arXiv subjects

P. J. Baker

Publications and source records attributed to P. J. Baker.

At least 19 recordsLinked to original sources

arXiv2025

Anisotropic skyrmion and multi-$q$ spin dynamics in centrosymmetric Gd$_2$PdSi$_3$

Skyrmions are particle-like vortices of magnetization with non-trivial topology, which are usually stabilized by Dzyaloshinskii-Moriya interactions (DMI) in noncentrosymmetric bulk materials. Exceptions are centrosymmetric Gd- and Eu-based skyrmion-lattice (SkL) hosts with zero DMI, where both the SkL stabilization mechanisms and magnetic ground states remain controversial. We address these here by investigating both the static and dynamical spin properties of the centrosymmetric SkL host Gd$_2$PdSi$_3$ using muon spectroscopy ($μ$SR). We find that spin fluctuations in the non-coplanar SkL phase are highly anisotropic, implying that spin anisotropy plays a prominent role in stabilizing this phase. We also observe strongly-anisotropic spin dynamics in the ground-state (IC-1) incommensurate magnetic phase of the material, indicating that it hosts a meron-like multi-$q$ structure. In contrast, the higher-field, coplanar IC-2 phase is found to be single-$q$ with nearly-isotropic spin dynamics.

cond-mat.str-el↗

arXiv2024

Spinons in a new Shastry-Sutherland lattice magnet Pr$_2$Ga$_2$BeO$_7$

Identifying the elusive spinon excitations in quantum spin liquid (QSL) materials is what scientists have long sought for. Recently, thermal conductivity ($κ$) has emerged to be a decisive probe because the fermionic nature of spinons leads to a characteristic nonzero linear $κ_0/T$ term while approaching zero Kelvin. So far, only a few systems have been reported to exhibit such term. Here, we report a $κ_0/T \approx$ 0.01 WK$^{-2}$m$^{-1}$, the largest $κ_0/T$ value ever observed in magnetic oxide QSL candidates, in a new quantum magnet Pr$_2$Ga$_2$BeO$_7$ with a Shastry-Sutherland lattice (SSL). Its QSL nature is further supported by the power-law temperature dependence of the specific heat, a plateau of muon spin relaxation rate, and gapless inelastic neutron spectra. Our theoretical analysis reveals that the introduction of XY spin anisotropy is the key for Pr$_2$Ga$_2$BeO$_7$ to be the first QSL realized on the SSL, after more than four decades of extensive studies on this celebrated magnetically frustrated lattice.

cond-mat.str-el↗

arXiv2022

Valence bond glass state in the 4$d^1$ fcc antiferromagnet Ba$_2$LuMoO$_6$

$B$-site ordered 4$d^1$ and 5$d^1$ double perovskites have a number of potential novel ground states including multipolar order, quantum spin liquids and valence bond glass states. These arise from the complex interactions of spin-orbital entangled $J_{eff}$ = 3/2 pseudospins on the geometrically frustrated fcc lattice. The 4$d^1$ Mo$^{5+}$ perovskite Ba$_2$YMoO$_6$ has been suggested to have a valence bond glass ground state. Here we report on the low temperature properties of powder samples of isostructural Ba$_2$LuMoO$_6$: the only other known cubic 4$d^1$ perovskite with one magnetic cation. Our muon spectroscopy experiments show that magnetism in this material remains dynamic down to 60 mK without any spin freezing or magnetic order. A singlet-triplet excitation with a gap of $Δ$ = 28 meV is observed in inelastic neutron scattering. These results are interpreted as a disordered valence bond glass ground state similar to Ba$_2$YMoO$_6$. Our results highlight the differences of the 4$d^1$ double perovskites in comparison to cubic 5$d^1$ analogues, which have both magnetic and multipolar order.

cond-mat.str-el↗

arXiv2021

Muon sites in PbF2 and YF3: decohering environments and the role of anion Frenkel defects

Muons implanted into ionic fluorides often lead to a so-called F-mu-F state, in which the time evolution of the muon spin contains information about the geometry and nature of the muon site. Nuclei more distant from the muon than the two nearest-neighbor fluorine ions result in decoherence of the F-mu-F system and this can yield additional quantitative information about the state of the muon. We demonstrate how this can be applied to the determination of muon sites within the ionic fluorides alpha-PbF2 and YF3 which contain fluoride ions in different crystallographic environments. Our results can be used to distinguish between different crystal phases and reveal the presence of anion Frenkel defects in alpha-PbF2.

cond-mat.stat-mech↗

arXiv2021

Magnetic order and disorder in a quasi-two-dimensional quantum Heisenberg antiferromagnet with randomized exchange

We present an investigation of the effect of randomizing exchange strengths in the $S=1/2$ square lattice quasi-two-dimensional quantum Heisenberg antiferromagnet (QuinH)$_2$Cu(Cl$_{x}$Br$_{1-x}$)$_{4}\cdot$2H$_2$O (QuinH$=$Quinolinium, C$_9$H$_8$N$^+$), with $0\leq x \leq 1$. Pulsed-field magnetization measurements allow us to estimate an effective in-plane exchange strength $J$ in a regime where exchange fosters short-range order, while the temperature $T_{\mathrm{N}}$ at which long range order (LRO) occurs is found using muon-spin relaxation, allowing us to construct a phase diagram for the series. We evaluate the effectiveness of disorder in suppressing $T_{\mathrm{N}}$ and the ordered moment size and find an extended disordered phase in the region $0.4 \lesssim x \lesssim 0.8$ where no magnetic order occurs, driven by quantum effects of the exchange randomness.

cond-mat.str-el↗

arXiv2020

From magnetic order to quantum disorder: a $μ$SR study of the Zn-barlowite series of $S={\frac{1}{2}}$ kagomé antiferromagnets, Zn$_{x}$Cu$_{4-x}$(OH)$_{6}$FBr

We report a comprehensive muon spectroscopy study of the Zn-barlowite series of $S={\frac{1}{2}}$ kagomé antiferromagnets, Zn$_x$Cu$_{4-x}$(OH)$_{6}$FBr, for $x=0.00$ to $0.99(1)$. By combining muon spin relaxation and rotation measurements with state-of-the-art density-functional theory muon-site calculations, we observe the formation of both $μ$--F and $μ$--OH complexes in Zn-barlowite. From these stopping sites, implanted muon spins reveal the suppression of long-range magnetic order into a possible quantum spin liquid state upon increasing concentration of Zn-substitution. In the parent compound ($x=0$), static long-range magnetic order below $T_{\mathsf{N}}=15$ K manifests itself in the form of spontaneous oscillations in the time-dependent muon asymmetry signal consistent with the dipolar fields expected from the calculated muon stopping sites and the previously determined magnetic structure of barlowite. Meanwhile, in the $x=1.0$ end-member of the series---in which antiferromagnetic kagomé layers of Cu$^{2+}$ $S={\frac{1}{2}}$ moments are decoupled by diamagnetic Zn$^{2+}$ ions---we observe that dynamic magnetic moment fluctuations persist down to at least 50 mK, indicative of a quantum disordered ground state. We demonstrate that this crossover from a static to dynamic magnetic ground state occurs for compositions of Zn-barlowite with $x>0.5$, which bears resemblance to dynamical behaviour of the widely studied Zn-paratacamite series that contains the quantum spin liquid candidate herbertsmithite.

cond-mat.str-el↗

arXiv2019

Magnetic Microphase Inhomogeneity as a Thermodynamic Precursor of Ground State Phase Separation in Weakly Coupled Spin-$\frac{3}{2}$ Chains

$γ$-CoV$_{2}$O$_{6}$ is a quasi one-dimensional spin-$\frac{3}{2}$ magnet that possesses two distinct magnetic orders in the ground state with modulation vectors $k_\mathrm{1}$ = ($\frac{1}{2}$, 0, 0) and $k_\mathrm{2}$ = ($\frac{1}{4}$, 0, -$\frac{1}{4}$), respectively. Here, we use muon spin relaxation and rotation to reveal the thermodynamics of the magnetic phase separation in this compound. In the paramagnetic (PM) region, short-range correlated spin clusters emerge at $T_\mathrm{m}$ $\simeq$ 26 K at the $\it{partial}$ expense of the PM volume. Upon further cooling, we show that these emergent clusters become spatially coherent at $T_\mathrm{N2}$ = 7.5 K and eventually form the $k_\mathrm{2}$ order at $T^{\star}$ = 5.6 K, while the remaining PM spins are driven into the $k_\mathrm{1}$ state at $T_\mathrm{N1}$ = 6.6 K. These results stress magnetic microphase inhomogeneity as a thermodynamic precursor for the ground state phase separation in weakly coupled spin-$\frac{3}{2}$ chains.

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↗

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

Opposites Attract, Muons as Direct Probes for Iodide Diffusion in Methyl Ammonium Lead Iodide

The volume of research into organo-lead hailde perovskites is increasing rapidly, with perovskite solar cell efficiencies reaching as high as 22 percent. There is considerable evidence that mobile ions in the perovskite strongly influence the properties of the solar cell, with the majority of studies carried out on whole cells under bias. Here we use muon spin relaxation to directly probe iodide diffusion in methyl ammonium lead iodide (MAPI). This is the first time that has been used to detect iodide diffusion in any material and the results provide valuable insight into the movement of ions in lead halide perovskites. The experiment was carried out in the dark with no external biases applied and allowed us to calculate a diffusion coefficient of 1.6 x10-14 cm2/s for iodide in MAPI at 300 K.

cond-mat.mtrl-sci↗

arXiv2017

Long-range dynamical magnetic order and spin tunneling in the cooperative paramagnetic states of the pyrochlore analogous spinel antiferromagnets CdYb2X4 (X = S, Se)

Magnetic systems with spins sitting on a lattice of corner sharing regular tetrahedra have been particularly prolific for the discovery of new magnetic states for the last two decades. The pyrochlore compounds have offered the playground for these studies, while little attention has been comparatively devoted to other compounds where the rare earth R occupies the same sub-lattice, e.g. the spinel chalcogenides CdR2X4 (X = S, Se). Here we report measurements performed on powder samples of this series with R = Yb using specific heat, magnetic susceptibility, neutron diffraction and muon-spin-relaxation measurements. The two compounds are found to be magnetically similar. They long-range order into structures described by the Γ_5 irreducible representation. The magnitude of the magnetic moment at low temperature is 0.77 (1) and 0.62 (1) mu_B for X = S and Se, respectively. Persistent spin dynamics is present in the ordered states. The spontaneous field at the muon site is anomalously small, suggesting magnetic moment fragmentation. A double spin-flip tunneling relaxation mechanism is suggested in the cooperative paramagnetic state up to 10 K. The magnetic space groups into which magnetic moments of systems of corner-sharing regular tetrahedra order are provided for a number of insulating compounds characterized by null propagation wavevectors.

cond-mat.str-el↗

arXiv2017

Slow spin tunneling in the paramagnetic phase of the pyrochlore Nd2Sn2O7

The insulating pyrochlore compound Nd2Sn2O7 has been shown to undergo a second order magnetic phase transition at Tc ~ 0.91 K to a noncoplanar all-in--all-out magnetic structure of the Nd3+ magnetic moments. An anomalously slow paramagnetic spin dynamics has been evidenced from neutron backscattering and muon spin relaxation (muSR). In the case of muSR this has been revealed through the strong effect of a 50 mT longitudinal field on the spin-lattice relaxation rate. Here, motivated by a recent successful work performed for Yb2Ti2O7 and Yb2Sn2O7, analyzing the shape of the muSR longitudinal polarization function, we substantiate the existence of extremely slow paramagnetic spin dynamics in the microsecond time range for Nd2Sn2O7. Between 1.7 and 7 K, this time scale is temperature independent. This suggests a double spin-flip tunneling relaxation mechanism to be at play, probably involving spin substructures such as tetrahedra. Unexpectedly, the standard deviation of the field distribution at the muon site increases as the system is cooled. This exotic spin dynamics is in sharp contrast with the dynamics above 100 K which is driven by the Orbach relaxation mechanism involving single Nd3+ magnetic moments.

cond-mat.str-el↗

arXiv2017

Coexistence of magnetism and superconductivity in separate layers of the iron-based superconductor Li_{1-x}Fe_{x}(OH)Fe_{1-y}Se

The magnetic properties attributed to the hydroxide layer of Li1-xFex(OH)Fe1-ySe have been elucidated by the study of superconducting and nonsuperconducting members of this family. Both ac magnetometry and muon spin relaxation measurements of nonsuperconductors find a magnetic state existing below approximately 10 K which exhibits slow relaxation of magnetization. This magnetic state is accompanied by a low-temperature heat capacity anomaly present in both superconducting and nonsuperconducting variants suggesting that the magnetism persists into the superconducting state. The estimated value of magnetic moment present within the hydroxide layer supports a picture of a glassy magnetic state, probably comprising clusters of iron ions of varying cluster sizes distributed within the lithium hydroxide layer.

cond-mat.supr-con↗

arXiv2017

Quantum-critical spin dynamics in a Tomonaga-Luttinger liquid studied with muon-spin relaxation

We demonstrate that quantum-critical spin dynamics can be probed in high magnetic fields using muon-spin relaxation ($μ^{+}$SR). Our model system is the strong-leg spin ladder bis(2,3-dimethylpyridinium) tetrabromocuprate (DIMPY). In the gapless Tomonaga-Luttinger liquid phase we observe finite-temperature scaling of the $μ^{+}$SR $1/T_1$ relaxation rate which allows us to determine the Luttinger parameter $K$. We discuss the benefits and limitations of local probes compared with inelastic neutron scattering.

cond-mat.str-el↗

arXiv2016

Commensurate lattice distortion in the layered titanium oxypnictides Na$_{2}$Ti$_{2}Pn_{2}$O ($Pn =$ As, Sb) determined by X-ray diffraction

We report single crystal X-ray diffraction measurements on Na$_2$Ti$_{2}Pn_{2}$O ($Pn$ = As, Sb) which reveal a charge superstructure that appears below the density wave transitions previously observed in bulk data. From symmetry-constrained structure refinements we establish that the associated distortion mode can be described by two propagation vectors, ${\bf q}_{1} = (1/2, 0, l)$ and ${\bf q}_{2} = (0, 1/2, l)$, with $l=0$ (Sb) or $l = 1/2$ (As), and primarily involves in-plane displacements of the Ti atoms perpendicular to the Ti--O bonds. The results provide direct evidence for phonon-assisted charge density wave order in Na$_2$Ti$_{2}Pn_{2}$O and identify a proximate ordered phase that could compete with superconductivity in doped BaTi$_{2}$Sb$_{2}$O.

cond-mat.supr-con↗

arXiv2016

Novel magnetism on a honeycomb lattice in a-RuCl3 studied by muon spin rotation

Muon spin rotation measurements have been performed on a powder sample of a-RuCl3, a layered material which previously has been proposed to be a quantum magnet on a honeycomb lattice close to a quantum spin liquid ground state. Our data reveal two distinct phase transitions at 11 K and 14 K which we interpret as originating from the onset of three-dimensional order and in-plane magnetic order, respectively. We identify, with the help of density functional theory calculations, likely muon stopping sites and combine these with dipolar field calculations to show that the two measured muon rotation frequencies are consistent with two inequivalent muon sites within a zig-zag antiferromagnetic structure proposed previously.

cond-mat.str-el↗

arXiv2016

Structural and magnetic properties of the 5$d^2$ double perovskites Sr$_2 B$ReO$_6$ ($B$ $=$ Y, In)

We have performed magnetic susceptibility, heat capacity, neutron powder diffraction, and muon spin relaxation experiments to investigate the magnetic ground states of the 5$d^2$ double perovskites Sr$_2$YReO$_6$ and Sr$_2$InReO$_6$. We find that Sr$_2$YReO$_6$ is a spin glass, while Sr$_2$InReO$_6$ hosts a non-magnetic singlet state. By making detailed comparisons with other 5$d^2$ double perovskites, we argue that a delicate interplay between spin-orbit coupling, non-cubic crystal fields, and exchange interactions plays a key role in the great variation of magnetic ground states observed for this family of materials.

cond-mat.str-el↗

arXiv2015

The magnetic ground state of two isostructual polymeric quantum magnets, [Cu(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$ and [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$, investigated with neutron powder diffraction

The magnetic ground state of two isostructural coordination polymers (i) the quasi two-dimensional S = 1/2 square-lattice antiferromagnet [Cu(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$; and (ii) a new compound [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$, were examined with neutron powder diffraction measurements. We find the ordered moments of the Heisenberg S = 1/2 Cu(II) ions in [Cu(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$ are 0.6(1)$μ_{B}$, whilst the ordered moments for the Co(II) ions in [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$ are 3.02(6)$μ_{B}$. For Cu(II), this reduced moment indicates the presence of quantum fluctuations below the ordering temperature. We show from heat capacity and electron spin resonance measurements, that due to the crystal electric field splitting of the S = 3/2 Co(II) ions in [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$, this isostructual polymer also behaves as an effective spin-half magnet at low temperatures. The Co moments in [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$ show strong easy-axis anisotropy, neutron diffraction data which do not support the presence of quantum fluctuations in the ground state and heat capacity data which are consistent with 2D or close to 3D spatial exchange anisotropy.

cond-mat.str-el↗