Quantum Spin Liquid Candidate Research Articles

Algebraic charge dynamics of the quantum spin liquid β′−EtMe3Sb[Pd(dmit)2]2

Nuclear spin-lattice (1/T1) and spin-spin (1/T2) relaxation rates of the cation sites of a quantum spin-liquid candidate b'-EtMe3Sb[Pd(dmit)2]2 and its deuterated sample are presented. The enhanced 1/T1 of 1H and 2D are well analyzed considering the rotations of methyl- and ethyl-groups of the cation with the activation energies of 200K and 1200K respectively. The 1/T1 and 1/T2 at the Sb site that is located on the 2-fold rotation axis remain active down to the lowest temperature with an algebraic temperature dependence of the correlation time as has been observed in the ac response of the dielectric constants.

Design and Preparation of a Quantum Spin Liquid Candidate κ-(ET)2Ag2(CN)3 Having a Nearby Superconductivity

Abstract Similar to the first quantum spin liquid (QSL) candidate, κ-(ET)2Cu2(CN)3 (1), newly prepared κ-(ET)2Ag2(CN)3 (2) is a dimer Mott insulator with a QSL ground state at ambient pressure and exhibits metallic and superconducting states next to the QSL state under pressure, where ET is bis(ethylenedithio)tetrathiafulvalene. The packing of the ET dimer, which corresponds to a single spin site (S = 1/2), in 2 is similar to that in 1. Salt 2 afforded a two-dimensional equilateral triangular spin lattice having strong geometrical spin frustration (t′/t = 0.967) similar to 1 (t′/t = 1.09), where t and t′ are the interdimer transfer interactions. The geometric relationship between the spin site and the opening in the anion layer in 2 is considerably different from that in 1, resulting in more dispersed packing of ET dimers, narrower bandwidth W, and larger on-site Coulomb repulsion energy U for 2 than 1. As a consequence, 2 has a higher electron correlation U/W, more robust QSL state for wider pressure range and is allocated far away from the itinerant region compared to those of 1. The narrower bandwidth is consistent with a higher superconducting critical temperature for 2 than 1 under pressure.

Gapped Spin-1/2 Spinon Excitations in a New Kagome Quantum Spin Liquid Compound Cu3Zn(OH)6FBr**Supported by the National Key Research and Development Program of China under Grant Nos 2016YFA0300502, 2016YFA0300503, 2016YFA0300604, 2016YF0300300 and 2016YFA0300802, the National Natural Science Foundation of China under Grant Nos 11421092, 11474330, 11574359, 11674406, 11374346 and 11674375, the National Basic Research Program of China (973 Program) under Grant

We report a new kagome quantum spin liquid candidate Cu3Zn(OH)6FBr, which does not experience any phase transition down to 50 mK, more than three orders lower than the antiferromagnetic Curie-Weiss temperature (∼200 K). A clear gap opening at low temperature is observed in the uniform spin susceptibility obtained from 19F nuclear magnetic resonance measurements. We observe the characteristic magnetic field dependence of the gap as expected for fractionalized spin-1/2 spinon excitations. Our experimental results provide firm evidence for spin fractionalization in a topologically ordered spin system, resembling charge fractionalization in the fractional quantum Hall state.

Thermal Hall Effect in a Phonon-Glass Ba_{3}CuSb_{2}O_{9}.

A distinct thermal Hall signal is observed in a quantum spin liquid candidate Ba_{3}CuSb_{2}O_{9}. The transverse thermal conductivity shows a power-law temperature dependence below 50K, where a spin gap opens. We suggest that because of the very low longitudinal thermal conductivity and the thermal Hall signals, a phonon Hall effect is induced by strong phonon scattering of orphan Cu^{2+} spins formed in the random domains of the Cu^{2+}-Sb^{5+} dumbbells in Ba_{3}CuSb_{2}O_{9}.

Importance of spin-orbit coupling in layered organic salts

We investigate the spin-orbit coupling (SOC) effects in $\ensuremath{\alpha}$- and $\ensuremath{\kappa}$-phase BEDT-TTF and BEDT-TSF organic salts. Contrary to the assumption that SOC in organics is negligible due to light C, S, and H atoms, we show the relevance of such an interaction in a few representative cases. In the weakly correlated regime, SOC manifests primarily in the opening of energy gaps at degenerate band touching points. This effect becomes especially important for Dirac semimetals such as $\ensuremath{\alpha}\ensuremath{-}{(\mathrm{ET})}_{2}{\mathrm{I}}_{3}$. Furthermore, in the magnetic insulating phase, SOC results in additional anisotropic exchange interactions, which provide a compelling explanation for the puzzling field-induced behavior of the quantum spin-liquid candidate $\ensuremath{\kappa}\ensuremath{-}{(\mathrm{ET})}_{2}{\mathrm{Cu}}_{2}{(\mathrm{CN})}_{3}$. We conclude by discussing the importance of SOC for the description of low-energy properties in organics.

Optical Properties of a Quantum Spin Liquid Candidate Material, κ-(BEDT-TTF)2Ag2(CN)3

We investigated the electronic states of a quantum spin liquid candidate material, κ-(BEDT-TTF)2Ag2(CN)3, using optical methods. In reflectivity measurements, we observed the polarization dependence of electronic transitions, which reflects the crystal structure and anisotropic charge excitation. Raman scattering measurements revealed that the broad magnetic excitation mode is located below 600 cm−1. This spectral feature indicates the spin-liquid nature of the candidate material. The charge-sensitive molecular-vibrational modes observed in infrared and Raman spectra are broader than those of typical BEDT-TTF compounds, which indicate a possibility of dynamic charge fluctuation. By comparing the optical spectra of κ-(BEDT-TTF)2Ag2(CN)3 with a well-investigated spin-liquid candidate κ-(BEDT-TTF)2Cu2(CN)3, we found common optical properties of BEDT-TTF-based spin-liquid candidates. The dynamic fluctuations of charge on a BEDT-TTF dimer are independent of the arrangement of BEDT-TTF molecules and anion layers.

Absence of Magnetic Thermal Conductivity in the Quantum Spin-Liquid Candidate YbMgGaO_{4}.

We present the ultralow-temperature specific heat and thermal conductivity measurements on single crystals of YbMgGaO_{4}, which was recently argued to be a promising candidate for a quantum spin liquid (QSL). In a zero magnetic field, a large magnetic contribution of specific heat is observed, and exhibits a power-law temperature dependence (C_{m}∼T^{0.74}). On the contrary, we do not observe any significant contribution of thermal conductivity from magnetic excitations. In magnetic fields H≥6 T, the exponential T dependence of C_{m} and the enhanced thermal conductivity indicate a magnon gap of the fully polarized state. The absence of magnetic thermal conductivity at the zero field in this QSL candidate puts a strong constraint on the theories of its ground state.

Continuous excitations of the triangular-lattice quantum spin liquid YbMgGaO4

A quantum spin liquid (QSL) is an exotic state of matter in which electrons' spins are quantum entangled over long distances, but do not show symmetry-breaking magnetic order in the zero-temperature limit. The observation of QSL states is a central aim of experimental physics, because they host collective excitations that transcend our knowledge of quantum matter; however, examples in real materials are scarce. Here, we report neutron-scattering measurements on YbMgGaO4, a QSL candidate in which Yb3+ ions with effective spin-1/2 occupy a triangular lattice. Our measurements reveal a continuum of magnetic excitations - the essential experimental hallmark of a QSL - at very low temperature (0.06 K). The origin of this peculiar excitation spectrum is a crucial question, because isotropic nearest-neighbor interactions do not yield a QSL ground state on the triangular lattice. Using measurements of the magnetic excitations close to the field-polarized state, we identify antiferromagnetic next-nearest-neighbor interactions in the presence of planar anisotropy as key ingredients for QSL formation in YbMgGaO4.

Optical, transport and magnetic properties of new compound CeCd3P3

We have found that CeCd3P3 crystallizes into a hexagonal ScAl3C3-type structure. The optical, transport and magnetic properties of CeCd3P3 were investigated by measuring the diffuse reflectance, electrical resistivity and magnetization. CeCd3P3 is a semiconductor with a fundamental band gap of approximately 0.75 eV. The 4f electrons of Ce3+ ions are well localized but do not show long-range order down to 0.48 K, presumably due to the geometrical frustration of Ce atoms. The magnetic ordering temperature is possibly lower than that of isostructural CeZn3P3 (0.75 K). Because several f-electron compounds with the ScAl3C3-type structure are quantum spin systems, CeCd3P3 may be a candidate for quantum spin liquid. On the other hand, the relatively large band gap compared to approximately 0.4 eV in CeZn3P3, would not be in accordance with the observation of the photoinduced Kondo effect, providing a potentially new range of applications for devices based on the Kondo effect.

Spin-1 [formula omitted] ferromagnetic Heisenberg model with an easy-plane crystal field on the cubic lattice: A bosonic approach

We examine the phase diagram of the spin-1 J1−J2−J3 ferromagnetic Heisenberg model with an easy-plane crystal field on the cubic lattice, in which J1 is the ferromagnetic exchange interaction between nearest neighbors, J2 is the antiferromagnetic exchange interaction between next-nearest neighbors and J3 is the antiferromagnetic exchange interaction between next-next-nearest neighbors. Using the bond-operator formalism, we investigate the phase transitions between the disordered paramagnetic phase and the ordered ones. We show that the nature of the quantum phase transitions changes as the frustration parameters (J2J1, J3J1) are varied. The zero-temperature phase diagram exhibits second- and first-order transitions, depending on the energy gap behavior. Remarkably, we find a disordered nonmagnetic phase, even in the absence of a crystal field, which is suggested to be a quantum spin liquid candidate. We also depict the phase diagram at finite temperature for some values of crystal field and frustration parameters.

Selectively doping barlowite for quantum spin liquid: A first-principles study

Barlowite $Cu_4(OH)_6FBr$ is a newly found mineral containing $Cu^{2+}$ kagome planes. Despite similarities in many aspects to Herbertsmithite $Cu_3Zn(OH)_6Cl_2$, the well-known quantum spin liquid (QSL) candidate, intrinsic Barlowite turns out not to be a QSL, possibly due to the presence of $Cu^{2+}$ ions in between kagome planes that induce interkagome magnetic interaction [PRL, 113, 227203 (2014)]. Using first-principles calculation, we systematically study the feasibility of selective substitution of the interkagome Cu ions with isovalent nonmagnetic ions. Unlike previous speculation of using larger dopants, such as $Cd^{2+}$ and $Ca^{2+}$, we identify the most ideal stoichiometric doping elements to be Mg and Zn in forming $Cu_3Mg(OH)_6FBr$ and $Cu_3Zn(OH)_6FBr$ with the highest site selectivity and smallest lattice distortion. The equilibirium anti-site disorder in Mg/Zn- doped Barlowite is estimated to be one order of magnitude lower than that in Herbertsmithite. The single-electron band structure and orbital component analysis show that the proposed selective doping effectively mitigates the difference between Barlowite and Herbertsmithite.

Gapless chiral spin liquid in a kagome Heisenberg model

Motivated by recent experiments on the Heisenberg S=1/2 quantum spin liquid candidate material kapellasite, we classify all possible chiral (time-reversal symmetry breaking) spin liquids with fermionic spinons on the kagome lattice. We obtain the phase diagram for the physically relevant extended Heisenberg model, comparing the energies of a wide range of microscopic variational wave functions. We propose that, at low temperature, kapellasite exhibits a gapless chiral spin liquid phase with spinon Fermi surfaces. This two-dimensional state inherits many properties of the nearby one-dimensional phase of decoupled anti-ferromagnetic spin chains, but also shows some remarkable differences. We discuss the spin structure factors and other physical properties.

Gapless quantum spin liquid in the S = 1/2 anisotropic kagome antiferromagnet ZnCu3(OH)6SO4

We have successfully synthesized the new S = 1/2 anisotropic kagome antiferromagnet ZnCu3(OH)6SO4 and determined its structure by synchrotron x-ray diffraction. No magnetic ordering is observed down to 50 mK, despite a moderately high Weiss temperature of Θw ∼ −79 K, indicating that the compound is a new quantum spin liquid (QSL) candidate. A linear temperature dependence of the magnetic heat capacity is found at 6 ∼ 15 K and below 0.6 K. Temperature-independent intrinsic susceptibilities are observed exactly in both temperature ranges. This consistently suggests a gapless QSL below 0.6 K, which may evolve from an unconventional quantum spin state at higher temperatures (6 ∼ 15 K).

High-Pressure Sequence ofBa3NiSb2O9Structural Phases: NewS=1Quantum Spin Liquids Based onNi2+

Two new gapless quantum spin-liquid candidates with S = 1 (Ni(2+)) moments: the 6H-B phase of Ba(3)NiSb(2)O(9) with a Ni(2+)-triangular lattice and the 3C phase with a Ni(2/3)Sb(1/3)-three-dimensional edge-shared tetrahedral lattice were obtained under high pressure. Both compounds show no magnetic order down to 0.35 K despite Curie-Weiss temperatures θ(CW) of -75.5 (6H-B) and -182.5 K (3C), respectively. Below ~25 K, the magnetic susceptibility of the 6H-B phase saturates to a constant value χ(0) = 0.013 emu/mol, which is followed below 7 K by a linear-temperature-dependent magnetic specific heat (C(M)) displaying a giant coefficient γ = 168 mJ/mol K(2). Both observations suggest the development of a Fermi-liquid-like ground state. For the 3C phase, the C(M) perpendicular T(2) behavior indicates a unique S = 1, 3D quantum spin-liquid ground state.

Thermal‐Transport Studies on Two‐Dimensional Quantum Spin Liquids

Quantum spin liquids (QSLs) are fluidlike states of quantum spins in which the long-range ordered state is destroyed by quantum fluctuations. The ground state of QSLs and their exotic phenomena, which have been extensively discussed for decades, have yet to be identified. We employ thermal-transport measurements on newly discovered QSL candidates κ-(BEDT-TTF)(2)Cu(2)(CN)(3) and EtMe(3)Sb[Pd(dmit)(2)](2), and report that the two organic insulators have different QSLs characterized by different elementary excitations. In κ-(BEDT-TTF)(2)Cu(2)(CN)(3), heat transport is thermally activated at low temperatures, and this suggests the presence of a spin gap in this QSL. In stark contrast, in EtMe(3)Sb[Pd(dmit)(2)](2), a sizable linear temperature dependence of thermal conductivity is clearly resolved in the zero-temperature limit, and shows gapless excitation with a long mean free path (ca. 1000 lattice distances). Such a long mean free path demonstrates a novel feature of QSL as a quantum-condensed state with long-distance coherence.

Quantum Excitations in Quantum Spin Ice

A form of quantum electrodynamics emerges from interacting spins at low temperatures in the spin ice $Y\phantom{\rule{0}{0ex}}{b}_{2}\phantom{\rule{0}{0ex}}T\phantom{\rule{0}{0ex}}{i}_{2}\phantom{\rule{0}{0ex}}{O}_{7}$.

Spin Liquid State in theS=1/2Triangular LatticeBa3CuSb2O9

The synthesis and characterization of Ba3CuSb2O9, which has a layered array of Cu2+ spins in a triangular lattice, are reported. The magnetic susceptibility and neutron scattering experiments of this material show no magnetic ordering down to 0.2 K with a θ(CW) = -55 K. The magnetic specific heat reveals a T-linear dependence with a γ = 43.4 mJ K(-2) mol(-1) below 1.4 K. These observations suggest that Ba3CuSb2O9 is a new quantum spin liquid candidate with a S = 1/2 triangular lattice.