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arXiv:0907.1710 · Physical Review B

Weak Mott insulators on the triangular lattice: Possibility of a gapless nematic quantum spin liquid

Tarun Grover, Nandini Trivedi, T. Senthil, Patrick A. Lee

Published Jun 18, 2010• 96 citations
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Abstract

We study the energetics of Gutzwiller projected BCS states of various symmetries for the triangular lattice antiferromagnet with a four-particle ring exchange using variational Monte Carlo methods. In a range of parameters the energetically favored state is found to be a projected ${d}_{{x}^{2}\ensuremath{-}{y}^{2}}$ paired state which breaks lattice rotational symmetry. We show that the properties of this nematic or orientationally ordered paired spin-liquid state as a function of temperature and pressure can account for many of the experiments on organic materials. We also study the ring-exchange model with ferromagnetic Heisenberg exchange and find that among the studied ans\"atze, a projected $f$-wave state is the most favorable.

DOI
10.1103/physrevb.81.245121

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We study the energetics of Gutzwiller projected BCS states of various symmetries for the triangular lattice antiferromagnet with a four-particle ring exchange using variational Monte Carlo methods. In a range of parameters the energetically favored state is found to be a projected dx2\ensuremath−y2{d}_{{x}^{2}\ensuremath{-}{y}^{2}}dx2\ensuremath−y2​ paired state which breaks lattice rotational symmetry. We show that the properties of this nematic or orientationally ordered paired spin-liquid state as a function of temperature and pressure can account for many of the experiments on organic materials. We also study the ring-exchange model with ferromagnetic Heisenberg exchange and find that among the studied ans"atze, a projected fff-wave state is the most favorable.
Previous investigations have suggested that the simplest spin-orbital model on the simplest frustrated lattice can host a nematic quantum spin-orbital liquid state. Namely, the orbital degeneracy of the SU(4) Kugel-Khomskii model tends to enhance quantum fluctuations and stabilize a quantum spin-orbital liquid exhibiting stripy features on the triangular lattice, as revealed by the state-of-the-art method of the density matrix renormalization group boosted by Gutzwiller projected wave functions. In this work, using the variational quantum Monte Carlo method, we study several spin-orbital liquid states, including a uniform $\ensuremath{\pi}$-flux state, three stripy states, and a plaquette state, on the $L\ifmmode\times\else\texttimes\fi{}L$ torus up to L=24L=24L=24. It turns out that one of these stripy states, called the ``stripe-II'' state, is energetically favored. This ground state breaks the C6{C}_{6}C6​ symmetry of the lattice, resulting in a reduced C2{C}_{2}C2​ symmetry and doubled unit cells while preserving the SU(4) spin-orbital rotation symmetry. Such a nematic quantum spin-orbital liquid state can be characterized by a parton Fermi surface (FS) consisting of open orbits in the Brillouin zone, in contrast to the circular FS of the uniform $\ensuremath{\pi}$-flux state.
Previous investigations have suggested that the simplest spin-orbital model on the simplest frustrated lattice can host a nematic quantum spin-orbital liquid state. Namely, the orbital degeneracy of the SU(4) Kugel-Khomskii (KK) model tends to enhance quantum fluctuations and stabilize a quantum spin-orbital liquid exhibiting stripy features on the triangular lattice, as revealed by the state-of-the-art method of the density matrix renormalization group boosted by Gutzwiller projected wave functions. In this work, using the variational quantum Monte Carlo method, we have studied several spin-orbital liquid states, including a uniform πππ flux state, three stripy states, and a plaquette state, on the L×LL\times{}LL×L torus up to L=24L=24L=24. It turns out that one of these stripy states, called the "stripe-II" state, is energetically favored. This ground state breaks the C6C_6C6​ symmetry of the lattice, resulting in a reduced C2C_2C2​ symmetry and doubled unit cells, while preserving the SU(4) spin-orbital rotation symmetry. Such a nematic quantum spin-orbital liquid state can be characterized by a parton Fermi surface (FS) consisting of open orbits in the Brillouin zone, in contrast to the circular FS of the uniform πππ-flux state.
Recent experiments on triangular lattice organic Mott insulators have found evidence for a two-dimensional (2D) spin liquid in close proximity to the metal-insulator transition. A Gutzwiller wave function study of the triangular lattice Heisenberg model with a four-spin ring exchange term appropriate in this regime has found that the projected spinon Fermi sea state has a low variational energy. This wave function, together with a slave particle-gauge theory analysis, suggests that this putative spin liquid possesses spin correlations that are singular along surfaces in momentum space, i.e., ``Bose surfaces.'' Signatures of this state, which we will refer to as a ``spin Bose metal'' (SBM), are expected to manifest in quasi-one-dimensional (quasi-1D) ladder systems: the discrete transverse momenta cut through the 2D Bose surface leading to a distinct pattern of 1D gapless modes. Here, we search for a quasi-1D descendant of the triangular lattice SBM state by exploring the Heisenberg plus ring model on a two-leg triangular strip (zigzag chain). Using density matrix renormalization group (DMRG) supplemented by variational wave functions and a bosonization analysis, we map out the full phase diagram. In the absence of ring exchange the model is equivalent to the ${J}_{1}\text{\ensuremath{-}}{J}_{2}$ Heisenberg chain, and we find the expected Bethe-chain and dimerized phases. Remarkably, moderate ring exchange reveals a new gapless phase over a large swath of the phase diagram. Spin and dimer correlations possess singular wave vectors at particular ``Bose points'' (remnants of the 2D Bose surface) and allow us to identify this phase as the hoped for quasi-1D descendant of the triangular lattice SBM state. We use bosonization to derive a low-energy effective theory for the zigzag spin Bose metal and find three gapless modes and one Luttinger parameter controlling all power law correlations. Potential instabilities out of the zigzag SBM give rise to other interesting phases such as a period-3 valence bond solid or a period-4 chirality order, which we discover in the DMRG. Another interesting instability is into a spin Bose-metal phase with partial ferromagnetism (spin polarization of one spinon band), which we also find numerically using the DMRG.
By using the variational Monte Carlo technique, we study the spin-12\frac{1}{2}21​ XXZ antiferromagnetic model (with easy-plane anisotropy) on the kagome lattice. A class of Gutzwiller projected fermionic states with a spin Jastrow factor is considered to describe either spin liquids [with U(1)U(1)U(1) or Z2{Z}_{2}Z2​ symmetry] or magnetically ordered phases [with q=(0,0)\mathbf{q}=(0,0)q=(0,0) or $\mathbf{q}=(4\ensuremath{\pi}/3,0)$]. We find that the magnetic states are not stable in the thermodynamic limit. Moreover, there is no energy gain to break the gauge symmetry from U(1)U(1)U(1) to Z2{Z}_{2}Z2​ within the spin-liquid states, as previously found in the Heisenberg model. The best variational wave function is therefore the U(1)U(1)U(1) Dirac state, supplemented by the spin Jastrow factor. Furthermore, a vanishing S=2S=2S=2 spin gap is obtained at the variational level, in the whole regime from the XYXYXY to the Heisenberg model.
It is widely believed that the U(1)U(1)U(1) spin liquid with a large spinon Fermi surface (SFS state) can be realized in the spin-$\frac{1}{2}\phantom{\rule{4pt}{0ex}}{J}_{1}\text{\ensuremath{-}}{J}_{4}$ model on the triangular lattice, when the ring exchange coupling J4{J}_{4}J4​ is sufficiently strong to suppress the ${120}^{\ensuremath{\circ}}$ magnetic ordered state. This belief is supported by many variational studies on this model and seems to be consistent with the observations on the organic spin liquid materials such as $\ensuremath{\kappa}$-(BEDT-TTF)2Cu2(CN)3{\mathrm{TTF})}_{2}{\mathrm{Cu}}_{2}{(\mathrm{CN})}_{3}TTF)2​Cu2​(CN)3​ and EtMe3Sb[Pd(dmit)2]2{\mathrm{EtMe}}_{3}\mathrm{Sb}{[\mathrm{Pd}{(\mathrm{dmit})}_{2}]}_{2}EtMe3​Sb[Pd(dmit)2​]2​, which are systems close to their Mott transition and thus have large J4{J}_{4}J4​. Here we show through systematic variational search that such a state is never favored in the ${J}_{1}\text{\ensuremath{-}}{J}_{4}$ model on the triangular lattice. Instead, a state with broken spatial symmetry is favored in the most probable parameter regime for the SFS state and has an energy much lower than that of the SFS state and other proposed variational states. More specifically, we find that for ${J}_{4}\ensuremath{\ge}0.09{J}_{1}$, the model favors a valence bond solid state with a $4\ifmmode\times\else\texttimes\fi{}6$ period in its local spin correlation pattern and has a variational energy that is about 55%5 lower than that of the SFS state. This state is separated from the $\ensuremath{\pi}$-flux state for ${J}_{4}\ensuremath{\le}0.045{J}_{1}$ by an intermediate symmetry-breaking phase with a zigzag pattern in its local spin correlation. We find that the variational phase diagram we got is in qualitative agreement with that obtained from exact diagonalization on a $6\ifmmode\times\else\texttimes\fi{}6$ cluster.
Experimental quest for the hypothetical "quantum spin liquid" state has recently met a few promising candidate materials including organic salts κ-(ET)2Cu2(CN)3 and EtMe3Sb[Pd(dmit)2]2, S=1/2 triangular-lattice Heisenberg antiferromagnets consisting of molecular dimers. These compounds exhibit no magnetic ordering nor the spin freezing down to very low temperature, while various physical quantities exhibit gapless behaviors. Recent dielectric measurements revealed the glassy dielectric response suggesting the random freezing of the electric polarization degrees of freedom. Inspired by this observation, we propose as a minimal model of the observed quantum spin-liquid behavior the S=1/2 antiferromagnetic Heisenberg on the triangular lattice with a quenched randomness in the exchange interaction. We study both zero- and finite-temperature properties of the model by an exact diagonalization method, to find that when the randomness exceeds a critical value the model exhibits a quantum spin-liquid ground state. This randomness-induced quantum spin-liquid state exhibits gapless behaviors including the temperature-linear specific heat. The results provide a consistent explanation of the recent experimental observations on organic salts.