Suppression of Superconductivity and Nematic Order in Fe$_{1-y}$Se$_{1-x}$S$_x$ (0$\leq$$x$$\leq$1, $y$$\leq$0.1) Crystals by Anion Height Disorder

TL;DR

This study reveals that in Fe$_{1-y}$Se$_{1-x}$S$_x$ crystals, superconductivity and nematic order suppression are linked to disorder in Fe vibrations along the c-axis, rather than the traditional anion height correlation.

Contribution

It demonstrates that disorder in Fe vibrations, caused by S substitution, suppresses $T_c$ and nematic transition, challenging the conventional correlation with anion height in Fe-based superconductors.

Findings

$T_c$ and $T_s$ are suppressed by disorder in Fe vibrations.

Disorder arises from random S substitution causing tetrahedral deformation.

Traditional correlation between $T_c$ and anion height does not hold in these alloys.

Abstract

Connections between crystal chemistry and critical temperature $T_c$ have been in the focus of superconductivity, one of the most widely studied phenomena in physics, chemistry and materials science alike. In most Fe-based superconductors, materials chemistry and physics conspire so that $T_c$ correlates with the average anion height above the Fe plane, i. e. with the geometry of the FeAs4 or FeCh4 (Ch = Te, Se, or S) tetrahedron. By synthesizing Fe$_{1-y}$Se$_{1-x}$S$_x$ (0$\leq$$x$$\leq$1, $y$$\leq$0.1), we find that in alloyed crystals $T_c$ is not correlated with the anion height like it is for most other Fe superconductors. Instead, changes in $T_c$($x$) and tetragonal-to-orthorombic (nematic) transition $T_s$($x$) upon cooling are correlated with disorder in Fe vibrations in the direction orthogonal to Fe planes, along the crystallographic c-axis. The disorder stems from the random nature of S substitution, causing deformed Fe(Se,S)4 tetrahedra with different Fe-Se and Fe-S bond distances. Our results provide evidence of $T_c$ and $T_s$ suppression by disorder in anion height. The connection to local crystal chemistry may be exploited in computational prediction of new superconducting materials with Fe/S building blocks.