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Valence Bonds in Random Quantum Magnets: Theory and Application to YbMgGaO4

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 Added by Itamar Kimchi
 Publication date 2017
  fields Physics
and research's language is English




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We analyze the effect of quenched disorder on spin-1/2 quantum magnets in which magnetic frustration promotes the formation of local singlets. Our results include a theory for 2d valence-bond solids subject to weak bond randomness, as well as extensions to stronger disorder regimes where we make connections with quantum spin liquids. We find, on various lattices, that the destruction of a valence-bond solid phase by weak quenched disorder leads inevitably to the nucleation of topological defects carrying spin-1/2 moments. This renormalizes the lattice into a strongly random spin network with interesting low-energy excitations. Similarly when short-ranged valence bonds would be pinned by stronger disorder, we find that this putative glass is unstable to defects that carry spin-1/2 magnetic moments, and whose residual interactions decide the ultimate low energy fate. Motivated by these results we conjecture Lieb-Schultz-Mattis-like restrictions on ground states for disordered magnets with spin-1/2 per statistical unit cell. These conjectures are supported by an argument for 1d spin chains. We apply insights from this study to the phenomenology of YbMgGaO$_4$, a recently discovered triangular lattice spin-1/2 insulator which was proposed to be a quantum spin liquid. We instead explore a description based on the present theory. Experimental signatures, including unusual specific heat, thermal conductivity, and dynamical structure factor, and their behavior in a magnetic field, are predicted from the theory, and compare favorably with existing measurements on YbMgGaO$_4$ and related materials.



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Since its proposal by Anderson, resonating valence bonds (RVB) formed by a superposition of fluctuating singlet pairs have been a paradigmatic concept in understanding quantum spin liquids (QSL). Here, we show that excitations related to singlet breaking on nearest-neighbor bonds describe the high-energy part of the excitation spectrum in YbMgGaO4, the effective spin-1/2 frustrated antiferromagnet on the triangular lattice, as originally considered by Anderson. By a thorough single-crystal inelastic neutron scattering (INS) study, we demonstrate that nearest-neighbor RVB excitations account for the bulk of the spectral weight above 0.5 meV. This renders YbMgGaO4 the first experimental system where putative RVB correlations restricted to nearest neighbors are observed, and poses a fundamental question of how complex interactions on the triangular lattice conspire to form this unique many-body state.
DC-magnetization data measured down to 40 mK speak against conventional freezing and reinstate YbMgGaO$_4$ as a triangular spin-liquid candidate. Magnetic susceptibility measured parallel and perpendicular to the $c$-axis reaches constant values below 0.1 and 0.2 K, respectively, thus indicating the presence of gapless low-energy spin excitations. We elucidate their nature in the triple-axis inelastic neutron scattering experiment that pinpoints the low-energy ($E$ $leq$ $J_0$ $sim$ 0.2 meV) part of the excitation continuum present at low temperatures ($T$ $<$ $J_0$/$k_B$), but emph{completely} disappearing upon warming the system above $T$ $gg$ $J_0$/$k_B$. In contrast to the high-energy part at $E$ $>$ $J_0$ that is rooted in the breaking of nearest-neighbor valence bonds and persists to temperatures well above $J_0$/$k_B$, the low-energy one originates from the rearrangement of the valence bonds and thus from the propagation of unpaired spins. We further extend this picture to herbertsmithite, the spin-liquid candidate on the kagome lattice, and argue that such a hierarchy of magnetic excitations may be a universal feature of quantum spin liquids.
We present a large-N variational approach to describe the magnetism of insulating doped semiconductors based on a disorder-generalization of the resonating-valence-bond theory for quantum antiferromagnets. This method captures all the qualitative and even quantitative predictions of the strong-disorder renormalization group approach over the entire experimentally relevant temperature range. Finally, by mapping the problem on a hard-sphere fluid, we could provide an essentially exact analytic solution without any adjustable parameters.
The Kagome Heisenberg antiferromagnet is mapped onto an effective Hamiltonian on the star superlattice by Contractor Renormalization. Comparison of ground state energies on large lattices to Density Matrix Renormalization Group justifies truncation of effective interactions at range 3. Within our accuracy, magnetic and translational symmetries are not broken (i.e. a spin liquid ground state). However, we discover doublet spectral degeneracies which signal the onset of p6 - chirality symmetry breaking. This is understood by simple mean field analysis. Experimentally, the p6 chiral order parameter should split the optical phonons degeneracy near the zone center. Addition of weak next to nearest neighbor coupling is discussed.
Hard-spin mean-field theory has recently been applied to Ising magnets, correctly yielding the absence and presence of an interface roughening transition respectively in $d=2$ and $d=3$ dimensions and producing the ordering-roughening phase diagram for isotropic and anisotropic systems. The approach has now been extended to the effects of quenched random pinning centers and missing bonds on the interface of isotropic and anisotropic Ising models in $d=3$. We find that these frozen impurities cause domain boundary roughening that exhibits consecutive thresholding transitions as a function interaction of anisotropy. For both missing-bond and pinning-center impurities, for moderately large values the anisotropy, the systems saturate to the solid-on-solid limit, exhibiting a single universal curve for the domain boundary width as a function of impurity concentration.
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