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B. Lake

Publications and source records attributed to B. Lake.

At least 55 records · Page 3Linked to original sources

Magnetic excitations in the S = 1/2 antiferromagnetic-ferromagnetic chain compound BaCu2V2O8 at zero and finite temperature

Unlike most quantum systems which rapidly become incoherent as temperature is raised, strong correlations persist at elevated temperatures in $S=1/2$ dimer magnets, as revealed by the unusual asymmetric lineshape of their excitations at finite temperatures. Here we quantitatively explore and parameterize the strongly correlated magnetic excitations at finite temperatures using the high resolution inelastic neutron scattering on the model compound BaCu$_2$V$_2$O$_8$ which we show to be an alternating antiferromagnetic-ferromagnetic spin$-1/2$ chain. Comparison to state of the art computational techniques shows excellent agreement over a wide temperature range. Our findings hence demonstrate the possibility to quantitatively predict coherent behavior at elevated temperatures in quantum magnets.

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Investigation of the magnetic structure and crystal field states of pyrochlore antiferromagnet Nd2Zr2O7

We present synchrotron x-ray diffraction, neutron powder diffraction and time-of-flight inelastic neutron scattering measurements on the rare earth pyrochlore oxide Nd2Zr2O7 to study the ordered state magnetic structure and cystal field states. The structural characterization by high-resolution synchrotron x-ray diffraction confirms that the pyrochlore structure has no detectable O vacancies or Nd/Zr site mixing. The neutron diffraction reveals long range all-in/all-out antiferromagnetic order below T_N ~ 0.4 K with propagation vector k = (0 0 0) and an ordered moment of 1.26(2) μ_B/Nd at 0.1 K. The ordered moment is much smaller than the estimated moment of 2.65 μ_B/Nd for the local <111> Ising ground state of Nd3+ (J=9/2) suggesting that the ordering is partially suppressed by quantum fluctuations. The strong Ising anisotropy is further confirmed by the inelastic neutron scattering data which reveals a well-isolated dipolar-octupolar type Kramers doublet ground state. The crystal field level scheme and ground state wavefunction have been determined.

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Observation of long range magnetic ordering in pyrohafnate Nd2Hf2O7: A neutron diffraction study

We have investigated the physical properties of a pyrochlore hafnate Nd2Hf2O7 using ac magnetic susceptibility χ_ac(T), dc magnetic susceptibility χ(T), isothermal magnetization M(H) and heat capacity C_p(T) measurements, and determined the magnetic ground state by neutron powder diffraction study. An upturn is observed below 6 K in C_p(T)/T, however both C_p(T) and χ(T) do not show any clear anomaly down to 2 K. The χ_ac(T) shows a well pronounced anomaly indicating an antiferromagnetic transition at T_N = 0.55 K. The long range antiferromagnetic ordering is confirmed by neutron diffraction. The refinement of neutron diffraction pattern reveals an all-in/all-out antiferromagnetic structure, where for successive tetrahedra, the four Nd3+ magnetic moments point alternatively all-into or all-out-of the tetrahedron, with an ordering wavevector k = (0, 0, 0) and an ordered state magnetic moment of m = 0.62(1) μ_B/Nd at 0.1 K. The ordered moment is strongly reduced reflecting strong quantum fluctuations in ordered state.

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Investigations of the effect of nonmagnetic Ca substitution for magnetic Dy on spin-freezing in Dy2Ti2O7

Physical properties of partially Ca substituted hole-doped Dy2Ti2O7 have been investigated by ac magnetic susceptibility χ_ac(T), dc magnetic susceptibility χ(T), isothermal magnetization M(H) and heat capacity C_p(T) measurements on Dy1.8Ca0.2Ti2O7. The spin-ice system Dy2Ti2O7 exhibits a spin-glass type freezing behavior near 16 K. Our frequency dependent χ_ac(T) data of Dy1.8Ca0.2Ti2O7 show that the spin-freezing behavior is significantly influenced by Ca substitution. The effect of partial nonmagnetic Ca2+ substitution for magnetic Dy3+ is similar to the previous study on nonmagnetic isovalent Y3+ substituted Dy2-xYxTi2O7 (for low levels of dilution), however the suppression of spin-freezing behavior is substantially stronger for Ca than Y. The Cole-Cole plot analysis reveals semicircular character and a single relaxation mode in Dy1.8Ca0.2Ti2O7 as for Dy2Ti2O7. No noticeable change in the insulating behavior of Dy2Ti2O7 results from the holes produced by 10% Ca2+ substitution for Dy3+ ions.

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Spinon Confinement in the One-Dimensional Ising-Like Antiferromagnet SrCo2V2O8

For quasi-one dimensional quantum spin systems theory predicts the occurrence of a confinement of spinon excitation due to interchain couplings. Here we investigate the system SrCo2V2O8, a realization of the weakly-coupled Ising-like XXZ antiferromagnetic chains, by terahertz spectroscopy with and without applied magnetic field. At low temperatures a series of excitations is observed, which split in a Zeeman-like fashion in an applied magnetic field. These magnetic excitations are identified as the theoretically predicted spinon-pair excitations. Using a one dimensional Schrödinger equation with a linear confinement potential imposed by weak interchain couplings, the hierarchy of the confined spinons can be fully described.

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Consequences of critical interchain couplings and anisotropy on a Haldane chain

Effects of interchain couplings and anisotropy on a Haldane chain have been investigated by single crystal inelastic neutron scattering and density functional theory (DFT) calculations on the model compound SrNi$_2$V$_2$O$_8$. Significant effects on low energy excitation spectra are found where the Haldane gap ($Δ_0 \approx 0.41J$; where $J$ is the intrachain exchange interaction) is replaced by three energy minima at different antiferromagnetic zone centers due to the complex interchain couplings. Further, the triplet states are split into two branches by single-ion anisotropy. Quantitative information on the intrachain and interchain interactions as well as on the single-ion anisotropy are obtained from the analyses of the neutron scattering spectra by the random phase approximation (RPA) method. The presence of multiple competing interchain interactions is found from the analysis of the experimental spectra and is also confirmed by the DFT calculations. The interchain interactions are two orders of magnitude weaker than the nearest-neighbour intrachain interaction $J$ = 8.7~meV. The DFT calculations reveal that the dominant intrachain nearest-neighbor interaction occurs via nontrivial extended superexchange pathways Ni--O--V--O--Ni involving the empty $d$ orbital of V ions. The present single crystal study also allows us to correctly position SrNi$_2$V$_2$O$_8$ in the theoretical $D$-$J_{\perp}$ phase diagram [T. Sakai and M. Takahashi, Phys. Rev. B 42, 4537 (1990)] showing where it lies within the spin-liquid phase.

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Linear spin wave theory for single-Q incommensurate magnetic structures

Linear spin wave theory provides the leading term in the calculation of the excitation spectra of long-range ordered magnetic systems as a function of $1/\sqrt{S}$. This term is acquired using the Holstein-Primakoff approximation of the spin operator and valid for small $δS$ fluctuations of the ordered moment. We propose an algorithm that allows magnetic ground states with general moment directions and single-Q incommensurate ordering wave vector using a local coordinate transformation for every spin and a rotating coordinate transformation for the incommensurability. Finally we show, how our model can determine the spin wave spectrum of the magnetic C-site langasites with incommensurate order.

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Magnetic correlations of the quasi-one-dimensional half-integer spin-chain antiferromagnets Sr$M_2$V$_2$O$_8$ ($M$ = Co, Mn)

Magnetic correlations of two iso-structural quasi-one-dimensional (1D) antiferromagnetic spin-chain compounds Sr$M_2$V$_2$O$_8$ ($M$ = Co, Mn) have been investigated by magnetization and powder neutron diffraction. Two different collinear antiferromagnetic (AFM) structures, characterized by the propagation vectors, $k$ = (0 0 1) and $k$ = (0 0 0), have been found below $\sim$ 5.2 K and $\sim$ 42.2 K for the Co- and Mn-compounds, respectively. For the Mn-compound, AFM chains (along the $c$ axis) order ferromagnetically within the $ab$ plane, whereas, for the Co-compound, AFM chains order ferro-/antiferromagnetically along the $a/b$ direction. The critical exponent study confirms that the Co- and Mn-compounds belong to the Ising and Heisenberg universality classes, respectively. For both compounds, short-range spin-spin correlations are present over a wide temperature range above $T_N$. The reduced ordered moments at base temperature (1.5 K) indicate the presence of quantum fluctuations in both compounds due to the quasi-1D magnetic interactions.

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Quantum spin chain as a potential realization of the Nersesyan-Tsvelik model

It is well established that long-range magnetic order is suppressed in magnetic systems whose interactions are low-dimensional. The prototypical example is the S-1/2 Heisenberg antiferromagnetic chain (S-1/2 HAFC) whose ground state is quantum critical. In real S-1/2 HAFC compounds interchain coupling induces long-range magnetic order although with a suppressed ordered moment and reduced Néel temperature compared to the Curie-Weiss temperature. Recently, it was suggested that order can also be suppressed if the interchain interactions are frustrated, as for the Nersesyan-Tsvelik model. Here, we study the new S-1/2 HAFC, (NO)[Cu(NO3)3]. This material shows extreme suppression of order which furthermore is incommensurate revealing the presence of frustration consistent with the Nersesyan-Tsvelik model.

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High-field spectroscopy of singlet-triplet transitions in the spin-dimer systems Sr3Cr2O8 and Ba3Cr2O8

Magnetic excitations in the isostructural spin-dimer systems Sr3Cr2O8 and Ba3Cr2O8 are probed by means of high-field electron spin resonance at sub-terahertz frequencies. Three types of magnetic modes were observed. One mode is gapless and corresponds to transitions within excited states, while two other sets of modes are gapped and correspond to transitions from the ground to the first excited states. The selection rules of the gapped modes are analyzed in terms of a dynamical Dzyaloshinskii-Moriya interaction, suggesting the presence of phonon-assisted effects in the low-temperature spin dynamics of Sr3Cr2O8 and Ba3Cr2O8

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Field Induced Magnetic Ordering and Single-ion Anisotropy in the Quasi-1D Haldane Chain Compound SrNi2V2O8: A Single Crystal investigation

Field-induced magnetic ordering in the Haldane chain compound SrNi$_{2}$V$_{2}$O$_{8}$ and effect of anisotropy have been investigated using single crystals. Static susceptibility, inelastic neutron scattering, high-field magnetization, and low temperature heat-capacity studies confirm a non-magnetic spin-singlet ground state and a gap between the singlet ground state and triplet excited states. The intra-chain exchange interaction is estimated to be $J \sim 8.9{\pm}$0.1 meV. Splitting of the dispersions into two modes with minimum energies 1.57 and 2.58 meV confirms the existence of single-ion anisotropy $D(S^z){^2}$. The value of {\it D} is estimated to be $-0.51{\pm}0.01$ meV and the easy axis is found to be along the crystallographic {\it c}-axis. Field-induced magnetic ordering has been found with two critical fields [$μ_0H_c^{\perp c} = 12.0{\pm}$0.2 T and $μ_0H_c^{\parallel c} = 20.8{\pm}$0.5 T at 4.2 K]. Field-induced three-dimensional magnetic ordering above the critical fields is evident from the heat-capacity, susceptibility, and high-field magnetization study. The Phase diagram in the {\it H-T} plane has been obtained from the high-field magnetization. The observed results are discussed in the light of theoretical predictions as well as earlier experimental reports on Haldane chain compounds.

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Multispinon continua at zero and finite temperature in a near-ideal Heisenberg chain

The space- and time-dependent response of many-body quantum systems is the most informative aspect of their emergent behaviour. The dynamical structure factor, experimentally measurable using neutron scattering, can map this response in wavevector and energy with great detail, allowing theories to be quantitatively tested to high accuracy. Here, we present a comparison between neutron scattering measurements on the one-dimensional spin-1/2 Heisenberg antiferromagnet KCuF3, and recent state-of-the-art theoretical methods based on integrability and density matrix renormalization group simulations. The unprecedented quantitative agreement shows that precise descriptions of strongly correlated states at all distance, time and temperature scales are now possible, and highlights the need to apply these novel techniques to other problems in low-dimensional magnetism.

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Exciton-magnon transitions in the frustrated chromium antiferromagnets CuCrO2, alpha-CaCr2O4, CdCr2O4, and ZnCr2O4

We report on optical transmission spectroscopy of the Cr-based frustrated triangular antiferromagnets CuCrO2 and alpha-CaCr2O4, and the spinels CdCr2O4 and ZnCr2O4 in the near-infrared to visible-light frequency range. We explore the possibility to search for spin correlations far above the magnetic ordering temperature and for anomalies in the magnon lifetime in the magnetically ordered state by probing exciton-magnon sidebands of the spin-forbidden crystal-field transitions of the Cr3+ ions (spin S = 3/2). In CuCrO2 and alpha-CaCr2O4 the appearance of fine structures below T_N is assigned to magnon sidebands by comparison with neutron scattering results. The temperature dependence of the line width of the most intense sidebands in both compounds can be described by an Arrhenius law. For CuCrO2 the sideband associated with the 4A2 -> 2T2 transition can be observed even above T_N. Its line width does not show a kink at the magnetic ordering temperature and can alternatively be described by a Z2 vortex scenario proposed previously for similar materials. The exciton-magnon features in alpha-CaCr2O4 are more complex due to the orthorhombic distortion. While for CdCr2O4 magnon sidebands are identified below T_N and one sideband excitation is found to persist across the magnetic ordering transition, only a weak fine structure related to magnetic ordering has been observed in ZnCr2O4.

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Low-energy magnetic excitations in the quasi-one-dimensional spin-1 chain compound SrNi2V2O8

Multi-frequency electron spin resonance (ESR) transmission spectra have been measured as function of temperature and magnetic field on single crystals of the quasi-one-dimensional spin-1 chain compound SrNi2V2O8 in the GHz frequency range. Magnetic resonance modes above 50 K have been observed with an effective g-factor of 2.24 at 100 K. Below 30 K, intra-triplet excitations have been observed in the ESR spectra, which reveal the presence of single-ion anisotropy with D = -0.29 meV.

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Asymmetric Thermal Lineshape Broadening in a Gapped 3-Dimensional Antiferromagnet - Evidence for Strong Correlations at Finite Temperature

It is widely believed that magnetic excitations become increasingly incoherent as temperature is raised due to random collisions which limit their lifetime. This picture is based on spin-wave calculations for gapless magnets in 2 and 3 dimensions and is observed experimentally as a symmetric Lorentzian broadening in energy. Here, we investigate a three-dimensional dimer antiferromagnet and find unexpectedly that the broadening is asymmetric - indicating that far from thermal decoherence, the excitations behave collectively like a strongly correlated gas. This result suggests that a temperature activated coherent state of quasi-particles is not confined to special cases like the highly dimerized spin-1/2 chain but is found generally in dimerized antiferromagnets of all dimensionalities and perhaps gapped magnets in general.

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Orbital fluctuations and orbital order below the Jahn-Teller transition in Sr3Cr2O8

We report on the magnetic and phononic excitation spectrum of Sr3Cr2O8 determined by THz and infrared (IR) spectroscopy, and electron spin resonance (ESR) measurements across the Jahn-Teller transition, which is detected by specific-heat measurements to occur at T_{JT} = 285 K. We identify the singlet-triplet excitations in the dimerized ground state and estimate the exchange couplings in the system. Moreover, ESR absorptions were observed up to T* = 120 K with a linewidth proportional to exp{-Delta/k_{B}T} and Delta/k_{B} = 388 K indicating a phonon-mediated spin relaxation via the excited orbital state of the Cr $e$ doublet in the orbitally ordered state. In contrast to the expected drastic change of the IR active phonons upon entering the low-symmetry Jahn-Teller distorted phase below T_{JT}, we find an extended regime T*<T<T_{JT} where the IR active phonons change only gradually with decreasing temperature. This regime is associated with strong fluctuations in the orbital and lattice degrees of freedom in agreement with the loss of the ESR signal above T*. Using the measured magnetic and phononic excitation spectrum we model the orbital contribution to the specific heat and find the persistence of strong fluctuations far below T_{JT}.

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Magnetic soft modes in the locally distorted triangular antiferromagnet alpha-CaCr2O4

In this paper 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-CaCr2O4 which has 120° structure but lies very close to the phase boundary. This is verified by inelastic neutron scattering which reveals unusual roton-like minima at reciprocal space points different from those corresponding to the magnetic order.

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Magnetic field-induced instability of the cooperative paramagnetic state in Zn$_x$Co$_{4-x}$(OD)$_6$Cl$_2$

Using elastic and inelastic neutron scattering techniques with and without application of an external magnetic field $H$, the magnetic ground states of Zn$_x$Co$_{4-x}$(OD)$_6$Cl$_2$ ($x=0,1$) were studied. Our results show that for $x=0$, the ground state is a magnetic long-range ordered (LRO) state where each tetrahedron forms an "umbrella"-type structure. On the other hand, for $x=1$, no static ordering was observed down to 1.5 K, which resembles the behavior found in the isostructural quantum system Zn$_x$Cu$_{4-x}$(OD)$_6$Cl$_2$. When $H$ field is applied, however the $x=1$ system develops the same LRO state as $x=0$. This indicates that the $x=1$ disordered state is in the vicinity of the $x=0$ ordered state.

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