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- ItemPressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet α-RuCl3(College Park, MD : American Physical Society, 2018) Bastien, G.; Garbarino, G.; Yadav, R.; Martinez-Casado, F.J.; Beltrán, Rodríguez, R.; Stahl, Q.; Kusch, M.; Limandri, S.P.; Ray, R.; Lampen-Kelley, P.; Mandrus, D.G.; Nagler, S.E.; Roslova, M.; Isaeva, A.; Doert, T.; Hozoi, L.; Wolter, A.U.B.; Büchner, B.; Geck, J.; Van Den Brink, J.Magnetization and high-resolution x-ray diffraction measurements of the Kitaev-Heisenberg material α-RuCl3 reveal a pressure-induced crystallographic and magnetic phase transition at a hydrostatic pressure of p∼0.2 GPa. This structural transition into a triclinic phase is characterized by a very strong dimerization of the Ru-Ru bonds, accompanied by a collapse of the magnetic susceptibility. Ab initio quantum-chemistry calculations disclose a pressure-induced enhancement of the direct 4d-4d bonding on particular Ru-Ru links, causing a sharp increase of the antiferromagnetic exchange interactions. These combined experimental and computational data show that the Kitaev spin-liquid phase in α-RuCl3 strongly competes with the crystallization of spin singlets into a valence bond solid.