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arXiv 1303.2869physics.atom-phcond-mat.mes-hallphysics.atm-clusphysics.chem-ph
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电子-电子干涉在电子波包超快时间分辨成像中的作用

Role of electron-electron interference in ultrafast time-resolved imaging of electronic wavepackets

Gopal Dixit, Robin Santra

摘要:

超快时间分辨x射线散射是一种新兴的方法,可以实时和实时地对复杂的化学和生物过程中电子电荷分布的动态演化进行成像。最近,对于来自电子波包的超短X射线脉冲的散射,光-物质相互作用的半经典和量子电动力学(QED)理论之间的差异被正式地证明,并且通过针对原子氢中的电子波包计算的散射图案来直观地说明[Proc. Natl. Acad. Sci.美国,{ \bf 109},11636(2012)]。在这项工作中,我们提出了一个详细的分析时间分辨的X射线散射的样品中包含的非稳态和稳态电子的混合物内的两个理论。在多电子系统中,研究了一个非稳态电子与多个稳态电子之间的散射干涉对总散射信号的影响。一般来说,QED和半经典理论提供了不同的结果散射干涉的贡献,这取决于探测器的能量分辨率和X射线脉冲的持续时间。本文通过一个氦原子中电子波包的x射线TRI的数值例子来说明本文的研究结果。结果表明,在半经典理论中,含时散射干涉为零,相应的斑图由非含时散射干涉的散射贡献所支配;而在量子电动力学理论中,含时散射干涉的贡献并不为零,相应的斑图由非定常电子散射的散射贡献所支配.

英文摘要:

Ultrafast time-resolved x-ray scattering is an emerging approach to image the dynamical evolution of the electronic charge distribution during complex chemical and biological processes in real-space and real-time. Recently, the differences between semiclassical and quantum-electrodynamical (QED) theory of light-matter interaction for scattering of ultrashort x-ray pulses from the electronic wavepacket were formally demonstrated and visually illustrated by scattering patterns calculated for an electronic wavepacket in atomic hydrogen [Proc. Natl. Acad. Sci. U.S.A., {\bf 109}, 11636 (2012)]. In this work, we present a detailed analysis of time-resolved x-ray scattering from a sample containing a mixture of non-stationary and stationary electrons within both the theories. In a many-electron system, the role of scattering interference between a non-stationary and several stationary electrons to the total scattering signal is investigated. In general, QED and semiclassical theory provide different results for the contribution from the scattering interference, which depends on the energy resolution of the detector and the x-ray pulse duration. The present findings are demonstrated by means of a numerical example of x-ray TRI for an electronic wavepacket in helium. It is shown that the time-dependent scattering interference vanishes within semiclassical theory and the corresponding patterns are dominated by the scattering contribution from the time-independent interference, whereas the time-dependent scattering interference contribution does not vanish in the QED theory and the patterns are dominated by the scattering contribution from the non-stationary electron scattering.

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