arXiv subjects

K. A. Ross

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

At least 19 recordsLinked to original sources

arXiv2024

Dipolar spin ice regime proximate to an all-in-all-out Néel ground state in the dipolar-octupolar pyrochlore Ce$_2$Sn$_2$O$_7$

The dipolar-octupolar (DO) pyrochlores, R$_2$M$_2$O$_7$ (R = Ce, Sm, Nd), are key players in the search for realizable novel quantum spin liquid (QSL) states as a large parameter space within the DO pyrochlore phase diagram is theorized to host QSL states of both dipolar and octupolar nature. New single crystals and powders of Ce$_2$Sn$_2$O$_7$, synthesized by hydrothermal techniques, present an opportunity for a new characterization of the exchange parameters in Ce$_2$Sn$_2$O$_7$ using the near-neighbor $XYZ$ model Hamiltonian associated with DO pyrochlores. Utilizing quantum numerical linked cluster expansion fits to heat capacity and magnetic susceptibility measurements, and classical Monte Carlo calculations to the diffuse neutron diffraction of the new hydrothermally grown Ce$_2$Sn$_2$O$_7$ samples, we place Ce$_2$Sn$_2$O$_7$'s ground state within the ordered dipolar all-in-all-out (AIAO) Néel phase, with quantum Monte Carlo calculations showing a transition to long-range order at temperatures below those accessed experimentally. Indeed, our new neutron diffraction measurements on the hydrothermally grown Ce$_2$Sn$_2$O$_7$ powders show a broad signal at low scattering wave vectors, reminiscent of a \textit{dipolar} spin ice, in striking contrast from previous powder neutron diffraction on samples grown from solid-state synthesis, which found diffuse scattering at high scattering wave vectors associated with magnetic {\it octupoles} and suggested an octupolar quantum spin ice state. We conclude that new hydrothermally grown Ce$_2$Sn$_2$O$_7$ samples host a finite-temperature proximate dipolar spin ice phase, above the expected transition to AIAO Néel order.

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arXiv2023

Quantum Spin Ice Response to a Magnetic Field in the Dipole-Octupole Pyrochlore Ce$_2$Zr$_2$O$_7$

We report new heat capacity measurements on single crystal Ce$_2$Zr$_2$O$_7$ down to $\sim$ 0.1 K in a magnetic field along the $[1,\bar{1}, 0]$ direction. These new measurements show that the broad hump in the zero-field heat capacity moves higher in temperature with increasing field strength and is split into two humps by the $[1,\bar{1}, 0]$ field at $\sim$ 2 T. These separate features are due to the decomposition of the pyrochlore lattice into effectively decoupled chains for fields in this direction: one set of chains ($α$-chains) is polarized by the field while the other ($β$-chains) remains free. Our theoretical modelling suggests that the $β$-chains are close to a critical state, with nearly-gapless excitations. We also report new elastic and inelastic neutron scattering measurements on single crystal Ce$_2$Zr$_2$O$_7$ in $[1, \bar{1}, 0]$ and $[0, 0, 1]$ magnetic fields at temperatures down to 0.03 K. The elastic scattering behaves consistently with the formation of independent chains for a $[1, \bar{1}, 0]$ field, while the $[0, 0, 1]$ field produces a single field-induced magnetic Bragg peak at $(0, 2, 0)$ and equivalent wavevectors, indicating a polarized spin ice for fields above $\sim$ 3 T. For both $[1, \bar{1}, 0]$ and $[0, 0, 1]$ fields, our inelastic neutron scattering results show an approximately-dispersionless continuum of scattering that increases in both energy and intensity with increasing field strength. By modelling the complete set of experimental data using numerical linked cluster and semiclassical molecular dynamics calculations, we demonstrate the dominantly multipolar nature of the exchange interactions in Ce$_2$Zr$_2$O$_7$ and the smallness of the parameter $θ$ which controls the mixing between dipolar and octupolar degrees of freedom. These results support previous estimates of the microscopic exchange parameters.

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arXiv2022

Reply to "Comment on: 'Case for a U(1)$_π$ Quantum Spin Liquid Ground State in the Dipole-Octupole Pyrochlore $\mathrm{Ce}_2\mathrm{Zr}_2\mathrm{O}_7$' "

In his comment [arXiv:2209.03235], S. W. Lovesey argues that our analysis of neutron scattering experiments performed on Ce$_2$Zr$_2$O$_7$ is invalid. Lovesey argues that we have not properly accounted for the higher-order multipolar contributions to the magnetic scattering and that our use of pseudospin-$1/2$ operators to describe the scattering is inappropriate. In this reply, we show that the multipolar corrections discussed by Lovesey only become significant at scattering wavevectors exceeding those accessed in our experiments. This in no way contradicts or undermines our work, which never claimed a direct observation of scattering from higher-order multipoles. We further show that Lovesey's objections to our use of pseudospins are unfounded, and that the pseudospin operators are able to describe all magnetic scattering processes at the energy scale of our experiments, far below the crystal field gap. Finally, we comment on certain assumptions in Lovesey's calculations of the scattering amplitude which are inconsistent with experiment.

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arXiv2022

Single-ion properties of the transverse-field Ising model material CoNb$_2$O$_6$

CoNb$_2$O$_6$ is one of the few materials that is known to approximate the one-dimensional transverse-field Ising model (1D-TFIM) near its quantum critical point. It has been inferred that Co$^{2+}$ acts as a pseudo-spin 1/2 with anisotropic exchange interactions that are largely Ising-like, enabling the realization of the TFIM. However, the behavior of CoNb$_2$O$_6$ is known to diverge from the ideal TFIM under transverse magnetic fields that are far from the quantum critical point, requiring the consideration of additional anisotropic, bond-dependent (Kitaev-like) terms in the microscopic pseudo-spin 1/2 Hamiltonian. These terms are expected to be controlled in part by single-ion physics, namely the wavefunction for the pseudo-spin 1/2 angular momentum doublet. Here, we present the results of both inelastic neutron scattering measurements and electron paramagnetic resonance spectroscopy on CoNb$_2$O$_6$, which elucidate the single-ion physics of Co$^{2+}$ in CoNb$_2$O$_6$ for the first time. We find that the system is well-described by an intermediate spin-orbit coupled Hamiltonian, and the ground state is a well-isolated Kramers doublet with an anisotropic $g$-tensor. We provide the approximate wavefunctions for this doublet, which we expect will be useful in theoretical investigations of the anisotropic exchange interactions.

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arXiv2021

The case for a U(1)$_π$ Quantum Spin Liquid Ground State in the Dipole-Octupole Pyrochlore Ce$_2$Zr$_2$O$_7$

The Ce$^{3+}$ pseudospin-$\frac{1}{2}$ degrees of freedom in the pyrochlore magnet Ce$_2$Zr$_2$O$_7$ are known to possess dipole-octupole (DO) character, making it a candidate for novel quantum spin liquid (QSL) ground states at low temperatures. We report new polarized neutron diffraction at low temperatures, as well as heat capacity ($C_p$) measurements on single crystal Ce$_2$Zr$_2$O$_7$. The former bears both similarities and differences from that measured in the canonical dipolar spin ice compound Ho$_2$Ti$_2$O$_7$, while the latter rises sharply at low temperatures, initially plateauing near 0.08 K, before falling off towards a high temperature zero beyond 3 K. Above $\sim$0.5 K, the $C_p$ data set can be fit to the results of a quantum numerical linked cluster (NLC) calculation, carried out to 4$^{\mathrm{th}}$ order, that allows estimates for the terms in the near-neighbour XYZ Hamiltonian expected for such DO pyrochlore systems. Fits of the same theory to the temperature dependence of the magnetic susceptibility and unpolarized neutron scattering complement this analysis. A comparison between the resulting best fit NLC calculation and the polarized neutron diffraction shows both agreement and discrepancies, mostly in the form of zone-boundary diffuse scattering in the non-spin flip channel, which are attributed to interactions beyond near-neighbours. The lack of an observed thermodynamic anomaly and the constraints on the near-neighbour XYZ Hamiltonian suggest that Ce$_2$Zr$_2$O$_7$ realizes a U(1)$_π$ QSL state at low temperatures, and one that likely resides near the boundary between dipolar and octupolar character.

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arXiv2021

Microscopics of Quantum Annealing in the Disordered Dipolar Ising Ferromagnet LiHo$_{x}$Y$_{1-x}$F$_4$

Quantum annealing (QA) refers to an optimization process that uses quantum fluctuations to find the global minimum of a rugged energy landscape with many local minima. Conceptually, QA is often framed in the context of the disordered transverse field Ising model, in which a magnetic field applied perpendicular to the Ising axis tunes the quantum fluctuations and enables the system to tunnel through energy barriers, and hence reach the ground state more quickly. A solid state material closely related to this model, LiHo$_{0.45}$Y$_{0.55}$F$_4$, was shown to exhibit faster dynamics after a QA protocol, compared to thermal annealing (TA), but little is known about the actual process of optimization involved or the nature of the spin correlations in the state that is reached. Here, we report on the microscopics of QA in this material using diffuse magnetic neutron scattering. Comparing a QA to a TA protocol that reach the same end-point, we find very similar final diffuse scattering which consists of pinch-point scattering, largely consistent with critical scattering near a phase boundary in the dipolar Ising ferromagnetic model. However, comparing the time evolution at the end of the protocols, we find that the spin correlations evolve more significantly after TA, suggesting that QA produces a state closer to equilibrium. We also observe experimental evidence that the transverse field produces random fields, which had been previously predicted for this material and studied in other contexts. Thus, while the material does exhibit a quantum speedup under quantum annealing conditions, it is not a simple annealing problem; the energy landscape being optimized is changing as the optimization proceeds.

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arXiv2021

Low Temperature Domain Wall Freezing and Non-Equilibrium Dynamics in the Transverse-Field Ising Model Material CoNb$_2$O$_6$

CoNb$_2$O$_6$ is a rare realization of the transverse field Ising model (TFIM), making it a useful tool for studying both equilibrium and non-equilibrium many-body quantum physics. Despite a large body of work dedicated to characterizing this material, details of the ordered states in the presence of relatively weak transverse fields have not been discussed in detail. Here, we present a detailed study of CoNb$_2$O$_6$ via ac susceptibility measurements in order to further characterize its low temperature behavior in the presence of a transverse field. Specifically, we call attention to an unconventional freezing transition in zero-field below T$_F$ = 1.2~K, occurring \emph{within} the well-known commensurate antiferromagnetic (CAFM) state that onsets at $T_{N2}$ = 1.9~K. We performed a series of transverse-field quenches into this frozen state, which resulted in a slowly relaxing susceptibility, $χ^{\prime}(t)$, that followed a logarithmic decay within the time range measured. We discuss the frozen state in the context of the freezing of previously discussed "free" chains arising from domain walls between the four degenerate sublattices of the CAFM state. We also attempted to observe Kibble-Zurek scaling by quenching the transverse field into the frozen state at different rates. This produced a null result; the behavior can be fully explained by coarsening of domains over the timescale of the quenches. The absence of a clear Kibble-Zurek scaling is itself surprising, given the proposed ubiquity of the phenomenon for general second order phase transitions.

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arXiv2021

Magnetic Properties of the Ising-like Rare Earth Pyrosilicate: D-Er$_{2}$Si$_{2}$O$_{7}$

Ising-like spin-1/2 magnetic materials are of interest for their ready connection to theory, particularly in the context of quantum critical behavior. In this work we report detailed studies of the magnetic properties of a member of the rare earth pyrosilicate family, D-Er$_{2}$Si$_{2}$O$_{7}$, which is known to display a highly anisotropic Ising-like g-tensor and effective spin-1/2 magnetic moments. We used powder neutron diffraction, powder inelastic neutron spectroscopy (INS), and single crystal AC susceptibility to characterize its magnetic properties. Neutron diffraction enabled us to determine the magnetic structure below the known transition temperature ($T_{N}$ = 1.9 K) in zero field, confirming that the magnetic state is a four-sublattice antiferromagnetic structure with two non-collinear Ising axes, as was previously hypothesized. Our powder INS data revealed a gapped excitation at zero field, consistent with anisotropic (possibly Ising) exchange. An applied field of 1 T produces a mode softening, which is consistent with a field-induced second order phase transition. To assess the relevance of D-Er$_{2}$Si$_{2}$O$_{7}$ to the transverse field Ising model, we performed AC susceptibility measurements on a single crystal with the magnetic field oriented in the direction transverse to the Ising axes. This revealed a transition at 2.65 T at 0.1 K, a field significantly higher than the mode-softening field observed by powder INS, showing that the field-induced phase transitions are highly field-direction dependent as expected. These measurements suggest that D-Er$_{2}$Si$_{2}$O$_{7}$ may be a candidate for further exploration related to the transverse field Ising model.

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arXiv2021

Néel Ordering in the Distorted Honeycomb Pyrosilicate: C-Er$_{2}$Si$_{2}$O$_{7}$

The rare-earth pyrosilicate family of compounds (RE$_{2}$Si$_{2}$O$_{7}$) hosts a variety of polymorphs, some with honeycomb-like geometries of the rare-earth sublattices, and the magnetism has yet to be deeply explored in many of the cases. Here we report on the ground state properties of C-Er$_{2}$Si$_{2}$O$_{7}$. C-Er$_{2}$Si$_{2}$O$_{7}$ crystallizes in the C2/m space group and the Er$^{3+}$ atoms form a distorted honeycomb lattice in the $a$-$b$ plane. We have utilized specific heat, DC susceptibility, and neutron diffraction measurements to characterize C-Er$_{2}$Si$_{2}$O$_{7}$. Our specific heat and DC susceptibility measurements show signatures of antiferromagnetic ordering at 2.3 K. Neutron powder diffraction confirms this transition temperature and the relative intensities of the magnetic Bragg peaks are consistent with a collinear Néel state in the magnetic space group C2'/m, with ordered moment of 6.61 $μ_{B}$ canted 13$^{\circ}$ away from the $c$-axis toward the $a$-axis. These results are discussed in relation to the isostructural quantum dimer magnet compound Yb$_{2}$Si$_{2}$O$_{7}$.

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arXiv2021

Understanding Reentrance in Frustrated Magnets: the Case of the Er$_2$Sn$_2$O$_7$ Pyrochlore

Reentrance, the return of a system from an ordered phase to a previously encountered less-ordered one as a controlled parameter is continuously varied, is a recurring theme found in disparate physical systems, from condensed matter to black holes. While diverse in its many incarnations and generally unsuspected, the cause of reentrance at the microscopic level is often not investigated thoroughly. Here, through detailed characterization and theoretical modeling, we uncover the microscopic mechanism behind reentrance in the strongly frustrated pyrochlore antiferromagnet Er$_2$Sn$_2$O$_7$. Taking advantage of the recent advance in rare earth stannate single crystal synthesis, we use heat capacity measurements to expose that Er$_2$Sn$_2$O$_7$ exhibits multiple instances of reentrance in its magnetic field $B$ vs. temperature $T$ phase diagram for magnetic fields along three cubic high symmetry directions. Through classical Monte Carlo simulations, mean field theory and classical linear spin-wave expansions, we argue that the origins of the multiple occurrences of reentrance observed in Er$_2$Sn$_2$O$_7$ are linked to soft modes. Depending on the field direction, these arise either from a direct $T=0$ competition between the field-evolved ground states, or from a field-induced enhancement of the competition with a distinct zero-field antiferromagnetic phase. In both scenarios, the phase competition enhances thermal fluctuations which entropically stabilize a specific ordered phase. This results in an increased transition temperature for certain field values and thus the reentrant behavior. Our work represents a detailed examination into the mechanisms responsible for reentrance in a frustrated magnet and may serve as a template for the interpretation of reentrant phenomena in other physical systems.

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arXiv2020

Unravelling competing microscopic interactions at a phase boundary: a single crystal study of the metastable antiferromagnetic pyrochlore Yb$_{2}$Ge$_{2}$O$_{7}$

We report inelastic neutron scattering measurements from our newly synthesized single crystals of the structurally metastable antiferromagnetic pyrochlore Yb$_{2}$Ge$_{2}$O$_{7}$. We determine the four symmetry-allowed nearest-neighbor anisotropic exchange parameters via fits to linear spin wave theory supplemented by fits of the high-temperature specific heat. The exchange parameters so-determined are strongly correlated to the values determined for the $g$-tensor components, as previously observed for the related Yb pyrochlore Yb$_{2}$Ti$_{2}$O$_{7}$. To address this issue, we directly determined the $g$-tensor from electron paramagnetic resonance of 1% Yb-doped Lu$_{2}$Ge$_{2}$O$_{7}$, thus enabling an unambiguous determination of the exchange parameters. Our results show that Yb$_{2}$Ge$_{2}$O$_{7}$ resides extremely close to the classical phase boundary between an antiferromagnetic $Γ_5$ phase and a splayed ferromagnet phase. By juxtaposing our results with recent ones on Yb$_{2}$Ti$_{2}$O$_{7}$, our work illustrates that the Yb pyrochlore oxides represent ideal systems for studying quantum magnets in close proximity to classical phase boundaries.

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arXiv2019

Partial Antiferromagnetic Helical Order in Fe$_3$PO$_4$O$_3$

Magnetic frustration in Fe$_3$PO$_4$O$_3$ has been shown to produce to an unusual magnetic state below T$_N = 163$ K, where incommensurate antiferromagnetic order is restricted to nanosized needle-like domains, as inferred from neutron powder diffraction. Here we show using single-crystal neutron diffraction that Fe$_3$PO$_4$O$_3$ does not exhibit a preferred ordering wavevector direction in the $ab$ plane despite having a well-defined ordering wavevector length. This results in the observation of continuous rings of scattering rather than satellite Bragg peaks. The lack of a preferred incommensurate ordering wavevector direction can be understood in terms of an antiferromagnetic Heisenberg model with nearest-neighbor ($J_1$) and second-neighbor ($J_2$) interactions, which produces a quasi-degenerate manifold of ordering wavevectors. This state appears to be similar to the partially ordered phase of MnSi, but in Fe$_3$PO$_4$O$_3$ arises in a frustrated antiferromagnet rather than a chiral ferromagnet.

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arXiv2019

Novel Strongly Spin-Orbit Coupled Quantum Dimer Magnet: Yb$_2$Si$_2$O$_7$

The quantum dimer magnet (QDM) is the canonical example of quantum magnetism. The QDM state consists of entangled nearest-neighbor spin dimers and often exhibits a field-induced triplon Bose-Einstein condensate (BEC) phase. We report on a new QDM in the strongly spin-orbit coupled, distorted honeycomb-lattice material Yb$_2$Si$_2$O$_7$. Our single crystal neutron scattering, specific heat, and ultrasound velocity measurements reveal a gapped singlet ground state at zero field with sharp, dispersive excitations. We find a field-induced magnetically ordered phase reminiscent of a BEC phase, with exceptionally low critical fields of $H_{c1} \sim 0.4$ T and $H_{c2} \sim 1.4$ T. Using inelastic neutron scattering in an applied magnetic field we observe a Goldstone mode (gapless to within $δE$ = 0.037 meV) that persists throughout the entire field-induced magnetically ordered phase, suggestive of the spontaneous breaking of U(1) symmetry expected for a triplon BEC. However, in contrast to other well-known cases of this phase, the high-field ($μ$$_0$$H\geq1.2$T) part of the phase diagram in Yb$_2$Si$_2$O$_7$ is interrupted by an unusual regime signaled by a change in the field dependence of the ultrasound velocity and magnetization, as well as the disappearance of a sharp anomaly in the specific heat. These measurements raise the question of how anisotropy in strongly spin-orbit coupled materials modifies the field induced phases of QDMs.

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arXiv2019

Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce$_2$Zr$_2$O$_7$

Neutron scattering measurements on the pyrochlore magnet Ce$_2$Zr$_2$O$_7$ reveal an unusual crystal field splitting of its lowest $J$=5/2 multiplet, such that its ground state doublet is composed of m$_J$=$\pm$3/2, giving these doublets a dipole - octupole (DO) character with local Ising anisotropy. Its magnetic susceptibility shows weak antiferromagnetic correlations with $θ_{CW}$=-0.4(2)K, leading to a naive expectation of an All-In, All-Out ordered state at low temperatures. Instead our low energy inelastic neutron scattering measurements show a dynamic quantum spin ice state, with suppressed scattering near |$\textbf{Q}$|=0, and no long range order at low temperatures. This is consistent with recent theory predicting symmetry enriched U(1) quantum spin liquids for such DO doublets decorating the pyrochlore lattice. Finally, we show that disorder, especially oxidation of powder samples, is important in Ce$_2$Zr$_2$O$_7$ and could play an important role in the low temperature behaviour of this material.

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arXiv2018

Low frequency spin dynamics in XY quantum spin ice Yb$_2$Pt$_2$O$_7$

The XY pyrochlore Yb$_2$Ti$_2$O$_7$, with pseudo spin 1/2 at the Yb$^{3+}$ site, has been celebrated as potential host for the quantum spin ice state. The substitution of non-magnetic Ti with Pt gives Yb$_2$Pt$_2$O$_7$, a system with remarkably similar magnetic properties. The large nuclear gyromagnetic ratio ($γ_{n}/2 π= 9.15$~MHz/T) of $^{195}$Pt makes Yb$_2$Pt$_2$O$_7$ an ideal material for NMR investigation of its unconventional magnetic properties. Based on the $^{195}$Pt nuclear spin-lattice relaxation rate $1/T_1$ and the magnetic specific heat $C_{p}$ measured in a broad range of magnetic field $B_{ext}$, we demonstrate that the field-induced magnon gap linearly decreases with $B_{ext}$ but additional low energy mode of spin excitations emerge below $\sim 0.5$~T.

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arXiv2018

Behavior of the breathing pyrochlore lattice Ba$_3$Yb$_2$Zn$_5$O$_{11}$ in applied magnetic field

The breathing pyrochlore lattice material Ba$_3$Yb$_2$Zn$_5$O$_{11}$ exists in the nearly decoupled limit, in contrast to most other well-studied breathing pyrochlore compounds. As a result, it constitutes a useful platform to benchmark theoretical calculations of exchange interactions in insulating Yb$^{3+}$ magnets. Here we study Ba$_3$Yb$_2$Zn$_5$O$_{11}$ at low temperatures in applied magnetic fields as a further probe of the physics of this model system. Experimentally, we consider the behavior of polycrystalline samples of Ba$_3$Yb$_2$Zn$_5$O$_{11}$ with a combination of inelastic neutron scattering and heat capacity measurements down to 75 mK and up to fields of 10 T. Consistent with previous work, inelastic neutron scattering finds a level crossing near 3 T, but no significant dispersion of the spin excitations is detected up to the highest applied fields. Refinement of the theoretical model previously determined at zero field can reproduce much of the inelastic neutron scattering spectra and specific heat data. A notable exception is a low temperature peak in the specific heat near 0.1 K. This may indicate the scale of interactions between tetrahedra or may reflect undetected disorder in Ba$_3$Yb$_2$Zn$_5$O$_{11}$.

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arXiv2018

Short range order in the quantum XXZ honeycomb lattice material BaCo$_2$(PO$_4$)$_2$

We present observations of highly frustrated quasi two-dimensional (2D) magnetic correlations in the honeycomb lattice layers of the S$_{eff}$ = 1/2 compound $γ$-BaCo$_2$(PO$_4$)$_2$ ($γ$-BCPO). Specific heat shows a broad peak comprised of two weak kink features at $T_{N1} \sim$ 6 K and $T_{N2} \sim$ 3.5 K, the relative weights of which can be modified by sample annealing. Neutron powder diffraction measurements reveal short range quasi-2D order that is established below $T_{N1}$ and $T_{N2}$, at which two separate, incompatible, short range magnetic orders onset: commensurate antiferromagnetic correlations with correlation length $ξ_c = 60\pm2$ Å\ ($T_{N1}$) and in quasi-2D helical domains with $ξ_h = 350 \pm 11$ Å\ ($T_{N2}$). The ac magnetic susceptibility response lacks frequency dependence, ruling out spin freezing. Inelastic neutron scattering data on $γ$-BCPO is compared with linear spin wave theory, and two separate parameter regions of the XXZ $J_1$-$J_2$-$J_3$ model with ferromagnetic nearest-neighbor exchange $J_1$ are favored, both near regions of high classical degeneracy. High energy coherent excitations ($\sim 10$ meV) persist up to at least 40 K, suggesting strong in-plane correlations persist above $T_N$. These data show that $γ$-BCPO is a rare highly frustrated, quasi-2D S$_{eff}$ = 1/2 honeycomb lattice material which resists long range magnetic order and spin freezing.

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arXiv2017

Tuning the antiferromagnetic helical pitch length and nanoscale domain size in Fe$_3$PO$_4$O$_3$ by magnetic dilution

The insulating magnetic material Fe3PO4O3 features a non-centrosymmetric lattice composed of Fe^{3+} triangular units. Frustration, due to competing near neighbor ($J_1$) and next nearest neighbor ($J_2$) antiferromagnetic interactions, was recently suggested to be the origin of an antiferromagnetic helical ground state with unusual needle-like nanoscale magnetic domains in Fe3PO4O3. Magnetic dilution is shown here to tune the ratio of these magnetic interactions, thus providing deeper insight into this unconventional antiferromagnet. Dilution of the Fe^{3+} lattice in Fe3PO4O3 was accomplished by substituting non-magnetic Ga^{3+} to form the solid solution series Fe_{3-x}Ga_xPO4O3 with $x = 0.012, 0.06, 0.25, 0.5, 1.0, 1.5$. Magnetic susceptibility and neutron powder diffraction data from this series are presented. A continuous decrease of the both the helical pitch length and the domain size is observed with increasing dilution up to at least $x = 0.25$, while for $x \ge 0.5$, the compounds lack long range magnetic order entirely. The decrease in the helical pitch length with increasing $x$ can be qualitatively understood by reduction of the ratio of $J_2/J_1$ in the Heisenberg model, consistent with mean field considerations. Intriguingly, the magnetic correlation length in the $ab$ plane remains nearly equal to the pitch length for each value of $x \le 0.25$, showing that the two quantities are intrinsically connected in this unusual antiferromagnet.

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