Protocol for observing molecular dipole excitations by attosecond self-streaking
Protocol for observing molecular dipole excitations by attosecond self-streaking
复制标题
通过阿秒自条纹观察分子偶极子激发的协议
DOI：
10.1103/physreva.92.061403
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发表时间：
2015
影响因子：
2.9
通讯作者：
J. Burgdoerfer
中科院分区：
文献类型：
--
作者：
G. Wachter;S. Nagele;S.A. Sato;R. Pazourek;M. Wais;C. Lemell;X.-M. Tong;K. Yabana;J. Burgdoerfer
我们提出了一个协议，探测超快的演化和相干电子激发在时域中的分子由分子本身产生的本征条纹场退相。在内嵌富勒烯的相干电子运动是由一个中等强度的飞秒紫外可见光脉冲，导致相干振荡的分子偶极矩，持续结束后的激光脉冲。由此产生的时间依赖的分子近场探测通过从中心氖原子的光发射的动量调制的时间延迟的阿秒XUV脉冲。我们的从头算依赖于时间的密度泛函理论和经典的轨迹模拟预测，这种自我条纹信号准确地跟踪分子偶极振荡在真实的时间。我们讨论的基本过程，并给出了一个分析模型，抓住了欧拉初始模拟的本质。
We propose a protocol to probe the ultrafast evolution and dephasing of coherent electronic excitation in molecules in the time domain by the intrinsic streaking field generated by the molecule itself. Coherent electronic motion in the endohedral fullereneis initiated by a moderately intense femtosecond UV-visible pulse leading to coherent oscillations of the molecular dipole moment that persist after the end of the laser pulse. The resulting time-dependent molecular near field is probed through the momentum modulation of photoemission from the central neon atom by a time-delayed attosecond XUV pulse. Ourab initiotime-dependent density functional theory and classical trajectory simulations predict that this self-streaking signal accurately traces the molecular dipole oscillations in real time. We discuss the underlying processes and give an analytical model that captures the essence of ourab initiosimulations.