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T. G. Perring

Publications and source records attributed to T. G. Perring.

At least 19 recordsLinked to original sources

Low energy phonons in single crystal ZrW$_{2}$O$_{8}$

ZrW$_{2}$O$_{8}$ is the prototypical example of a material exhibiting negative thermal expansion (NTE). It is now widely accepted that in ZrW$_{2}$O$_{8}$, and in many other framework materials exhibiting NTE, a collection of low energy phonon modes, as opposed to just one or two, are responsible for the anomalous thermal properties. However, quantitative verification and analysis of the density functional theory (DFT) calculations which underpin this proposal are still lacking. In particular, probing the low energy phonons directly throughout reciprocal space using inelastic neutron scattering, as opposed to other techniques which only probe the Brillouin zone center, is technically challenging and hence rarely done. Here we report inelastic neutron scattering measurements in a large number of Brillouin zones over a 400 K temperature range. We find excellent agreement between DFT calculations and experimental data at low temperature. However, the shifts in phonon modes predicted by DFT due to the reduction in lattice parameter (warming) are not observed. This is most likely due to counteractive anharmonic effects, which we verified using finite temperature molecular dynamics (MD) calculations. Notwithstanding, both DFT and MD results are consistent with NTE in ZrW$_{2}$O$_{8}$ arising from the tension effect, and by extension this explanation is supported by the neutron scattering results.

cond-mat.mtrl-sci

Low-energy Spin Dynamics of Quantum Spin Liquid Candidate $NaYbSe_{2}$

The family of rare earth chalcogenides $ARECh_{2}$ (A = alkali or monovalent ions, RE = rare earth, and Ch = O, S, Se, and Te) appears as an inspiring playground for studying quantum spin liquids (QSL). The crucial low-energy spin dynamics remain to be uncovered. By employing muon spin relaxation ($μ$SR) and zero-field (ZF) AC susceptibility down to 50 mK, we are able to identify the gapless QSL in $NaYbSe_{2}$, a representative member with an effective spin-1/2, and explore its unusual spin dynamics. The ZF $μ$SR experiments unambiguously rule out spin ordering or freezing in $NaYbSe_{2}$ down to 50 mK, two orders of magnitude smaller than the exchange coupling energies. The spin relaxation rate, $λ$, approaches a constant below 0.3 K, indicating finite spin excitations featured by a gapless QSL ground state. This is consistently supported by our AC susceptibility measurements. The careful analysis of the longitudinal field (LF) $μ$SR spectra reveals a strong spatial correlation and a temporal correlation in the spin-disordered ground state, highlighting the unique feature of spin entanglement in the QSL state. The observations allow us to establish an experimental H-T phase diagram. The study offers insight into the rich and exotic magnetism of the rare earth family.

cond-mat.str-el

Carrier Tuning of Stoner Ferromagnetism in ThCr$_{\mathbf{2}}$Si$_{\mathbf{2}}$-Structure Cobalt Arsenides

CaCo$_{2-y}$As$_2$ is an unusual itinerant magnet with signatures of extreme magnetic frustration. The conditions for establishing magnetic order in such itinerant frustrated magnets, either by reducing frustration or increasing electronic correlations, is an open question. Here we use results from inelastic neutron scattering and magnetic susceptibility measurements and density functional theory calculations to show that hole doping in Ca(Co$_{1-x}$Fe$_{x}$)$_{2-y}$As$_{2}$ suppresses magnetic order by quenching the magnetic moment while maintaining the same level of magnetic frustration. The suppression is due to tuning the Fermi energy away from a peak in the electronic density of states originating from a flat conduction band. This results in the complete elimination of the magnetic moment by $x\approx0.25$, providing a clear example of a Stoner-type transition.

cond-mat.str-el

Spin texture induced by non-magnetic doping and spin dynamics in 2D triangular lattice antiferromagnet h-Y(Mn,Al)O3

Novel effects induced by nonmagnetic impurities in frustrated magnets and quantum spin liquid represent a highly nontrivial and interesting problem. A theoretical proposal of extended modulated spin structures induced by doping of such magnets, distinct from the well-known skyrmions has attracted significant interest. Here, we demonstrate that nonmagnetic impurities can produce such extended spin structures in h-YMnO3, a triangular antiferromagnet with noncollinear magnetic order. Using inelastic neutron scattering (INS), we measured the full dynamical structure factor in Al-doped h-YMnO3 and confirmed the presence of magnon damping with a clear momentum dependence. Our theoretical calculations can reproduce the key features of the INS data, supporting the formation of the proposed spin textures. As such, our study provides the first experimental confirmation of the impurity-induced spin textures. It offers new insights and understanding of the impurity effects in a broad class of noncollinear magnetic systems.

cond-mat.str-el

Charge disproportionation and nano phase separation in $R$SrNiO$_4$

We have successfully grown centimeter-sized layered $R$SrNiO$_4$ single crystals under high oxygen pressures of 120 bar by the floating zone technique. This enabled us to perform neutron scattering experiments where we observe close to quarter-integer magnetic peaks below $\sim$77 K that are accompanied by steep upwards dispersing spin excitations. Within the high-frequency Ni-O bond stretching phonon dispersion, a softening at the propagation vector for a checkerboard modulation can be observed. Together with our spin wave simulations these observations reveal that this Ni$^{3+}$ system exhibits charge disproportionation with charges segregating into a checkerboard pattern within a nano phase separation scenario rather than showing a Jahn-Teller effect.

cond-mat.str-el

Momentum-dependent magnon lifetime in the metallic non-collinear triangular antiferromagnet CrB2

Non-collinear magnetic order arises for various reasons in several magnetic systems and exhibits interesting spin dynamics. Despite its ubiquitous presence, little is known of how magnons, otherwise stable quasiparticles, decay in these systems, particularly in metallic magnets. Using inelastic neutron scattering, we examine the magnetic excitation spectra in a metallic non-collinear antiferromagnet CrB$_{2}$, in which Cr atoms form a triangular lattice and display incommensurate magnetic order. Our data show intrinsic magnon damping and continuum-like excitations that cannot be explained by linear spin wave theory. The intrinsic magnon linewidth $Γ(q,E_{q})$ shows very unusual momentum dependence, which our analysis shows to originate from the combination of two-magnon decay and the Stoner continuum. By comparing the theoretical predictions with the experiments, we identify where in the momentum and energy space one of the two factors becomes more dominant. Our work constitutes a rare comprehensive study of the spin dynamics in metallic non-collinear antiferromagnets. It reveals, for the first time, definite experimental evidence of the higher-order effects in metallic antiferromagnets.

cond-mat.str-el

Crystalline Electric-Field Excitations in Quantum Spin Liquids Candidate $NaYbSe_{2}$

Very recently we revealed a large family of triangular lattice quantum spin liquid candidates named rare-earth chalcogenides, which features a high-symmetry structure without structural/charge disorders and spin impurities, and may serve as an ideal platform exploring spin liquid physics. The knowledge of crystalline electric-field (CEF) excitations is an essential step to explore the fundamental magnetism of rare-earth spin systems. Here we employed inelastic neutron scattering (INS) and Raman scattering (RS) to carry out a comprehensive CFE investigation on $NaYbSe_{2}$, a promising representative of the family. By comparison with its nonmagnetic compound $NaLuSe_{2}$, we are able to identify the CEF excitations at 15.8, 24.3 and 30.5 meV at 5K. The selected cuts of the INS spectra are well re-produced with a large anisotropy of $g$ factors ($g_{ab}:g_{c}\sim3:1$). Further, the CEF excitations are explained well by our calculations based on the point charge model. Interestingly, $NaYbSe_{2}$ exhibits an unusual CEF shift to higher energies with increasing temperatures, and the Raman mode close to the first CEF excitation shows an anomalously large softening with decreasing temperatures. The absence of the anomalies in $NaLuSe_{2}$ clearly demonstrates a CEF-phonon coupling not reported in the family. It can be understood in term of the weaker electronegativity of Se. The fact that the smallest first CEF excitation in the sub-family of $NaYbCh_{2}$ is $\sim$ 180K (Ch=O, S, Se), guarantees that the sub-family can be strictly described with an effective S=1/2 picture at sufficiently low temperatures. Interestingly the CEF-phonon coupling revealed here may present alternative possibilities to manipulate the spin systems.

cond-mat.str-el

Temperature dependence of the $(π,0)$ anomaly in the excitation spectrum of the 2D quantum Heisenberg antiferromagnet

It is well established that in the low-temperature limit, the two-dimensional quantum Heisenberg antiferromagnet on a square lattice (2DQHAFSL) exhibits an anomaly in its spectrum at short-wavelengths on the zone-boundary. In the vicinity of the $(π,0)$ point the pole in the one-magnon response exhibits a downward dispersion, is heavily damped and attenuated, giving way to an isotropic continuum of excitations extending to high energies. The origin of the anomaly and the presence of the continuum are of current theoretical interest, with suggestions focused around the idea that the latter evidences the existence of spinons in a two-dimensional system. Here we present the results of neutron inelastic scattering experiments and Quantum Monte Carlo calculations on the metallo-organic compound Cu(DCOO)$_2\cdot 4$D$_2$O (CFTD), an excellent physical realisation of the 2DQHAFSL, designed to investigate how the anomaly at $(π,0)$ evolves up to finite temperatures $T/J\sim2/3$. Our data reveal that on warming the anomaly survives the loss of long-range, three-dimensional order, and is thus a robust feature of the two-dimensional system. With further increase of temperature the zone-boundary response gradually softens and broadens, washing out the $(π,0)$ anomaly. This is confirmed by a comparison of our data with the results of finite-temperature Quantum Monte Carlo simulations where the two are found to be in good accord. At lower energies, in the vicinity of the antiferromagnetic zone centre, there was no significant softening of the magnetic excitations over the range of temperatures investigated.

cond-mat.str-el

Kagome modes, a new route to ultralow thermal conductivity?

From next generation gas turbines to scavenging waste heat from car exhausts, finding new materials with ultra-low thermal conductivity ($κ$) has the potential to lead to large gains in device efficiency. Crystal structures with inherently low $κ$ are consequently desirable, but candidate materials are rare and often difficult to make. Using first principles calculations and inelastic neutron scattering we have studied the pyrochlore La$_2$Zr$_2$O$_7$ which has been proposed as a next generation thermal barrier. We find that there is a highly anharmonic, approximately flat, vibrational mode associated with the kagome planes. Our results suggest that this mode is responsible for the low thermal conductivity observed in the pyrochlores and that kagome compounds will be a fruitful place to search for other low $κ$ materials.

cond-mat.mtrl-sci

Upgrade to the MAPS neutron time-of-flight chopper spectrometer

The MAPS direct geometry time-of-flight chopper spectrometer at the ISIS pulsed neutron and muon source has been in operation since 1999 and its novel use of a large array of position-sensitive neutron detectors paved the way for a later generations of chopper spectrometers around the world. Almost two decades of experience of user operations on MAPS, together with lessons learned from the operation of new generation instruments, led to a decision to perform three parallel upgrades to the instrument. These were to replace the primary beamline collimation with supermirror neutron guides, to install a disk chopper, and to modify the geometry of the poisoning in the water moderator viewed by MAPS. Together these upgrades were expected to increase the neutron flux substantially, to allow more flexible use of repetition rate multiplication and to reduce some sources of background. Here we report the details of these upgrades, and compare the performance of the instrument before and after their installation, as well as to Monte Carlo simulations. These illustrate that the instrument is performing in line with, and in some respects in excess of, expectations. It is anticipated that the improvement in performance will have a significant impact on the capabilities of the instrument. A few examples of scientific commissioning are presented to illustrate some of the possibilities.

physics.ins-det

Coexistence of ferromagnetic and stripe antiferromagnetic spin fluctuations in SrCo$_2$As$_2$

We use inelastic neutron scattering to study energy and wave vector dependence of spin fluctuations in SrCo$_2$As$_2$, derived from SrFe$_{2-x}$Co$_x$As$_2$ iron pnictide superconductors. Our data reveals the coexistence of antiferromagnetic (AF) and ferromagnetic (FM) spin fluctuations at wave vectors $\textbf{Q}_{\rm AF}$=(1,0) and $\textbf{Q}_{\rm FM}$=(0,0)/(2,0), respectively. By comparing neutron scattering results with those of dynamic mean field theory calculation and angle-resolved photoemission spectroscopy experiments, we conclude that both AF and FM spin fluctuations in SrCo$_2$As$_2$ are closely associated with a flat band of the $e_g$ orbitals near the Fermi level, different from the $t_{2g}$ orbitals in superconducting SrFe$_{2-x}$Co$_x$As$_2$. Therefore, Co-substitution in SrFe$_{2-x}$Co$_x$As$_2$ induces a $t_{2g}$ to $e_g$ orbital switching, and is responsible for FM spin fluctuations detrimental to the singlet pairing superconductivity.

cond-mat.str-el

Magnetic excitations in bulk multiferroic two-dimensional triangular lattice antiferromagnet (Lu,Sc)FeO$_3$

Non-collinear two-dimensional triangular lattice antiferromagnets (2D TLAF) are currently an area of very active research due to their unique magnetic properties, which lead to non-trivial quantum effects that experimentally manifest themselves in the spin excitation spectra. Recent examples of such insulating 2D TLAF include (Y,Lu)MnO$_3$, LiCrO$_2$, and CuCrO$_2$. Hexagonal LuFeO3 is a recently synthesized 2D TLAF which exhibits properties of an ideal multiferroic material, partially because of the high spin ($S=5/2$) and strong magnetic super-exchange interactions. We report the full range of spin dynamics in a bulk single crystal of (Lu$_{0.6}$Sc$_{0.4}$)FeO$_3$ (Sc doping to stabilize the hexagonal structure) measured via time-of-flight inelastic neutron scattering. Modeling with linear spin wave theory yields a nearest neighbor exchange coupling of $J$ = 4.0(2) meV (DFT calculations for $h$-LuFeO$_3$ predicted a value of 6.31 meV) and anisotropy values of $K_D$ = 0.17(1) meV (easy plane) and $K_A$~=~-0.05(1)~meV (local easy axis). It is observed that the magnon bandwidth of the spin wave spectra is twice as large for $h$-(Lu,Sc)FeO$_3$ as it is for $h$-LuMnO$_3$.

cond-mat.str-el

Magnetic interactions in PdCrO$_2$ and their effects on its magnetic structure

We report a neutron scattering study of the metallic triangular lattice antiferromagnet PdCrO$_2$. Powder neutron diffraction measurements confirm that the crystalline space group symmetry remains $R\bar{3}m$ below $T_N$. This implies that magnetic interactions consistent with the crystal symmetry do not stabilise the non-coplanar magnetic structure which was one of two structures previously proposed on the basis of single crystal neutron diffraction measurements. Inelastic neutron scattering measurements find two gaps at low energies which can be explained as arising from a dipolar-type exchange interaction. This symmetric anisotropic interaction also stabilises a magnetic structure very similar to the coplanar magnetic structure which was also suggested by the single crystal diffraction study. The higher energy magnon dispersion can be modelled by linear spin wave theory with exchange interactions up to sixth nearest-neighbors, but discrepancies remain which hint at additional effects unexplained by the linear theory.

cond-mat.str-el

Spontaneous decays of magneto-elastic excitations in noncollinear antiferromagnet (Y,Lu)MnO3

When magnons and phonons, the fundamental quasiparticles of the solid, are coupled to one another, they form a new hybrid quasi-particle, leading to novel phenomena and interesting applications. Despite its wide-ranging importance, however, detailed experimental studies on the underlying Hamiltonian is rare for actual materials. Moreover, the anharmonicity of such magnetoelastic excitations remains largely unexplored although it is essential for a proper understanding of their diverse thermodynamic behaviour as well as intrinsic zero-temperature decay. Here we show that in noncollinear antiferromagnets, a strong magnon-phonon coupling can significantly enhance the anharmonicity, resulting in the creation of magnetoelastic excitations and their spontaneous decay. By measuring the spin waves over the full Brillouin zone and carrying out anharmonic spin wave calculations using a Hamiltonian with an explicit magnon-phonon coupling, we have identified a hybrid magnetoelastic mode in (Y,Lu)MnO3 and quantified its decay rate and the exchange-striction coupling term required to produce it. Our work has wide implications for understanding of the spin-phonon coupling and the resulting excitations of the broad classes of noncollinear magnets.

cond-mat.mtrl-sci

Spin excitations used to probe the nature of the exchange coupling in the magnetically ordered ground state of Pr$_{0.5}$Ca$_{0.5}$MnO$_{3}$

We have used time-of-flight inelastic neutron scattering to measure the spin wave spectrum of the canonical half-doped manganite Pr$_{0.5}$Ca$_{0.5}$MnO$_{3}$, in its magnetic and orbitally ordered phase. The data, which cover multiple Brillouin zones and the entire energy range of the excitations, are compared with several different models that are all consistent with the CE-type magnetic order, but arise through different exchange coupling schemes. The Goodenough model, i.e. an ordered state comprising strong nearest neighbor ferromagnetic interactions along zig-zag chains with antiferromagnetic inter-chain coupling, provides the best description of the data, provided that further neighbor interactions along the chains are included. We are able to rule out a coupling scheme involving formation of strongly bound ferromagnetic dimers, i.e. Zener polarons, on the basis of gross features of the observed spin wave spectrum. A model with weaker dimerization reproduces the observed dispersion but can be ruled out on the basis of discrepancies between the calculated and observed structure factors at certain positions in reciprocal space. Adding further neighbor interactions results in almost no dimerization, i.e. recovery of the Goodenough model. These results are consistent with theoretical analysis of the degenerate double exchange model for half-doping, and provide a recipe for how to interpret future measurements away from half-doping, where degenerate double exchange models predict more complex ground states.

cond-mat.str-el

Electron doping evolution of the magnetic excitations in NaFe$_{1-x}$Co$_x$As

We use time-of-flight (ToF) inelastic neutron scattering (INS) spectroscopy to investigate the doping dependence of magnetic excitations across the phase diagram of NaFe$_{1-x}$Co$_x$As with $x=0, 0.0175, 0.0215, 0.05,$ and $0.11$. The effect of electron-doping by partially substituting Fe by Co is to form resonances that couple with superconductivity, broaden and suppress low energy ($E\le 80$ meV) spin excitations compared with spin waves in undoped NaFeAs. However, high energy ($E> 80$ meV) spin excitations are weakly Co-doping dependent. Integration of the local spin dynamic susceptibility $χ^{\prime\prime}(ω)$ of NaFe$_{1-x}$Co$_x$As reveals a total fluctuating moment of 3.6 $μ_B^2$/Fe and a small but systematic reduction with electron doping. The presence of a large spin gap in the Co-overdoped nonsuperconducting NaFe$_{0.89}$Co$_{0.11}$As suggests that Fermi surface nesting is responsible for low-energy spin excitations. These results parallel Ni-doping evolution of spin excitations in BaFe$_{2-x}$Ni$_x$As$_2$, confirming the notion that low-energy spin excitations coupling with itinerant electrons are important for superconductivity, while weakly doping dependent high-energy spin excitations result from localized moments.

cond-mat.supr-con

HORACE: software for the analysis of data from single crystal spectroscopy experiments at time-of-flight neutron instruments

The HORACE suite of programs has been developed to work with large multiple-measurement data sets collected from time-of-flight neutron spectrometers equipped with arrays of position-sensitive detectors. The software allows exploratory studies of the four dimensions of reciprocal space and excitation energy to be undertaken, enabling multi-dimensional subsets to be visualized, algebraically manipulated, and models for the scattering to simulated or fitted to the data. The software is designed to be an extensible framework, thus allowing user-customized operations to be performed on the data. Examples of the use of its features are given for measurements exploring the spin waves of the simple antiferromagnet RbMnF$_{3}$ and ferromagnetic iron, and the phonons in URu$_{2}$Si$_{2}$.

physics.data-an

Spin Waves and Spatially Anisotropic Exchange Interactions in the $\mathrm{S=2}$ Stripe Antiferromagnet Rb$_{0.8}$Fe$_{1.5}$S$_2$

An inelastic neutron scattering study of the spin waves corresponding to the stripe antiferromagnetic order in insulating Rb$_{0.8}$Fe$_{1.5}$S$_2$ throughout the Brillouin zone is reported. The spin wave spectra are well described by a Heisenberg Hamiltonian with anisotropic in-plane exchange interactions. Integrating the ordered moment and the spin fluctuations results in a total moment squared of $27.6\pm4.2μ_B^2$/Fe, consistent with $\mathrm{S \approx 2}$. Unlike $X$Fe$_2$As$_2$ ($X=$ Ca, Sr, and Ba), where the itinerant electrons have a significant contribution, our data suggest that this stripe antiferromagnetically ordered phase in Rb$_{0.8}$Fe$_{1.5}$S$_2$ is a Mott-like insulator with fully localized $3d$ electrons and a high-spin ground state configuration. Nevertheless, the anisotropic exchange couplings appear to be universal in the stripe phase of Fe pnictides and chalcogenides.

cond-mat.supr-con