X-ray absorption spectroscopy investigation of the electronic structure of superconducting FeSe_x single crystals

¹ Institute of Physics, Academia Sinica - Taipei 11529, Taiwan
² National Synchrotron Radiation Research Center - Hsinchu 30076, Taiwan
³ Department of Physics, Tamkang University - Tamsui, Taipei County, Taiwan
⁴ Advanced Light Source, Lawrence Berkeley National Laboratory - Berkeley, CA 94720, USA

^a clchen@phys.sinica.edu.tw
^b rao@phys.sinica.edu.tw

Received: 16 September 2010
Accepted: 21 January 2011

Abstract

X-ray absorption spectroscopy (XAS) Fe K-edge spectra of the FeSe_x (x = 1–0.8) single crystals cleaved in situ under vacuum reveal characteristic Fe 4sp states and a lattice distortion. The Se K-edge spectra point to a strong Fe 3d-Se 4p hybridization giving rise to itinerant charge carriers. A formal charge of ∼1.8+ for Fe and ∼2.2− for Se was evaluated from these spectra in the FeSe_x (x = 0.88). The charge balance between Fe and Se is assigned to itinerant electrons located in the Fe-Se hybridization bond. As x decreases the 4p hole count increases and a crystal structure distortion is observed that in turn causes the Fe separation in the ab-plane change from 4p orbital to varying (modulating) coordination. Powder X-ray diffraction (XRD) measurements also show a slight increase in lattice parameters as x decreases (increasing Se deficiency).