Coherent Control of Bond Making

Abstract

We demonstrate for the first time coherent control of bond making, a milestone on the way to coherent control of photo-induced bimolecular chemical reactions. In strong-field multiphoton femtosecond photoassociation experiments, we find the yield of detected magnesium dimer molecules to be enhanced for positively chirped pulses and suppressed for negatively chirped pulses. Our ab initio model shows that control is achieved by purification via Franck-Condon filtering combined with chirp-dependent Raman transitions. Experimental closed-loop phase optimization using a learning algorithm yields an improved pulse that utilizes vibrational coherent dynamics in addition to chirp-dependent Raman transitions. Our results show that coherent control of binary photo-reactions is feasible even under thermal conditions.

References in corpus (1)

• The $A^1{\Sigma }_u^{+}$ + (1)${}^1{\Pi }_u$ system of Mg${}_2$

Cited by in corpus (4)

• Theoretical description of circular dichroism in photoelectron angular distributions of randomly oriented chiral molecules after multi-photon photoionization
• Towards controlling the dissociation probability by light-induced conical intersections
• Directional Quantum-Controlled Chemistry: Generating Aligned Ultracold Molecules via Photoassociation
• Transition moments between excited electronic states from the Hermitian formulation of the coupled cluster quadratic response function