arXiv subjects

J. L. Manson

Publications and source records attributed to J. L. Manson.

At least 19 recordsLinked to original sources

arXiv2026

Heterometallic spin-1/2 quantum magnet under hydrostatic pressure

We investigate the properties of CuVOF$_4$(H$_2$O)$_6$$\cdot$H$_2$O, in which two different spin species, Cu(II) and V(IV), form antiferromagnetic spin-1/2 dimers with weak interdimer coupling provided via hydrogen bonding. Using radio-frequency susceptometry and electron-spin resonance (ESR), we show how the temperature-magnetic field spin-dimer phase diagram evolves as a function of applied hydrostatic pressure and correlate this with pressure-induced changes to the crystal structure. These results, coupled with pressure-tuned DFT calculations, confirm the prior prediction that the primary exchange interaction is mediated via an unusual mechanism in which the V(IV) ions provide considerable spin density to the oxygen that joins the two spins in each dimer and which lies along the Jahn-Teller axis of the Cu(II) ion. In addition, the dissimilarity in the spins that make up each dimer unit leads to a non-linear field dependence of the electronic energy levels as detected in the ESR measurements.

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arXiv2025

Single-ion anisotropy driven chiral magnetic order in a spin-1 antiferromagnetic chain

Chirality in magnetic systems gives rise to a wide range of exotic phenomena, yet its influence in $S=1$ chains remains largely unexplored. Here, we present a comprehensive experimental study of a chiral antiferromagnetic (AFM) $S=1$ chain, [Ni(pym)(H$_{2}$O)$_{4}$]SO$_{4} \cdot$ H$_{2}$O (pym = pyrimidine), where the Ni(II) octahedral orientation exhibits a four-fold chiral periodicity. Muon spin rotation measurements indicate the onset of long-range magnetic order below $T_{\rm N} = 1.82(2)\,\mathrm{K}$. Neutron diffraction measurements reveal a chiral AFM order driven by a chiral modulation of the easy-axis anisotropy direction, rather than the typical scenario of Dzyaloshinskii-Moriya interactions, geometrical frustration or higher-order interactions. Inelastic neutron scattering (INS) measurements reveal dispersive spin-wave excitations well described by linear spin-wave theory, with Hamiltonian parameters $J_{0} = 6.81(1)\,\mathrm{K}$ (intrachain exchange), $J'_{1\rm a} = -0.091(1)\,\mathrm{K}$ (interchain exchange), and $D = -3.02(1)\,\mathrm{K}$ (easy-axis single-ion anisotropy). These parameters are further validated by Monte Carlo simulations of the magnetisation. Additionally, the INS data reveal multiple dispersionless bands, suggesting the presence of further excitations beyond the scope of our linear spin-wave theory.

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arXiv2024

Pseudo-easy-axis anisotropy in antiferromagnetic $S=1$ diamond-lattice systems Ni$X_{2}$(pym)$_{2}$

We investigate the magnetic properties of $S=1$ antiferromagnetic diamond lattice, Ni$X_{2}$(pyrimidine)$_{2}$ ($X$ = Cl, Br), hosting a single-ion anisotropy (SIA) orientation which alternates between neighbouring sites. Through neutron diffraction measurements of the $X$ = Cl compound, the ordered state spins are found to align collinearly along a pseudo-easy-axis, a unique direction created by the intersection of two easy planes. Similarities in the magnetization, exhibiting spin-flop transitions, and the magnetic susceptibility in the two compounds imply that the same magnetic structure and a pseudo-easy-axis is also present for $X$ = Br. We estimate the Hamiltonian parameters by combining analytical calculations and Monte-Carlo (MC) simulations of the spin-flop and saturation field. The MC simulations also reveal that the spin-flop transition occurs when the applied field is parallel to the pseudo-easy-axis. Contrary to conventional easy-axis systems, there exist field directions perpendicular to the pseudo-easy-axis for which the magnetic saturation is approached asymptotically and no symmetry-breaking phase transition is observed at finite fields.

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arXiv2024

Magnetic properties of a staggered $S=1$ chain Ni(pym)(H$_{2}$O)$_{2}$(NO$_{3}$)$_{2}$ with an alternating single-ion anisotropy direction

Materials composed of spin-1 antiferromagnetic (AFM) chains are known to adopt complex ground states which are sensitive to the single-ion-anisotropy (SIA) energy ($D$), and intrachain ($J_{0}$) and interchain ($J'_{i}$) exchange energy scales. While theoretical and experimental studies have extended this model to include various other energy scales, the effect of the lack of a common SIA axis is not well explored. Here we investigate the magnetic properties of Ni(pyrimidine)(H$_{2}$O)$_{2}$(NO$_{3}$)$_{2}$, a chain compound where the tilting of Ni octahedra leads to a 2-fold alternation of the easy-axis directions along the chain. Muon-spin relaxation measurements indicate a transition to long-range order at $T_{\text{N}}=2.3$\,K and the magnetic structure is initially determined to be antiferromagnetic and collinear using elastic neutron diffraction experiments. Inelastic neutron scattering measurements were used to find $J_{0} = 5.107(7)$\,K, $D = 2.79(1)$\,K, $J'_{2}=0.18(3)$\,K and a rhombic anisotropy energy $E=0.19(9)$\,K. Mean-field modelling reveals that the ground state structure hosts spin canting of $ϕ\approx6.5^{\circ}$, which is not detectable above the noise floor of the elastic neutron diffraction data. Monte-Carlo simulation of the powder-averaged magnetization, $M(H)$, is then used to confirm these Hamiltonian parameters, while single-crystal $M(H)$ simulations provide insight into features observed in the data.

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arXiv2023

Asymmetric phase diagram and dimensional crossover in a system of spin-1/2 dimers under applied hydrostatic pressure

We present the magnetic and structural properties of [Cu(pyrazine)$_{0.5}$(glycine)]ClO$_4$ under applied pressure. As previously reported, at ambient pressure this material consists of quasi-two-dimensional layers of weakly coupled antiferromagnetic dimers which undergo Bose-Einstein condensation of triplet excitations between two magnetic field-induced quantum critical points (QCPs). The molecular building blocks from which the compound is constructed give rise to exchange strengths that are considerably lower than those found in other $S = 1/2$ dimer materials, which allows us to determine the pressure evolution of the entire field-temperature magnetic phase diagram using radio-frequency magnetometry. We find that a distinct phase emerges above the upper field-induced transition at elevated pressures and also show that an additional QCP is induced at zero-field at a critical pressure of $p_{\rm c} = 15.7(5)$ kbar. Pressure-dependent single-crystal X-ray diffraction and density functional theory calculations indicate that this QCP arises primarily from a dimensional crossover driven by an increase in the interdimer interactions between the planes. While the effect of quantum fluctuations on the lower field-induced transition is enhanced with applied pressure, quantum Monte Carlo calculations suggest that this alone cannot explain an unconventional asymmetry that develops in the phase diagram.

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arXiv2021

Anomalous magnetic exchange in a dimerized quantum-magnet composed of unlike spin species

We present here a study of the magnetic properties of the antiferromagnetic dimer material CuVOF$_4$(H$_2$O)$_6\cdot$H$_2$O, in which the dimer unit is composed of two different $S = 1/2$ species, Cu(II) and V(IV). An applied magnetic field of $μ_0H_{\rm c1} = 13.1(1)~\rm T$ is found to close the singlet-triplet energy gap, the magnitude of which is governed by the antiferromagnetic intradimer, $J_0 \approx 21~\rm K$, and interdimer, $J' \approx 1~\rm K$, exchange energies, determined from magnetometry and electron-spin resonance measurements. The results of density functional theory (DFT) calculations are consistent with the experimental results and predicts antiferromagnetic coupling along all nearest-neighbor bonds, with the magnetic ground state comprising spins of different species aligning antiparallel to one another, while spins of the same species are aligned parallel. The magnetism in this system cannot be accurately described by the overlap between localized V orbitals and magnetic Cu orbitals lying in the Jahn-Teller (JT) plane, with a tight-binding model based on such a set of orbitals incorrectly predicting that interdimer exchange should be dominant. DFT calculations indicate significant spin density on the bridging oxide, suggesting instead an unusual mechanism in which intradimer exchange is mediated through the O atom on the Cu(II) JT axis.

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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.

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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.

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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.

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arXiv2017

Adiabatic physics of an exchange-coupled spin-dimer system: magnetocaloric effect, zero-point fluctuations, and possible two-dimensional universal behavior

We present the magnetic and thermal properties of the bosonic-superfluid phase in a spin-dimer network using both quasistatic and rapidly-changing pulsed magnetic fields. The entropy derived from a heat-capacity study reveals that the pulsed-field measurements are strongly adiabatic in nature and are responsible for the onset of a significant magnetocaloric effect (MCE). In contrast to previous predictions we show that the MCE is not just confined to the critical regions, but occurs for all fields greater than zero at sufficiently low temperatures. We explain the MCE using a model of the thermal occupation of exchange-coupled dimer spin-states and highlight that failure to take this effect into account inevitably leads to incorrect interpretations of experimental results. In addition, the heat capacity in our material is suggestive of an extraordinary contribution from zero-point fluctuations and appears to indicate universal behavior with different critical exponents at the two field-induced critical points. The data are consistent with a two-dimensional nature of spin excitations in the system.

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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.

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arXiv2015

Magnetism in a family of $S = 1$ square lattice antiferromagnets Ni$X_2$(pyz)$_2$ ($X = $ Cl, Br, I, NCS; pyz = pyrazine)

The crystal structures of Ni$X_2$(pyz)$_2$ ($X$ = Cl (\textbf{1}), Br (\textbf{2}), I (\textbf{3}) and NCS (\textbf{4})) were determined at 298~K by synchrotron X-ray powder diffraction. All four compounds consist of two-dimensional (2D) square arrays self-assembled from octahedral NiN$_4$$X_2$ units that are bridged by pyz ligands. The 2D layered motifs displayed by \textbf{1}-\textbf{4} are relevant to bifluoride-bridged [Ni(HF$_2$)(pyz)$_2$]$Z$F$_6$ ($Z$ = P, Sb) which also possess the same 2D layers. In contrast, terminal $X$ ligands occupy axial positions in \textbf{1}-\textbf{4} and cause a staggering of adjacent layers. Long-range antiferromagnetic order occurs below 1.5 (Cl), 1.9 (Br and NCS) and 2.5~K (I) as determined by heat capacity and muon-spin relaxation. The single-ion anisotropy and $g$ factor of \textbf{2}, \textbf{3} and \textbf{4} are measured by electron spin resonance where no zero--field splitting was found. The magnetism of \textbf{1}-\textbf{4} crosses a spectrum from quasi-two-dimensional to three-dimensional antiferromagnetism. An excellent agreement was found between the pulsed-field magnetization, magnetic susceptibility and $T_\textrm{N}$ of \textbf{2} and \textbf{4}. Magnetization curves for \textbf{2} and \textbf{4} calculated by quantum Monte Carlo simulation also show excellent agreement with the pulsed-field data. \textbf{3} is characterized as a three-dimensional antiferromagnet with the interlayer interaction ($J_\perp$) slightly stronger than the interaction within the two-dimensional [Ni(pyz)$_2$]$^{2+}$ square planes ($J_\textrm{pyz}$).

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arXiv2015

Spin diffusion in the low-dimensional molecular quantum Heisenberg antiferromagnet Cu(pyz)(NO$_{3}$)$_{2}$ detected with implanted muons

We present the results of muon-spin relaxation measurements of spin excitations in the one-dimensional quantum Heisenberg antiferromagnet Cu(pyz)(NO$_{3}$)$_{2}$. Using density-functional theory we propose muon sites and assess the degree of perturbation the muon probe causes on the system. We identify a site involving the muon forming a hydroxyl-type bond with an oxygen on the nitrate group that is sensitive to the characteristic spin dynamics of the system. Our measurements of the spin dynamics show that in the temperature range $T_{\mathrm{N}} J$ and that in the related two-dimensional system Cu(pyz)$_2$(ClO$_4$)$_{2}$.

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arXiv2013

Controlling magnetic order and quantum disorder in one- and zero-dimensional molecule-based magnets

We investigate the structural and magnetic properties of two molecule-based magnets synthesized from the same starting components. Their different structural motifs promote contrasting exchange pathways and consequently lead to markedly different magnetic ground states. Through examination of their structural and magnetic properties we show that [Cu(pyz)(H$_{2}$O)(gly)$_{2}$](ClO$_{4}$)$_{2}$ may be considered a quasi-one-dimensional quantum Heisenberg antiferromagnet while the related compound [Cu(pyz)(gly)](ClO$_{4}$), which is formed from dimers of antiferromagnetically interacting Cu$^{2+}$ spins, remains disordered down to at least 0.03 K in zero field, but shows a field-temperature phase diagram reminiscent of that seen in materials showing a Bose-Einstein condensation of magnons.

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arXiv2013

Evolution of magnetic interactions in a pressure-induced Jahn-Teller driven magnetic dimensionality switch

We present the results of high-field magnetization and muon-spin relaxation measurements on the coordination polymer CuF_2(H_2O)_2(pyrazine) in pressures up to 22.5 kbar. We observe a transition from a quasi-two-dimensional to a quasi-one-dimensional antiferromagnetic phase at 9.1 kbar, driven by a rotation of the Jahn-Teller axis. Long-range antiferromagnetic ordering is seen in both regimes, as well as a phase separation in the critical pressure region. The magnetic dimensionality switching as pressure is increased is accompanied by a halving of the primary magnetic exchange energy J and a fivefold decrease in the ordering temperature T_N. J decreases gradually with pressure in the two-dimensional phase, and then increases in the one-dimensional regime. We relate both effects to the changes in the crystal structure with applied pressure.

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arXiv2012

Magnetic properties of the S=1/2 quasi square lattice antiferromagnet CuF2(H2O)2(pyz) (pyz=pyrazine) investigated by neutron scattering

We have performed elastic and inelastic neutron experiments on single crystal samples of the coordination polymer compound CuF2(H2O)2(pyz) (pyz=pyrazine) to study the magnetic structure and excitations. The elastic neutron diffraction measurements indicate a collinear antiferromagnetic structure with moments oriented along the [0.7 0 1] real-space direction and an ordered moment of 0.60 +/- 0.03 muB/Cu. This value is significantly smaller than the single ion magnetic moment, reflecting the presence of strong quantum fluctuations. The spin wave dispersion from magnetic zone center to the zone boundary points (0.5 1.5 0) and (0.5 0 1.5) can be described by a two dimensional Heisenberg model with a nearest neighbor magnetic exchange constant J2d = 0.934 +/-0.0025 meV. The inter-layer interaction Jperp in this compound is less than 1.5% of J2d. The spin excitation energy at the (0.5 0.5 0.5) zone boundary point is reduced when compared to the (0.5 1 0.5) zone boundary point by ~10.3 +/- 1.4 %. This zone boundary dispersion is consistent with quantum Monte Carlo and series expansion calculations which include corrections for quantum fluctuations to linear spin wave theory.

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arXiv2009

Magnetic properties of the quasi-two-dimensional S = 1/2 Heisenberg antiferromagnet [Cu(pyz)2(HF2)]PF6

We report on high-field magnetization, specific-heat and electron spin resonance (ESR) studies of the quasi-two-dimensional spin-1/2 Heisenberg antiferromagnet [Cu(pyz)2(HF2)]PF6. The frequency-field diagram of ESR modes below TN = 4.38 K is described in the frame of the meanfield theory, confirming a collinear magnetic structure with an easy-plane anisotropy. The obtained results allowed us to determine the anisotropy/exchange interaction ratio, A/J = 0.003, and the upper limit for the inter/intra-plane exchange-interaction ratio, J'/J = 1/16. It is argued that despite the onset of 3D long-range magnetic ordering the magnetic properties of this material (including high-magnetic-field magnetization and non-monotonic field dependence of the Neel temperature) are strongly affected by two-dimensional spin correlations.

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arXiv2009

A new collective phenomenon arising from spin anisotropic perturbations to a Heisenberg square lattice manifested in paramagnetic resonance experiments

We report unexpected behaviour in a family of Cu spin- 1/2 systems, in which an apparent gap in the low energy magneto-optical absorption spectrum opens at low temperature. This previously unreported collective phenomenon arises at temperatures where the energy of the dominant exchange interaction exceeds the thermal energy. Simulations of the observed shifts in electron paramagnetic resonance spectral weight, which include spin anisotropy, reproduce this behavior yielding the magnitude of the spin anisotropy in these compounds.

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