New insights into the structural properties of κ-(BEDT-TTF)2Ag2(CN)3 spin liquid

Acta Crystallogr B Struct Sci Cryst Eng Mater. 2020 Aug 1;76(Pt 4):581-590. doi: 10.1107/S2052520620005545. Epub 2020 Jul 8.


Here, the first accurate study is presented of the room-temperature and 100 K structures of one of the first organic spin liquids, κ-(BEDT-TTF)2Ag2(CN)3. It is shown that the monoclinic structure determined previously is only the average one. It is shown that the exact structure presents triclinic symmetry with two non-equivalent dimers in the unit cell. But surprisingly this does not lead to a sizeable charge disproportionation between dimers. The difference from the analogue compound κ-(BEDT-TTF)2Cu2(CN)3 which also presents a spin liquid phase is discussed in detail. The data provided here show the importance of the anionic layer and in particular the transition metal position in the process of symmetry breaking. The possible impact of the symmetry breaking, albeit weak, on the spin-liquid mechanism and the influence of various disorders on the physical properties of this system is also discussed.

Keywords: Mott transition; X-ray diffraction; geometrical frustration; molecular spin liquids.