Interplay between External High Pressure and Intrinsic Jahn-Teller Effect in the Compression Behavior of Clinoatacamite.

ABSTRACT

Clinoatacamite (γ-Cu2(OH)3Cl) possesses a geometrically frustrated kagome lattice for the S = 1/2 antiferromagnetic spin system. Thus, it is deemed as the mother compound of many promising quantum spin liquid materials. Here, we synthesized clinoatacamite consisting of homogeneous octahedron-like particles with an average size of 1-2 µm via a hydrothermal strategy. Clinoatacamite crystallizes in a monoclinic lattice composed of Jahn-Teller distorted Cu(OH)6 and Cu(OH)4Cl2 octahedrons. The bonding nature of clinoatacamite is characterized using Raman scattering and FTIR absorption spectroscopies, which reveal the existence of trimeric hydrogen bonds. The magnetic measurements indicate that at temperatures below about 6 K, the magnetic response of the prepared samples is dominated by weak ferromagnetic contributions. The compression behavior is investigated by in situ high-pressure synchrotron radiation X-ray diffraction and Raman scattering spectroscopy. An isostructural phase transition is observed at about 8.4 GPa, which is evidenced by the anomalies in the variation curves of the lattice parameters and Raman scattering frequencies with pressure. The occurrence of the isostructural phase transition is attributed to the competition and cooperation of the external pressure and intrinsic Jahn-Teller effect, together with the interplay of intrastructural hydrogen bonding.