Abstract

The general picture established so far for the links between superconductivity and magnetic ordering in iron chalcogenide Fe1+y(Te1-xSex) is that the substitution of Se for Te directly drives the system from the antiferromagnetic end into the superconducting regime. Here, we report on the observation of a ferromagnetic component that developed together with the superconducting transition in Fe-excess Fe1.12Te1-xSex crystals using neutron and x-ray diffractions, resistivity, magnetic susceptibility and magnetization measurements. The superconducting transition is accompanied by a negative thermal expansion of the crystalline unit cell and an electronic charge redistribution, where a small portion of the electronic charge flows from around the Fe sites toward the Te/Se sites. First-principles calculations show consistent results, revealing that the excess Fe ions play a more significant role in affecting the magnetic property in the superconducting state than in the normal state and the occurrence of an electronic charge redistribution through the superconducting transition.

Highlights

  • Configuration of the conduction and magnetic components

  • The development of an additional ferromagnetic component in the superconducting state is identified, which links directly to the occurrence of electronic charge redistribution, in which a small portion of the electronic charges around the Fe(1) and Fe(2) sites flow to the Te/Se sites on cooling through the superconducting transition

  • In the compounds with excess Fe ions, the divalent Te/Se bonds are shared among the Fe(1) ions on the lattice sites and the Fe(2) ions on the interstitial sites

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Summary

Introduction

Configuration of the conduction and magnetic components. The goal of this study is to search for the ferromagnetic component that links directly to the superconductivity in Fe-excess Fe(Te,Se). The low-temperature magnetic phase, which coexists with superconductivity, involves the ordering of the Fe(1) and Fe(2) ions. The formation of superconducting pairs drives the electrons to flow from the Fe sites to the Te/Se sites, which alters the numbers of Fe2+ ions on the lattice and the excess sites. It is this change in valence of the magnetic sites that drives the system to develop an additional ferromagnetic component in the superconducting state

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