Weak-Field Coherent Control of Ultrafast Molecule Making

TL;DR

This paper demonstrates the feasibility of weak-field coherent control of ultrafast molecule formation from hot reactants, using resonance-mediated two-photon excitation with chirped femtosecond pulses, opening new pathways for chemical reaction control.

Contribution

It provides the first experimental evidence that weak-field coherent control can be effective even under hot, thermally challenging conditions, with results supported by ab initio calculations.

Findings

Negative chirps increase molecule yield.

Weak-field control is feasible under hot conditions.

Experimental results agree with ab initio simulations.

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 molecules 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 results are in excellent agreement. New routes to CCBP are opened.