arXiv subjects

H. C. Walker

Publications and source records attributed to H. C. Walker.

At least 37 records · Page 2Linked to original sources

arXiv2019

Fractionalized excitations in the partially magnetized spin liquid candidate YbMgGaO4

Quantum spin liquids (QSLs) are exotic states of matter characterized by emergent gauge structures and fractionalized elementary excitations. The recently discovered triangular lattice antiferromagnet YbMgGaO$_4$ is a promising QSL candidate, and the nature of its ground state is still under debate. Here, we use neutron scattering to study the spin excitations in YbMgGaO$_4$ under various magnetic fields. Our data reveal a dispersive spin excitation continuum with clear upper and lower excitation edges under a weak magnetic field ($H=2.5$ T). Moreover, a spectral crossing emerges at the $Γ$ point at the Zeeman-split energy. The corresponding redistribution of the spectral weight and its field-dependent evolution are consistent with the theoretical prediction based on the inter-band and intra-band spinon particle-hole excitations associated with the Zeeman-split spinon bands, implying the presence of fractionalized excitations and spinon Fermi surfaces in the partially magnetized YbMgGaO$_4$.

cond-mat.str-el↗

arXiv2019

Multi-phase competition in quantum $XY$ pyrochlore antiferromagnet CdYb$_{2}$Se$_{4}$: zero and applied magnetic field study

We study magnetic behaviour of the Yb$^{3+}$ ions on a frustrated pyrochlore lattice in the spinel {\CYS}. The crystal-electric field parameters deduced from high-energy inelastic neutron scattering reveal well-isolated ytterbium ground state doublet with a weakly Ising character. Magnetic order studied by powder neutron diffraction evolves from the $XY$-type antiferromagnetic $Γ_5$ state to a splayed ice-like ferromagnet (both with k=0) in applied magnetic field with $B_c$=3 T. Low-energy inelastic neutron scattering identifies weakly dispersive magnetic bands around 0.72 meV starting at $\mid\bf{Q}\mid$ = 1.1 Å$^{-1}$~ at zero field, which diminish with field and vanish above 3 T. We explain the observed magnetic behaviour in framework of the nearest-neighbour anisotropic exchange model for effective $S=1/2$ Kramers doublets on the pyrochlore lattice. The estimated exchanges position the {\CYS} spinel close to the phase boundary between the $Γ_5$ and splayed ferromagnet states, similar to the Yb-pyrochlores suggesting an important role of the competition between these phases.

cond-mat.str-el↗

arXiv2019

Plaquette instability competing with bicollinear ground state in detwinned FeTe

We use inelastic neutron scattering to show that long-range spin waves arising from the static bicollinear antiferromagnetic (AF) order in FeTe, which have twofold rotational symmetry in a fully detwinned crystal, rapidly dissolve above $E\approx 26$ meV into ridges of scattering with fourfold rotational symmetry and a nearly isotropic magnetic fluctuation spectrum. With increasing temperature above $T_N\approx 68$ K, the twofold spin waves change into broad regions of scattering with fourfold symmetry. Since the scattering patterns from plaquette magnetic order generated within a bilinear biquadratic Hamiltonian have fourfold rotational symmetry consistent with the high-energy, spin-isotropic spin waves of FeTe, we conclude that the bicollinear AF state in FeTe is quasidegenerate with plaquette magnetic order, providing evidence for the strongly frustrated nature of the local moments in iron chalcogenide family of iron-based superconductors.

cond-mat.str-el↗

arXiv2019

Magnon-polaron excitations in the noncollinear antiferromagnet Mn$_3$Ge

We present the detailed inelastic neutron scattering measurements of the noncollinear antiferromagnet Mn$_3$Ge. Time-of-flight and triple-axis spectroscopy experiments were conducted at the temperature of 6~K, well below the high magnetic ordering temperature of 370~K. The magnetic excitations have a 5-meV gap and display an anisotropic dispersive mode reaching $\simeq 90$~meV at the boundaries of the magnetic Brillouin zone. The spectrum at the zone center shows two additional excitations that demonstrate characteristics of both magnons and phonons. The \textit{ab initio} lattice-dynamics calculations show that these can be associated with the magnon-polaron modes resulting from the hybridization of the spin fluctuations and the low-energy optical phonons. The observed magnetoelastic coupling agrees with the previously found negative thermal expansion in this compound and resembles the features reported in the spectroscopic studies of other antiferromagnets with the similar noncollinear spin structures.

cond-mat.str-el↗

arXiv2019

Impact of the first order antiferromagnetic phase transition on the paramagnetic spin excitations and nematic phase of SrFe$_2$As$_2$

Understanding the nature of the electronic nematic phase in iron pnictide superconductors is important for elucidating its impact on high-temperature superconductivity. Here we use transport and inelastic neutron scattering to study spin excitations and in-plane resistivity anisotropy in uniaxial pressure detwinned BaFe$_2$As$_2$ and SrFe$_2$As$_2$, the parent compounds of iron pnictide superconductors. While BaFe$_2$As$_2$ exhibits weakly first order tetragonal-to-orthorhombic structural and antiferromagnetic (AF) phase transitions below $T_s > T_N\approx 138$ K, SrFe$_2$As$_2$ has strongly coupled first order structural and AF transitions below $T_s= T_N\approx 210$ K. We find that the direct signatures of the nematic phase persist to lower temperatures above the phase transition in the case of SrFe$_2$As$_2$ compared to BaFe$_2$As$_2$. Our findings support the conclusion that the strongly first-order nature of the magnetic transition in SrFe$_2$As$_2$ weakens the nematic phase and resistivity anisotropy in the system.

cond-mat.supr-con↗

arXiv2019

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↗

arXiv2019

Critical fluctuations in the spin-orbit Mott insulator Sr$_3$Ir$_2$O$_7$

X-ray magnetic critical scattering measurements and specific heat measurements were performed on the perovskite iridate Sr$_3$Ir$_2$O$_7$. We find that the magnetic interactions close to the Néel temperature $T_N$ = 283.4(2) K are three-dimensional. This contrasts with previous studies which suggest two-dimensional behaviour like Sr$_2$IrO$_4$. Violation of the Harris criterion ($dν>2$) means that weak disorder becomes relevant. This leads a rounding of the antiferromagnetic phase transition at $T_N$, and modifies the critical exponents relative to the clean system. Specifically, we determine that the critical behaviour of Sr$_3$Ir$_2$O$_7$ is representative of the diluted 3D Ising universality class.

cond-mat.str-el↗

arXiv2018

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↗

arXiv2018

NaYbS$_2$ - a new planar spin-$\frac{1}{2}$ triangular-lattice magnet and putative spin liquid

Platelike high-quality NaYbS$_{2}$ rhombohedral single crystals with lateral dimensions of a few mm have been grown and investigated in great detail by bulk methods like magnetization and specific heat, but also by local probes like nuclear magnetic resonance (NMR), electron-spin resonance (ESR), muon-spin relaxation ($μ$SR), and inelastic neutron scattering (INS) over a wide field and temperature range. Our single-crystal studies clearly evidence a strongly anisotropic quasi-2D magnetism and an emerging spin-orbit entangled $S=1/2$ state of Yb towards low temperatures together with an absence of long-range magnetic order down to 260~mK. In particular, the clear and narrow Yb ESR lines together with narrow $^{23}$Na NMR lines evidence an absence of inherent structural distortions in the system, which is in strong contrast to the related spin-liquid candidate YbMgGaO$_{4}$ falling within the same space group $R\overline{3}m$. This identifies NaYbS$_{2}$ as a rather pure spin-1/2 triangular lattice magnet and a new putative quantum spin liquid.

cond-mat.str-el↗

arXiv2018

Tuning the $S = 1/2$ square-lattice antiferromagnet Sr$_2$Cu(Te$_{1-x}$W$_x$)O$_6$ from Néel order to quantum disorder to columnar order

The spin-1/2 square-lattice Heisenberg model is predicted to have a quantum disordered ground state when magnetic frustration is maximized by competing nearest-neighbor $J_1$ and next-nearest-neighbor $J_2$ interactions ($J_2/J_1 \approx 0.5$). The double perovskites Sr$_2$CuTeO$_6$ and Sr$_2$CuWO$_6$ are isostructural spin-1/2 square-lattice antiferromagnets with Néel ($J_1$ dominates) and columnar ($J_2$ dominates) magnetic order, respectively. Here we characterize the full isostructural solid solution series Sr$_2$Cu(Te$_{1-x}$W$_x$)O$_6$ ($0 \leq x \leq 1$) tunable from Néel order to quantum disorder to columnar order. A spin-liquid-like ground state was previously observed for the $x$ = 0.5 phase, but we show that the magnetic order is suppressed below 1.5 K in a much wider region of $x \approx$ 0.1-0.6. This coincides with significant $T$-linear terms in the low-temperature specific heat. However, density functional theory calculations predict most of the materials are not in the highly frustrated $J_2/J_1 \approx 0.5$ region square-lattice Heisenberg model. Thus, a combination of both magnetic frustration and quenched disorder is the likely origin of the spin-liquid-like state in $x$ = 0.5.

cond-mat.str-el↗

arXiv2018

Anharmonic magnon excitations in noncollinear and charge-ordered RbFe$^{2+}$Fe$^{3+}$F$_6$

RbFe$^{2+}$Fe$^{3+}$F$_6$ is an example of a charge ordered antiferromagnet where iron sites, with differing valences, are structurally separated into two interpenetrating sublattices. The low temperature magnetically ordered Fe$^{2+}$ ($S$=2) and Fe$^{3+}$ ($S$=5/2) moments form a noncollinear orthogonal structure with the Fe$^{3+}$ site displaying a reduced static ordered moment. Neutron spectroscopy on single crystals finds two distinct spin wave branches with a dominant coupling along the Fe$^{3+}$ chain axis ($b$-axis). High resolution spectroscopic measurements find an intense energy and momentum broadened magnetic band of scattering bracketing a momentum-energy region where two magnon processes are kinematically allowed. These anharmonic excitations are enhanced in this non collinear magnet owing to the orthogonal spin arrangement.

cond-mat.str-el↗

arXiv2018

Spin Waves in Detwinned BaFe$_2$As$_2$

Understanding magnetic interactions in the parent compounds of high-temperature superconductors forms the basis for determining their role for the mechanism of superconductivity. For parent compounds of iron pnictide superconductors such as $A$Fe$_2$As$_2$ ($A=$ Ba, Ca, Sr), although spin excitations have been mapped out throughout the entire Brillouin zone (BZ), measurements were carried out on twinned samples and did not allow for a conclusive determination of the spin dynamics. Here we use inelastic neutron scattering to completely map out spin excitations of $\sim$100\% detwinned BaFe$_2$As$_2$. By comparing observed spectra with theoretical calculations, we conclude that the spin excitations can be well described by an itinerant model with important contributions from electronic correlations.

cond-mat.supr-con↗

arXiv2018

Vesignieite: a $S = \frac{1}{2}$ kagome antiferromagnet with dominant third-neighbor exchange

The spin-$\frac{1}{2}$ kagome antiferromagnet is an archetypal frustrated system predicted to host a variety of exotic magnetic states. We show using neutron scattering measurements that deuterated vesignieite BaCu$_{3}$V$_{2}$O$_{8}$(OD)$_{2}$, a fully stoichiometric $S=1/2$ kagome magnet with $<$1% lattice distortion, orders magnetically at $T_{\mathrm{N}}=9$K into a multi-k coplanar variant of the predicted triple-k octahedral structure. We find this structure is stabilized by a dominant antiferromagnetic 3$^{\mathrm{rd}}$-neighbor exchange $J_3$ with minor 1$^{\mathrm{st}}$- or 2$^{\mathrm{nd}}$--neighbour exchange. The spin-wave spectrum is well described by a $J_3$-only model including a tiny symmetric exchange anisotropy.

cond-mat.str-el↗

arXiv2018

Spin-liquid-like state in a spin-1/2 square-lattice antiferromagnet perovskite induced by $d^{10}$-$d^0$ cation mixing

A quantum spin liquid state has long been predicted to arise in spin-1/2 Heisenberg square-lattice antiferromagnets at the boundary region between Néel (nearest-neighbor interaction dominates) and columnar (next-nearest-neighbor dominates) antiferromagnetic order. However, there are no known compounds in this region. Here we use $d^{10}$-$d^0$ cation mixing to tune the magnetic interactions on the square lattice while simultaneously introducing disorder. We find spin-liquid-like behavior in the double perovskite Sr$_2$Cu(Te$_{0.5}$W$_{0.5}$)O$_6$, where the isostructural end phases Sr$_2$CuTeO$_6$ and Sr$_2$CuWO$_6$ are Néel and columnar type antiferromagnets, respectively. We show that magnetism in Sr$_2$Cu(Te$_{0.5}$W$_{0.5}$)O$_6$ is entirely dynamic down to 19 mK. Additionally, we observe at low temperatures for Sr$_2$Cu(Te$_{0.5}$W$_{0.5}$)O$_6$, similar to several spin liquid candidates, a plateau in muon spin relaxation rate and a strong $T$-linear dependence in specific heat. Our observations for Sr$_2$Cu(Te$_{0.5}$W$_{0.5}$)O$_6$ highlight the role of disorder in addition to magnetic frustration in spin liquid physics.

cond-mat.str-el↗

arXiv2017

Magnetic structure and spin wave excitations in the multiferroic magnetic metal-organic framework (CD$_3$)$_2$ND$_2$[Mn(DCO$_2$)$_3$]

We report the magnetic diffraction pattern and spin wave excitations in (CD$_3$)$_2$ND$_2$[Mn(DCO$_2$)$_3$] measured using elastic and inelastic neutron scattering. The magnetic structure is shown to be a G-type antiferromagnet with moments pointing along the $b$ axis. By comparison with simulations based on linear spin wave theory, we have developed a model for the magnetic interactions in this multiferroic metal-organic framework material. The interactions form a three-dimensional network with antiferromagnetic nearest-neighbour interactions along three directions of $J_1=-0.103(8)$~meV, $J_2=-0.032(8)$~meV and $J_3=-0.035(8)$~meV.

cond-mat.str-el↗

arXiv2017

Evidence for a spinon Fermi surface in a triangular lattice quantum spin liquid candidate

A quantum spin liquid is an exotic quantum state of matter in which spins are highly entangled and remain disordered down to zero temperature. Such a state of matter is potentially relevant to high-temperature superconductivity and quantum-information applications, and experimental identification of a quantum spin liquid state is of fundamental importance for our understanding of quantum matter. Theoretical studies have proposed various quantum-spin-liquid ground states, most of which are characterized by exotic spin excitations with fractional quantum numbers (termed `spinon'). Here, we report neutron scattering measurements that reveal broad spin excitations covering a wide region of the Brillouin zone in a triangular antiferromagnet YbMgGaO4. The observed diffusive spin excitation persists at the lowest measured energy and shows a clear upper excitation edge, which is consistent with the particle-hole excitation of a spinon Fermi surface. Our results therefore point to a QSL state with a spinon Fermi surface in YbMgGaO4 that has a perfect spin-1/2 triangular lattice as in the original proposal of quantum spin liquids.

cond-mat.str-el↗

arXiv2017

Magnetic excitations from the two-dimensional interpenetrating Cu framework in Ba$_2$Cu$_3$O$_4$Cl$_2$

We report detailed neutron scattering studies on Ba$_2$Cu$_3$O$_4$Cl$_2$. The compound consists of two interpenetrating sublattices of Cu, labeled as Cu$_{\rm A}$ and Cu$_{\rm B}$, each of which forms a square-lattice Heisenberg antiferromagnet. The two sublattices order at different temperatures and effective exchange couplings within the sublattices differ by an order of magnitude. This yields an inelastic neutron spectrum of the Cu$_{\rm A}$ sublattice extending up to 300 meV and a much weaker dispersion of Cu$_{\rm B}$ going up to around 20 meV. Using a single-band Hubbard model we derive an effective spin Hamiltonian. From this, we find that linear spin-wave theory gives a good description to the magnetic spectrum. In addition, a magnetic field of 10 T is found to produce effects on the Cu$_{\rm B}$ dispersion that cannot be explained by conventional spin-wave theory.

cond-mat.str-el↗

arXiv2017

Resonant x-ray spectroscopy of uranium intermetallics at the U $M_{4,5}$ edges

We present resonant x-ray emission spectroscopic (RXES) data from the uranium intermetallics UPd$_3$, USb, USn$_3$ and URu$_2$Si$_2$, at the U $M_{4,5}$ edges and compare the data to those from the well-localized $5f^2$ semiconductor UO$_2$. The technique is especially sensitive to any oxidation of the surface, and this was found on the USb sample, thus preventing a good comparison with a material known to be $5f^3$. We have found a small energy shift between UO$_2$ and UPd$_3$, both known to have localized $5f^2$ configurations, which we ascribe to the effect of conduction electrons in UPd$_3$. The spectra from UPd$_3$ and URu$_2$Si$_2$,are similar, strongly suggesting a predominant $5f^2$ configuration for URu$_2$Si$_2$. The valence-band resonant inelastic x-ray scattering (RIXS) provides information on the U $P_3$ transitions (at about $18$~eV) between the U $5f$ and U $6p$ states, as well as transitions of between $3$ and $7$~eV from the valence band into the unoccupied $5f$ states. These transitions are primarily involving mixed ligand states (O $2p$ or Pd, Ru $4d$) and U $5f$ states. Calculations are able to reproduce both these low-energy transitions reasonably well.

cond-mat.str-el↗