Abstract
The development of the laser some twelve years ago has resulted in the creation and/or the resuscitation of a number of experimental disciplines involving measurements of energy transfer, chemical reaction rates, high resolution spectroscopy as well as nonlinear effects. In the last three years more and more work involving the use of lasers has been reported on in the literature and a number of excellent review articles has been published dealing with many specific experimental and theoretical subfields(1) The audience tuned to laser and laser related research has steadily expanded to include widely varying disciplines ranging from Engineers to Chemists and from Artists to Meteorologists and is reflected in a variety of professional publications tailored for more or less specific audiences; but even a brief survey of the most widely read physical chemistry journals will convince anyone that one of the most extensive applications of the laser has been in the field of energy transfer studies. The study of energy transfer between the various internal modes and translation has been a topic of fundamental research for a number of decades, yet the detailed probing and “preparation” of well defined vibrational, rotational or electronically excited species have always been at best difficult. The availability of a monochromatic, high power, short pulse duration, and almost tunable sources was a boon to chemists, since the new research tool offered the intriguing possibility of measuring the rate constants for processes taking place between molecules “prepared” in well defined quantum states. As a field within a field, the specific application of vibrational excitation of molecules and the subsequent measurement of the various relaxation rates has received the most attention; partly due, no doubt, to the properties of the molecular lasers available in the infrared region and partly due to the significance of vibrational excitation on the rate and mechanism of chemical reactions.