Center for Free-Electron Laser Science, DESY, Notkestrasse 85, D-22607 Hamburg, Germany.
Proc Natl Acad Sci U S A. 2012 Jul 17;109(29):11636-40. doi: 10.1073/pnas.1202226109. Epub 2012 Jul 2.
Imaging the quantum motion of electrons not only in real-time, but also in real-space is essential to understand for example bond breaking and formation in molecules, and charge migration in peptides and biological systems. Time-resolved imaging interrogates the unfolding electronic motion in such systems. We find that scattering patterns, obtained by X-ray time-resolved imaging from an electronic wavepacket, encode spatial and temporal correlations that deviate substantially from the common notion of the instantaneous electronic density as the key quantity being probed. Surprisingly, the patterns provide an unusually visual manifestation of the quantum nature of light. This quantum nature becomes central only for non-stationary electronic states and has profound consequences for time-resolved imaging.
实时、实空间地成像电子的量子运动,对于理解分子中的键断裂和形成以及肽和生物系统中的电荷迁移等现象至关重要。时间分辨成像是对这些系统中展开的电子运动进行探测的一种方法。我们发现,通过 X 射线时间分辨成像从电子波包中获得的散射图样,编码了空间和时间相关性,这些相关性与瞬时电子密度作为被探测的关键量的常见概念有很大的偏离。令人惊讶的是,这些图样提供了光的量子性质的一种异常直观的表现。这种量子性质仅对于非定态电子态是核心的,并且对时间分辨成像有深远的影响。