New iron-based Heusler compounds Fe2YZ: Comparison with theoretical predictions of the crystal structure and magnetic properties

TL;DR

This study synthesizes and characterizes new Fe2YZ Heusler compounds, revealing they adopt an inverse cubic structure contrary to previous predictions, and compares experimental results with ab-initio calculations to understand their stability.

Contribution

It provides experimental validation and comparison of the crystal structure and magnetic properties of Fe2YZ Heusler compounds with theoretical predictions, highlighting the role of atomic disorder.

Findings

Most synthesized compounds adopt inverse cubic Heusler structure.

Disorder levels vary among compounds, affecting stability.

Good agreement between experimental magnetic moments and calculations.

Abstract

The present work reports on the new soft ferromagnetic Heusler phases Fe2NiGe, Fe2CuGa, and Fe2CuAl, which in previous theoretical studies have been predicted to exist in a tetragonal regular Heusler structure. Together with the known phases Fe2CoGe and Fe2NiGa these materials have been synthesized and characterized by powder XRD, 57 Fe M\"ossbauer spectroscopy, SQUID and EDX measurements. In particular M\"ossbauer spectroscopy was used to monitor the degree of local atomic order/disorder and to estimate magnetic moments at the Fe sites from the hyperfine fields. It is shown that in contrast to the previous predictions all the materials except Fe2NiGa basically adopt the inverse cubic Heusler (X-) structure with differing degrees of disorder. The disorder is more enhanced in case of Fe2NiGa, which was predicted as an inverse Heusler phase. The experimental data are compared with results from ab-inito electronic structure calculations on LDA level incorporating the effects of atomic disorder by using the coherent potential approximation (CPA). A good agreement between calculated and experimental magnetic moments is found for the cubic inverse Heusler phases. Model calculations on various atomic configurations demonstrate that antisite disorder tends to enhance the stability of the X-structure. Given the fundamental scientific and technological importance of tetragonal Heusler phases the present results call for further investigations to unravel the factors stabilizing tetragonal Heusler materials.