CaCu2(SeO3)2Cl2: spin-1/2 Heisenberg chain compound with complex frustrated interchain couplings

We report the crystal structure, magnetization measurements, and band-structure calculations for the spin-1/2 quantum magnet CaCu2(SeO3)2Cl2. The magnetic behavior of this compound is well reproduced by a uniform spin-1/2 chain model with the nearest-neighbor exchange of about 133 K. Due to the peculiar crystal structure, spin chains run in the direction almost perpendicular to the structural chains. We find an exotic regime of frustrated interchain couplings owing to two inequivalent exchanges of 10 K each. Peculiar superexchange paths grant an opportunity to investigate bond-randomness effects under partial Cl-Br substitution.Comment: Extended version: 9 pages, 7 figures, 4 table

Magnetism of coupled spin tetrahedra in ilinskite-type KCu5_{5}O2_2(SeO3_3)2_2Cl3_3

Synthesis, thermodynamic properties, and microscopic magnetic model of ilinskite-type KCu$_{5}$O$_2$(SeO$_3$)$_2$Cl$_3$ built by corner-sharing Cu$_4$ tetrahedra are reported, and relevant magnetostructural correlations are discussed. Quasi-one-dimensional magnetic behavior with the short-range order around 50\,K and the absence of long-range order down to at least 2\,K is observed experimentally and explained in terms of weakly coupled spin ladders (tubes) with a complex topology formed upon fragmentation of the tetrahedral network. This fragmentation is rooted in the non-trivial effect of the SeO$_3$ groups that render the Cu--O--Cu superexchange strongly ferromagnetic.Comment: 9 pages, 7 figure

High-frequency dielectric anomalies in a highly frustrated square kagome lattice nabokoite family compounds ACu7_7(TeO4_4)(SO4_4)5_5Cl (A=Na, K, Rb, Cs)

Nabokoite family compounds ACu$_7$(TeO$_4$)(SO$_4$)$_5$Cl (A=Na, K, Cs, Rb) are candidates for the experimental realization of highly-frustrated 2D square kagome lattice (SKL). Their magnetic subsystem includes SKL layers decorated by additional copper ions. All members of this family are characterized by quite high Curie-Weiss temperatures ($\sim 80-200$ K), but magnetic ordering was reported only for Na and K compounds at a much lower temperatures below 4 K. We report here results of the study of high-frequency ($\sim 10$ GHz) dielectric properties of this family of compounds. Our study revealed presence of the strong dielectric anomaly both in the real and imaginary parts of high-frequency dielectric permittivity for Na and K compounds approx. 100 and 26 K, correspondingly, presumably related to antiferroelectric ordering. Additionally, much weaker anomalies were observed at approximately 5K indicating possible interplay of magnetic and lattice degrees of freedom. We discuss possible relation between the structure rearrangements accompanying dielectric anomalies and a delayed magnetic ordering in the nabokoite family compounds.Comment: 12 pages, 8 figure

Cs7Sm11[TeO3]12Cl16 and Rb7Nd11[TeO3]12Br16, the new tellurite halides of the tetragonal Rb6LiNd11[SeO3]12Cl16 structure type

The authors thank the Russian Foundation for Basic Researches for the support of this work under Grants No. 14-03-00604_a and 12-03-92604-KO_a. The X-ray study of compound II was made possible due to M.V. Lomonosov Moscow State University Programm of Development. PL thanks the University of St Andrews and EPSRC for DTA Studentships to CB and LJD.Two new rare-earth – alkali – tellurium oxide halides were synthesized by a salt flux technique and characterized by single-crystal X-ray diffraction. The structures of the new compounds Cs7Sm11[TeO3]12Cl16 (I) and Rb7Nd11[TeO3]12Br16 (II) (both tetragonal, space group I4/mcm) correspond to the sequence of [MLn11(TeO3)12] and [M6×16] layers and bear very strong similarities to those of known selenite analogs. We discuss the trends in similarities and differences in compositions and structural details between the Se and Te compounds; more members of the family are predicted.PostprintPeer reviewe

Structural phase transitions in the kagome lattice based materials Cs2-xRbxSnCu3F12 (x = 0, 0.5, 1.0, 1.5)

The solid solution Cs2-xRbxSnCu3F12 (x = 0, 0.5, 1.0, 1.5) has been investigated crystallographically between 100 and 300 K using synchrotron X-ray powder diffraction and, in the case of x = 0, neutron powder diffraction.Comment: 14 pages, 9 figure

Quasi-1D XY Antiferromagnet Sr2Ni(SeO3)2Cl2 at Sakai-Takahashi Phase Diagram

Uniform quasi-one-dimensional integer spin compounds are of interest as a potential realization of the Haldane conjecture of a gapped spin liquid. This phase, however, has to compete with magnetic anisotropy and long-range ordered phases, the implementation of which depends on the ratio of interchain J′ and intrachain J exchange interactions and both uniaxial D and rhombic E single-ion anisotropies. Strontium nickel selenite chloride, Sr2Ni(SeO3)2Cl2, is a spin-1 chain system which passes through a correlations regime at Tmax ~ 12 K to long-range order at TN = 6 K. under external magnetic field it experiences the sequence of spin-flop at Bc1 = 9.0 T and spin-flip transitions Bc2 = 23.7 T prior to full saturation at Bsat = 31.0 T. Density functional theory provides values of the main exchange interactions and uniaxial anisotropy which corroborate the experimental findings. The values of J′/J = 0.083 and D/J = 0.357 place this compound into a hitherto unoccupied sector of the Sakai-Takahashi phase diagram. © 2021, The Author(s).Support by the P220 program of Government of Russia through the project 075-15-2021-604 is acknowledged. ANV acknowledges support by the RFBR Grant 19-02-00015. Work at Heidelberg was supported by BMBF via the project SpinFun (13XP5088) and by Deutsche Forschungsgemeinschaft (DFG) under Germany’s Excellence Strategy EXC2181/1-390900948 (the Heidelberg STRUCTURES Excellence Cluster) and through project KL 1824/13-1. We acknowledge the support of the HLD-HZDR, member of the European Magnetic Field Laboratory (EMFL). Theoretical calculations using density functional theory were supported by the Russian Science Foundation via project 20-62-46047. Experimental research was supported by the Russian Science Foundation via project 19-42-02010

Static and resonant properties of decorated square kagome lattice compound KCu7_7(TeO4_4)(SO4_4)5_5Cl

The magnetic subsystem of nabokoite, KCu$_7$(TeO$_4$)(SO$_4$)$_5$Cl, is constituted by buckled square kagome lattice of copper decorated by quasi-isolated Cu$^{2+}$ ions. This combination determines peculiar physical properties of this compound evidenced in electron spin resonance (ESR) spectroscopy, dielectric permittivity $\varepsilon$, magnetization $M$ and specific heat $C_p$ measurements. At lowering temperature, the magnetic susceptibility $\chi = M/H$ passes through broad hump at about 150 K inherent for low-dimensional magnetic systems and evidences sharp peak at antiferromagnetic phase transition at $T_N = 3.2$K. The $C_p(T)$ curve also exhibits sharp peak at $T_N$ readily suppressed by magnetic field and additional peak-like anomaly at $T_\textrm{peak}= 5.7$ K robust to magnetic field. The latter can be ascribed to low-lying singlet excitations filling the singlet-triplet gap in magnetic excitation spectrum of the square kagome lattice [J.Richter, O.Derzhko and J.Schnack, Phys. Rev. B 105, 144427 (2022)]. According to position of $T_\textrm{peak}$, the leading exchange interaction parameter $J$ in nabokoite is estimated to be about 60K. ESR spectroscopy provides indications that antiferromagnetic structure below $T_N$ is non-collinear. These complex thermodynamic and resonant properties signal the presence of two weakly coupled magnetic subsystems in nabokoite, namely spin-liquid with large singlet-triplet gap and antiferromagnet represented by decorating ions. Separate issue is the observation of antiferroelectric-type behavior in $\varepsilon$ at low temperatures, which tentatively reduces the symmetry and partially lifts frustration of magnetic interactions of decorating copper ions with buckled square kagome lattice.Comment: 13 pages, 13 figure