Weak-Field Coherent Control of Ultrafast Molecule Making

Abstract

Coherent control of ultrafast molecule making from colliding reactants is crucial for realizing coherent control of binary photoreactions (CCBP). To handle diverse excitation scenarios, feasibility with both weak and strong fields is essential. We experimentally demonstrate here the weak-field feasibility, achieving it even under thermally hot conditions typical of chemical reactions. The making of KAr complexes from hot pairs of colliding K and Ar atoms via resonance-mediated two-photon excitation is controlled by weak linearly chirped femtosecond pulses. Negative chirps enhance the yield. Our experimental and ab initio theoretical results are in excellent agreement. New routes to CCBP are opened.