Attosecond-recollision-controlled selective fragmentation of polyatomic molecules

TL;DR

This paper demonstrates how the optical waveform of intense few-cycle laser pulses can control the fragmentation of polyatomic molecules through recollision-induced ionization, enabling selective reactions on sub-femtosecond timescales.

Contribution

It introduces a method to control molecular fragmentation and isomerization using recollision dynamics driven by the laser waveform, combining experimental and theoretical analysis.

Findings

Selective fragmentation of polyatomic molecules achieved.

Recollision energy depends on laser waveform.

Control occurs on sub-femtosecond timescales.

Abstract

Control over various fragmentation reactions of a series of polyatomic molecules (acetylene, ethylene, 1,3-butadiene) by the optical waveform of intense few-cycle laser pulses is demonstrated experimentally. We show both experimentally and theoretically that the responsible mechanism is inelastic ionization from inner-valence molecular orbitals by recolliding electron wavepackets, whose recollision energy in few-cycle ionizing laser pulses strongly depends on the optical waveform. Our work demonstrates an efficient and selective way of pre-determining fragmentation and isomerization reactions in polyatomic molecules on sub-femtosecond time-scales.