arXiv subjects

Stephen J. Blundell

Publications and source records attributed to Stephen J. Blundell.

At least 37 records · Page 2Linked to original sources

arXiv2021

Studies on Novel Yb-based Candidate Triangular Quantum Antiferromagnets: Ba3YbB3O9 and Ba3YbB9O18

Yb-based triangular magnets have recently attracted attention as promising candidates to explore frustrated quantum magnetism. However, some candidates have turned out to have significant amounts of site disorder, which significantly affects the low-temperature magnetic behavior. To overcome this issue, Yb-based frustrated systems without structural disorder are required. In this paper, we report physical properties of two Yb-based triangular magnets Ba3YbB3O9 and Ba3YbB9O18, without structural disorder. Via magnetic susceptibility, magnetization, and muon spin rotation measurements, we verified that both Ba3YbB3O9 and, particularly studied for the first time, Ba3YbB9O18 do not show long range magnetic order or glass-like spin freezing down to 0.28 K, but show typical paramagnetic behavior.

cond-mat.str-el↗

arXiv2021

Magnetic ground-state of the one-dimensional ferromagnetic chain compounds $M$(NCS)$_2$(thiourea)$_2$; $M$ = Ni, Co

The magnetic properties of the two isostructural molecule-based magnets, Ni(NCS)$_{2}$(thiourea)$_{2}$, $S$ = 1, [thiourea = SC(NH$_2$)$_2$] and Co(NCS)$_{2}$(thiourea)$_{2}$, $S$ = 3/2, are characterised using several techniques in order to rationalise their relationship with structural parameters and ascertain magnetic changes caused by substitution of the spin. Zero-field heat capacity and muon-spin relaxation measurements reveal low-temperature long-range ordering in both compounds, in addition to Ising-like ($D < 0$) single-ion anisotropy ($D_{\rm{Co}} \sim$ -100 K, $D_{\rm{Ni}} \sim$ -10 K). Crystal and electronic structure, combined with DC-field magnetometry, affirm highly quasi-one-dimensional behaviour, with ferromagnetic intrachain exchange interactions $J_{\rm{Co}}\approx+4$ K and $J_{\rm{Ni}}\sim+100$ K and weak antiferromagnetic interchain exchange, on the order of $J'$ $\sim-0.1$ K. Electron charge and spin-density mapping reveals through-space exchange as a mechanism to explain the large discrepancy in $J$-values despite, from a structural perspective, the highly similar exchange pathways in both materials. Both species can be compared to the similar compounds $M$Cl$_2$(thiourea)$_4$, $M$ = Ni(II) (DTN) and Co(II) (DTC), where DTN is know to harbour two magnetic field-induced quantum critical points. Direct comparison of DTN and DTC with the compounds studied here shows that substituting the halide Cl$^-$ ion, for the NCS$^-$ ion, results in a dramatic change in both the structural and magnetic properties.

cond-mat.str-el↗

arXiv2020

Dynamic Spin Fluctuations in the Frustrated A-site Spinel CuAl2O4

We performed nuclear magnetic resonance (NMR) and muon spin relaxation (μSR) experiments to identify the magnetic ground state of the frustrated quantum A-site spinel, CuAl2O4. Our results verify that the ground state does not exhibit a long-range magnetic ordering, but a glass-like transition manifests at T*=2.3 K. However, the Gaussian shape and the weak longitudinal field dependence of μSR spectra below T* show that the ground state has dynamic spin fluctuations, distinct from those of conventional spin-glasses.

cond-mat.str-el↗

arXiv2020

Robustness of superconducting properties to transition metal substitution and impurity phases in Fe1-xVxSe

We have performed transverse- and zero-field muon spin rotation/relaxation experiments, as well as magnetometry measurements, on samples of Fe1-xVxSe and their Li+NH3 intercalates Li0.6(NH2)0.2(NH3)0.8 Fe1-x Vx Se. We examine the low vanadium substitution regime: x = 0.005, 0.01, and 0.02. The intercalation reaction significantly increases the critical temperature (Tc) and the superfluid stiffness for all x. The nonintercalated samples all exhibit Tc = 8.5 K while the intercalated samples all show an enhanced Tc > 40 K. Vanadium substitution has a negligible effect on Tc, but seems to suppress the superfluid stiffness for the nonintercalated samples and weakly enhance it for the intercalated materials. The optimal substitution level for the intercalated samples is found to be x = 0.01, with Tc = 41 K and λ_{ab}(0) = 0.18 μm. The nonintercalated samples can be modeled with either a single d-wave superconducting gap or with an anisotropic gap function based on recent quasiparticle imaging experiments, whereas the intercalates display multigap nodal behavior which can be fitted using s + d- or d + d-wave models. Magnetism, likely from iron impurities, appears after the intercalation reaction and coexists and competes with the superconductivity. However, it appears that the superconductivity is remarkably robust to the impurity phase, providing an avenue to stably improve the superconducting properties of transition metal substituted FeSe.

cond-mat.supr-con↗

arXiv2020

Competing pairing interactions responsible for the large upper critical field in a stoichiometric iron-based superconductor, CaKFe$_4$As$_4$

The upper critical field of multiband superconductors is an important quantity that can reveal the details about the nature of the superconducting pairing. Here we experimentally map out the complete upper critical field phase diagram of a stoichiometric superconductor, CaKFe$_4$As$_4$, up to 90T for different orientations of the magnetic field and at temperatures down to 4.2K. The upper critical fields are extremely large, reaching values close to ~3$T_c$ at the lowest temperature, and the anisotropy decreases dramatically with temperature leading to essentially isotropic superconductivity at 4.2K. We find that the temperature dependence of the upper critical field can be well described by a two-band model in the clean limit with band coupling parameters favouring intraband over interband interactions. The large Pauli paramagnetic effects together with the presence of the shallow bands is consistent with the stabilization of an FFLO state at low temperatures in this clean superconductor.

cond-mat.supr-con↗

arXiv2019

A Near-Ideal Molecule-Based Haldane Spin-Chain

The molecular coordination complex NiI$_2$(3,5-lut)$_4$ [where (3,5-lut) $=$ (3,5-lutidine) $=$ (C$_7$H$_9$N)] has been synthesized and characterized by several techniques including synchrotron X-ray diffraction, ESR, SQUID magnetometry, pulsed-field magnetization, inelastic neutron scattering and muon spin relaxation. Templated by the configuration of 3,5-lut ligands the molecules pack in-registry with the Ni--I$\cdots$I--Ni chains aligned along the $c$--axis. This arrangement leads to through-space I$\cdots$I magnetic coupling which is directly measured for the first time in this work. The net result is a near-ideal realization of the $S = 1$ Haldane chain with $J = 17.5~\rm{K}$ and energy gaps of $Δ^{\parallel} = 5.3~{\rm K}$ $Δ^{\perp} =7.7~{\rm K}$, split by the easy-axis single-ion anisotropy $D=-1.2~{\rm K}$. The ratio $D/J = -0.07$ affords one of the most isotropic Haldane systems yet discovered, while the ratio $Δ_0/J = 0.40(1)$ (where $Δ_0$ is the average gap size) is close to its ideal theoretical value, suggesting a very high degree of magnetic isolation of the spin chains in this material. The Haldane gap is closed by orientation-dependent critical fields $μ_0H_{\rm c}^{\parallel} = 5.3~\rm{T}$ and $μ_0H_{\rm c}^{\perp} = 4.3~\rm{T}$, which are readily accessible experimentally and permit investigations across the entirety of the Haldane phase, with the fully polarized state occurring at $μ_0 H_{\rm s}^{\parallel}=46.0~\rm{T}$ and $μ_0 H_{\rm s}^{\perp}=50.7~\rm{T}$. The results are explicable within the so-called fermion model, in contrast to other reported easy-axis Haldane systems. Zero-field magnetic order is absent down to $20~{\rm mK}$ and emergent end-chain effects are observed in the gapped state, as evidenced by detailed low-temperature measurements.

cond-mat.str-el↗

arXiv2019

FeTi$_2$O$_5$: a spin Jahn-Teller transition enhanced by cation substitution

We have used muon-spin rotation, heat capacity and x-ray diffraction measurements in combination with density functional theory and dipole field calculations to investigate the crystal and magnetic structure of FeTi$_2$O$_5$. We observe a long range ordered state below $T_{\rm N}$=41.8(5) K with indications of significant correlations existing above this temperature. We determine candidate muon stopping sites in this compound, and find that our data are consistent with the spin Jahn-Teller driven antiferromagnetic ground state with $\boldsymbol{k}$=(1/2,1/2,0) reported for CoTi$_2$O$_5$ ($T_{\rm N}$=26 K). By comparing our data with calculated dipolar fields we can restrict the possible moment size and directions of the Fe$^{2+}$ ions.

cond-mat.str-el↗

arXiv2019

Determining the anisotropy and exchange parameters of polycrystalline spin-1 magnets

Although low-dimensional $S = 1$ antiferromagnets remain of great interest, difficulty in obtaining high-quality single crystals of the newest materials hinders experimental research in this area. Polycrystalline samples are more readily produced, but there are inherent problems in extracting the magnetic properties of anisotropic systems from powder data. Following a discussion of the effect of powder-averaging on various measurement techniques, we present a methodology to overcome this issue using thermodynamic measurements. In particular we focus on whether it is possible to characterise the magnetic properties of polycrystalline, anisotropic samples using readily available laboratory equipment. We test the efficacy of our method using the magnets [Ni(H$_{2}$O)$_{2}$(3,5-lutidine)$_{4}$](BF$_{4}$)$_{2}$ and Ni(H$_{2}$O)$_{2}$(acetate)$_{2}$(4-picoline)$_{2}$, which have negligible exchange interactions, as well as the antiferromagnet [Ni(H$_{2}$O)$_{2}$(pyrazine)$_{2}$](BF$_{4}$)$_{2}$, and show that we are able to extract the anisotropy parameters in each case. The results obtained from the thermodynamic measurements are checked against electron-spin resonance and neutron diffraction. We also present a density functional method, which incorporates spin-orbit coupling to estimate the size of the anisotropy in [Ni(H$_{2}$O)$_{2}$(pyrazine)$_{2}$](BF$_{4}$)$_{2}$.

cond-mat.str-el↗

arXiv2019

Magnetic Monopole Noise

Magnetic monopoles are hypothetical elementary particles exhibiting quantized magnetic charge $m_0=\pm(h/μ_0e)$ and quantized magnetic flux $Φ_0=\pm h/e$. A classic proposal for detecting such magnetic charges is to measure the quantized jump in magnetic flux $Φ$ threading the loop of a superconducting quantum interference device (SQUID) when a monopole passes through it. Naturally, with the theoretical discovery that a plasma of emergent magnetic charges should exist in several lanthanide-pyrochlore magnetic insulators, including Dy$_2$Ti$_2$O$_7$, this SQUID technique was proposed for their direct detection. Experimentally, this has proven extremely challenging because of the high number density, and the generation-recombination (GR) fluctuations, of the monopole plasma. Recently, however, theoretical advances have allowed the spectral density of magnetic-flux noise $S_Φ(ω,T)$ due to GR fluctuations of $\pm m_*$ magnetic charge pairs to be determined. These theories present a sequence of strikingly clear predictions for the magnetic-flux noise signature of emergent magnetic monopoles. Here we report development of a high-sensitivity, SQUID based flux-noise spectrometer, and consequent measurements of the frequency and temperature dependence of $S_Φ(ω,T)$ for Dy$_2$Ti$_2$O$_7$ samples. Virtually all the elements of $S_Φ(ω,T)$ predicted for a magnetic monopole plasma, including the existence of intense magnetization noise and its characteristic frequency and temperature dependence, are detected directly. Moreover, comparisons of simulated and measured correlation functions $C_Φ(t)$ of the magnetic-flux noise $Φ(t)$ imply that the motion of magnetic charges is strongly correlated because traversal of the same trajectory by two magnetic charges of same sign is forbidden.

cond-mat.quant-gas↗

arXiv2018

Magnetic phases of skyrmion-hosting GaV$_4$S$_{8-y}$Se$_{y}$ ($y = 0, 2, 4, 8$) probed with muon spectroscopy

We present the results of a muon-spin spectroscopy investigation of GaV$_4$S$_{8-y}$Se$_{y}$ with $y=0, 2, 4$ and 8. Zero-field measurements suggest that GaV$_{4}$Se$_{8}$ and GaV$_{4}$S$_{8}$ have distinct magnetic ground states, with the latter material showing an anomalous temperature-dependence of the local magnetic field. It is not possible to evolve the magnetic state continuously between these two systems, with the intermediate $y=2$ and $4$ materials showing glassy magnetic behaviour at low temperature. The skyrmion lattice (SkL) phase is evident in the $y=0$ and 8 materials through an enhanced response of the muon-spin relaxation to the emergent dynamics that accompany the SkL. For our polycrystalline samples of GaV$_4$Se$_{8}$, this enhanced dynamic response is confined to a smaller region of the magnetic field-temperature phase diagram than the previous reports of the SkL in single crystals.

cond-mat.mtrl-sci↗

arXiv2018

Ultra-high critical current densities, the vortex phase diagram and the effect of granularity of the stoichiometric high-Tc superconductor, CaKFe$_4$As$_4$

We present a comprehensive study of the critical current densities and the superconducting vortex phase diagram in the stoichiometric superconductor CaKFe$_4$As$_4$ which has a critical temperature of 35 K. We performed detailed magnetization measurements both of high quality single crystals for different orientations in an applied magnetic field up to 16 T and for a powder sample. We find an extremely large critical current density, Jc, up to 10$^8$ A/cm2 for single crystals when H||(ab) at 5 K, which remains robust in fields up to 16 T, being the largest of any other iron-based superconductor. The critical current density is reduced by a factor 10 in single crystals when H||c at 5 K and significantly suppressed by the presence of grain boundaries in the powder sample. We also observe the presence of the fishtail effect in the magnetic hysteresis loops of single crystals when H||c. The flux pinning force density and the pinning parameters suggest that the large critical current could be linked to the existence of point core and surface pinning. Based on the vortex phase diagram and the large critical current densities, CaKFe$_4$As$_4$ is now established as a potential iron-based superconductor candidate for practical applications.

cond-mat.supr-con↗

arXiv2018

Spin Jahn-Teller antiferromagnetism in CoTi$_2$O$_5$

We have used neutron powder diffraction to solve the magnetic structure of orthorhombic CoTi$_2$O$_5$, showing that the long-range ordered state below 26 K identified in our muon-spin rotation experiments is antiferromagnetic with propagation vector ${\bf k}=(\pm \frac{1}{2}, \frac{1}{2}, 0)$ and moment of 2.72(1)$μ_{\rm B}$ per Co$^{2+}$ ion. This long range magnetic order is incompatible with the experimentally determined crystal structure because the imposed symmetry completely frustrates the exchange coupling. We conclude that the magnetic transition must therefore be associated with a spin Jahn-Teller effect which lowers the structural symmetry and thereby relieves the frustration. These results show that CoTi$_2$O$_5$ is a highly unusual low symmetry material exhibiting a purely spin-driven lattice distortion critical to the establishment of an ordered magnetic ground state.

cond-mat.str-el↗

arXiv2018

Observation of a crossover from nodal to gapped superconductivity in Lu$_x$Zr$_{1-x}$B$_{12}$

We have determined the superconducting and magnetic properties of four samples of Lu$_x$Zr$_{1-x}$B$_{12}$ ($x=0.04$, $0.07$, $0.17$, and $0.8$) using muon spin rotation ($μ$SR) and magnetometry measurements. We observed a strong magnetic signal in both the $μ$SR and magnetometry data in one sample ($x=0.07$), likely caused by the formation of static moments of size $\approx 1\,μ_{\rm B}$ due to a clustering effect of the Lu$^{3+}$ ions. In all other samples, we find only a small magnetic signal in the $μ$SR data thought to originate from boron nuclei in the B$_{12}$ cages. The superconductivity is found to evolve with $x$, with a decrease in $x$ resulting in an increase in critical temperature and a decrease of the penetration depth. Most remarkably, we find the formation of nodes in the superconducting gap for $x \leq 0.17$, providing a new example of an $s$-to-$d$-wave crossover in a superconductor.

cond-mat.supr-con↗

arXiv2018

Two-gap superconductivity with line nodes in CsCa$_2$Fe$_4$As$_4$F$_2$

We report the results of a muon-spin rotation ($μ$SR) experiment to determine the superconducting ground state of the iron-based superconductor CsCa$_2$Fe$_4$As$_4$F$_2$ with $T_{\rm c} \approx 28.3\,$K. This compound is related to the fully-gapped superconductor CaCsFe$_4$As$_4$, but here the Ca-containing spacer layer is replaced with one containing Ca$_2$F$_2$. The temperature evolution of the penetration depth strongly suggests the presence of line nodes and is best modelled by a system consisting of both an $s$- and a $d$-wave gap. We also find a potentially magnetic phase which appears below $\approx 10\,$K but does not appear to compete with the superconductivity. This compound contains the largest alkali atom in this family of superconductors and our results yield a value for the in-plane penetration depth of $λ_{ab}(T=0)=423(5)\,$nm.

cond-mat.supr-con↗

arXiv2017

Proposal for the Detection of Magnetic Monopoles in Spin Ice via Nanoscale Magnetometry

We present a proposal for applying nanoscale magnetometry to the search for magnetic monopoles in the spin ice materials holmium and dysprosium titanate. Employing Monte Carlo simulations of the dipolar spin ice model, we find that when cooled to below $1.5\,$K these materials exhibit a sufficiently low monopole density to enable the direct observation of magnetic fields from individual monopoles. At these temperatures we demonstrate that noise spectroscopy can capture the intrinsic fluctuations associated with monopole dynamics, allowing one to isolate the qualitative effects associated with both the Coulomb interaction between monopoles and the topological constraints implied by Dirac strings. We describe in detail three different nanoscale magnetometry platforms (muon spin rotation, nitrogen vacancy defects, and nanoSQUID arrays) that can be used to detect monopoles in these experiments, and analyze the advantages of each.

cond-mat.str-el↗

arXiv2017

Static and Fluctuating Magnetic Moments in the Ferroelectric Metal LiOsO$_3$

LiOsO$_3$ is the first example of a new class of material called a ferroelectric metal. We performed zero-field and longitudinal-field $μ$SR, along with a combination of electronic structure and dipole field calculations, to determine the magnetic ground state of LiOsO$_3$. We find that the sample contains both static Li nuclear moments and dynamic Os electronic moments. Below $\approx 0.7\,$K, the fluctuations of the Os moments slow down, though remain dynamic down to 0.08$\,$K. We expect this could result in a frozen-out, disordered ground state at even lower temperatures.

cond-mat.str-el↗

arXiv2017

Quantum Griffiths phase inside the ferromagnetic phase of Ni$_{1-x}$V$_x$

We study by means of bulk and local probes the d-metal alloy Ni$_{1-x}$V$_x$ close to the quantum critical concentration, $x_c \approx 11.6\%$, where the ferromagnetic transition temperature vanishes. The magnetization-field curve in the ferromagnetic phase takes an anomalous power-law form with a nonuniversal exponent that is strongly $x$-dependent and mirrors the behavior in the paramagnetic phase. Muon spin rotation experiments demonstrate inhomogeneous magnetic order and indicate the presence of dynamic fluctuating magnetic clusters. These results provide strong evidence for a quantum Griffiths phase on the ferromagnetic side of the quantum phase transition.

cond-mat.str-el↗

arXiv2016

Robustness of superconductivity to competing magnetic phases in tetragonal FeS

We have determined the superconducting and magnetic properties of a hydrothermally synthesized powder sample of tetragonal FeS using muon spin rotation (μSR). The superconducting properties are entirely consistent with those of a recently published study, showing fully gapped behavior and giving a penetration depth of λ_{ab} = 204(3) nm. However, our zero-field μSR data are rather different and indicate the presence of a small, non-superconducting magnetic phase within the sample. These results highlight that sample-to-sample variations in magnetism can arise in hydrothermally prepared phases, but interestingly the superconducting behavior is remarkably insensitive to these variations.

cond-mat.supr-con↗