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Single Photon K − 2 and K − 1 K − 1 Double Core Ionization in C 2 H 2 n ( n = 1 – 3 ), CO, and N 2 as a Potential New Tool for Chemical Analysis

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TLDR
The cross section variation for single photon K(-1)K (-1) double core ionization in the C(2)H(2n) sequence and in the isoelectronic C(1-3) hydrocarbon sequence, N (2) and CO molecules validates a knock-out mechanism in which a primary ionized 1s photoelectron ejects another 1s electron of the neighbor atom.
Abstract
We have observed single photon double $K$-shell photoionization in the ${\mathrm{C}}_{2}{\mathrm{H}}_{2n}$ ($n=1--3$) hydrocarbon sequence and in ${\mathrm{N}}_{2}$ and CO, using synchrotron radiation and electron coincidence spectroscopy. Our previous observations of the ${K}^{\ensuremath{-}2}$ process in these molecules are extended by the observations of a single photon double photoionization with one core hole created at each of the two neighboring atoms in the molecule (${K}^{\ensuremath{-}1}{K}^{\ensuremath{-}1}$ process). In the ${\mathrm{C}}_{2}{\mathrm{H}}_{2n}$ sequence, the spectroscopy of ${K}^{\ensuremath{-}1}{K}^{\ensuremath{-}1}$ states is much more sensitive to the bond length than conventional electron spectroscopy for chemical analysis spectroscopy based on single $K$-shell ionization. The cross section variation for single photon ${K}^{\ensuremath{-}1}{K}^{\ensuremath{-}1}$ double core ionization in the ${\mathrm{C}}_{2}{\mathrm{H}}_{2n}$ sequence and in the isoelectronic ${\mathrm{C}}_{2}{\mathrm{H}}_{2}$, ${\mathrm{N}}_{2}$ and CO molecules validates a knock-out mechanism in which a primary ionized $1s$ photoelectron ejects another $1s$ electron of the neighbor atom. The specific Auger decay from such states is clearly observed in the CO case.

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Journal ArticleDOI

Highly Accurate Prediction of Core Spectra of Molecules at Density Functional Theory Cost: Attaining Sub-electronvolt Error from a Restricted Open-Shell Kohn–Sham Approach

TL;DR: In this paper, the square gradient minimization (SGM) algorithm was used to obtain spin-pure restricted open-shell Kohn-Sham (ROKS) energies for core excited states of molecules.
Journal ArticleDOI

Modeling of the spectroscopy of core electrons with density functional theory

TL;DR: In this paper, an overview of current developments to apply DFT and TDDFT to study the key techniques of X-ray photoelectron spectroscopy, X −ray absorption, X−ray emission, and resonant inelastic X -ray scattering is presented.
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Using X-ray free-electron lasers for spectroscopy of molecular catalysts and metalloenzymes

TL;DR: The current state of the art of X-ray spectroscopy studies at XFELs is described and some new techniques currently under development are highlighted, including real-time molecular movies of metalloenzymes and catalysts in solution, while chemical reactions are taking place.
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