arXiv subjects

M. B. Stone

Publications and source records attributed to M. B. Stone.

At least 55 records · Page 3Linked to original sources

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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arXiv2019

Frustrated Magnetism in Mott Insulating (V$_{1-x}$Cr$_x$)$_2$O$_3$

V2O3 famously features all four combinations of paramagnetic vs antiferromagnetic, and metallic vs insulating states of matter in response to %-level doping, pressure in the GPa range, and temperature below 300 K. Using time-of-flight neutron spectroscopy combined with density functional theory calculations of magnetic interactions, we have mapped and analyzed the inelastic magnetic neutron scattering cross section over a wide range of energy and momentum transfer in the chromium stabilized antiferromagnetic and paramagnetic insulating phases (AFI & PI). Our results reveal an important magnetic frustration and degeneracy of the PI phase which is relieved by the rhombohedral to monoclinic transition at $T_N=185$ K due to a significant magneto-elastic coupling. This leads to the recognition that magnetic frustration is an inherent property of the paramagnetic phase in $\rm (V_{1-x}Cr_x)_2O_3$ and plays a key role in suppressing the magnetic long range ordering temperature and exposing a large phase space for the paramagnetic Mott metal-insulator transition to occur.

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arXiv2019

Evolution of Magnetic Double Helix and Quantum Criticality near a Dome of Superconductivity in CrAs

At ambient pressure CrAs undergoes a first-order transition into a double-helical magnetic state at TN = 265 K, which is accompanied by a structural transition. The recent discovery of pressure-induced superconductivity in CrAs makes it important to clarify the nature of quantum phase transitions out of its coupled structural/helimagnetic order. Here we show, via neutron diffraction on the single-crystal CrAs under hydrostatic pressure (P), that the combined order is suppressed at Pc ~ 10 kbar, near which bulk superconductivity develops with a maximal transition temperature Tc ~ 2 K. We further show that the coupled order is also completely suppressed by phosphorus doping in CrAs1-xPx at a critical xc ~ 0.05, above which inelastic neutron scattering evidenced persistent antiferromagnetic correlations, providing a possible link between magnetism and superconductivity. In line with the presence of antiferromagnetic fluctuations near Pc (xc), the A coefficient of the quadratic temperature dependence of resistivity exhibits a dramatic enhancement as P (x) approaches Pc (xc), around which Res(T) has a non-Fermi-liquid form. Accordingly, the electronic specific-heat coefficient of CrAs1-xPx peaks out around xc. These properties provide clear evidences for quantum criticality, which we interpret as originating from a nearly second-order helimagnetic quantum phase transition that is concomitant with a first-order structural transition. Our findings in CrAs highlight the distinct characteristics of quantum criticality in bad metals, thereby bringing out new insights into the physics of unconventional superconductivity such as occurring in the high-Tc iron pnictides.

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arXiv2018

Low-energy antiferromagnetic spin fluctuations limit the coherent superconducting gap in cuprates

Motivated by recent attention to a potential antiferromagnetic quantum critical point at $x_c\sim 0.19$, we have used inelastic neutron scattering to investigate the low-energy spin excitations in crystals of La$_{2-x}$Sr$_x$CuO$_4$ bracketing $x_c$. We observe a peak in the normal-state spin-fluctuation weight at $\sim20$~meV for both $x=0.21$ and 0.17, inconsistent with quantum critical behavior. The presence of the peak raises the question of whether low-energy spin fluctuations limit the onset of superconducting order. Empirically evaluating the spin gap $Δ_{\rm spin}$ in the superconducting state, we find that $Δ_{\rm spin}$ is equal to the coherent superconducting gap $Δ_c$ determined by electronic spectroscopies. To test whether this is a general result for other cuprate families, we have checked through the literature and find that $Δ_c\leΔ_{\rm spin}$ for cuprates with uniform $d$-wave superconductivity. We discuss the implications of this result.

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arXiv2018

Neutron Scattering Investigation of Rhenium Orbital Ordering in $3d-5d$ Double Perovskite Ca$_2$FeReO$_6$

We have carried out inelastic neutron scattering experiments to study magnetic excitations in ordered double perovskite Ca$_2$FeReO$_6$. We found a well-defined magnon mode with a bandwidth of $\sim$50meV below the ferri-magnetic ordering temperature ($T_c\sim$520K), similar to previously studied Ba$_2$FeReO$_6$. The spin excitation is gapless for most temperatures within the magnetically ordered phase. However, a spin gap of $\sim$10meV opens up below $\sim$150K, which is well below the magnetic ordering temperature but coincides with a previously reported metal-insulator transition and onset of structural distortion. The observed temperature dependence of spin gap provides strong evidence for ordering of Re orbitals at $\sim$150~K, in accordance with earlier proposal put forward by Oikawa $\it{et.\,al}$ based on neutron diffraction [J. Phys. Soc. Jpn., $\bf{72}$, 1411 (2003)] as well as recent theoretical work by Lee and Marianetti [Phys. Rev. B, $\bf{97}$, 045102 (2018)]. The presence of separate orbital and magnetic ordering in Ca$_2$FeReO$_6$ suggests weak coupling between spin and orbital degrees of freedom and hints towards a sub-dominant role played by spin orbit coupling in describing its magnetism. In addition, we observed only one well-defined magnon band near magnetic zone boundary, which is incompatible with simple ferrimagnetic spin waves arising from Fe and Re local moments, but suggests a strong damping of Re magnon mode.

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arXiv2018

Amplitude mode in the planar triangular antiferromagnet Na$_{0.9}$MnO$_2$

Amplitude modes arising from symmetry breaking in materials are of broad interest in condensed matter physics. These modes reflect an oscillation in the amplitude of a complex order parameter, yet are typically unstable and decay into oscillations of the order parameter's phase. This renders stable amplitude modes rare, and exotic effects in quantum antiferromagnets have historically provided a realm for their detection. Here we report an alternate route to realizing amplitude modes in magnetic materials by demonstrating that an antiferromagnet on a two-dimensional anisotropic triangular lattice ($α$-Na$_{0.9}$MnO$_2$) exhibits a long-lived, coherent oscillation of its staggered magnetization field. Our results show that geometric frustration of Heisenberg spins with uniaxial single-ion anisotropy can renormalize the interactions of a dense two-dimensional network of moments into largely decoupled, one-dimensional chains that manifest a longitudinally polarized bound state. This bound state is driven by the Ising-like anisotropy inherent to the Mn$^{3+}$ ions of this compound.

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arXiv2018

Spin-gap and two-dimensional magnetic excitations in Sr2IrO4

Time-of-flight inelastic neutron scattering measurements on Sr2IrO4 single crystals were performed to access the spin Hamiltonian in this canonical Jeff=1/2 spin-orbital Mott insulator. The momentum of magnetic scattering at all inelastic energies that were measured is revealed to be $L$-independent, indicative of idealized two-dimensional in-plane correlations. By probing the in-plane energy and momentum dependence up to ~80 meV we model the magnetic excitations and define a spin-gap of 0.6(1) meV. Collectively the results indicate that despite the strong spin-orbit entangled isospins an isotropic two-dimensional S=1/2 Heisenberg model Hamiltonian accurately describes the magnetic interactions, pointing to a robust analogy with unconventional superconducting cuprates.

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arXiv2018

Physical properties of the trigonal binary compound Nd$_2$O$_3$

We have studied the physical properties of Nd$_2$O$_3$ with neutron diffraction, inelastic neutron scattering, heat capacity, and magnetic susceptibility measurements. Nd$_2$O$_3$ crystallizes in a trigonal structure, with Nd$^{3+}$ ions surrounded by cages of 7 oxygen anions. The crystal field spectrum consists of four excitations spanning the energy range 3-60 meV. The refined eigenfunctions indicate XY-spins in the $ab$ plane. The Curie-Weiss temperature of $θ_{CW}=-23.7(1)$ K was determined from magnetic susceptibility measurements. Heat capacity measurements show a sharp peak at 550 mK and a broader feature centered near 1.5 K. Neutron diffraction measurements show that the 550 mK transition corresponds to long-range anti-ferromagnetic order implying a frustration index of $θ_{CW}/T_N\approx43$. These results indicate that Nd$_2$O$_3$ is a structurally and chemically simple model system for frustration caused by competing interactions with moments with predominate XY anisotropy.

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arXiv2018

Spin gaps in the ordered states of La$_2$LiXO$_6$ (X = Ru, Os) and their relation to distortion of the cubic double perovskite structure in 4$d^3$ and 5$d^3$ magnets

Time-of-flight inelastic neutron scattering measurements have been carried out on polycrystalline samples of the 4$d^3$ and 5$d^3$ double pervoskite antiferromagnets La$_2$LiRuO$_6$ and La$_2$LiOsO$_6$. These reveal the development of an inelastic spin gap in La$_2$LiRuO$_6$ and La$_2$LiOsO$_6$ of $\sim$ 1.8(8) meV and 6(1) meV, below their respective ordering temperatures, $T_N$, $\sim$ 23.8 K and 30 K. The bandwidth of the spin excitations is shown to be $\sim$ 5.7(9) to 12(1) meV, respectively, at low temperatures. Spin gaps are surprising in such magnets as the t$_{2g}$ levels of Ru$^{5+}$ or Os$^{5+}$ are expected to be half-filled, resulting in an anticipated orbital singlet for both materials. We compare these results in monoclinic double perovskites La$_2$LiRuO$_6$ and La$_2$LiOsO$_6$ with those in cubic Ba$_2$YRuO$_6$ and Ba$_2$YOsO$_6$, as well as with those in the more strongly monoclinic La$_2$NaRuO$_6$, La$_2$NaOsO$_6$, and Sr$_2$ScOsO$_6$, and model the inelastic magnetic scattering with linear spin wave theory using minimal anisotropic exchange interactions. We discuss the possible role of the distortion of the face-centered cubic, double perovskite structure on the spin gap formation and geometric frustration in these materials, and show that $T_N$ scales with the top of the spin wave band in all members of these families that display long range order.

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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.

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arXiv2018

Magneto-elastic induced vibronic bound state in the spin ice pyrochlore Ho$_2$Ti$_2$O$_7$

The single ion physics of Ho$_2$Ti$_2$O$_7$ is well-understood to produce strong Ising anisotropy, which is an essential ingredient to its low-temperature spin ice state. We present inelastic neutron scattering measurements on Ho$_2$Ti$_2$O$_7$ that reveal a clear inconsistency with its established single ion Hamiltonian. Specifically, we show that a crystal field doublet near 60~meV is split by approximately 3~meV. Furthermore, this crystal field splitting is not isolated to Ho$_2$Ti$_2$O$_7$ but can also be found in its chemical pressure analogs, Ho$_2$Ge$_2$O$_7$ and Ho$_2$Sn$_2$O$_7$. We demonstrate that the origin of this effect is a vibronic bound state, resulting from the entanglement of a phonon and crystal field excitation. We derive the microscopic Hamiltonian that describes the magneto-elastic coupling and provides a quantitative description of the inelastic neutron spectra.

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arXiv2018

Origin of magnetic excitation gap in double perovskite Sr$_2$FeOsO$_6$

Sr$_2$FeOsO$_6$ is an insulating double perovskite compound which undergoes antiferromagnetic transitions at 140 K ($T_{N1}$) and 67 K ($T_{N2}$). To study the underlying electronic and magnetic interactions giving rise to this behavior we have performed inelastic neutron scattering (INS) and resonant inelastic x-ray scattering (RIXS) experiments on polycrystalline samples of Sr$_2$FeOsO$_6$. The INS data reveal that the spectrum of spin excitations remains ungapped below T$_{N1}$, however below T$_{N2}$ a gap of 6.8 meV develops. The RIXS data reveals splitting of the T$_{2g}$ multiplet consistent with that seen in other 5d$^3$ osmium based double perovskites. Together these results suggest that spin-orbit coupling is important for ground state selection in 3d-5d$^3$ double perovskite materials.

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arXiv2018

Magnetic excitations of the Cu$^{2+}$ quantum spin chain in Sr$_3$CuPtO$_6$

We report the magnetic excitation spectrum as measured by inelastic neutron scattering for a polycrystalline sample of Sr$_3$CuPtO$_6$. Modeling the data by the 2+4 spinon contributions to the dynamical susceptibility within the chains, and with interchain coupling treated in the random phase approximation, accounts for the major features of the powder-averaged structure factor. The magnetic excitations broaden considerably as temperature is raised, persisting up to above 100 K and displaying a broad transition as previously seen in the susceptibility data. No spin gap is observed in the dispersive spin excitations at low momentum transfer, which is consistent with the gapless spinon continuum expected from the coordinate Bethe ansatz. However, the temperature dependence of the excitation spectrum gives evidence of some very weak interchain coupling.

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arXiv2018

Non-Fermi surface nesting driven commensurate magnetic ordering in Fe-doped Sr$_2$RuO$_4$

Sr$_2$RuO$_4$, an unconventional superconductor, is known to possess an incommensurate spin density wave instability driven by Fermi surface nesting. Here we report a static spin density wave ordering with a commensurate propagation vector $q_c$ = (0.25 0.25 0) in Fe-doped Sr$_2$RuO$_4$, despite the magnetic fluctuations persisting at the incommensurate wave vectors $q_{ic}$ = (0.3 0.3 L) as in the parent compound. The latter feature is corroborated by the first principles calculations, which show that Fe substitution barely changes the nesting vector of the Fermi surface. These results suggest that in addition to the known incommensurate magnetic instability, Sr$_2$RuO$_4$ is also in proximity to a commensurate magnetic tendency that can be stabilized via Fe doping.

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arXiv2017

Growth and structural characterization of large superconducting crystals of La$_{2-x}$Ca$_{1+x}$Cu$_2$O$_{6}$

Large crystals of La$_{2-x}$Ca$_{1+x}$Cu$_2$O$_{6}$ (La-Ca-2126) with $x=0.10$ and 0.15 have been grown and converted to bulk superconductors by high-pressure oxygen annealing. The superconducting transition temperature, $T_c$, is as high as 55~K; this can be raised to 60~K by post-annealing in air. Here we present structural and magnetic characterizations of these crystals using neutron scattering and muon spin rotation techniques. While the as-grown, non-superconducting crystals are single phase, we find that the superconducting crystals contain 3 phases forming coherent domains stacked along the $c$ axis: the dominant La-Ca-2126 phase, very thin (1.5 unit-cell) intergrowths of La$_2$CuO$_4$, and an antiferromagnetic La$_8$Cu$_8$O$_{20}$ phase. We propose that the formation and segregation of the latter phases increases the Ca concentration of the La-Ca-2126, thus providing the hole-doping that supports superconductivity.

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$_{7}$.

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arXiv2017

Destabilization of magnetic order in a dilute Kitaev spin liquid candidate

The insulating honeycomb magnet $α$-RuCl$_{3}$ exhibits fractionalized excitiations that signal its proximity to a Kitaev quantum spin liquid (QSL) state, however, at $T=0$, fragile long-range magnetic order arises from non-Kitaev terms in the Hamiltonian. Spin vacancies in the form of Ir$^{3+}$ substituted for Ru are found to destabilize this long-range order. Neutron diffraction and bulk characterization of Ru$_{1-x}$Ir$_{x}$Cl$_{3}$ show that the magnetic ordering temperature is suppressed with increasing $x$ and evidence of zizag magnetic order is absent for $x>0.3$. Inelastic neutron scattering demonstrates that the signature of fractionalized excitations is maintained over the full range of $x$ investigated. The depleted lattice without magnetic order thus hosts a spin-liquid-like ground state that may indicate the relevance of Kitaev physics in the magnetically dilute limit of RuCl$_{3}$.

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arXiv2017

Suppression of the antiferromagnetic order when approaching the superconducting state in a phase-separated crystal of K$_x$Fe$_{2-y}$Se$_2$

We have combined elastic and inelastic neutron scattering techniques, magnetic susceptibility and resistivity measurements to study single-crystal samples of K$_x$Fe$_{2-y}$Se$_2$, which contain the superconducting phase that has a transition temperature of $\sim$31 K. In the inelastic neutron scattering measurements, we observe both the spin-wave excitations resulting from the block antiferromagnetic ordered phase and the resonance that is associated with the superconductivity in the superconducting phase, demonstrating the coexistence of these two orders. From the temperature dependence of the intensity of the magnetic Bragg peaks, we find that well before entering the superconducting state, the development of the magnetic order is interrupted, at $\sim$42 K. We consider this result to be evidence for the physical separation of the antiferromagnetic and superconducting phases; the suppression is possibly due to the proximity effect of the superconducting fluctuations on the antiferromagnetic order.

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