Magnetic-field- and pressure-induced quantum phase transition in CsFeCl3_3 proved via magnetization measurement

We have performed magnetization measurements of the gapped quantum magnet CsFeCl$_3$ at temperatures ($T$) down to 0.5\,K at ambient pressure and down to 1.8\,K at hydrostatic pressures ($P$) of up to 1.5\,GPa. The lower-field ($H$) phase boundary of the field-induced ordered phase at ambient pressure is found to follow the power-law behavior expressed by the formula $H_{\rm N}(T)$\,$-$\,$H_{\rm c}$\,$\propto$\,$T_{\rm N}^{\phi}$. The application of pressure extends the phase boundary to both a lower field and higher temperature. Above the critical pressure $P_{\rm c}$\,$\sim$\,0.9\,GPa, the transition field $H_{\rm N}$ associated with the excitation gap becomes zero, and a signature of the magnetic phase transition is found in the $T$-dependence of magnetization in a very low applied field. This suggests that CsFeCl$_3$ exhibits a pressure-induced magnetic phase transition at $P_{\rm c}$.Comment: 8 pages, 8 figures, to appear in Phys. Rev.

Experimental Verification of the Universality of Magnetic-Field-Induced Bose-Einstein Condensation of Magnons

CsFeBr$_3$ is an $S\,{=}\,1$ hexagonal antiferromagnet that has a singlet ground state owing to its large easy-plane single-ion anisotropy. The critical behavior of the magnetic-field-induced phase transition for a magnetic field parallel to the $c$ axis, which can be described by the Bose-Einstein condensation (BEC) of magnons under the $U(1)$ symmetry, was investigated via magnetization and specific heat measurements down to 0.1$\,$K. For the specific heat measurement, we have developed a method of effectively suppressing the torque acting on a sample with strong anisotropy that uses the spin dimer compound Ba$_2$CoSi$_2$O$_6$Cl$_2$ with large and anisotropic Van Vleck paramagnetism. The temperature dependence of the transition field $H_{\rm c}(T)$ was found to follow the power-law $H_{\rm c}(T)\,{-}\,H_{\rm c}\,{\propto}\,T^{\phi}$ with a critical exponent of ${\phi}\,{=}\,1.50\,{\pm}\,0.02$ and critical field of $H_{\rm c}\,{=}\,2.60$ T. This result verifies the universality of the three-dimensional BEC of magnons described by ${\phi}_{\rm BEC}\,{=}\,3/2$.Comment: 5 pages, 3 figures, to appear in Phys. Rev.

Strong Suppression of Magnetic Ordering in an S = 1/2 Square-Lattice Heisenberg Antiferromagnet Sr2CuTeO6

We report the magnetic susceptibility and the low-temperature specific heat of a double perovskite compound, Sr2CuTeO6, which is expected as the spin-1/2 square-lattice Heisenberg antiferromagnet with nearest-neighbor J1 and next-nearest-neighbor J2 exchange interactions. The specific heat exhibits a sharp lambda-like anomaly at TN = 4.8 K indicative of magnetic ordering, which is much lower than those in isostructural A2CuMO6 with A = Ba, Sr and M = W, Mo. This indicates the strong suppression of magnetic ordering in Sr2CuTeO6. We estimate the exchange constant J1/kB ~ 80 K and J2/J1 < 0.07 from magnetic susceptibility data using Pade approximation of high temperature expansion and quantum Monte Carlo method. The strong suppression of magnetic ordering in Sr2CuTeO6 should be ascribed to the weekness of the interlayer exchange.Comment: 3 pages, 3 Figures, to appear in J. Phys. Soc. Jp

Quantum phase transition between disordered and ordered states in the spin-1/2 kagome lattice antiferromagnet (Rb1−x_{1-x}Csx_{x})2_2Cu3_3SnF12_{12}

We have systematically investigated the variation of the exchange parameters and the ground state in the $S = 1/2$ kagome-lattice antiferromagnet (Rb$_{1-x}$Cs$_{x}$)$_2$Cu$_3$SnF$_{12}$, via magnetic measurements using single crystals. One of the parent compounds, Rb$_2$Cu$_3$SnF$_{12}$, which has a distorted kagome lattice accompanied by four sorts of nearest-neighbor exchange interaction, has a disordered ground state described by a pinwheel valence-bond-solid state. The other parent compound, Cs$_2$Cu$_3$SnF$_{12}$, which has a uniform kagome lattice at room temperature, has an ordered ground state with the $q$ = 0 spin structure. The analysis of magnetic susceptibilities shows that with increasing cesium concentration $x$, the exchange parameters increase with the tendency to be uniform. It was found that the ground state is disordered for $x$ 0.53. The pseudogap observed for $x$ 0.53 approach zero at $x_{\rm c}$ $\simeq$ 0.53. This is indicative of the occurrence of a quantum phase transition at $x_{\rm c}$.Comment: 8 pages, 8 figures, to appear in Phys. Rev.

Magnetic Phase Diagram of the S=1/2 Triangular-Lattice Heisenberg Antiferromagnet Ba3CoNb2O9

We report the results of low-temperature thermal and magnetic measurements on Ba$_3$CoNb$_2$O$_9$ powder, described as a uniform triangular-lattice antiferromagnet (TLAF) with a fictitious spin-1/2. Ba$_3$CoNb$_2$O$_9$ is found to undergo two-step antiferromagnetic transitions at $T_{\rm N1}=1.39~{\rm K}$ and $T_{\rm N2}=1.13~{\rm K}$. As the magnetic field is increased, both $T_{\rm N1}$ and $T_{\rm N2}$ monotonically decrease. The magnetic field vs temperature phase diagram indicates that the exchange interactions are nearly of the Heisenberg type with weak easy-axis anisotropy and that the exchange interaction between triangular lattices is crucial, in contrast to the case of the quasi-two-dimensional TLAF Ba$_3$CoSb$_2$O$_9$ [Susuki {\it et al}., Phys. Rev. Lett. \textbf{110}, 267201 (2013)].Comment: 14 pages, 6 Figures, to appear in Phys. Rev.

Quasi-two-dimensional Bose-Einstein condensation of lattice bosons in spin-1/2 XXZ ferromagnet K2_2CuF4_4

K$_2$CuF$_4$ is magnetically described as a spin-1/2, quasi-two-dimensional (2D), square-lattice XXZ ferromagnet with weak easy-plane anisotropy. The magnetic ordering for an applied magnetic field $H$ parallel to the $c$ axis is equivalent to the Bose\,--\,Einstein condensation (BEC) of lattice bosons, as discussed by Matsubara and Matsuda [Prog. Theor. Phys. \textbf{16}, 569 (1956)]. Magnetization and specific heat measurements were performed to obtain the temperature vs magnetic field phase diagram for $H\,{\parallel}\,c$. The phase boundary between polarized and ordered phases was found to be expressed by the power law $H_{\rm c}(T)\,{-}\,H_{\rm c}(0)\,{\propto}\,T^\phi$ with exponent $\phi\,{\approx}\,1.0$ in a wide temperature range, in agreement with the theory of quasi-2D BEC.Comment: 5 pages, 4 figures, accepted for publication in Physics. Rev.

Field-driven successive phase transitions in quasi-two-dimensional frustrated antiferromagnet Ba2_2CoTeO6_6 and highly degenerate classical ground states

We report the results of magnetization and specific heat measurements of Ba$_2$CoTeO$_6$ composed of two subsystems A and B, which are magnetically described as an $S\,{=}\,1/2$ triangular-lattice Heisenberg-like antiferromagnet and a $J_1-J_2$ honeycomb-lattice Ising-like antiferromagnet, respectively. These two subsystems were found to be approximately decoupled. Ba$_2$CoTeO$_6$ undergoes magnetic phase transitions at $T_{\rm N1}\,{=}\,12.0$ K and $T_{\rm N2}\,{=}\,3.0$ K, which can be interpreted as the orderings of subsystems B and A, respectively. Subsystem A exhibits a magnetization plateau at one-third of the saturation magnetization for the magnetic field $H$ perpendicular to the $c$ axis owing to the quantum order-by-disorder, whereas for $H\,{\parallel}\,c$, subsystem B shows three-step metamagnetic transitions with magnetization plateaus at zero, one-third and one-half of the saturation magnetization. The analysis of the magnetization process for subsystem B shows that the classical ground states at these plateaus are infinitely degenerate within the Ising model.Comment: 7 pages, 8 figure

Valence-Bond-Glass State with Singlet Gap in the Spin-1/2 Square-Lattice Random J1J_1-J2J_2 Heisenberg Antiferromagnet Sr2_2CuTe1−x_{1-x}Wx_xO6_6

The double-perovskite compounds Sr$_2$CuTeO$_6$ and Sr$_2$CuWO$_6$ are magnetically described as quasi-two-dimensional spin-1/2 square-lattice $J_1{-}J_2$ Heisenberg antiferromagnets with predominant $J_1$ and $J_2$ exchange interactions, respectively. We report the low-temperature magnetic properties of Sr$_2$CuTe$_{1-x}$W$_x$O$_6$ with randomness in the magnitudes of $J_1$ and $J_2$. It was found that the low-temperature specific heat for $0.1\leq x \leq 0.5$ has a large component proportional to the temperature $T$ above 1.2 K, although the low-temperature specific heat for the two parent systems is approximately proportional to $T^3$. With decreasing temperature below 1.2 K, the $T$-linear component decreases rapidly toward zero, which is insensitive to the magnetic field up to 9 T. This is suggestive of the singlet excitation decoupled from the magnetic field. The NMR spectrum for $x=0.2$ exhibits no long-range order down to 1.8 K. These results indicates that the ground state of Sr$_2$CuTe$_{1-x}$W$_x$O$_6$ is a valence-bond-glass state with singlet gaps.Comment: 6 pages, 5 figure

Magnetic Structure of the S = 1/2S\,{=}\,1/2 Quasi-Two-Dimensional Square-Lattice Heisenberg Antiferromagnet Sr2_2CuTeO6_6

The magnetic structure of the double perovskite compound Sr$_2$CuTeO$_6$ was determined from neutron powder diffraction data. This material is magnetically described as an $S\,{=}\,1/2$ quasi-two-dimensional square-lattice Heisenberg model with antiferromagnetic nearest-neighbor and next-nearest-neighbor interactions. Sr$_2$CuTeO$_6$ undergoes a magnetic phase transition at $T_{\rm N}\,{\simeq}\,29\,$ K. The spin structure below $T_{\rm N}$ is N\'{e}el antiferromagnetic on the square lattice, which means that the nearest-neighbor interaction ($J_1$) is stronger than the next-nearest-neighbor interaction ($J_2$), in contrast to other isostructural compounds such as Ba$_2$CuWO$_6$ and Sr$_2$CuWO$_6$, for which $|J_1|\,{<}\,|J_2|$ is realized.Comment: 6 pages, 7 figures, to appear in Phys. Rev.

Magnetization Process and Collective Excitations in the S=1/2 Triangular-Lattice Heisenberg Antiferromagnet Ba3CoSb2O9

We have performed high-field magnetization and ESR measurements on Ba$_3$CoSb$_2$O$_9$ single crystals, as a representative two-dimensional spin-1/2 Heisenberg antiferromagnet on a uniform triangular lattice, and have determined all the magnetic parameters. For an applied magnetic field $H$ parallel to the $ab$-plane, the entire magnetization curve including the plateau at one-third of the saturation magnetization ($M_\mathrm{s}$) is in excellent agreement with the results of theoretical calculations except an anomaly near $(3/5)M_\mathrm{s}$, indicative of an additional field-induced transition. However, for $H\,{\parallel}\,c$, the magnetization curve exhibits a cusp near $M_\mathrm{s}/3$. Paramagnetic resonance signals above the N\'eel temperature indicate the nearly isotropic $g$-factor. A detailed analysis of the collective ESR modes observed in the ordered state, combined with the magnetization process, provides evidence of the weak easy-plane anisotropy.Comment: 5 pages, 4 figure