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亚埃分辨率和阿秒分辨率下的轨道成像:迈向原子化学?

Imaging orbitals with attosecond and Ångström resolutions: toward attochemistry?

机构信息

CEA-Saclay, IRAMIS, Service des Photons, Atomes et Molécules, 91191 Gif-sur-Yvette, France.

出版信息

Rep Prog Phys. 2012 Jun;75(6):062401. doi: 10.1088/0034-4885/75/6/062401. Epub 2012 May 17.

Abstract

The recently developed attosecond light sources make the investigation of ultrafast processes in matter possible with unprecedented time resolution. It has been proposed that the very mechanism underlying the attosecond emission allows the imaging of valence orbitals with Ångström space resolution. This controversial idea together with the possibility of combining attosecond and Ångström resolutions in the same measurements has become a hot topic in strong-field science. Indeed, this could provide a new way to image the evolution of the molecular electron cloud during, e.g. a chemical reaction in 'real time'. Here we review both experimental and theoretical challenges raised by the implementation of these prospects. In particular, we show how the valence orbital structure is encoded in the spectral phase of the recombination dipole moment calculated for Coulomb scattering states, which allows a tomographic reconstruction of the orbital using first-order corrections to the plane-wave approach. The possibility of disentangling multi-channel contributions to the attosecond emission is discussed as well as the necessary compromise between the temporal and spatial resolutions.

摘要

最近开发的阿秒光源使得可以以前所未有的时间分辨率研究物质中的超快过程。有人提出,阿秒发射的基本机制允许以埃空间分辨率成像价轨道。这个有争议的想法以及在相同测量中结合阿秒和埃分辨率的可能性,已经成为强场科学中的一个热门话题。事实上,这可以为在“实时”化学等反应过程中,提供一种新的方法来对分子电子云的演化进行成像。在这里,我们综述了实现这些前景所带来的实验和理论挑战。特别是,我们展示了价轨道结构是如何编码在库仑散射态计算的复合偶极矩的光谱相位中的,这允许使用对平面波方法的一阶修正对轨道进行层析重建。还讨论了将阿秒发射的多通道贡献分离开的可能性,以及时间和空间分辨率之间的必要折衷。

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