Magnetosynthesis Effect on the Structure and Ground State of Cu2+-Based Antiferromagnets
Micaela E Primer1, Anna A Berseneva1, Ayesha Ulde2
1Materials Science Center, National Laboratory of the Rockies, Golden, Colorado 80401, United States.
None:
Synthetic variables can have an outsized influence on the crystal structure and magnetic properties of a material, particularly those of quantum materials. In this work, we investigate the impact of synthesis under a magnetic field (magnetosynthesis) on the crystal structure and magnetic properties of several Cu2+ (S = 1/2)-based materials with antiferromagnetic interactions and varying levels of magnetic frustration, from simple antiferromagnets to a quantum spin liquid. Here, we develop methods to apply small (0.09-0.37 T) magnetic fields during low-temperature hydrothermal, evaporative, and rehydration syntheses of the simple antiferromagnet CuCl2·2H2O, the canted antiferromagnet (Cu,Zn)3Cl4(OH)2·2H2O, the frustrated and canted antiferromagnet atacamite Cu2(OH)3Cl, and the highly frustrated quantum spin liquid herbertsmithite Cu3Zn(OH)6Cl2. We report the first single-crystal X-ray structural determination of the Cu3Cl4(OH)2·2H2O structure type and probe the stability of this phase both experimentally and computationally. Atacamite Cu2(OH)3Cl synthesized under a 0.19 T field experiences a 0.15 K (∼3%) decrease in its Néel transition temperature. This result suggests that magnetosynthesis with small applied fields may have a very subtle influence upon the magnetic properties of moderately magnetically frustrated 3d materials.
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