文摘
Minerals of the atacamite group such as herbertsmithite and kapellasite have recently attracted enormous attention as the S = ½ Kagomé antiferromagnets for achieving the quantum spin liquid (QSL) state with diverse technological applications. Herein we report on the synthesis of the newly discovered mineral centennialite by using an unconventional “solid-state” reaction method at 463 K. Synthetic centennialite, Ca1.06Cu2.94Cl2.01(OH)5.99·0.73H2O, has been characterized by scanning electron microscopy, electron microprobe analyses, Fourier-transform infrared spectroscopy, thermogravimetric and differential scanning calorimetric analyses, single-crystal X-ray diffraction structure refinements, and magnetic susceptibility measurements. The crystal structure of centennialite is characterized by a perfect (threefold symmetry) Kagomé layer with <5 % substitution between Ca and Cu and therefore differs from those of herbertsmithite and kapellasite, in which 15–25 % mixing between similar Zn and Cu atoms dramatically affects the QSL state. Centennialite remains antiferromagnetic down to ~7 K with a moderate spin frustration (i.e., a Weiss temperature θ = −56 K and a spin frustration parameter f = 8), but exhibits a canted antiferromagnetic ordering with a ferromagnetic component at lower temperatures. Keywords Centennialite Synthesis Kagomé lattice Spin frustration S = ½ antiferromagnet