Abstract

Optical excitation of material transitions by adiabatic passage with frequency modulated (chirped) laser pulses is a useful spectroscopic tool.^1,2 Here we demonstrate that picosecond frequency modulated laser pulses produce more efficient population transfer, and more selective excitation than equivalent (same spectral bandwidth) nearly transform limited laser pulses. We apply frequency modulated pulses to gas-phase and condensed phase systems. We also point out the "robustness", or insensitivity of the properties of the material excitation to the parameters of the laser field, that is inherent to the adiabatic process. The robustness obtainable by adiabatic passage will ultimately prove useful to laboratory applications of theoretical schemes which require frequency modulated ultrashort laser pulses to control chemical reaction dynamics.³

© 1992 The Author(s)