Theory of optimal laser pulses for selective transitions between molecular eigenstates

Abstract

We present a new theoretical approach to optimal laser pulses designed for selective transitions between molecular eigenstates, within the semiclassical dipole approximation. Optimization proceeds iteratively, starting from a rather arbitrary, e.g. continuous wave, reference and yielding efficient modulations of the laser field intensities, frequencies, and phases. The method is verified by successful application to state-selective vibrational excitation of a Morse oscillator representing the OH bond in H 2O by a subpicosecond laser pulse. The present theory is also compared with complementary approaches to optimal laser pulses inducing selective dissociations or excitations to bond-selective stretches in model polymers.