arXiv subjects

K. A. Ross

Publications and source records attributed to K. A. Ross.

At least 37 records · Page 2Linked to original sources

arXiv2017

Magnetic order and spin dynamics in the helical magnetic system Fe$_3$PO$_4$O$_3$

The 3$d$-electronic spin dynamics and the magnetic order in Fe$_3$PO$_4$O$_3$ were investigated by muon spin rotation and relaxation ($μ$SR) and $^{57}$Fe Mössbauer spectroscopy. Zero-field (ZF)-$μ$SR and $^{57}$Fe Mössbauer studies confirm static long range magnetic ordering below $T_{\mathrm{N}}$ $\approx$ 164\,K. Both transverse-field (TF) and ZF-$μ$SR results evidence 100\% magnetic volume fraction in the ordered state. The ZF-$μ$SR time spectra can be best described by a Bessel function, which is consistent with the helical magnetic structure proposed by neutron scattering experiments. The Mössbauer spectra are described in detail by considering the specific angular distribution of the local hyperfine field $B_{\mathrm{hyp}}$ with respect to the local electric field gradient. The $μ$SR spin-lattice relaxation rate exhibits two peaks: One at the magnetic ordering temperature related to critical magnetic fluctuations and another peak at 35\,K signaling the presence of a secondary low energy scale in Fe$_3$PO$_4$O$_3$.

cond-mat.str-el↗

arXiv2017

Ground state selection under pressure in the quantum pyrochlore magnet Yb2Ti2O7

A quantum spin liquid is a novel state of matter characterized by quantum entanglement and the absence of any broken symmetry. In condensed matter, the frustrated rare-earth pyrochlore magnets Ho$_2$Ti$_2$O$_7$ and Dy$_2$Ti$_2$O$_7$, so-called spin ices, exhibit a classical spin liquid state with fractionalized thermal excitations (magnetic monopoles). Evidence for a quantum spin ice, in which the magnetic monopoles become long range entangled and an emergent quantum electrodynamics arises, seems within reach. The magnetic properties of the quantum spin ice candidate Yb$_2$Ti$_2$O$_7$ have eluded a global understanding and even the presence or absence of static magnetic order at low temperatures is controversial. Here we show that sensitivity to pressure is the missing key to the low temperature behaviour of Yb$_2$Ti$_2$O$_7$. By combining neutron diffraction and muon spin relaxation on a stoichiometric sample under pressure, we evidence a magnetic transition from a disordered, non-magnetic, ground state to a splayed ferromagnetic ground state.

cond-mat.str-el↗

arXiv2017

Single-ion properties of the $S_{eff}$ = 1/2 XY antiferromagnetic pyrochlores, Na$A^{\prime}$Co$_2$F$_7$ ($A^{\prime} = $ Ca$^{2+}$, Sr$^{2+}$)

The antiferromagnetic pyrochlore material NaCaCo$_2$F$_7$ is a thermal spin liquid over a broad temperature range (~ 140 K down to $T_F = 2.4 $K), in which magnetic correlations between Co$^{2+}$ dipole moments explore a continuous manifold of antiferromagnetic XY states. The thermal spin liquid is interrupted by spin freezing at a temperature that is ~ 2 % of the mean field interaction strength, leading to short range static XY clusters with distinctive relaxation dynamics. Here we report the low energy inelastic neutron scattering response from the related compound NaSrCo$_2$F$_7$, confirming that it hosts the same static and dynamic spin correlations as NaCaCo$_2$F$_7$. We then present the single-ion levels of Co$^{2+}$ in these materials as measured by inelastic neutron scattering. An intermediate spin orbit coupling model applied to an ensemble of trigonally distorted octahedral crystal fields accounts for the observed transitions. The single-ion ground state of Co$^{2+}$ is a Kramers doublet with a strongly XY-like $g$-tensor ($g_{xy}/g_{z}$ ~ 3). The local disorder inherent from the mixed pyrochlore $A$ sites (Na$^{+}$/Ca$^{2+}$ and Na$^{+}$/Sr$^{2+}$) is evident in these measurements as exaggerated broadening of some of the levels. A simple model that reproduces the salient features of the single-ion spectrum produces approximately 8.4 % and 4.1 % variation in the $z$ and $xy$ components of the $g$-tensor, respectively. This study confirms that an $S_{eff} =1/2$ model with XY antiferromagnetic exchange and weak exchange disorder serves as a basic starting point in understanding the low temperature magnetic behavior of these strongly frustrated magnets.

cond-mat.str-el↗

arXiv2017

Disordered Route to the Coulomb Quantum Spin Liquid: Random Transverse Fields on Spin Ice in Pr$_2$Zr$_2$O$_7$

Inelastic neutron scattering reveals a broad continuum of excitations in Pr$_2$Zr$_2$O$_7$, the temperature and magnetic field dependence of which indicate a continuous distribution of quenched transverse fields ($Δ$) acting on the non-Kramers Pr$^{3+}$ crystal field ground state doublets. Spin-ice correlations are apparent within 0.2 meV of the Zeeman energy. A random phase approximation provides an excellent account of the data with a transverse field distribution $ρ(Δ)\propto (Δ^2+Γ^2)^{-1}$ where $ Γ=0.27(1)$ meV. Established during high temperature synthesis due to an underlying structural instability, it appears disorder in Pr$_2$Zr$_2$O$_7$ actually induces a quantum spin liquid.

cond-mat.str-el↗

arXiv2016

Gapless quantum excitations from an Ice-like Splayed Ferromagnetic ground state in stoichiometric Yb2Ti2O7

The ground state of the quantum spin ice candidate magnet Yb2Ti2O7 is known to be sensitive to weak disorder at the 1 percent level which occurs in single crystals grown from the melt. Powders produced by solid state synthesis tend to be stoichiometric and display large and sharp heat capacity anomalies at relatively high temperatures, with Tc about 0.26 K. We have carried out neutron elastic and inelastic measurements on well characterized and equilibrated stoichiometric powder samples of Yb2Ti2O7 which show resolution-limited Bragg peaks to appear at low temperatures, but whose onset correlates with temperatures much higher than Tc. The corresponding magnetic structure is best described as an ice-like splayed ferromagnet. The spin dynamics in Yb2Ti2O7 are shown to be gapless on an energy scale smaller than 0.09 meV at all temperatures, and organized into a continuum of scattering with vestiges of highly overdamped ferromagnetic spin waves present. These excitations differ greatly from conventional spin waves predicted for Yb2Ti2O7 s mean field ordered state, but appear robust to weak disorder as they are largely consistent with those displayed by non stoichiometric crushed single crystals and single crystals, as well as by powder samples of Yb2Ti2O7 s sister quantum magnet Yb2Sn2O7.

cond-mat.str-el↗

arXiv2015

Neutron Spectroscopic Study of Crystalline Electric Field Excitations in Stochiometric and Lightly Stuffed Yb2Ti2O7

Time-of-flight neutron spectroscopy has been used to determine the crystalline electric field (CEF) Hamiltonian, eigenvalues and eigenvectors appropriate to the $J$ = 7/2 Yb$^{3+}$ ion in the candidate quantum spin ice pyrochlore magnet $\rm Yb_2Ti_2O_7$. The precise ground state (GS) of this exotic, geometrically-frustrated magnet is known to be sensitive to weak disorder associated with the growth of single crystals from the melt. Such materials display weak "stuffing" wherein a small proportion, $\approx$ 2\%, of the non-magnetic Ti$^{4+}$ sites are occupied by excess Yb$^{3+}$. We have carried out neutron spectroscopic measurements on a stoichiometric powder sample of Yb$_2$Ti$_2$O$_7$, as well as a crushed single crystal with weak stuffing and an approximate composition of Yb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ with $x$ = 0.046. All samples display three CEF transitions out of the GS, and the GS doublet itself is identified as primarily composed of m$_J$ = $\pm$1/2, as expected. However,"stuffing" at low temperatures in Yb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ induces a similar finite CEF lifetime as is induced in stoichiometric Yb$_2$Ti$_2$O$_7$ by elevated temperature. We conclude that an extended strain field exists about each local "stuffed" site, which produces a distribution of random CEF environments in the lightly stuffed Yb$_{2+x}$Ti$_{2-x}$O$_{7+y}$, in addition to producing a small fraction of Yb-ions in defective environments with grossly different CEF eigenvalues and eigenvectors.

cond-mat.str-el↗

arXiv2014

Strict limit on in-plane ordered magnetic dipole moment in URu2Si2

Neutron diffraction is used to examine the polarization of weak static antiferromagnetism in high quality single crystalline URu2Si2. As previously documented, elastic Bragg-like diffraction develops for temperature T<T_{HO}= 17.5 K at q=(100) but not at wave vector transfer q=(001). The peak width indicates correlation lengths ξ_c=230(12) Å\ and ξ_a=240(15) Å. The integrated intensity of the T-dependent peaks corresponds to a sample averaged c-oriented staggered moment of μ_{c}=0.022(1) μ_B at T=1.7 K. The absence of T-dependent diffraction at q=(001) places a limit μ_{\perp}<0.0011 μ_B on an f- or d-orbital based in-plane staggered magnetic dipole moment, which is associated with multipolar orders proposed for URu_2Si_2.

cond-mat.str-el↗

arXiv2014

Order by Disorder Spin Wave Gap in the XY Pyrochlore Magnet Er2Ti2O7

The recent determination of a robust spin Hamiltonian for the anti-ferromagnetic XY pyrochlore Er2Ti2O7 reveals a most convincing case of the "order by quantum disorder" (ObQD) mechanism for ground state selection. This mechanism relies on quantum fluctuations to remove an accidental symmetry of the magnetic ground state, and selects a particular ordered spin structure below T_N=1.2K. The removal of the continuous degeneracy results in an energy gap in the spectrum of spin wave excitations, long wavelength pseudo-Goldstone modes. We have measured the ObQD spin wave gap at a zone center in Er2Ti2O7, using low incident energy neutrons and the time-of-flight inelastic scattering method. We report a gap of Delta =0.053 +/- 0.006 meV, which is consistent with upper bounds placed on it from heat capacity measurements and roughly consistent with theoretical estimate of ~ 0.02 meV, further validating the spin Hamiltonian that led to that prediction. The gap is observed to vary with square of the order parameter, and goes to zero for T ~ T_N.

cond-mat.str-el↗

arXiv2014

Liquid-like correlations in single crystalline Y2Mo2O7: an unconventional spin glass

The spin glass behavior of Y2Mo2O7 has puzzled physicists for nearly three decades. Free of bulk disorder within the resolution of powder diffraction methods, it is thought that this material is a rare realization of a spin glass resulting from weak disorder such as bond disorder or local lattice distortions. Here, we report on the single crystal growth of Y2Mo2O7. Using neutron scattering, we present unique isotropic magnetic diffuse scattering arising beneath the spin glass transition despite having a well-ordered structure at the bulk level. Despite our attempts to model the diffuse scattering using a computationally exhaustive search of a class of simple spin Hamiltonians, we were unable to replicate the experimentally observed energy-integrated (diffuse) neutron scattering. A T^2-temperature dependence in the heat capacity and density functional theory calculations hint at significant frozen degeneracy in both the spin and orbital degrees of freedom resulting from spin-orbital coupling (Kugel-Khomskii type) and random fluctuations in the Mo environment at the local level.

cond-mat.mtrl-sci↗

arXiv2013

Temperature and Magnetic Field Dependence of Spin Ice Correlations in the Pyrochlore Magnet Tb2Ti2O7

We present a parametric study of the diffuse magnetic scattering at (1/2,1/2,1/2) positions in reciprocal space, ascribed to a frozen antiferromagnetic spin ice state in single crystalline Tb2Ti2O7. Our high-resolution neutron scattering measurements show that the elastic (-0.02 meV < E < 0.02 meV) (1/2,1/2,1/2) scattering develops strongly below ~275 mK, and correlates with the opening of a spin gap of ~0.06-0.08 meV over most of the Brillouin zone. The concomitant low-lying magnetic spin excitations are weakly dispersive and appear to soften near the (1/2,1/2,1/2) wave vector at 80 mK. The nature of the transition at 275 mK has many characteristics of spin glass behavior, consistent with ac-susceptibility measurements. The application of a magnetic field of 0.075 T applied along the [1-10] direction destroys the (1/2,1/2,1/2) elastic scattering, revealing the fragility of this short-range ordered ground state. We construct a refined H-T phase diagram for Tb2Ti2O7 and [1-10] fields which incorporates this frozen spin ice regime and the antiferromagnetic long-range order previously known to be induced in relatively large fields. Specific heat measurements on the same crystal reveal a sharp anomaly at Tc~450 mK and no indication of a transition near ~275 mK. We conclude that the higher temperature specific heat peak is not related to the magnetic ordering but is likely a signal of other, nonmagnetic, correlations.

cond-mat.str-el↗

arXiv2013

Unconventional Magnetic Ground State in Yb$_2$Ti$_2$O$_7$

We report low temperature specific heat and muon spin relaxation/rotation ($μ$SR) measurements on both polycrystalline and single crystal samples of the pyrochlore magnet Yb$_2$Ti$_2$O$_7$. This system is believed to possess a spin Hamiltonian supporting a Quantum Spin Ice (QSI) ground state and to display sample variation in its low temperature heat capacity. Our two samples exhibit extremes of this sample variation, yet our $μ$SR measurements indicate a similar disordered low temperature state down to 16 mK in both. We report little temperature dependence to the spin relaxation and no evidence for ferromagnetic order, in contrast to recent reports by Chang \emph{et al.} (Nat. Comm. {\bf 3}, 992 (2012)). Transverse field (TF) $μ$SR measurements show changes in the temperature dependence of the muon Knight shift which coincide with heat capacity anomalies. We are therefore led to propose that Yb$_2$Ti$_2$O$_7$ enters a hidden order ground state below $T_c\sim265$ mK where the nature of the ordered state is unknown but distinct from simple long range order.

cond-mat.str-el↗

arXiv2013

Antiferromagnetic Spin Ice Correlations at (1/2,1/2,1/2) in the Ground State of the Pyrochlore Magnet Tb2Ti2O7

We present high-resolution single crystal time-of-flight neutron scattering measurements on the candidate quantum spin liquid pyrochlore Tb2Ti2O7 at low temperature and in a magnetic field. At ~70 mK and in zero field, Tb2Ti2O7 reveals diffuse magnetic elastic scattering at (1/2,1/2,1/2) positions in reciprocal space, consistent with short-range correlated regions based on a two-in, two-out spin ice configuration on a doubled conventional unit cell. This elastic scattering is separated from very low-energy magnetic inelastic scattering by an energy gap of ~0.06-0.08 meV. The elastic signal disappears under the application of small magnetic fields and upon elevating temperature. Pinch-point-like elastic diffuse scattering is observed near (1,1,1) and (0,0,2) in zero field at ~70 mK, in agreement with Fennell et al. (Ref. 1), supporting the quantum spin ice interpretation of Tb2Ti2O7.

cond-mat.str-el↗

arXiv2013

Two Dimensional Incommensurate and Three Dimensional Commensurate Magnetic Order and Fluctuations in $La_{2-x}Ba_{x}CuO_{4}$

We present neutron scattering measurements on single crystals of lightly doped $La_{2-x}Ba_{x}CuO_{4}$, with $0 \leq x \leq? 0.035$. These reveal the evolution of the magnetism in this prototypical doped Mott insulator from a three dimensional (3D) commensurate (C) antiferromagnetic ground state, which orders at a relatively high TN, to a two dimensional (2D) incommensurate (IC) ground state with finite ranged static correlations, which appear below a relatively low effective TN. At low temperatures, the 2D IC magnetism co-exists with the 3D C magnetism for doping concentrations as low as ? 0.0125. We find no signal of a 3D C magnetic ground state by x $\sim$? 0.025, consistent with the upper limit of x $\sim$? 0.02 observed in the sister family of doped Mott insulators, $La_{2-x}Sr_{x}CuO_{4}$. The 2D IC ground states observed for $0.0125 \leq x \leq 0.035$ are diagonal, and are rotated by 45 degrees within the orthorhombic basal plane compared with those previously reported for samples with superconducting ground states: $La_{2-x}Ba_{x}CuO_{4}$, with $0.05 \leq? x \leq? 0.095. We construct a phase diagram based solely on magnetic order parameter measurements, which displays much of the complexity of standard high temperature superconductivity phase diagrams discussed in the literature. Analysis of high energy-resolution inelastic neutron scattering at moderately low temperatures shows a progressive depletion of the very low energy dynamic magnetic susceptibility as x increases from 0.0125 to 0.035. This low energy, dynamic susceptibility falls off? with increasing temperature on a scale much higher than the effective 2D IC TN appropriate to these materials. Appreciable dynamic 2D IC magnetic fluctuations inhabit much of the "pseudogap" regime of the phase diagram.

cond-mat.supr-con↗

arXiv2013

Lightly stuffed pyrochlore structure of single-crystalline Yb2Ti2O7 grown by the optical floating zone technique

Recent neutron scattering and specific heat studies on the pyrochlore Yb2Ti2O7 have revealed variations in its magnetic behavior below 265mK. In the best samples, a sharp anomaly in the specific heat is observed at T=265mK. Other samples, especially single crystals, have broad features in the specific heat which vary in sharpness and temperature depending on the sample, indicating that the magnetic ground state may be qualitatively different in such samples. We performed detailed comparisons of the chemical structure of a pulverised single crystal of Yb2Ti2O7, grown by the floating zone technique, to a sintered powder sample of Yb2Ti2O7. Rietveld refinements of neutron powder diffraction data on these samples reveal that the crushed single crystal is best described as a "stuffed" pyrochlore, Yb2(Ti(2-x)Yb(x))O7-(x/2) with x = 0.046(4), despite perfectly stoichiometric starting material. Substituting magnetic Yb3+ on the non-magnetic Ti4+ sublattice would introduce random exchange bonds and local lattice deformations. These are expected to be the mechanism leading to of the variation of the delicate magnetic ground state of Yb2Ti2O7. Determination of the cubic cell length, a, could be useful as a method for characterizing the stoichiometry of non- pulverised single crystals at room temperature.

cond-mat.str-el↗

arXiv2012

Thermodynamic properties of the Yb2Ti2O7 pyrochlore as a function of temperature and magnetic field: validation of a quantum spin ice exchange Hamiltonian

The thermodynamic properties of the pyrochlore Yb2Ti2O7 material are calculated using the numericallinked-cluster (NLC) calculation method for an effective anisotropic-exchange spin-1/2 Hamiltonian with parameters recently determined by fitting the neutron scattering spin wave data obtained at high magnetic field h. Magnetization, M(T,h), as a function of temperature T and for different magnetic fields h applied along the three high symmetry directions [100], [110] and [111], are compared with experimental measurements on the material for temperature T>1.8K. The excellent agreement between experimentally measured and calculated M(T,h) over the entire temperature and magnetic field range considered provides strong quantitative validation of the effective Hamiltonian. It also confirms that fitting the high-field neutron spin wave spectra in the polarized paramagnetic state is an excellent method for determining the microscopic exchange constants of rare-earth insulating magnets that are described by an effective spin-1/2 Hamiltonian. Finally, we present results which demonstrate that a recent analysis of the polarized neutron scattering intensity of Yb2Ti2O7 using a random phase approximation (RPA) method [Chang et al., Nature Communications {3}, 992 (2012)] does not provide a good description of M(T,h) for $T\lesssim 10$ K, that is in the entire temperature regime where correlations become non-negligible.

cond-mat.str-el↗

arXiv2012

Dimensional Evolution of Spin Correlations in the Magnetic Pyrochlore Yb2Ti2O7

The pyrochlore material Yb2Ti2O7 displays unexpected quasi-two-dimensional (2D) magnetic correlations within a cubic lattice environment at low temperatures, before entering an exotic disordered ground state below T=265mK. We report neutron scattering measurements of the thermal evolution of the 2D spin correlations in space and time. Short range three dimensional (3D) spin correlations develop below 400 mK, accompanied by a suppression in the quasi-elastic (QE) scattering below ~ 0.2 meV. These show a slowly fluctuating ground state with spins correlated over short distances within a kagome-triangular-kagome (KTK) stack along [111], which evolves to isolated kagome spin-stars at higher temperatures. Furthermore, low-temperature specific heat results indicate a sample dependence to the putative transition temperature that is bounded by 265mK, which we discuss in the context of recent mean field theoretical analysis.

cond-mat.str-el↗

arXiv2010

Magnetoelastics of a spin liquid: X-ray diffraction studies of Tb2Ti2O7 in pulsed magnetic fields

We report high resolution single crystal x-ray diffraction measurements of the frustrated pyrochlore magnet Tb2Ti2O7, collected using a novel low temperature pulsed magnet system. This instrument allows characterization of structural degrees of freedom to temperatures as low as 4.4 K, and in applied magnetic fields as large as 30 Tesla. We show that Tb2Ti2O7 manifests intriguing structural effects under the application of magnetic fields, including strongly anisotropic giant magnetostriction, a restoration of perfect pyrochlore symmetry in low magnetic fields, and ultimately a structural phase transition in high magnetic fields. It is suggested that the magnetoelastic coupling thus revealed plays a significant role in the spin liquid physics of Tb2Ti2O7 at low temperatures.

cond-mat.str-el↗

arXiv2010

Two Dimensional Kagome Correlations and Field Induced Order in the Ferromagnetic XY Pyrochlore Yb2Ti2O7

Neutron scattering measurements show the ferromagnetic XY pyrochlore Yb2Ti2O7 to display strong quasi-two dimensional (2D) spin correlations at low temperature, which give way to long range order (LRO) under the application of modest magnetic fields. Rods of scattering along < 111 > directions due to these 2D spin correlations imply a magnetic decomposition of the cubic pyrochlore system into decoupled kagome planes. A magnetic field of ~0.5 T applied along the [1-10] direction induces a transition to a 3D LRO state characterized by long-lived, dispersive spin waves. Our measurements map out a complex low temperature-field phase diagram for this exotic pyrochlore magnet.

cond-mat.str-el↗