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Register a new userCharacterizing random-singlet state in two-dimensional frustrated quantum magnets and implications for the double perovskite Sr$_2$CuTe$_{1-x}$W$_{x}$O$_6$
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Motivated by experimental observation of the non-magnetic phase in the compounds with frustration and disorder, we study the ground state of the spin-$1/2$ square-lattice Heisenberg model with randomly distributed nearest-neighbor $J_1$ and next-nearest-neighbor $J_2$ couplings. By using the density matrix renormalization group (DMRG) calculation on cylinder system with circumference up to $10$ lattice sites, we identify a disordered phase between the Neel and stripe magnetic phase with growing $J_2 / J_1$ in the presence of strong randomness. The vanished spin-freezing parameter indicates the absent spin glass order. The large-scale DMRG results unveil the size-scaling behaviors of the spin-freezing parameter, the power-law decay of average spin correlation, and the exponential decay of typical spin correlation, which all agree with the corresponding behavior in the one-dimensional random singlet (RS) state and characterize the RS nature of this non-magnetic state. The DMRG simulation also opens new insight and opportunities for characterizing a class of non-magnetic states in two-dimensional frustrated magnets with disorder. We also compare with existing experiments and suggest more measurements for understanding the spin-liquid-like behavior in the double perovskite Sr$_2$CuTe$_{1-x}$W$_{x}$O$_6$.
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Double-perovskite oxides that contain both 3d and 5d transition metal elements have attracted growing interest as they provide a model system to study the interplay of strong electron interaction and large spin-orbit coupling (SOC). Here, we report on experimental and theoretical studies of the magnetic and electronic properties of double-perovskites (La$_{1-x}$Sr$_x$)$_2$CuIrO$_6$ ($x$ = 0.0, 0.1, 0.2, and 0.3). The undoped La$_2$CuIrO$_6$ undergoes a magnetic phase transition from paramagnetism to antiferromagnetism at T$_N$ $sim$ 74 K and exhibits a weak ferromagnetic behavior below $T_C$ $sim$ 52 K. Two-dimensional magnetism that was observed in many other Cu-based double-perovskites is absent in our samples, which may be due to the existence of weak Cu-Ir exchange interaction. First-principle density-functional theory (DFT) calculations show canted antiferromagnetic (AFM) order in both Cu$^{2+}$ and Ir$^{4+}$ sublattices, which gives rise to weak ferromagnetism. Electronic structure calculations suggest that La$_2$CuIrO$_6$ is an SOC-driven Mott insulator with an energy gap of $sim$ 0.3 eV. Sr-doping decreases the magnetic ordering temperatures ($T_N$ and $T_C$) and suppresses the electrical resistivity. The high temperatures resistivity can be fitted using a variable-range-hopping model, consistent with the existence of disorders in these double-pervoskite compounds.
Remarkably, doping isovalent $d^{10}$ and $d^0$ cations onto the $B$ site in $A_2B$$B$O$_6$ double perovskites has the power to direct the magnetic interactions between magnetic $B$ cations. This is due to changes in orbital hybridization, which favors different superexchange pathways, and leads to the formation of alternative magnetic structures depending on whether $B$ is $d^{10}$ or $d^0$. Furthermore, the competition generated by introducing mixtures of $d^{10}$ and $d^0$ cations can drive the material into the realms of exotic quantum magnetism. Here, a W$^{6+}$ $d^0$ dopant was introduced to a $d^{10}$ hexagonal perovskite Ba$_2$CuTeO$_6$, which possesses a spin ladder geometry of Cu$^{2+}$ cations, creating a Ba$_2$CuTe$_{1-x}$W$_x$O$_6$ solid solution ($x$ = 0 - 0.3). Neutron and synchrotron X-ray diffraction show that W$^{6+}$ is almost exclusively substituted for Te$^{6+}$ on the corner-sharing site within the spin ladder, in preference to the face-sharing site between ladders. This means the intra-ladder interactions are selectively tuned by the $d^0$ cations. Bulk magnetic measurements suggest this suppresses magnetic ordering in a similar manner to that observed for the spin-liquid like material Sr$_2$CuTe$_{1-x}$W$_x$O$_6$. This further demonstrates the utility of $d^{10}$ and $d^0$ dopants as a tool for tuning magnetic ground states in a wide range of perovskites and perovskite-derived structures.
The double-perovskite A$_2$BBO$_6$ with heavy transition metal ions on the ordered B sites is an important family of compounds to study the interplay between electron correlation and spin-orbit coupling (SOC). Here we prepared high-quality Sr$_2$MgReO$_6$ powder and single-crystal samples and performed non-resonant and resonant synchrotron x-ray diffraction experiments to investigate its magnetic ground state. By combining the magnetic susceptibility and heat capacity measurements, we conclude that Sr$_2$MgReO$_6$ exhibits a layered antiferromagnetic (AF) order at temperatures below $sim$ 55 K with a propagation vector q = (001), which contrasts the previously suspected spin glass state. Our works clarify the magnetic order in Sr$_2$MgReO$_6$ and demonstrate it as a candidate system to look for magnetic octupolar orders and exotic spin dynamics.
We study effects of disorder (randomness) in a 2D square-lattice $S=1/2$ quantum spin system, the $J$-$Q$ model with a 6-spin interaction $Q$ supplementing the Heisenberg exchange $J$. In the absence of disorder the system hosts antiferromagnetic (AFM) and columnar valence-bond-solid (VBS) ground states. The VBS breaks $Z_4$ symmetry, and in the presence of arbitrarily weak disorder it forms domains. Using QMC simulations, we demonstrate two kinds of such disordered VBS states. Upon dilution, a removed site leaves a localized spin in the opposite sublattice. These spins form AFM order. For random interactions, we find a different state, with no order but algebraically decaying mean correlations. We identify localized spinons at the nexus of domain walls between different VBS patterns. These spinons form correlated groups with the same number of spinons and antispinons. Within such a group, there is a strong tendency to singlet formation, because of spinon-spinon interactions mediated by the domain walls. Thus, no long-range AFM order forms. We propose that this state is a 2D analog of the well-known 1D random singlet (RS) state, though the dynamic exponent $z$ in 2D is finite. By studying the T-dependent magnetic susceptibility, we find that $z$ varies, from $z=2$ at the AFM--RS phase boundary and larger in the RS phase The RS state discovered here in a system without geometric frustration should correspond to the same fixed point as the RS state recently proposed for frustrated systems, and the ability to study it without Monte Carlo sign problems opens up opportunities for further detailed characterization of its static and dynamic properties. We also discuss experimental evidence of the RS phase in the quasi-two-dimensional square-lattice random-exchange quantum magnets Sr$_2$CuTe$_{1-x}$W$_x$O$_6$.
We study the magnetic properties of CaFeTi$_2$O$_6$ (CFTO) by high-field magnetization and specific heat measurements. While the magnetic susceptibility data yield a vanishingly small Curie-Weiss temperature, the magnetic moments are not fully polarized in magnetic field up to 60 T, which reveals a large spin exchange energy scale. Yet, the system shows no long range magnetic order but a spin-glass-like state below 5.5 K in zero field, indicating strong magnetic frustration in this system. Applying magnetic field gradually suppresses the spin-glass-like state and gives rise to a potential quantum spin liquid state whose low-temperature specific heat exhibits a $T^{1.6}$ power-law. Crucially, conventional mechanisms for frustration do not apply to this system as it possesses neither apparent geometrical frustration nor exchange frustration. We suggest that the orbital modulation of exchange interaction is likely the source of hidden frustration in CFTO, and its full characterization may open a new route in the quest for quantum spin liquids.
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