Control of recollision wave packets for molecular orbital tomography using short laser pulses

Abstract. The tomographic imaging of arbitrary molecular orbitals via high-order harmonic generation requires that electrons recollide from one direction only. Within a semi-classical model, we show that extremely short phase-stabilized laser pulses offer control over the momentum distribution of the returning electrons. By adjusting the carrier-envelope phase, recollisions can be forced to occur from mainly one side, while retaining a broad energy spectrum. The signatures of the semi-classical distributions are observed in harmonic spectra obtained by numerical solution of the time-dependent Schrödinger equation.