受激阿秒X射线拉曼散射揭示的纠缠价电子-空穴动力学
Entangled Valence Electron-Hole Dynamics Revealed by Stimulated Attosecond X-ray Raman Scattering.
作者信息
Healion Daniel, Zhang Yu, Biggs Jason D, Govind Niranjan, Mukamel Shaul
机构信息
Dept. of Chemistry, University of California, 450 Rowland Hall, Irvine, California 92697, USA, and William R. Wiley Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, P. O. Box 999, Richland, Washington 99352, USA.
出版信息
J Phys Chem Lett. 2012 Aug 8;3(17):2326-2331. doi: 10.1021/jz300981w.
Abstract
We show that broadband x-ray pulses can create wavepackets of valence electrons and holes localized in the vicinity of a selected atom (nitrogen, oxygen or sulfur in cysteine) by stimulated resonant Raman scattering. The subsequent dynamics reveals highly correlated motions of entangled electrons and hole quasiparticles. This information goes beyond the time-dependent total charge density derived from x-ray diffraction.
摘要
我们表明，宽带X射线脉冲可以通过受激共振拉曼散射产生局域在选定原子（半胱氨酸中的氮、氧或硫）附近的价电子和空穴波包。随后的动力学揭示了纠缠电子和空穴准粒子的高度相关运动。这些信息超越了由X射线衍射得出的随时间变化的总电荷密度。
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Migration of holes: numerical algorithms and implementation.
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Multielectron wave-packet propagation: general theory and application.多电子波包传播：一般理论与应用。
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