Non-Lorentzian resonance and product control in two-photon photodissociation

Abstract

We demonstrate that detuning in two-photon processes can yield non-Lorentzian resonances in the photodissociation spectra by accurately computing the second-order transition amplitudes. Both the one-colour and the two-colour processes are discussed. In one-colour two-photon processes, non-lorentzian resonances may be obtained due to the detunings in the intermediate and final states, when the final states are predissociating. The product branching ratios may change significantly in the vicinity of non-Lorentzian resonances when the built-in interference in the final state manifold affects the dynamics. In two-colour two-photon processes, quantum interference between the (v(1) + v(2)) and (v(2) + v(1)) processes can give rapidly changing product branching ratios near the non-lorentzian resonances, suggesting the potential of controlling product distributions in two-photon photodissociation processes.