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The pyrochlore material Nd_{2}Zr_{2}O_{7} with an "all-in-all-out" (AIAO) magnetic order shows novel quantum moment fragmentation with gapped flat dynamical spin ice modes. The parametrized spin Hamiltonian with a dominant frustrated ferromagnetic transverse term reveals a proximity to a U(1) spin liquid. Here we study the magnetic excitations of Nd_{2}Zr_{2}O_{7} above the ordering temperature (T_{N}) using high-energy-resolution inelastic neutron scattering. We find strong spin ice correlations at zero energy with the disappearance of gapped magnon excitations of the AIAO order. It seems that the gap to the dynamical spin ice closes above T_{N} and the system enters a quantum spin ice state competing with and suppressing the AIAO order. Classical Monte Carlo simulations, molecular dynamics, and quantum boson calculations support the existence of a Coulombic phase above T_{N}. Our findings relate the magnetic ordering of Nd_{2}Zr_{2}O_{7} with the Higgs mechanism and provide explanations for several previously reported experimental features.
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The frustrated pyrochlore magnet Yb_{2}Ti_{2}O_{7} has the remarkable property that it orders magnetically but has no propagating magnons over wide regions of the Brillouin zone. Here we use inelastic neutron scattering to follow how the spectrum evolves in cubic-axis magnetic fields. At high fields we observe, in addition to dispersive magnons, a two-magnon continuum, which grows in intensity upon reducing the field and overlaps with the one-magnon states at intermediate fields leading to strong renormalization of the dispersion relations, and magnon decays. Using heat capacity measurements we find that the low- and high-field regions are smoothly connected with no sharp phase transition, with the spin gap increasing monotonically in field. Through fits to an extensive data set of dispersion relations combined with magnetization measurements, we reevaluate the spin Hamiltonian, finding dominant quantum exchange terms, which we propose are responsible for the anomalously strong fluctuations and quasiparticle breakdown effects observed at low fields.
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The spinel FeSc_{2}S_{4} has been proposed to realize a near-critical spin-orbital singlet (SOS) state, where entangled spin and orbital moments fluctuate in a global singlet state on the verge of spin and orbital order. Here we report powder inelastic neutron scattering measurements that observe the full bandwidth of magnetic excitations and we find that spin-orbital triplon excitations of an SOS state can capture well key aspects of the spectrum in both zero and applied magnetic fields up to 8.5 T. The observed shift of low-energy spectral weight to higher energies upon increasing applied field is naturally explained by the entangled spin-orbital character of the magnetic states, a behavior that is in strong contrast to spin-only singlet ground state systems, where the spin gap decreases upon increasing applied field.
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The discovery of magnetic bistability in Mn_{12} more than 20 years ago marked the birth of molecular magnetism, an extremely fertile interdisciplinary field and a powerful route to create tailored magnetic nanostructures. However, the difficulty to determine interactions in complex polycentric molecules often prevents their understanding. Mn_{12} is an outstanding example of this difficulty: although it is the forefather and most studied of all molecular nanomagnets, an unambiguous determination of even the leading magnetic exchange interactions is still lacking. Here we exploit four-dimensional inelastic neutron scattering to portray how individual spins fluctuate around the magnetic ground state, thus fixing the exchange couplings of Mn_{12} for the first time. Our results demonstrate the power of four-dimensional inelastic neutron scattering as an unrivaled tool to characterize magnetic clusters.
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The low-temperature thermal and transport properties of an unusual kind of crystal exhibiting minimal molecular positional and tilting disorder have been measured. The material, namely, low-dimensional, highly anisotropic pentachloronitrobenzene has a layered structure of rhombohedral parallel planes in which the molecules execute large-amplitude in-plane as well as concurrent out-of-plane librational motions. Our study reveals that low-temperature glassy anomalies can be found in a system with minimal disorder due to the freezing of (mostly in-plane) reorientational jumps of molecules between equivalent crystallographic positions with partial site occupation. Our findings will pave the way to a deeper understanding of the origin of the above-mentioned universal glassy properties at low temperature.
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The challenge of one-dimensional systems is to understand their physics beyond the level of known elementary excitations. By high-resolution neutron spectroscopy in a quantum spin-ladder material, we probe the leading multiparticle excitation by characterizing the two-magnon bound state at zero field. By applying high magnetic fields, we create and select the singlet (longitudinal) and triplet (transverse) excitations of the fully spin-polarized ladder, which have not been observed previously and are close analogs of the modes anticipated in a polarized Haldane chain. Theoretical modeling of the dynamical response demonstrates our complete quantitative understanding of these states.
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The conduction electrons in a metal experience competing interactions with each other and the atomic nuclei. This competition can lead to many types of magnetic order in metals. For example, in chromium the electrons order to form a spin-density-wave (SDW) antiferromagnetic state. A magnetic field may be used to perturb or tune materials with delicately balanced electronic interactions. Here, we show that the application of a magnetic field can induce SDW magnetic order in a quasi-2D metamagnetic metal, where none exists in the absence of the field. We use magnetic neutron scattering to show that the application of a large (B ≈ 8 T) magnetic field to the perovskite metal Sr3Ru2O7 (refs 3-7) can be used to tune the material through two magnetically ordered SDW states. The ordered states exist over relatively small ranges in field (â²0.4 T), suggesting that their origin is due to a new mechanism related to the electronic fine structure near the Fermi energy, possibly combined with the stabilizing effect of magnetic fluctuations. The magnetic field direction is shown to control the SDW domain populations, which naturally explains the strong resistivity anisotropy or 'electronic nematic' behaviour observed in this material.
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Properties of the depleted Heisenberg spin ladder material series (C_{7}H_{10}N)_{2}Cu_{1-z}Zn_{z}Br_{4} have been studied by the combination of magnetic measurements and neutron spectroscopy. Disorder-induced degrees of freedom lead to a specific magnetic response, described in terms of emergent strongly interacting "spin island" objects. The structure and dynamics of the spin islands is studied by high-resolution inelastic neutron scattering. This allows us to determine their spatial shape and to observe their mutual interactions, manifested by strong spectral in-gap contributions.
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We find evidence for long-range and short-range (ζ=70 Å at 4 K) incommensurate magnetic order on the quasi-face-centered-cubic (fcc) lattices of the monoclinic double perovskites La2NaRuO6 and La2NaOsO6, respectively. Incommensurate magnetic order on the fcc lattice has not been predicted by mean field theory, but may arise via a delicate balance of inequivalent nearest neighbor and next nearest neighbor exchange interactions. In the Ru system with long-range order, inelastic neutron scattering also reveals a spin gap Δ â¼ 2.75 meV. Magnetic anisotropy is generally minimized in the more familiar octahedrally coordinated 3d3 systems, so the large gap observed for La2NaRuO6 may result from the significantly enhanced value of spin-orbit coupling in this 4d(3) material.
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A new family of superconductors containing layers of iron arsenide has attracted considerable interest because of their high transition temperatures (T(c)), some of which are >50 K, and because of similarities with the high-T(c) copper oxide superconductors. In both the iron arsenides and the copper oxides, superconductivity arises when an antiferromagnetically ordered phase has been suppressed by chemical doping. A universal feature of the copper oxide superconductors is the existence of a resonant magnetic excitation, localized in both energy and wavevector, within the superconducting phase. This resonance, which has also been observed in several heavy-fermion superconductors, is predicted to occur when the sign of the superconducting energy gap takes opposite values on different parts of the Fermi surface, an unusual gap symmetry which implies that the electron pairing interaction is repulsive at short range. Angle-resolved photoelectron spectroscopy shows no evidence of gap anisotropy in the iron arsenides, but such measurements are insensitive to the phase of the gap on separate parts of the Fermi surface. Here we report inelastic neutron scattering observations of a magnetic resonance below T(c) in Ba(0.6)K(0.4)Fe(2)As(2), a phase-sensitive measurement demonstrating that the superconducting energy gap has unconventional symmetry in the iron arsenide superconductors.
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Inelastic neutron scattering is used to measure the spin excitation spectrum of the Heisenberg S=1/2 ladder material (C7H10N)2CuBr4 in its entirety, both in the gapped spin liquid and the magnetic field-induced Tomonaga-Luttinger spin liquid regimes. A fundamental change of the spin dynamics is observed between these two regimes. Density matrix renormalization group calculations quantitatively reproduce and help understand the observed commensurate and incommensurate excitations. The results validate long-standing quantum field-theoretical predictions but also test the limits of that approach.
Asunto(s)
Campos Magnéticos , Teoría Cuántica , Alcanos/química , Bromuros/química , Cobre/químicaRESUMEN
High degeneracy in ground states leads to the generation of exotic zero-energy modes, a representative example of which is the formation of molecular spin-liquid-like fluctuations in a frustrated magnet. Here we present single-crystal inelastic neutron scattering results for the frustrated magnet MgCr(2)O(4), which show that a common set of finite-energy molecular spin excitation modes is sustained in both the liquid-like phase above magnetic ordering temperature T(N) and an ordered phase with an extremely complex magnetic structure below T(N). Based on this finding, we propose the concept of high degeneracy in excited states, which promotes local resonant elementary excitations. This concept is expected to have ramifications on our understanding of excitations in many complex systems, including not only spin but also atomic liquids, complex order systems, and amorphous systems.
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In this Letter, we explore the phase diagram and excitations of a distorted triangular lattice antiferromagnet. The unique two-dimensional distortion considered here is very different from the "isosceles"-type distortion that has been extensively investigated. We show that it is able to stabilize a 120° spin structure for a large range of exchange interaction values, while new structures are found for extreme distortions. A physical realization of this model is α-CaCr(2)O(4), which has a 120° structure but lies very close to the phase boundary. This is verified by inelastic neutron scattering which reveals unusual rotonlike minima at reciprocal space points different from those corresponding to the magnetic order.
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Using the inelastic neutron scattering technique, we measured the spin wave dispersion over the entire Brillouin zone of room temperature multiferroic BiFeO(3) single crystals with magnetic excitations extending to as high as 72.5 meV. The full spin waves can be explained by a simple Heisenberg Hamiltonian with a nearest-neighbor exchange interaction (J=4.38 meV), a next-nearest-neighbor exchange interaction (J'=0.15 meV), and a Dzyaloshinskii-Moriya-like term (D=0.107 meV). This simple Hamiltonian determined, for the first time, for BiFeO(3) provides a fundamental ingredient for understanding the novel magnetic properties of BiFeO(3).
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We report inelastic neutron scattering measurements of the resonant spin excitations in Ba(1-x)K(x)Fe(2)As(2) over a broad range of electron band filling. The fall in the superconducting transition temperature with hole doping coincides with the magnetic excitations splitting into two incommensurate peaks because of the growing mismatch in the hole and electron Fermi surface volumes, as confirmed by a tight-binding model with s(±)-symmetry pairing. The reduction in Fermi surface nesting is accompanied by a collapse of the resonance binding energy and its spectral weight, caused by the weakening of electron-electron correlations.
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When the transition temperature of a continuous phase transition is tuned to absolute zero, new ordered phases and physical behaviour emerge in the vicinity of the resulting quantum critical point. Sr3Ru2O7 can be tuned through quantum criticality with magnetic field at low temperature. Near its critical field Bc it displays the hallmark T-linear resistivity and a [Formula: see text] electronic heat capacity behaviour of strange metals. However, these behaviours have not been related to any critical fluctuations. Here we use inelastic neutron scattering to reveal the presence of collective spin fluctuations whose relaxation time and strength show a nearly singular variation with magnetic field as Bc is approached. The large increase in the electronic heat capacity and entropy near Bc can be understood quantitatively in terms of the scattering of conduction electrons by these spin-fluctuations. On entering the spin-density-wave ordered phase present near Bc, the fluctuations become stronger suggesting that the order is stabilised through an "order-by-disorder" mechanism.
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A thorough crystal structure determination at very low temperature of (CuCl)LaNb2O7, originally proposed as a spin-1/2 square-lattice antiferromagnet, is reported thanks to the use of single-crystal x-ray diffraction and powder neutron diffraction. State-of-the-art calculations (maximum entropy method) reveal that (CuCl)LaNb2O7 is orthorhombic with Pbam symmetry. First-principles calculations demonstrate that the dominant magnetic interactions are antiferromagnetic between fourth nearest neighbors with a Cu-Cl-Cl-Cu exchange path, which lead to the formation of spin singlets. The two strongest interactions between the singlets are ferromagnetic, which makes (CuCl)LaNb2O7 the first system of ferromagnetically coupled Shastry-Sutherland quantum spin singlets.
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Phonons are the main source of relaxation in molecular nanomagnets, and different mechanisms have been proposed in order to explain the wealth of experimental findings. However, very limited experimental investigations on phonons in these systems have been performed so far, yielding no information about their dispersions. Here we exploit state-of-the-art single-crystal inelastic neutron scattering to directly measure for the first time phonon dispersions in a prototypical molecular qubit. Both acoustic and optical branches are detected in crystals of [VO(acac)[Formula: see text]] along different directions in the reciprocal space. Using energies and polarisation vectors calculated with state-of-the-art Density Functional Theory, we reproduce important qualitative features of [VO(acac)[Formula: see text]] phonon modes, such as the presence of low-lying optical branches. Moreover, we evidence phonon anti-crossings involving acoustic and optical branches, yielding significant transfers of the spin-phonon coupling strength between the different modes.
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The organic-inorganic lead-halide perovskites are composed of organic molecules imbedded in an inorganic framework. The compounds with general formula CH3NH3PbX 3 (MAPbX 3) display large photovoltaic efficiencies for halogens X = Cl, Br, and I in a wide variety of sample geometries and preparation methods. The organic cation and inorganic framework are bound by hydrogen bonds that tether the molecules to the halide anions, and this has been suggested to be important to the optoelectronic properties. We have studied the effects of this bonding using time-of-flight neutron spectroscopy to measure the molecular dynamics in CH3NH3PbCl3 (MAPbCl3). Low-energy/high-resolution neutron backscattering reveals thermally activated molecular dynamics with a characteristic temperature of ~95 K. At this same temperature, higher-energy neutron spectroscopy indicates the presence of an anomalous broadening in energy (reduced lifetime) associated with the molecular vibrations. By contrast, neutron powder diffraction shows that a spatially long-range structural phase transitions occurs at 178 K (cubic â tetragonal) and 173 K (tetragonal â orthorhombic). The large difference between these two temperature scales suggests that the molecular and inorganic lattice dynamics in MAPbCl3 are actually decoupled. With the assumption that underlying physical mechanisms do not change with differing halogens in the organic-inorganic perovskites, we speculate that the energy scale most relevant to the photovoltaic properties of the lead-halogen perovskites is set by the lead-halide bond, not by the hydrogen bond.
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Signatures of absence of a long-range ordered magnetic ground state down to 0.36 K are observed in magnetic susceptibility, specific heat, thermal/electrical transport and inelastic neutron scattering data of the quasi-skutterudite compound Pr3Rh4Sn13 which crystallizes in the Yb3Rh4Sn13-type structure with a cage-like network of Sn atoms. In this structure, Pr3+ occupies a lattice site with D 2d point symmetry having a ninefold degeneracy corresponding to J = 4. The magnetic susceptibility of Pr3Rh4Sn13 shows only a weak temperature dependence below 10 K; otherwise remaining paramagnetic-like in the range, 10 K-300 K. From the inelastic neutron scattering intensity of Pr3Rh4Sn13 recorded at different temperatures, we identify excitations at 4.5(7) K, 5.42(6) K, 10.77(5) K, 27.27(5) K, 192.28(4) K and 308.33(3) K through a careful peak analysis. However, no signatures of long-range magnetic order are observed in the neutron data down to 1.5 K, which is also confirmed by the specific heat data down to 0.36 K. A broad Schottky-like peak is recovered for the magnetic part of the specific heat, C 4f, which suggests the role of crystal electric fields of Pr3+ . A crystalline electric field model consisting of 7 levels was applied to C 4f which leads to the estimation of energy levels at 4.48(2) K, 6.94(4) K, 11.23(8) K, 27.01(5) K, 193.12(6) K and 367.30(2) K. The CEF energy levels estimated from the heat capacity analysis are in close agreement with the excitation energies seen in the neutron data. The Sommerfeld coefficient estimated from the analysis of magnetic specific heat is [Formula: see text] mJ K-2 mol-Pr which suggests the formation of heavy itinerant quasi-particles in Pr3Rh4Sn13. Combining inelastic neutron scattering results, analysis of the specific heat data down to 0.36 K, magnetic susceptibility and, electrical and thermal transport, we establish the absence of long-range ordered magnetic ground state in Pr3Rh4Sn13.