arXiv subjects

C. R. Wiebe

Publications and source records attributed to C. R. Wiebe.

At least 19 recordsLinked to original sources

arXiv2022

Synthesis, physical and magnetic properties of CuAlCr$_4$S$_8$: a new Cr-based breathing pyrochlore

We present the synthesis and physical properties of a new breathing pyrochlore magnet CuAlCr$_4$S$_8$ with the help of synchrotron x-ray diffraction (XRD), magnetization under ambient and applied hydrostatic pressure, heat capacity, and muon spin relaxation/rotation ($μ$SR) measurements. CuAlCr$_4$S$_8$ exhibits positive thermal expansion with concave upward temperature dependence. We observed a sharp antiferromagnetic ordering transition of a purely magnetic nature at 20 K, which shifts by as much as 3.2 K on the application of 600 MPa pressure. The breathing factor (B$_f$ = $J'/J$) in breathing pyrochlores can be an important parameter to tune the magnetic ground states of the pyrochlore lattice. The breathing factor can be modulated through breathing ratio, the ratio of sizes of the two tetrahedra, by using different elements at A and A' sites in the breathing pyrochlore structure. We find that CuAlCr$_4$S$_8$ has a breathing ratio of 1.0663(8), which is comparable to other sulfur breathing pyrochlores.

cond-mat.str-el↗

arXiv2021

Non-magnetic ion site disorder effects on the quantum magnetism of a spin-1/2 equilateral triangular lattice antiferromagnet

With the motivation to study how non-magnetic ion site disorder affects the quantum magnetism of Ba3CoSb2O9, a spin-1/2 equilateral triangular lattice antiferromagnet, we performed DC and AC susceptibility, specific heat, elastic and inelastic neutron scattering measurements on single crystalline samples of Ba2.87Sr0.13CoSb2O9 with Sr doping on non-magnetic Ba2+ ion sites. The results show that Ba2.87Sr0.13CoSb2O9 exhibits (i) a two-step magnetic transition at 2.7 K and 3.3 K, respectively; (ii) a possible canted 120-degree spin structure at zero field with reduced ordered moment as 1.24μB/Co; (iii) a series of spin state transitions for both H // ab-plane and H // c-axis. For H // ab-plane, the magnetization plateau feature related to the up-up-down phase is significantly suppressed; (iv) an inelastic neutron scattering spectrum with only one gapped mode at zero field, which splits to one gapless and one gapped mode at 9 T. All these features are distinctly different from those observed for the parent compound Ba3CoSb2O9, which demonstrates that the non-magnetic ion site disorder (the Sr doping) plays a complex role on the magnetic properties beyond the conventionally expected randomization of the exchange interactions. We propose the additional effects including the enhancement of quantum spin fluctuations and introduction of a possible spatial anisotropy through the local structural distortions.

cond-mat.str-el↗

arXiv2021

Absence of moment fragmentation in the mixed $B$-site pyrochlore Nd$_{2}$GaSbO$_{7}$

Nd-based pyrochlore oxides of the form Nd$_{2}B_{2}$O$_{7}$ have garnered a significant amount of interest owing to the moment fragmentation physics observed in Nd$_{2}$Zr$_{2}$O$_{7}$ and speculated in Nd$_{2}$Hf$_{2}$O$_{7}$. Notably this phenomenon is not ubiquitous in this family, as it is absent in Nd$_{2}$Sn$_{2}$O$_{7}$, which features a smaller ionic radius on the $B$-site. Here, we explore the necessary conditions for moment fragmentation in the Nd pyrochlore family through a detailed study of the mixed $B$-site pyrochlore Nd$_{2}$GaSbO$_{7}$. The $B$-site of this system is characterized by significant disorder and an extremely small average ionic radius. Similarly to Nd$_{2}$Sn$_{2}$O$_{7}$, we find no evidence for moment fragmentation through our bulk characterization and neutron scattering experiments, indicating that chemical pressure (and not necessarily the $B$-site disorder) plays a key role in the presence or absence of this phenomenon in this material family. Surprisingly, the presence of significant $B$-site disorder in Nd$_{2}$GaSbO$_{7}$ does not generate a spin glass ground state and instead the same all-in-all-out magnetic order identified in other Nd pyrochlores is found here.

cond-mat.str-el↗

arXiv2020

Intertwined Magnetic Dipolar and Electric Quadrupolar Correlations in the Pyrochlore Tb$_2$Ge$_2$O$_7$

We present a comprehensive experimental and theoretical study of the pyrochlore Tb$_2$Ge$_2$O$_7$, an exemplary realization of a material whose properties are dominated by competition between magnetic dipolar and electric quadrupolar correlations. The dipolar and quadrupolar correlations evolve over three distinct regimes that we characterize via heat capacity, elastic and inelastic neutron scattering. In the first regime, above $T^*=1.1$ K, significant quadrupolar correlations lead to an intense inelastic mode that cannot be accounted for within a scenario with solely magnetic dipole-dipole correlations. The onset of extended dipole correlations occurs in the intermediate regime, between $T^*=1.1$ K and $T_c = 0.25$ K, with the formation of a collective paramagnetic state characterized by extended ferromagnetic canted spin ice domains. Here, long-range order is impeded not only by the usual frustration operating in classical spin ice systems, but also by a competition between dipolar and quadrupolar correlations. Finally, in the lowest temperature regime, below $T_c=0.25$ K, there is an abrupt and significant increase in the dipole ordered moment. The majority of the ordered moment remains tied up in the ferromagnetic spin ice-like state, but an additional $\mathbf{k}=(0,0,1)$ antiferromagnetic order parameter also develops. Simultaneously, the spectral weight of the inelastic mode, which is a proxy for the quadrupolar correlations, is observed to drop, indicating that dipole order ultimately wins out. Tb$_2$Ge$_2$O$_7$ is therefore a remarkable platform to study intertwined dipolar and quadrupolar correlations in a magnetically frustrated system and provides important insights into the physics of the whole family of terbium pyrochlores.

cond-mat.str-el↗

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.

cond-mat.str-el↗

arXiv2018

Dipolar-Octupolar Ising Antiferromagnetism in Sm$_2$Ti$_2$O$_7$: A Moment Fragmentation Candidate

Over the past two decades, the magnetic ground states of all rare earth titanate pyrochlores have been extensively studied, with the exception of Sm$_2$Ti$_2$O$_7$. This is, in large part, due to the very high absorption cross-section of naturally-occurring samarium, which renders neutron scattering infeasible. To combat this, we have grown a large, isotopically-enriched single crystal of Sm$_2$Ti$_2$O$_7$. Using inelastic neutron scattering, we determine that the crystal field ground state for Sm$^{3+}$ is a dipolar-octupolar doublet with Ising anisotropy. Neutron diffraction experiments reveal that Sm$_2$Ti$_2$O$_7$ orders into the all-in, all-out magnetic structure with an ordered moment of 0.44(7) $μ_B$ below $T_N=0.35$ K, consistent with expectations for antiferromagnetically-coupled Ising spins on the pyrochlore lattice. Zero-field muon spin relaxation measurements reveal an absence of spontaneous oscillations and persistent spin fluctuations down to 0.03 K. The combination of the dipolar-octupolar nature of the Sm$^{3+}$ moment, the all-in, all-out ordered state, and the low-temperature persistent spin dynamics make this material an intriguing candidate for moment fragmentation physics.

cond-mat.str-el↗

arXiv2018

Evidence for negative thermal expansion in the superconducting precursor phase SmFeAsO

The fluorine-doped rare-earth iron oxypnictide series SmFeAsO$_{1-x}$F$_x$ (0 $\leq x \leq$ 0.10) was investigated with high resolution powder x-ray scattering. In agreement with previous studies, the parent compound SmFeAsO exhibits a tetragonal-to-orthorhombic structural distortion at T$\rm{_{S}}$~=~130~K which is rapidly suppressed by $x \simeq$ 0.10 deep within the superconducting dome. The change in unit cell symmetry is followed by a previously unreported magnetoelastic distortion at 120~K. The temperature dependence of the thermal expansion coefficient $α_{V}$ reveals a rich phase diagram for SmFeAsO: (i) a global minimum at 125 K corresponds to the opening of a spin-density wave instability as measured by pump-probe femtosecond spectroscopy whilst (ii) a global maximum at 110 K corresponds to magnetic ordering of the Sm and Fe sublattices as measured by magnetic x-ray scattering. At much lower temperatures than T$\rm{_{N}}$, SmFeAsO exhibits a significant negative thermal expansion on the order of -40~ppm~$\cdot$~K$^{-1}$ in contrast to the behavior of other rare-earth oxypnictides such as PrFeAsO and the actinide oxypnictide NpFeAsO where the onset of $α<$ 0 only appears in the vicinity of magnetic ordering. Correlating this feature with the temperature and doping dependence of the resistivity and the unit cell parameters, we interpret the negative thermal expansion as being indicative of the possible condensation of itinerant electrons accompanying the opening of a SDW gap, consistent with transport measurements.

cond-mat.supr-con↗

arXiv2017

Evidence for the Confinement of Magnetic Monopoles in Quantum Spin Ice

Magnetic monopoles are hypothesised elementary particles connected by Dirac strings that behave like infinitely thin solenoids. Despite decades of searches, free magnetic monopoles and their Dirac strings have eluded experimental detection, although there is substantial evidence for deconfined magnetic monopole quasiparticles in spin ice materials. Here we report the detection of a hierarchy of unequally-spaced magnetic excitations \emph{via} high resolution inelastic neutron spectroscopic measurements on the quantum spin ice candidate Pr$_{2}$Sn$_{2}$O$_{7}$. These excitations are well-described by a simple model of monopole pairs bound by a linear potential with an effective tension of 0.642(8) K~$\cdot$Å$^{-1}$ at 1.65~K. The success of the linear potential model suggests that these low energy magnetic excitations are direct spectroscopic evidence for the confinement of magnetic monopole quasiparticles in the quantum spin ice candidate Pr$_{2}$Sn$_{2}$O$_{7}$.

cond-mat.str-el↗

arXiv2017

Phase Competition in the Palmer-Chalker XY Pyrochlore Er$_2$Pt$_2$O$_7$

We report neutron scattering measurements on Er$_2$Pt$_2$O$_7$, a new addition to the XY family of frustrated pyrochlore magnets. Symmetry analysis of our elastic scattering data shows that Er$_2$Pt$_2$O$_7$ is the first XY pyrochlore to order into the $k=0$, $Γ_7$ magnetic structure (the Palmer-Chalker state), at $T_N = 0.38$ K. This contrasts with its sister XY pyrochlore antiferromagnets Er$_2$Ti$_2$O$_7$ and Er$_2$Ge$_2$O$_7$, both of which order into $Γ_5$ magnetic structures at much higher temperatures, $T_N=1.2$ K and $1.4$ K, respectively. In this temperature range, the magnetic heat capacity of Er$_2$Pt$_2$O$_7$ contains a broad anomaly centered at $T^*=1.5$ K. Our inelastic neutron scattering measurements reveal that this broad heat capacity anomaly sets the temperature scale for strong short-range spin fluctuations. Below $T_N = 0.38$ K, Er$_2$Pt$_2$O$_7$ displays a gapped spin wave spectrum with an intense, flat band of excitations at lower energy and a weak, diffusive band of excitations at higher energy. The flat band is well-described by classical spin wave calculations, but these calculations also predict sharp dispersive branches at higher energy, a striking discrepancy with the experimental data. This, in concert with the strong suppression of $T_N$, is attributable to enhanced quantum fluctuations due to phase competition between the $Γ_7$ and $Γ_5$ states that border each other within a classically predicted phase diagram.

cond-mat.str-el↗

arXiv2016

Relief of Frustration in the Heisenberg Pyrochlore Antiferromagnet Gd$_2$Pt$_2$O$_7$

The gadolinium pyrochlores, Gd$_2B_2$O$_7$, are amongst the best realizations of antiferromagnetically coupled Heisenberg spins on a pyrochlore lattice. We present a magnetic characterization of Gd$_2$Pt$_2$O$_7$, a unique member of this family. Magnetic susceptibility, heat capacity, and muon spin relaxation measurements show that Gd$_2$Pt$_2$O$_7$ undergoes an antiferromagnetic ordering transition at $T_N = 1.6$ K. This transition is strongly first order, as indicated by the sharpness of the heat capacity anomaly, thermal hysteresis in the magnetic susceptibility, and a non-divergent relaxation rate in $μ$SR. The form of the heat capacity below $T_N$ suggests that the ground state is an anisotropic collinear antiferromagnet with an excitation spectrum that is gapped by 0.245(1) meV. The ordering temperature in Gd$_2$Pt$_2$O$_7$, $T_N = 1.6$ K, is a substantial 160% increase from other gadolinium pyrochlores, which have been found to order at 1 K or lower. We attribute this enhancement in $T_N$ to the $B$-site cation, platinum, which, despite being non-magnetic, has a filled $5d$ $t_{2g}$ orbital and an empty $5d$ $e_g$ orbital that can facilitate superexchange. Thus, the magnetic frustration in Gd$_2$Pt$_2$O$_7$ is partially "relieved", thereby promoting magnetic order.

cond-mat.str-el↗

arXiv2016

Statics and dynamics of the highly correlated spin ice Ho2Ge2O7

The pyrochlore Ho2Ge2O7 is a new highly correlated spin ice material. Physical property measurements including x-ray diffraction, dc susceptibility and ac susceptibility, confirm that it shares the distinctive characteristics of other known spin ices. Polarized neutron scattering measurements on a powder sample, combined with reverse Monte Carlo (RMC) refinements, give unique information about the spin ice state in Ho2Ge2O7. RMC refinements are used to fit the powder magnetic diffuse scattering and predict the single crystal magnetic scattering of Ho2Ge2O7, demonstrating consistency with spin ice behavior.

cond-mat.str-el↗

arXiv2016

Universal Dynamic Magnetism in Yb-Pyrochlores with Disparate Ground States

The ytterbium pyrochlore magnets, Yb2B2O7 (B = Sn, Ti, Ge) are well described by S_eff = 1/2 quantum spins decorating a network of corner-sharing tetrahedra and interacting via anisotropic exchange. Structurally, only the non-magnetic B-site cation, and hence, primarily the lattice parameter, is changing across the series. Nonetheless, a range of magnetic behaviors are observed: the low temperature magnetism in Yb2Ti2O7 and Yb2Sn2O7 has ferromagnetic character, while Yb2Ge2O7 displays an antiferromagnetically ordered Neel state at low temperatures. While the static properties of the ytterbium pyrochlores are distinct, inelastic neutron scattering measurements reveal a common character to their exotic spin dynamics. All three ytterbium pyrochlores show a gapless continuum of spin excitations, resembling over-damped ferromagnetic spin waves at low Q. Furthermore, the specific heat of the series also follows a common form, with a broad, high-temperature anomaly followed by a sharp low-temperature anomaly at T_C or T_N. The novel spin dynamics we report correlate strongly with the broad specific heat anomaly only, remaining unchanged across the sharp anomaly. This result suggests that the primary order parameter in the ytterbium pyrochlores associated with the sharp anomaly is "hidden" and not simple magnetic dipole order.

cond-mat.str-el↗

arXiv2016

XY Antiferromagnetic Ground State in the Effective S=1/2 Pyrochlore Yb2Ge2O7

We report neutron scattering and muon spin relaxation measurements (muSR) on the pyrochlore antiferromagnet Yb2Ge2O7. Inelastic neutron scattering was used to probe the transitions between crystal electric field levels, allowing us to determine the eigenvalues and eigenvectors appropriate to the J=7/2 Yb3+ ion in this environment. The crystal electric field ground state doublet in Yb2Ge2O7 corresponds primarily to m_J = +/- 1/2 with local XY anisotropy, consistent with an S_eff = 1/2 description for the Yb moments. muSR measurements reveal the presence of an ordering transition at T_N = 0.57 K with persistent weak dynamics in the ordered state. Finally, we present neutron diffraction measurements that reveal a clear phase transition to the k = (000) Gamma_5 ground state with an ordered magnetic moment of 0.3(1) mu_B per Yb ion. We compare and contrast this phenomenology with the low temperature behavior of Yb2Ti2O7 and Er2Ti2O7, the prototypical S_eff = 1/2 XY pyrochlore magnets.

cond-mat.str-el↗

arXiv2015

Ground state selection in XY pyrochlore antiferromagnets R$_{2}$Ge$_{2}$O$_{7}$ (R = Er, Yb)

Elastic neutron scattering, ac susceptibility, and specific heat experiments on the pyrochlores Er$_{2}$Ge$_{2}$O$_{7}$ and Yb$_{2}$Ge$_{2}$O$_{7}$ show that both systems are antiferromagnetically ordered in the $Γ_5$ manifold. The ground state is a $ψ_{3}$ phase for the Er sample and a $ψ_{2}$ or $ψ_{3}$ phase for the Yb sample, which suggests "Order by Disorder"(ObD) physics. Furthermore, we unify the various magnetic ground states of all known R$_{2}$B$_{2}$O$_{7}$ (R = Er, Yb, B = Sn, Ti, Ge) compounds through the enlarged XY type exchange interaction $J_{\pm}$ under chemical pressure. The mechanism for this evolution is discussed in terms of the phase diagram proposed in the theoretical study [Wong et al., Phys. Rev. B 88, 144402, (2013)].

cond-mat.str-el↗

arXiv2015

Magnetic Frustration in Lead Pyrochlores

The rich phase diagrams of magnetically frustrated pyrochlores have maintained a high level of interest over the past 20 years. To experimentally explore these phase diagrams requires a means of tuning the relevant interactions. One approach to achieve this is chemical pressure, that is, varying the size of the non-magnetic cation. Here, we report on a new family of lead-based pyrochlores A$_2$Pb$_2$O$_7$ (A = Pr, Nd, Gd), which we have characterized with magnetic susceptibility and specific heat. Lead is the largest known possible B-site cation for the pyrochlore lattice. Thus, these materials significantly expand the phase space of the frustrated pyrochlores. Pr$_2$Pb$_2$O$_7$ has an absence of long-range magnetic order down to 400 mK and a spin ice-like heat capacity anomaly at 1.2 K. Thus, Pr$_2$Pb$_2$O$_7$ is a candidate for a quantum spin ice state, despite weaker exchange. Nd$_2$Pb$_2$O$_7$ transitions to a magnetically ordered state at 0.41 K. The Weiss temperature for Nd$_2$Pb$_2$O$_7$ is $θ_{\text{CW}}$ = $-$0.06 K, indicating close competition between ferromagnetic and antiferromagnetic interactions. Gd$_2$Pb$_2$O$_7$ is a Heisenberg antiferromagnet that transitions to long-range magnetic order at 0.81 K, in spite of significant site mixing. Below its ordering transition, we find a $T^{3/2}$ heat capacity dependence in Gd$_2$Pb$_2$O$_7$, confirmation of a ground state that is distinct from other gadolinium pyrochlores. These lead-based pyrochlores provide insight into the effects of weakened exchange on highly frustrated lattices and represent further realizations of several exotic magnetic ground states which can test theoretical models.

cond-mat.str-el↗

arXiv2014

Incipient Ferromagnetism in Tb2Ge2O7: Application of Chemical Pressure to the Enigmatic Spin Liquid, Tb2Ti2O7

The origin of the spin liquid state in Tb$_2$Ti$_2$O$_7$ has challenged experimentalists and theorists alike for nearly 20 years. To improve our understanding of the exotic magnetism in Tb$_2$Ti$_2$O$_7$, we have synthesized a chemical pressure analog, Tb$_2$Ge$_2$O$_7$. Germanium substitution results in a lattice contraction and enhanced exchange interactions. We have characterized the magnetic ground state of Tb$_2$Ge$_2$O$_7$ with specific heat, ac and dc magnetic susceptibility, and polarized neutron scattering measurements. Akin to Tb$_2$Ti$_2$O$_7$, there is no long-range order in Tb$_2$Ge$_2$O$_7$ down to 20 mK. The Weiss temperature of $-$19.2(1) K, which is more negative than that of Tb$_2$Ti$_2$O$_7$, supports the picture of stronger antiferromagnetic exchange. Polarized neutron scattering of Tb$_2$Ge$_2$O$_7$ reveals that at 3.5 K liquid-like correlations dominate in this system. However, below 1 K, the liquid-like correlations give way to intense short-range ferromagnetic correlations with a length scale related to the Tb-Tb nearest neighbor distance. Despite stronger antiferromagnetic exchange, the ground state of Tb$_2$Ge$_2$O$_7$ has ferromagnetic character, in stark contrast to the pressure-induced antiferromagnetic order observed in Tb$_2$Ti$_2$O$_7$.

cond-mat.str-el↗

arXiv2014

Liquid-like correlations in single crystalline Y2Mo2O7: an unconventional spin glass

The spin glass behavior of Y2Mo2O7 has puzzled physicists for nearly three decades. Free of bulk disorder within the resolution of powder diffraction methods, it is thought that this material is a rare realization of a spin glass resulting from weak disorder such as bond disorder or local lattice distortions. Here, we report on the single crystal growth of Y2Mo2O7. Using neutron scattering, we present unique isotropic magnetic diffuse scattering arising beneath the spin glass transition despite having a well-ordered structure at the bulk level. Despite our attempts to model the diffuse scattering using a computationally exhaustive search of a class of simple spin Hamiltonians, we were unable to replicate the experimentally observed energy-integrated (diffuse) neutron scattering. A T^2-temperature dependence in the heat capacity and density functional theory calculations hint at significant frozen degeneracy in both the spin and orbital degrees of freedom resulting from spin-orbital coupling (Kugel-Khomskii type) and random fluctuations in the Mo environment at the local level.

cond-mat.mtrl-sci↗

arXiv2011

AC Susceptibility and Electron Spin Resonance Studies of Spin Dynamics in n Ba$_3$NbFe$_3$Si$_2$O$_{14}$: A Geometrically Frustrated Lattice

We report ac susceptibility and high-frequency electron spin resonance (ESR) measurements on the geometrically frustrated compound Ba$_3$NbFe$_3$Si$_2$O$_{14}$ with the Néel temperature $T_N=27 K$. An unusually large frequency-dependence of ac susceptibility in the temperature range of 20 - 100 K reveals a spin-glass-like behavior, signalling the presence of frustration related slow magnetic fluctuations. ESR experiments show a multi-step magnetic and spin chirality ordering process. For temperatures above 30 K, the weak temperature dependence of the ESR linewidth $ΔH_{pp}\propto T^{-p}$ with $p=0.8$ evidences the development of short-range correlated spin clusters. The critical broadening with $p =1.8$, persisting down to 14 K, indicates the coexistence of the short-range ordered spin clusters within a helically ordered state. Below 9.5 K, the anomalously large decrease of the linewidth reveals the stabilization of a long-range ordered state with one chirality.

cond-mat.str-el↗