Photonics Institute, Vienna University of Technology, A-1040 Vienna, Austria.
Phys Rev Lett. 2012 Dec 14;109(24):243001. doi: 10.1103/PhysRevLett.109.243001. Epub 2012 Dec 10.
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 wave packets, whose recollision energy in few-cycle ionizing laser pulses strongly depends on the optical waveform. Our work demonstrates an efficient and selective way of predetermining fragmentation and isomerization reactions in polyatomic molecules on subfemtosecond time scales.
实验证明，强少周期激光脉冲的光波形可以控制一系列多原子分子（乙炔、乙烯、1,3-丁二烯）的各种碎裂反应。我们从实验和理论上都表明，负责的机制是通过再碰撞电子波包从内价分子轨道进行非弹性电离，而在少周期电离激光脉冲中，再碰撞电子波包的再碰撞能量强烈依赖于光波形。我们的工作证明了在亚飞秒时间尺度上预先确定多原子分子的碎裂和异构化反应的一种有效和选择性的方法。
