Crystal growth and characterization of Fe$_{1+\delta}$Se$_{1-x}$Te$_x$ (0.5 $\leq$ $x$ $\leq$ 1) from LiCl/KCl flux

TL;DR

This study presents a new flux method for growing high-quality Fe$_{1+ ext{delta}}$Se$_{1-x}$Te$_x$ crystals, revealing how interstitial iron influences superconductivity, magnetic order, and electronic properties across different compositions.

Contribution

The paper introduces a stable LiCl/KCl flux growth technique that produces homogeneous Fe$_{1+ ext{delta}}$Se$_{1-x}$Te$_x$ crystals with improved quality and provides detailed insights into how interstitial iron affects their physical properties.

Findings

High-quality single crystals were successfully grown using LiCl/KCl flux.

Superconductivity is maximized at x=0.61 with $T_C$=14.3 K and low interstitial Fe.

Interstitial Fe $ ext{delta}$ increases sharply at high Te content, correlating with loss of superconductivity and emergence of antiferromagnetic order.

Abstract

An eutectic LiCl/KCl flux method in a horizontal configuration has been used to grow a series of homogeneous Fe$_{1+\delta}$Se$_{1-x}$Te$_x$ single crystals of high quality with 0.5 $\leq$ $x$ $\leq$ 1. Compared with previously used melt-growth method, the stable crystallization process in LiCl/KCl flux below their peritectic temperatures results in better homogeneity and crystalline perfection identified by energy dispersive spectrometer and x-ray diffraction. The interstitial Fe value $\delta$ remains small within 0.5 $\leq$ $x$ $\leq$ 0.85 where the superconducting temperature $T_C$ is not sensitive to the Te content with sharp superconducting transition widths $\Delta$$T_C$ < 1 K and a maximum of $T_C$ = 14.3 K at $x$ = 0.61. The value $\delta$ starts to increase quickly accompanied by a deviation of linear behavior of crystal lattice parameters as well as the broadening of $\Delta$$T_C$ = 2.1 K at $x$ = 0.91, then suddenly rises up to $\delta$ > 0.1 followed by the disappearance of superconductivity and emergence of antiferromagnetic order at x $\geq$ 0.96. We also observed a metallic to semiconducting transition in the normal state resistivity of Fe$_{1+\delta}$Se$_{1-x}$Te$_x$ with increasing Te content which is related to a localized electronic state induced by the interstitial Fe. The interstitial Fe value $\delta$ might be a key physical parameter to understand various properties of Fe$_{1+\delta}$Se$_{1-x}$Te$_x$ system.