arXiv subjects

S. J. Blundell

Publications and source records attributed to S. J. Blundell.

At least 37 records · Page 2Linked to original sources

arXiv2020

Extremely well isolated 2D spin-$1/2$ antiferromagnetic Heisenberg layers with small exchange coupling in the molecular-based magnet CuPOF

We report on a comprehensive characterization of the newly synthesized Cu$^{2+}$-based molecular magnet [Cu(pz)$_2$(2-HOpy)$_2$](PF$_6$)$_2$ (CuPOF), where pz = C$_4$H$_4$N$_2$ and 2-HOpy = C$_5$H$_4$NHO. From a comparison of theoretical modeling to results of bulk magnetometry, specific heat, $μ^+$SR, ESR, and NMR spectroscopy, this material is determined as an excellent realization of the 2D square-lattice $S=1/2$ antiferromagnetic Heisenberg model with a moderate intraplane nearest-neighbor exchange coupling of $J/k_\mathrm{B} = 6.80(5)$ K, and an extremely small interlayer interaction of about 1 mK. At zero field, the bulk magnetometry reveals a temperature-driven crossover of spin correlations from isotropic to $XY$ type, caused by the presence of a weak intrinsic easy-plane anisotropy. A transition to long-range order, driven by the low-temperature $XY$ anisotropy under the influence of the interlayer coupling, occurs at $T_\mathrm{N} = 1.38(2)$ K, as revealed by $μ^+$SR. In applied magnetic fields, our $^1$H-NMR data reveal a strong increase of the magnetic anisotropy, manifested by a pronounced enhancement of the transition temperature to commensurate long-range order at $T_\mathrm{N} =2.8$ K and 7 T.

cond-mat.str-el↗

arXiv2020

Magnetically driven loss of centrosymmetry in metallic Pb2CoOsO6

We report magnetic, transport, neutron diffraction, and muon spin rotation data showing that Pb$_2$CoOsO$_6$, a newly synthesized metallic double-perovskite with a centrosymmetric space group at room temperature, exhibits a continuous second-order phase transition at 45 K to a magnetically ordered state with a non-centrosymmetric space group. The absence of inversion symmetry is very uncommon in metals, particularly metallic oxides. In contrast to the recently reported ferroelectric-like structural transition in LiOsO$_3$, the phase transition in Pb$_2$CoOsO$_6$ is driven by a long-range collinear antiferromagnetic order, with propagation vector $\textbf{k} = (\frac{1}{2},0,\frac{1}{2})$, which relieves the frustration associated with the symmetry of themagnetic exchanges. This magnetically-driven loss of inversion symmetry represents a new frontier in the search for novel metallic behavior.

cond-mat.str-el↗

arXiv2020

Magnetism and Néel skyrmion dynamics in GaV$_{4}$S$_{8-y}$Se$_{y}$

We present an investigation of the influence of low-levels of chemical substitution on the magnetic ground state and N{\' e}el skyrmion lattice (SkL) state in GaV$_4$S$_{8-y}$Se$_y$, where $y =0, 0.1, 7.9$, and $8$. Muon-spin spectroscopy ($μ$SR) measurements on $y=0$ and 0.1 materials reveal the magnetic ground state consists of microscopically coexisting incommensurate cycloidal and ferromagnetic environments, while chemical substitution leads to the growth of localized regions of increased spin density. $μ$SR measurements of emergent low-frequency skyrmion dynamics show that the SkL exists under low-levels of substitution at both ends of the series. Skyrmionic excitations persist to temperatures below the equilibrium SkL in substituted samples, suggesting the presence of skyrmion precursors over a wide range of temperatures.

cond-mat.str-el↗

arXiv2020

Magnetic order and ballistic spin transport in a sine-Gordon spin chain

We report the results of muon-spin spectroscopy ($μ^+$SR) measurements on the staggered molecular spin chain [pym-Cu(NO$_3$)$_2$(H$_2$O)$_2$] (pym = pyrimidine), a material previously described using sine-Gordon field theory. Zero-field $μ^+$SR reveals a long range magnetically-ordered ground state below a transition temperature $T_\mathrm{N}=0.22(1)$ K. Using longitudinal-field (LF) $μ^+$SR we investigate the dynamic response in applied magnetic fields $0< B < 500$ mT and find evidence for ballistic spin transport. Our LF $μ^+$SR measurements on the chiral spin chain [Cu(pym)(H$_2$O)$_4$]SiF$_6 \cdot $H$_2$O instead demonstrate one-dimensional spin diffusion and the distinct spin transport in these two systems likely reflects differences in their magnetic excitations.

cond-mat.str-el↗

arXiv2020

Observation of a neutron spin resonance in the bilayered superconductor CsCa2Fe4As4F2

We report inelastic neutron scattering (INS) investigations on the bilayer Fe-based superconductor CsCa2Fe4As4F4 above and below its superconducting transition temperature Tc = 28.9 K to investigate the presence of a neutron spin resonance. This compound crystallises in a body-centred tetragonal lattice containing asymmetric double layers of Fe2As2 separated by insulating CaF2 layers and is known to be highly anisotropic. Our INS study clearly reveals the presence of a neutron spin resonance that exhibits higher intensity at lower momentum transfer (Q) at 5K compared to 54 K, at an energy of 15 meV. The energy ER of the observed spin resonance is broadly consistent with the relationship E_R = 4.9 k_B T_c, but is slightly enhanced compared to the values observed in other Fe-based superconductors. We discuss the nature of the electron pairing symmetry by comparing the value of E_R with that deduced from the total superconducting gap value integrated over the Fermi surface.

cond-mat.supr-con↗

arXiv2020

Information and decoherence in a muon-fluorine coupled system

The unitary evolution of a quantum system preserves its coherence, but interactions between the system and its environment result in decoherence, a process in which the quantum information stored in the system becomes degraded. A spin-polarized positively-charged muon implanted in a fluoride crystal realises such a coherent quantum system, and the entanglement of muon and nearest-neighbour fluorine nuclear spins gives rise to an oscillatory time-dependence of the muon polarization which can be detected and measured. Here we show that the decohering effect of more distant nuclear spins can be precisely modelled, allowing a very detailed description of the decoherence processes coupling the muon-fluorine 'system' with its 'environment', and allowing us to track the system entropy as the quantum information degrades. These results show how to precisely quantify the spin relaxation of muons implanted into quantum entangled states in fluoride crystals, a feature that has hitherto only been described phenomenologically.

cond-mat.str-el↗

arXiv2019

Probing magnetic order and disorder in the one-dimensional molecular spin chains CuF2(pyz) and [Ln(hfac)3(boaDTDA)]n (Ln=Sm, La) using implanted muons

We present the results of muon-spin relaxation ($μ^{+}$SR) measurements on antiferromagnetic and ferromagnetic spin chains. In antiferromagnetic CuF$_{2}$(pyz) we identify a transition to long range magnetic order taking place at $T_{\mathrm{N}} = 0.6(1)$ K, allowing us to estimate a ratio with the intrachain exchange of $T_{\mathrm{N}}/|J| \approx 0.1$ and the ratio of interchain to intrachain exchange coupling as $|J'/J| \approx 0.05$. The ferromagnetic chain [Sm(hfac)$_{3}$(boaDTDA)]$_{n}$ undergoes an ordering transition at $T_{\mathrm{c}}=2.8(1)$ K, seen via a broad freezing of dynamic fluctuations on the muon (microsecond) timescale and implying $T_{\mathrm{c}}/|J| \approx 0.6$. The ordered radical moment continues to fluctuate on this timescale down to 0.3 K, while the Sm moments remain disordered. In contrast, the radical spins in [La(hfac)$_{3}$(boaDTDA)]$_{n}$ remain magnetically disordered down to $T=0.1$ K suggesting $T_{\mathrm{c}}/|J| < 0.17$.

cond-mat.str-el↗

arXiv2019

Local magnetism, magnetic order and spin freezing in the 'nonmetallic metal' FeCrAs

We present the results of x-ray scattering and muon-spin relaxation ($μ^{+}$SR) measurements on the iron-pnictide compound FeCrAs. Polarized non-resonant magnetic x-ray scattering results reveal the 120$^\circ$ periodicity expected from the suggested three-fold symmetric, non-collinear antiferromagnetic structure. $μ^+$SR measurements indicate a magnetically ordered phase throughout the bulk of the material below $T_\mathrm{N}$=105(5) K. There are signs of fluctuating magnetism in a narrow range of temperatures above $T_\mathrm{N}$ involving low-energy excitations, while at temperatures well below $T_\mathrm{N}$ behaviour characteristic of freezing of dynamics is observed, likely reflecting the effect of disorder in our polycrystalline sample. Using density functional theory we propose a distinct muon stopping site in this compound and assess the degree of distortion induced by the implanted muon.

cond-mat.str-el↗

arXiv2019

Unconventional field-induced spin gap in an $S = 1/2$ chiral staggered chain

We investigate the low-temperature magnetic properties of the molecule-based chiral spin chain [Cu(pym)(H$_2$O)$_4$]SiF$_6\cdot$H$_2$O (pym = pyrimidine). Electron-spin resonance, magnetometry and heat capacity measurements reveal the presence of staggered $g$ tensors, a rich low-temperature excitation spectrum, a staggered susceptibility and a spin gap that opens on the application of a magnetic field. These phenomena are reminiscent of those previously observed in non-chiral staggered chains, which are explicable within the sine-Gordon quantum-field theory. In the present case, however, although the sine-Gordon model accounts well for the form of the temperature-dependence of the heat capacity, the size of the gap and its measured linear field dependence do not fit with the sine-Gordon theory as it stands. We propose that the differences arise due to additional terms in the Hamiltonian resulting from the chiral structure of [Cu(pym)(H$_2$O)$_4$]SiF$_6\cdot$H$_2$O, particularly a uniform Dzyaloshinskii-Moriya coupling and a four-fold periodic staggered field.

cond-mat.str-el↗

arXiv2018

Spin dynamics and field-induced magnetic phase transition in the honeycomb Kitaev magnet $α$-Li$_2$IrO$_3$

The layered honeycomb iridate $α$-Li$_2$IrO$_3$ displays an incommensurate magnetic structure with counterrotating moments on nearest-neighbor sites, proposed to be stabilized by strongly-frustrated anisotropic Kitaev interactions between spin-orbit entangled Ir$^{4+}$ magnetic moments. Here we report powder inelastic neutron scattering measurements that observe sharply dispersive low-energy magnetic excitations centered at the magnetic ordering wavevector, attributed to Goldstone excitations of the incommensurate order, as well as an additional intense mode above a gap $Δ\simeq2.3$ meV. Zero-field muon-spin relaxation measurements show clear oscillations in the muon polarization below the Néel temperature $T_{\rm N}\simeq15$ K with a time-dependent profile consistent with bulk incommensurate long-range magnetism. Pulsed field magnetization measurements observe that only about half the saturation magnetization value is reached at the maximum field of 64 T. A clear anomaly near 25 T indicates a transition to a phase with reduced susceptibility. The transition field has a Zeeman energy comparable to the zero-field gapped mode, suggesting gap suppression as a possible mechanism for the field-induced transition.

cond-mat.str-el↗

arXiv2018

Microscopic effects of Dy-doping in the topological insulator Bi2Te3

Magnetic doping with transition metal ions is the most widely used approach to break timereversal symmetry in a topological insulator, a prerequisite for unlocking the TIs exotic potential. Recently, we reported the doping of Bi2Te3 thin films with rare earth ions, which, owing to their large magnetic moments, promise commensurately large magnetic gap openings in the topological surface states. However, only when doping with Dy has a sizable gap been observed in angle-resolved photoemission spectroscopy, which persists up to room-temperature. Although disorder alone could be ruled out as a cause of the topological phase transition, a fundamental understanding of the magnetic and electronic properties of Dy:Bi2Te3 remained elusive. Here, we present an X-ray magnetic circular dichroism, polarized neutron reflectometry, muon spin rotation, and resonant photoemission study of the microscopic magnetic and electronic properties. We find that the films are not simply paramagnetic but that instead the observed behavior can be well explained by the assumption of slowly fluctuating, inhomogeneous magnetic patches with increasing volume fraction as the temperature decreases. At liquid helium temperatures, a large effective magnetization can be easily introduced by the application of moderate magnetic fields, implying that this material is very suitable for proximity coupling to an underlying ferromagnetic insulator or in a heterostructure with transition metal-doped layers. However, the introduction of some charge carriers by the dopants cannot be excluded at least in these highly doped samples. Nevertheless, we find that the magnetic order is not mediated via the conduction channel in these rare earth doped samples and therefore magnetic order and carrier concentration are expected to be independently controllable. This is not generally the case for transition metal doped topological insulators.

cond-mat.mtrl-sci↗

arXiv2018

Evidence for $J_{\rm eff} = 0$ ground state and defect-induced spin glass behaviour in the pyrochlore osmate Y$_{2}$Os$_{2}$O$_{7}$

We present AC and DC magnetometry, heat capacity, muon spin relaxation ($μ$SR) and resonant inelastic X-ray scattering (RIXS) studies of the pyrochlore osmate Y$_2$Os$_2$O$_7$. We observe a non-zero effective moment governed by $\sqrt{f}μ_{\rm{eff}} = 0.417(1)\,μ_{\rm{B}}$ where $f$ is the fraction of Os sites which exhibit a spin, and spin freezing at temperature $T_{\rm f} \simeq 5\,$K, consistent with previous results. The field dependence of magnetisation data shows that the paramagnetic moment is most likely due to large moments $μ_{\rm eff} \simeq 3\,μ_{\rm B}$ on only a small fraction $f \simeq 0.02$ of Os sites. Comparison of single-ion energy level calculations with the RIXS data yields a non-magnetic $J_{\rm eff} = 0$ ground state on the Os$^{4+}$ sites. The spin-orbit interaction, Hund's coupling and trigonal distortion of OsO$_{6}$ octahedra are all important in modelling the experimentally observed spectra. We are able to rule out impurity effects, leaving disorder-related effects such as oxygen non-stoichiometry or site interchange between Os and Y ions as the most plausible explanation for the magnetic response in this material.

cond-mat.str-el↗

arXiv2018

Quantum magnetism in molecular spin ladders probed with muon-spin spectroscopy

We present the results of muon-spin spectroscopy ($μ^{+}$SR) measurements on the molecular spin ladder system (Hpip)$_{2}$CuBr$_{4(1-x)}$Cl$_{4x}$, [Hpip=(C$_{5}$H$_{12}$N)]. Using transverse field $μ^{+}$SR we are able to identify characteristic behaviour in each of the regions of the phase diagram of the $x=0$ strong-rung spin ladder system (Hpip)$_{2}$CuBr$_4$. Comparison of our results to those of the dimer-based molecular magnet Cu(pyz)(gly)(ClO$_{4}$) shows several common features. We locate the crossovers in partially disordered (Hpip)$_{2}$CuBr$_{4(1-x)}$Cl$_{4x}$ ($x=0.05$), where a region of behaviour intermediate between quantum disordered and Luttinger liquid-like is identified. Our interpretation of the results incorporates an analysis of the probable muon stopping states in (Hpip)$_{2}$CuBr$_4$ based on density functional calculations and suggests how the muon plus its local distortion can lead to a local probe unit with good sensitivity to the magnetic state. Using longitudinal field $μ^{+}$SR we compare the dynamic response of the $x=1$ strong-rung material (Hpip)$_{2}$CuCl$_{4}$ to that of the strong-leg material (C$_{7}$H$_{10}$N)$_{2}$CuBr$_{4}$ (known as DIMPY) and demonstrate that our results are in agreement with predictions based on interacting fermionic quasiparticle excitations in these materials.

cond-mat.str-el↗

arXiv2018

Multigap superconductivity in RbCa2Fe4As4F2 investigated using muSR measurements

The superconducting properties of the recently discovered double Fe$_2$As$_2$ layered high-$T_c$ superconductor RbCa$_2$Fe$_4$As$_4$F$_2$ with $T_c\approx$ 30~K have been investigated using magnetization, heat capacity, transverse-field (TF) and zero-field (ZF) muon-spin rotation/relaxation ($μ$SR) measurements. Our low field magnetization measurements and heat capacity (C$_p$) reveal an onset of bulk superconductivity with $T_{\bf c}\sim$ 30.0(4) K. Furthermore, the heat capacity exhibits a jump at $T_{\bf c}$ of $Δ$C$_p$/$T_{\bf c}$=94.6 (mJ/mole-K$^2$) and no clear effect of applied magnetic fields was observed on C$_p$(T) up to 9 T between 2 K and 5 K. Our analysis of the TF-$μ$SR results shows that the temperature dependence of the magnetic penetration depth is better described by a two-gap model, either isotropic $s$+$s$-wave or $s$+$d$-wave than a single gap isotropic $s$-wave or $d$-wave model for the superconducting gap. The presence of two superconducting gaps in RbCa$_2$Fe$_4$As$_4$F$_2$ suggests a multiband nature of the superconductivity, which is consistent with the multigap superconductivity observed in other Fe-based superconductors, including ACa$_2$Fe$_4$As$_4$F$_2$ (A=K and Cs). Furthermore, from our TF-$μ$SR study we have estimated an in-plane penetration depth $λ_{\mathrm{ab}}$$(0)$ =231.5(3) nm, superconducting carrier density $n_s = 7.45 \times 10^{26}~ $m$^{-3}$, and carrier's effective-mass $m^*$ = 2.45\textit{m}$_{e}$. Our ZF $μ$SR measurements do not reveal a clear sign of time reversal symmetry breaking at $T_{\bf c}$, but the temperature dependent relaxation between 150 K and 1.2 K might indicate the presence of spin-fluctuations. The results of our present study have been compared with those reported for other Fe pnictide superconductors.

cond-mat.supr-con↗

arXiv2018

Nodal multigap superconductivity in KCa$_2$Fe$_4$As$_4$F$_2$

We find evidence that the newly discovered Fe-based superconductor KCa$_2$Fe$_4$As$_4$F$_2$ ($T_c~=~33.36(7)$~K) displays multigap superconductivity with line nodes. Transverse field muon spin rotation ($μ$SR) measurements show that the temperature dependence of the superfluid density does not have the expected behavior of a fully-gapped superconductor, due to the lack of saturation at low temperatures. Moreover, the data cannot be well fitted using either single band models or a multiband $s$-wave model, yet are well described by two-gap models with line nodes on either one or both of the gaps. Meanwhile the zero-field $μ$SR results indicate a lack of time reversal symmetry breaking in the superconducting state, but suggest the presence of magnetic fluctuations. These results demonstrate a different route for realizing nodal superconductivity in iron-based superconductors. Here the gap structure is drastically altered upon replacing one of the spacer layers, indicating the need to understand how the pairing state is tuned by changes of the asymmetry between the pnictogens located either side of the Fe planes.

cond-mat.supr-con↗

arXiv2017

Strong coupling of microwave photons to antiferromagnetic fluctuations in an organic magnet

Coupling between a crystal of di(phenyl)-(2,4,6-trinitrophenyl)iminoazanium radicals and a superconducting microwave resonator is investigated in a circuit quantum electrodynamics (circuit QED) architecture. The crystal exhibits paramagnetic behavior above 4~K, with antiferromagnetic correlations appearing below this temperature, and we demonstrate strong coupling at base temperature. The magnetic resonance acquires a field angle dependence as the crystal is cooled down, indicating anisotropy of the exchange interactions. These results show that multispin modes in organic crystals are suitable for circuit QED, offering a platform for their coherent manipulation. They also utilize the circuit QED architecture as a way to probe spin correlations at low temperature.

cond-mat.mes-hall↗

arXiv2017

Local Magnetism and Spin Dynamics of the Frustrated Honeycomb Rhodate Li2RhO3

We report magnetization, heat capacity, 7Li - nuclear magnetic resonance (NMR), and muSR (muon spin roration) measurements on the honeycomb 4d5 spin liquid candidate Li2RhO3. The magnetization in small magnetic fields provides evidence of the partial spin-freezing of a small fraction of Rh4+ -moments at 6 K, whereas the Curie-Weiss behavior above 100 K suggests a pseudo-spin-1/2 paramagnet with a moment of about 2.2 muB. The magnetic specific heat (Cm) exhibits no field dependence and demonstrates the absence of long range magnetic order down to 0.35 K. Cm/T passes through a broad maximum at about 10 K and Cm=T^2 at low temperatures. Measurements of the spin-lattice relaxation rate (1/T1) reveal a gapless slowing down of spin fluctuations upon cooling with 1/T1=T^2.2. The results from NMR and muSR are consistent with a scenario in which a minority of Rh4+ moments are in a ahort-range correlated frozen state and coexist with a majority of moments in a liquid-like state that continue to fluctuate at low temperatures.

cond-mat.str-el↗

arXiv2017

Crystal structure and magnetic modulation in beta-Ce2O2FeSe2

We report a combination of X-ray and neutron diffraction studies, Mossbauer spectroscopy and muon spin relaxation (muSR) measurements to probe the structure and magnetic properties of the semiconducting beta-Ce2O2FeSe2 oxychalcogenide. We report a new structural description in space group Pna21 which is consistent with diffraction data and second harmonic generation measurements and reveal an order-disorder transition on one Fe site at TOD ~ 330 K. Susceptibility measurements, Mossbauer and muSR reveal antiferromagnetic ordering below TN = 86 K and more complex short range order above this temperature. 12 K neutron diffraction data reveal a modulated magnetic structure with q = 0.444 bN*.

cond-mat.mtrl-sci↗