少周期laser场中烃分子超快动力学的相位和强度依赖性
Phase- and intensity-dependence of ultrafast dynamics in hydrocarbon molecules in few-cycle laser fields
摘要：
在强激光场中，利用载波包络相位（CEP）对化学反应进行亚飞秒控制成为可能。我们研究了乙炔和丙二烯在750 nm强脉冲激光中的反应动力学控制，用反应显微镜记录离子碎片。我们发现，通过改变CEP和强度的激光脉冲，它是可能的，以引导质子在分子dications的运动，使控制去质子化和异构化反应。将实验结果与量子动力学模型的预测进行比较，其中控制是基于由激光波形操纵振动波包的相位。在CEP控制的乙炔去质子化的测量强度依赖性被很好地捕获的模型。然而，在乙炔异构化的情况下，我们发现实验和理论之间的强度依赖性的差异。对于丙二烯异构化反应，当光强度变化时，观察到CEP依赖的不对称性的反转，我们根据量子动力学模型对此进行了讨论。反转的不对称性被发现是一致的从非顺序到顺序双电离的过渡。
英文摘要：
In strong laser fields, sub-femtosecond control of chemical reactions with the carrier-envelope phase (CEP) becomes feasible. We have studied the control of reaction dynamics of acetylene and allene in intense few-cycle laser pulses at 750 nm, where ionic fragments are recorded with a reaction microscope. We find that by varying the CEP and intensity of the laser pulses it is possible to steer the motion of protons in the molecular dications, enabling control over deprotonation and isomerization reactions. The experimental results are compared to predictions from a quantum dynamical model, where the control is based on the manipulation of the phases of a vibrational wave packet by the laser waveform. The measured intensity dependence in the CEP-controlled deprotonation of acetylene is well captured by the model. In the case of the isomerization of acetylene, however, we find differences in the intensity dependence between experiment and theory. For the isomerization of allene, an inversion of the CEP-dependent asymmetry is observed when the intensity is varied, which we discuss in light of the quantum dynamical model. The inversion of the asymmetry is found to be consistent with a transition from non-sequential to sequential double ionization.
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