Structural Analysis of the Gd-Au-Al 1/1 Quasicrystal Approximant Phase across Its Composition-Driven Magnetic Property Changes.

GdAuAl Tsai-type 1/1 quasicrystal approximants (ACs) exhibit three magnetic orders that can be finely tuned by the valence electron concentration (/ ratio). This parameter has been considered to be crucial for controlling the long-range magnetic order in quasicrystals (QCs) and ACs. However, the nonlinear trend of the lattice parameter as a function of Au concentration suggests that GdAuAl 1/1 ACs are not following a conventional solid solution behavior. We investigated GdAuAl samples with values of 52, 53, 56, 61, 66, and 73 by single-crystal X-ray diffraction. Our analysis reveals that increasing Au/Al ordering with increasing leads to distortions in the icosahedral shell built of the Gd atoms and that trends observed in the interatomic Gd-Gd distances closely correlate with the magnetic property changes across different values. Our results demonstrate that the e/a ratio alone may be an oversimplified concept for investigating the long-range magnetic order in 1/1 ACs and QCs and that the mixing behavior of the nonmagnetic elements Au and Al plays a significant role in influencing the magnetic behavior of the GdAuAl 1/1 AC system. These findings will contribute to improved understanding towards tailoring magnetic properties in emerging materials.