Magnetic structure and uniaxial negative thermal expansion in antiferromagnetic CrSb

Negative thermal expansion (NTE) has been found in a growing number of ferromagnetic and ferrimagnetic materials; however, it remains a challenge to discover antiferromagnetic (AFM) NTE materials. Here, we report the uniaxial NTE properties of AFM intermetallic CrSb systematically, and reveal its uniaxial NTE mechanism for the first time. The present AFM intermetallic CrSb shows uniaxial NTE at high temperature and over a broad temperature window (αa = -6.55 × 10-6 K-1, 360-600 K). The direct experimental evidence of neutron powder diffraction reveals that NTE is induced by the AFM ordering of the Cr atom. The present study demonstrates that due to the transition from an AFM ordered structure to a paramagnetic disordered configuration, the negative contribution to the thermal expansion from the magnetovolume effect overwhelms the positive contribution from anharmonic phonon vibration. This study is of interest to find antiferromagnetic NTE materials.