Laboratoire de Chimie Physique-Matière et Rayonnement, Université Pierre et Marie Curie, 75231 Paris Cedex 05, France.
Proc Natl Acad Sci U S A. 2013 Sep 17;110(38):15201-6. doi: 10.1073/pnas.1306697110. Epub 2013 Sep 3.
Interferences in coherent emission of photoelectrons from two equivalent atomic centers in a molecule are the microscopic analogies of the celebrated Young's double-slit experiment. By considering inner-valence shell ionization in the series of simple hydrocarbons C2H2, C2H4, and C2H6, we show that double-slit interference is widespread and has built-in quantitative information on geometry, orbital composition, and many-body effects. A theoretical and experimental study is presented over the photon energy range of 70-700 eV. A strong dependence of the oscillation period on the C-C distance is observed, which can be used to determine bond lengths between selected pairs of equivalent atoms with an accuracy of at least 0.01 Å. Furthermore, we show that the observed oscillations are directly informative of the nature and atomic composition of the inner-valence molecular orbitals and that observed ratios are quantitative measures of elusive many-body effects. The technique and analysis can be immediately extended to a large class of compounds.
在分子中两个等效原子中心的光电子相干发射中的干涉是著名的杨氏双缝实验的微观类比。通过考虑简单碳氢化合物 C2H2、C2H4 和 C2H6 系列中的内壳层电离，我们表明双缝干涉是普遍存在的，并且具有关于几何形状、轨道组成和多体效应的内置定量信息。在 70-700 eV 的光子能量范围内进行了理论和实验研究。观察到了振荡周期强烈依赖于 C-C 距离，这可以用于以至少 0.01 Å 的精度确定选定的等效原子对之间的键长。此外，我们表明，观察到的振荡直接反映了内壳层分子轨道的性质和原子组成，并且观察到的比值是难以捉摸的多体效应的定量度量。该技术和分析可以立即扩展到一大类化合物。
