通过受激X射线拉曼过程对远程光致电子转移进行相干控制。
Coherent control of long-range photoinduced electron transfer by stimulated X-ray Raman processes.
作者信息
Dorfman Konstantin E, Zhang Yu, Mukamel Shaul
机构信息
Singapore Institute of Manufacturing Technology, Singapore 638075;
Department of Chemistry, University of California, Irvine, CA 92697;
出版信息
Proc Natl Acad Sci U S A. 2016 Sep 6;113(36):10001-6. doi: 10.1073/pnas.1610729113. Epub 2016 Aug 24.
Abstract
We show that X-ray pulses resonant with selected core transitions can manipulate electron transfer (ET) in molecules with ultrafast and atomic selectivity. We present possible protocols for coherently controlling ET dynamics in donor-bridge-acceptor (DBA) systems by stimulated X-ray resonant Raman processes involving various transitions between the D, B, and A sites. Simulations presented for a Ru(II)-Co(III) model complex demonstrate how the shapes, phases and amplitudes of the X-ray pulses can be optimized to create charge on demand at selected atoms, by opening up otherwise blocked ET pathways.
摘要
我们表明，与选定的核心跃迁共振的X射线脉冲可以以超快和原子选择性操纵分子中的电子转移（ET）。我们提出了通过涉及供体（D）、桥（B）和受体（A）位点之间各种跃迁的受激X射线共振拉曼过程来相干控制供体-桥-受体（DBA）系统中ET动力学的可能方案。针对Ru（II）-Co（III）模型配合物进行的模拟表明，如何通过打开原本受阻的ET途径来优化X射线脉冲的形状、相位和振幅，从而在选定原子上按需产生电荷。
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