We present time-of-flight neutron total scattering and polarized neutron scattering measurements of the magnetically frustrated compounds NaCaCo$_2$F$_7$ and NaSrCo$_2$F$_7$, which belong to a class of recently discovered pyrochlore compounds based o
n transition metals and fluorine. The magnetic pair distribution function (mPDF) technique is used to analyze and model the total scattering data in real space. We find that a previously-proposed model of short-range XY-like correlations with a length scale of 10-15 AA, combined with nearest-neighbor collinear antiferromagnetic correlations, accurately describes the mPDF data at low temperature, confirming the magnetic ground state in these materials. This model is further verified by the polarized neutron scattering data. From an analysis of the temperature dependence of the mPDF and polarized neutron scattering data, we find that short-range correlations persist on the nearest-neighbor length scale up to 200 K, approximately two orders of magnitude higher than the spin freezing temperatures of these compounds. These results highlight the opportunity presented by these new pyrochlore compounds to study the effects of geometric frustration at relatively high temperatures, while also advancing the mPDF technique and providing a novel opportunity to investigate a genuinely short-range-ordered magnetic ground state directly in real space.
Fe3PO4O3 forms a non-centrosymmetric lattice structure (space group R3m) comprising triangular motifs of Fe^{3+} coupled by strong antiferromagnetic interactions (|Theta_{CW}| > 900 K). Neutron diffraction from polycrystalline samples shows that stro
ng frustration eventually gives way to an ordered helical incommensurate structure below T_N = 163 K, with the helical axis in the hexagonal ab plane and a modulation length of ~ 86 AA. The magnetic structure consists of an unusual needle-like correlation volume that extends past 900 AA along the hexagonal c-axis but is limited to ~ 70 AA in the ab plane, despite the three-dimensional nature of the magnetic sublattice topology. The small in-plane correlation length, which persists to at least T = T_N/40, indicates a robust blocking of long-range order of the helical magnetic structure, and therefore stable domain walls, or other defect spin textures, must be abundant in Fe3PO7. Temperature dependent neutron powder diffraction reveals small negative thermal expansion below T_N. No change in lattice symmetry is observed on cooling through T_N, as revealed by high resolution synchrotron X-ray diffraction. The previously reported reduced moment of the Fe^{3+} ions (S=5/2), mu ~ 4.2 mu_B, is confirmed here through magnetization studies of a magnetically diluted solid solution series of compounds, Fe3-xGaxPO4O3, and is consistent with the refined magnetic moment from neutron diffraction 4.14(2) mu_B. We attribute the reduced moment to a modified spin density distribution arising from ligand charge transfer in this insulating oxide.
A single crystal of the Co2+ based pyrochlore NaCaCo2F7 was studied by inelastic neutron scattering. This frustrated magnet with quenched exchange disorder remains in a strongly correlated paramagnetic state down to one 60th of the Curie-Weiss temper
ature. Below T_f = 2.4 K, diffuse elastic scattering develops and comprises 30 +/- 10% of the total magnetic scattering, as expected for J_{eff} = 1/2 moments frozen on a time scale that exceeds hbar/delta E=3.8 ps. The diffuse scattering is consistent with short range XY antiferromagnetism with a correlation length of 16 AA. The momentum (Q) dependence of the inelastic intensity indicates relaxing XY-like antiferromagnetic clusters at energies below ~ 5.5 meV, and collinear antiferromagnetic fluctuations above this energy. The relevant XY configurations form a continuous manifold of symmetry-related states. Contrary to well-known models that produce this continuous manifold, order-by-disorder does not select an ordered state in NaCaCo2F7 despite evidence for weak (~12 %) exchange disorder. Instead, NaCaCo2F7 freezes into short range ordered clusters that span this manifold.
An important and continuing theme of modern solid state physics is the realization of exotic excitations in materials (e.g. quasiparticles) that have no analogy (or have not yet been observed) in the actual physical vacuum of free space. Although the
y are not fundamental particles, such quasiparticles do constitute the most basic description of the excited states of the vacuum in which they reside. In this regard the magnetic textures of the excited states of spin ices, magnetic pyrochlore oxides with dominant Ising interactions, are proposed to be modeled as effective magnetic charge monopoles. Recent inelastic neutron scattering experiments have established the pyrochlore material Yb$_2$Ti$_2$O$_7$ (YbTO) as a quantum spin ice, where in addition to the Ising interactions there are substantial transverse terms that may induce quantum dynamics and - in principle - coherent monopole motion. Here we report a combined time domain terahertz spectroscopy (TDTS) and microwave cavity study of YbTO to probe its complex dynamic magnetic susceptibility. We find that the form of the susceptibility is consistent with monopole motion and a magnetic monopole conductivity can be defined and measured. Using the unique phase sensitive capabilities of these techniques, we observe a sign change in the reactive part of the magnetic response. In generic models of monopole motion this is only possible through introducing inertial effects, e.g. a mass dependent term, to the equations of motion. Analogous to conventional electric charge systems, measurement of the conductivitys spectral weight allows us to derive a value for the magnetic monopole mass, which we find to be approximately 1800 electron masses. Our results establish the magnetic monopoles of quantum spin ice as true coherently propagating quasiparticles of this system.
Here we establish the systematic existence of a U(1) degeneracy of all symmetry-allowed Hamiltonians quadratic in the spins on the pyrochlore lattice, at the mean-field level. By extracting the Hamiltonian of Er2Ti2O7 from inelastic neutron scatterin
g measurements, we then show that the U(1)-degenerate states of Er2Ti2O7 are its classical ground states, and unambiguously show that quantum fluctuations break the degeneracy in a way which is confirmed by experiment. This is the first definitive observation of order-by-disorder in any material. We provide further verifiable consequences of this phenomenon, and several additional comparisons between theory and experiment.
We have developed an application of a one-dimensional micro-strip detector for capturing x-ray diffraction data in pulsed magnetic fields. This detector consists of a large array of 50 mu m-wide Si strips with a full-frame read out at 20 kHz. Its use
substantially improves data-collection efficiency and quality as compared to point detectors, because diffraction signals are recorded along an arc in reciprocal space in a time-resolved manner. By synchronizing with pulsed fields, the entire field dependence of a two-dimensional swath of reciprocal space may be determined using a small number of field pulses.
Recent work has highlighted remarkable effects of classical thermal fluctuations in the dipolar spin ice compounds, such as artificial magnetostatics, manifesting as Coulombic power-law spin correlations and particles behaving as diffusive magnetic m
onopoles. In this paper, we address quantum spin ice, giving a unifying framework for the study of magnetism of a large class of magnetic compounds with the pyrochlore structure, and in particular discuss Yb2Ti2O7 and extract its full set of Hamiltonian parameters from high field inelastic neutron scattering experiments. We show that fluctuations in Yb2Ti2O7 are strong, and that the Hamiltonian may support a Coulombic Quantum Spin Liquid ground state in low field and host an unusual quantum critical point at larger fields. This appears consistent with puzzling features in prior experiments on Yb2Ti2O7. Thus Yb2Ti2O7 is the first quantum spin liquid candidate in which the Hamiltonian is quantitatively known.
