on several organic molecules in solution. It is shown that a Brownian oscillator model for line broadening provides a full description for the optical dynamics in aprotic solutions. The dynamics of all systems studied is found to occur in the intermediate modulation regime, where the amplitude-DELTA and inverse correlation time-LAMBDA of the Brownian oscillator are about equal: DELTA/LAMBDA almost-equal-to 1. Isotopic substitution of either probe or solvent is shown to have no effect on the dynamics, from which it is concluded that the vibrational force field plays a minor role in determining the line shape. Four-wave mixing experiments with chirped femtosecond pulses yield intense coherent Raman scattering signals due to ground and excited-state vibrational coherences which are very effectively driven by the two instantaneous light fields whose frequency difference matches exactly a vibrational mode. It is shown that the "chirped" four-wave mixing signal near zero delay time only mimics the two-pulse photon echo if the system dynamics fall in the fast modulation limit: DELTA/LAMBDA

Original languageEnglish
Pages (from-to)347-370
Number of pages24
JournalJournal of photochemistry and photobiology a-Chemistry
Volume62
Issue number3
Publication statusPublished - 15-Jan-1992
Event15TH INTERNATIONAL CONF ON PHOTOCHEMISTRY - , France
Duration: 28-Jul-19912-Aug-1991

Event

15TH INTERNATIONAL CONF ON PHOTOCHEMISTRY

28/07/199102/08/1991

France

Event: Other

    Keywords

  • INTERMEDIATE STATE INTERACTION, ORDER OPTICAL PROCESSES, RAMAN EXCITATION PROFILES, FAST RELAXATION PROCESSES, PUMP-PROBE SPECTROSCOPY, NON-MARKOVIAN THEORY, CONDENSED PHASES, POLYATOMIC-MOLECULES, STOCHASTIC-MODELS, PHOTON-ECHOES

ID: 6307230