Abstract

We have recently initiated hard x-ray photoelectron spectroscopy experiments on heavy atoms and heavy-element containing molecules in gas phase by using synchrotron radiation up to 35 keV at SPring-8 undulator beamlines. We have successfully measured deep inner-shell photoelectron spectra, as well as L-MM and M-NN Auger electron spectra excited below and above the K-edge of heavy elements. Target specimens utilized for the preliminary experiments are Ar, Kr and Xe atoms, and also iodine in iodomethane (CH3I) and trifluoroiodomethane (CF3I) molecules, respectively. We show some selected results on the extracted core-hole lifetime broadenings for the iodine 1s core level of the CH3I molecule and also for the Xe 2s, 2p core levels, to compare with theoretical values. The L-MM Auger electron spectra of Kr recorded at 13 and 16.6 keV excitation energies are also shown as typical examples, and the spectrum measured above the K-edge, i.e. 14.327 keV, is analyzed based on theoretical calculations using the Hartree–Fock method. As a result, we give a tentative assignment for the double-core-hole hyper-satellite LL-LMM Auger transitions of the Kr atom.

Highlights

  • Hard x-ray photoelectron spectroscopy (HAXPES) at modern synchrotron radiation facilities is widely used nowadays and well known as one of the most powerful methods to directly investigate bulk electronic structure of condensed matter [1], owing to its intrinsic advantages, e.g. surface insensitivity and large probing depth, compared with PES using ultraviolet or soft x-ray radiation

  • The GALAXIES beamline at the SOLEIL synchrotron [2, 3] has been the only facility for high-resolution HAXPES experiments on atomic and molecular science and has been achieving significant results on double-core-hole spectroscopy [4,5,6,7], recoil effects [8,9,10], ultrafast phenomena [11,12,13], post-collision interaction (PCI) [14, 15], resonant Auger processes [16,17,18,19,20], and very recent studies on aqueous solution [21, 22]

  • This apparatus is usually installed at the soft x-ray undulator beamline BL17SU [27] (RIKEN beamline) at SPring-8, we move it to the hard x-ray undulator beamline for the gas-phase HAXPES experiments

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Summary

Introduction

Hard x-ray photoelectron spectroscopy (HAXPES) at modern synchrotron radiation facilities is widely used nowadays and well known as one of the most powerful methods to directly investigate bulk electronic structure of condensed matter [1], owing to its intrinsic advantages, e.g. surface insensitivity and large probing depth, compared with PES using ultraviolet or soft x-ray radiation. In 2016, at SPring-8, in order to advance the HAXPES as well as the hard x-ray induced Auger electron spectroscopy experiments on atomic and molecular science by making full use of the characteristic of such a high-energy and high-brilliance x-ray source, we have successfully upgraded an electron spectroscopy apparatus consisting of a hemispherical analyzer equipped with a gas-cell [25], which enables us to cover the kinetic energy up to 6 keV Such instrument had been previously utilized to diagnose the characteristics of optics designed for soft x-ray beamlines [26,27,28] and to carry out experiments using soft x-ray radiation [29,30,31].

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