Complex single-site magnetism and magnetotransport in single-crystalline Gd2AlSi3

Abstract

We present a detailed investigation of single-crystal samples of the magnetic compound Gd2AlSi3, which crystallizes in the α-ThSi2 type tetragonal structure. We report the temperature and magnetic field dependence of the magnetic susceptibility, magnetization, heat capacity, electrical resistivity, and magnetoresistance for magnetic fields applied along both the tetragonal c-axis and in the basal ab-plane. X-ray diffraction measurements confirm a centrosymmetric, I41/amd space group of the crystal structure. Despite single-site occupancy of the Gd position in this tetragonal structure, we identify two successive antiferromagnetic phase transitions at Ne\'el temperatures 32~K and 23~K via magnetic susceptibility, heat capacity and transport measurements, as well as a complex magnetic interaction with a magnetic anisotropy that plays an important role in the direction-dependent transport response. Our identification of multiple magnetic phases in Gd2AlSi3, where Gd is the only magnetic species, helps to elucidate the field-induced skyrmionic behavior in the Gd-based intermetallic compounds.

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