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Register a new userRearrangement of uncorrelated valence bonds evidenced by low-energy spin excitations in YbMgGaO4
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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.
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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.
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.
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.
The dynamics of S=1/2 quantum spins on a 2D square lattice lie at the heart of the mystery of the cuprates cite{Hayden2004,Vignolle2007,Li2010,LeTacon2011,Coldea2001,Headings2010,Braicovich2010}. In bulk cuprates such as LCO{}, the presence of a weak interlayer coupling stabilizes 3D N{e}el order up to high temperatures. In a truly 2D system however, thermal spin fluctuations melt long range order at any finite temperature cite{Mermin1966}. Further, quantum spin fluctuations transfer magnetic spectral weight out of a well-defined magnon excitation into a magnetic continuum, the nature of which remains controversial cite{Sandvik2001,Ho2001,Christensen2007,Headings2010}. Here, we measure the spin response of emph{isolated one-unit-cell thick layers} of LCO{}. We show that coherent magnons persist even in a single layer of LCO{} despite the loss of magnetic order, with no evidence for resonating valence bond (RVB)-like spin correlations cite{Anderson1987,Hsu1990,Christensen2007}. Thus these excitations are well described by linear spin wave theory (LSWT). We also observe a high-energy magnetic continuum in the isotropic magnetic response. This high-energy continuum is not well described by 2 magnon LSWT, or indeed any existing theories.
In strongly-correlated systems the electronic properties at the Fermi energy (EF) are intertwined with those at high energy scales. One of the pivotal challenges in the field of high-temperature superconductivity (HTSC) is to understand whether and how the high energy scale physics associated with Mott-like excitations (|E-E$_{F}$|>1 eV) is involved in the condensate formation. Here we show the interplay between the many-body high-energy CuO2 excitations at 1.5 and 2 eV and the onset of HTSC. This is revealed by a novel optical pump supercontinuum-probe technique, which provides access to the dynamics of the dielectric function in Bi$_2$Sr$_2$Ca$_{0.92}$Y$_{0.08}$Cu$_2$O$_{8+{delta}}$ over an extended energy range, after the photoinduced suppression of the superconducting pairing. These results unveil an unconventional mechanism at the base of HTSC both below and above the optimal hole concentration required to attain the maximum critical temperature (T$_c$).
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