Subcycle controlled charge-directed reactivity with few-cycle midinfrared pulses.
Subcycle controlled charge-directed reactivity with few-cycle midinfrared pulses.
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DOI：
10.1103/physrevlett.108.063002
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发表时间：
2012-02
影响因子：
8.6
通讯作者：
I. Znakovskaya;P. von den Hoff;G. Marcus;S. Zherebtsov;B. Bergues;X. Gu;Y. Deng;M. Vrakking;
中科院分区：
文献类型：
--
作者：
I. Znakovskaya;P. von den Hoff;G. Marcus;S. Zherebtsov;B. Bergues;X. Gu;Y. Deng;M. Vrakking;
分子中电子运动的转向可以通过波形控制的几个周期的激光来实现，并且可以控制光诱导化学反应的结果。然而，光的光学周期比最快的解离反应的持续时间短得多，严重限制了可以实现的控制程度。为了克服这一局限性，我们将控制计量学扩展到中红外，研究了2.1 μm处D（2）的典型解离电离。观察到D（2）（+）碎裂产生的定向D（+）离子发射的明显亚循环控制，证明了前所未有的电荷定向反应性。两个反应途径，显示定向离子发射，可以同时观察和控制的第一次。量子动力学计算阐明了解离通道，它们观察到的相位关系，和控制机制。
The steering of electron motion in molecules is accessible with waveform-controlled few-cycle laser light and may control the outcome of light-induced chemical reactions. An optical cycle of light, however, is much shorter than the duration of the fastest dissociation reactions, severely limiting the degree of control that can be achieved. To overcome this limitation, we extended the control metrology to the midinfrared studying the prototypical dissociative ionization of D(2) at 2.1 μm. Pronounced subcycle control of the directional D(+) ion emission from the fragmentation of D(2)(+) is observed, demonstrating unprecedented charge-directed reactivity. Two reaction pathways, showing directional ion emission, could be observed and controlled simultaneously for the first time. Quantum-dynamical calculations elucidate the dissociation channels, their observed phase relation, and the control mechanisms.