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Abstract
The toolbox for imaging molecules is well-equipped today. Some techniques visualize the geometrical structure, others the electron density or electron orbitals. Molecules are many-body systems for which the correlation between the constituents is decisive and the spatial and the momentum distribution of one electron depends on those of the other electrons and the nuclei. Such correlations have escaped direct observation by imaging techniques so far. Here, we implement an imaging scheme which visualizes correlations between electrons by coincident detection of the reaction fragments after high energy photofragmentation. With this technique, we examine the H2 two-electron wave function in which electron–electron correlation beyond the mean-field level is prominent. We visualize the dependence of the wave function on the internuclear distance. High energy photoelectrons are shown to be a powerful tool for molecular imaging. Our study paves the way for future time resolved correlation imaging at FELs and laser based X-ray sources.
Highlights
The toolbox for imaging molecules is well-equipped today
While the toolbox to image single electrons is well equipped, endeavors to directly examine an entangled two-electron wave function have, so far, not been successful and corresponding techniques are lacking. This is unfortunate, as electron correlation which shapes two-electron wavefunctions is of major importance across physics and chemistry
The singlephoton double ionization, i.e., the simultaneous emission of two electrons after photoabsorption, is only possible due to electron–electron correlation effects, as the photon cannot interact with two electrons simultaneously
Summary
The toolbox for imaging molecules is well-equipped today. Some techniques visualize the geometrical structure, others the electron density or electron orbitals. The photoionization differential cross section in the electron emission direction (θ, φ) (the socalled molecular frame photoelectron angular distribution, MFPAD) is proportional to the square of the Fourier transform (FT) of the initial state, φ0(k) (see methods section): dP dðcos θÞdk
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