arXiv subjects

J. F. Mitchell

Publications and source records attributed to J. F. Mitchell.

At least 73 records · Page 4Linked to original sources

arXiv2016

Magnetotransport of single crystalline YSb

We report magnetic field dependent transport measurements on a single crystal of cubic YSb together with first principles calculations of its electronic structure. The transverse magnetoresistance does not saturate up to 9 T and attains a value of 75,000 % at 1.8 K. The Hall coefficient is electron-like at high temperature, changes sign to hole-like between 110 and 50 K, and again becomes electron-like below 50 K. First principles calculations show that YSb is a compensated semimetal with a qualitatively similar electronic structure to that of isostructural LaSb and LaBi, but with larger Fermi surface volume. The measured electron carrier density and Hall mobility calculated at 1.8 K, based on a single band approximation, are 6.5$\times10^{20}/$cm$^{3}$ and 6.2$\times10^{4}$cm$^{2}$/Vs, respectively. These values are comparable with those reported for LaBi and LaSb. Like LaBi and LaSb, YSb undergoes a magnetic field-induced metal-insulator-like transition below a characteristic temperature T$_{m}$, with resistivity saturation below 13 K. Thickness dependent electrical resistance measurements show a deviation of the resistance behavior from that expected for a normal metal; however, they do not unambiguously establish surface conduction as the mechanism for the resistivity plateau.

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arXiv2016

Stacked Charge Stripes in Quasi-Two_Dimensional Trilayer Nickelate La4Ni3O8

The quasi-two-dimensional nickelate La4Ni3O8 (La-438) is an anion deficient n=3 Ruddlesden-Popper (R-P) phase that consists of trilayer networks of square planar Ni ions, formally assigned as Ni1+ and Ni2+ in a 2:1 ratio. While previous studies on polycrystalline samples have identified a 105 K phase transition with a pronounced electronic and magnetic response but weak lattice character, no consensus on the origin of this transition has been reached. Here we show using synchrotron x-ray diffraction on high-pO2 floating-zone grown single crystals that this transition is driven by a real space ordering of charge into a quasi-2D charge stripe ground state. The charge stripe superlattice propagation vector, q=(2/3, 0, 1), corresponds with that found in the related 1/3-hole doped single layer Ruddlesden-Popper nickelate, La5/3Sr1/3NiO4 (LSNO-1/3, Ni2.33+) with orientation at 45-degrees to the Ni-O bonds. Like LSNO-1/3, the charge stripes in La-438 are weakly correlated along the c axis to form a staggered ABAB stacking that minimizes the Coulomb repulsion among the stripes. Surprisingly, however, we find that the charge stripes within each trilayer of La-438 are stacked in phase from one layer to the next, at odds with any simple Coulomb repulsion argument.

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arXiv2015

Non percolative nature of the metal-insulator transition and persistence of local Jahn-Teller distortions in the rhombohedral regime of La$_{1-x}$Ca$_{x}$MnO$_{3}$

Evolution of the average and local crystal structure of Ca-doped LaMnO$_{3}$ has been studied across the metal to insulator (MI) and the orthorhombic to rhombohedral (OR) structural phase transitions over a broad temperature range for two Ca concentrations ($x = 0.18; 0.22$). Combined Rietveld and high real space resolution atomic pair distribution function (PDF) analysis of neutron total scattering data was carried out with aims of exploring the possibility of nanoscale phase separation (PS) in relation to MI transition, and charting the evolution of local Jahn-Teller (JT) distortion of MnO$_{6}$ octahedra across the OR transition at T$_{S}$ $\sim$ 720 K. The study utilized explicit two-phase PDF structural modeling, revealing that away from TMI there is no evidence for nanoscale phase coexistence. The local JT-distortions disappear abruptly upon crossing into the metallic regime both with doping and temperature, with only small temperature-independent signature of quenched disorder being observable at low temperature as compared to CaMnO$_{3}$. The results hence do not support the percolative scenario for the MI transition in La$_{1-x}$Ca$_{x}$MnO$_{3}$ based on PS, and question its ubiquity in the manganites. In contrast to LaMnO3 that exhibits long range orbital correlations and sizeable octahedral distortions at low temperature, the doped samples with compositions straddling the MI boundary exhibit correlations (in the insulating regime) limited to only $\sim$ 1 nm with observably smaller distortions. In $x = 0.22$ sample local JT-distortions are found to persist across the OR transition and deep into the R-phase (up to $\sim$ 1050 K) where they are crystallographically prohibited. Their magnitude and subnanometer spatial extent remain unchanged.

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arXiv2015

Structure and magnetism in $\rm LaCoO_3$

The temperature dependence of the hexagonal lattice parameter $c$ of single crystal $\rm LaCoO_3$ (LCO) with $H=0$ and $800$Oe, as well as LCO bulk powders with $H=0$, was measured using high-resolution x-ray scattering near the transition temperature $T_o\approx 35$K. The change of $c(T)$ is well characterized by a power law in $T-T_o$ for $T>T_o$ and by a temperature independent constant for $T<T_o$ when convoluted with a Gaussian function of width $8.5$K. This behavior is discussed in the context of the unusual magnetic behavior observed in LCO as well as recent generalized gradient approximation calculations.

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arXiv2015

Isotropic and Anisotropic Regimes of the Field-Dependent Spin Dynamics in Sr2IrO4: Raman Scattering Studies

A major focus of experimental interest in Sr2IrO4 has been to clarify how the magnetic excitations of this strongly spin-orbit coupled system differ from the predictions of anisotropic 2D spin-1/2 Heisenberg model and to explore the extent to which strong spin-orbit coupling affects the magnetic properties of iridates. Here, we present a high-resolution inelastic light (Raman) scattering study of the low energy magnetic excitation spectrum of Sr2IrO4 and doped Eu-doped Sr2IrO4 as functions of both temperature and applied magnetic field. We show that the high-field (H>1.5 T) in-plane spin dynamics of Sr2IrO4 are isotropic and governed by the interplay between the applied field and the small in-plane ferromagnetic spin components induced by the Dzyaloshinskii-Moriya interaction. However, the spin dynamics of Sr2IrO4 at lower fields (H<1.5 T) exhibit important effects associated with interlayer coupling and in-plane anisotropy, including a spin-flop transition at Hc in Sr2IrO4 that occurs either discontinuously or via a continuous rotation of the spins, depending upon the in-plane orientation of the applied field. These results show that in-plane anisotropy and interlayer coupling effects play important roles in the low-field magnetic and dynamical properties of Sr2IrO4.

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arXiv2015

Investigation of ferromagnetic domain behavior and phase transition at nanoscale in bilayer manganites

Understanding the underlying mechanism and phenomenology of colossal magnetoresistance in manganites has largely focused on atomic and nanoscale physics such as double exchange, phase separation, and charge order. Here we consider a more macroscopic view of manganite materials physics, reporting on the ferromagnetic domain behavior in a bilayer manganite sample with a nominal composition of La$_{2-2x}$Sr$_{1+2x}$Mn$_2$O$_7$ with $x=0.38$, studied using in-situ Lorentz transmission electron microscopy. The role of magnetocrystalline anisotropy on the structure of domain walls was elucidated. On cooling, magnetic domain contrast was seen to appear first at the Curie temperature within the $a-b$ plane. With further reduction in temperature, the change in area fraction of magnetic domains was used to estimate the critical exponent describing the ferromagntic phase transition. The ferromagnetic phase transition was accompanied by a distinctive nanoscale granular contrast close to the Curie temperature, which we infer to be related to the presence of ferromagnetic nanoclusters in a paramagnetic matrix, which has not yet been reported in bilayer manganites.

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arXiv2015

Direct Evidence for Dominant Bond-directional Interactions in a Honeycomb Lattice Iridate Na2IrO3

Heisenberg interactions are ubiquitous in magnetic materials and have been prevailing in modeling and designing quantum magnets. Bond-directional interactions offer a novel alternative to Heisenberg exchange and provide the building blocks of the Kitaev model, which has a quantum spin liquid (QSL) as its exact ground state. Honeycomb iridates, A2IrO3 (A=Na,Li), offer potential realizations of the Kitaev model, and their reported magnetic behaviors may be interpreted within the Kitaev framework. However, the extent of their relevance to the Kitaev model remains unclear, as evidence for bond-directional interactions remains indirect or conjectural. Here, we present direct evidence for dominant bond-directional interactions in antiferromagnetic Na2IrO3 and show that they lead to strong magnetic frustration. Diffuse magnetic x-ray scattering reveals broken spin-rotational symmetry even above Neel temperature, with the three spin components exhibiting nano-scale correlations along distinct crystallographic directions. This spin-space and real-space entanglement directly manifests the bond-directional interactions, provides the missing link to Kitaev physics in honeycomb iridates, and establishes a new design strategy toward frustrated magnetism.

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arXiv2014

Brownmillerite Ca2Co2O5: Synthesis, Stability, and Re-entrant Single-Crystal-to-Single-Crystal Structural Transitions

Ca2Co2O5 in the brownmillerite form was synthesized using a high-pressure optical-image floating zone furnace, and single crystals with dimensions up to 1.4x0.8x0.5 mm3 were obtained. At room temperature, Ca2Co2O5 crystallizes as a fully ordered brownmillerite variant in the orthorhombic space group Pcmb (No. 57) with unit cell parameters a=5.28960(10) Å, b=14.9240(2) Å, and c=10.9547(2) Å. With decreasing temperature, it undergoes a re-entrant sequence of first-order structural phase transitions (Pcmb to P2/c11 to P121/m1 to Pcmb) that is unprecedented among brownmillerites, broadening the family of space groups available to these materials and challenging current approaches for sorting the myriad variants of brownmillerite structures. Magnetic susceptibility data indicate antiferromagnetic ordering in Ca2Co2O5 occurs near 240 K, corroborated by neutron powder diffraction. Below 140 K, the specimen exhibits a weak ferromagnetic component directed primarily along the b axis that shows a pronounced thermal and magnetic history dependence.

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arXiv2014

Fermi Arcs in a Doped Pseudospin-1/2 Heisenberg Antiferromagnet

High temperature superconductivity in cuprates arises from an electronic state that remains poorly understood. We report the observation of a related electronic state in a non-cuprate material Sr2IrO4 in which the unique cuprate Fermiology is largely reproduced. Upon surface electron doping through in situ deposition of alkali-metal atoms, angle-resolved photoemission spectra of Sr2IrO4 display disconnected segments of zero-energy states, known as Fermi arcs, and a gap as large as 80 meV. Its evolution toward a normal metal phase with a closed Fermi surface as a function of doping and temperature parallels that in the cuprates. Our result suggests that Sr2IrO4 is a useful model system for comparison to the cuprates.

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arXiv2013

Cu(Ir$_{1-x}$Cr$_x$)$_2$S$_4$: a model system for studying nanoscale phase coexistence at the metal-insulator transition

Increasingly, nanoscale phase coexistence and hidden broken symmetry states are being found in the vicinity of metal-insulator transitions (MIT), for example, in high temperature superconductors, heavy fermion and colossal magnetoresistive materials, but their importance and possible role in the MIT and related emergent behaviors is not understood. Despite their ubiquity, they are hard to study because they produce weak diffuse signals in most measurements. Here we propose Cu(Ir$_{1-x}$Cr$_x$)$_2$S$_4$ as a model system, where robust local structural signals lead to key new insights. We demonstrate a hitherto unobserved coexistence of a Ir$^{4+}$ charge-localized dimer phase and Cr-ferromagnetism. The resulting phase diagram that takes into account the short range dimer order, is highly reminiscent of a generic MIT phase diagram similar to the cuprates. We suggest that the presence of quenched strain from dopant ions acts as an arbiter deciding between the competing ground states.

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arXiv2013

Minority-spin $t_{2g}$ states and the degree of spin polarization in ferromagnetic metallic La$_{2-2x}$Sr$_{1+2x}$Mn$_2$O$_7$ ($x=0.38$)

Using angle-resolved photoemission spectroscopy (ARPES), we investigate the electronic band structure and Fermi surface of ferromagnetic La$_{2-2x}$Sr$_{1+2x}$Mn$_2$O$_7$ ($x=0.38$). Besides the expected two hole pockets and one electron pocket of majority-spin $e_g$ electrons, we show an extra electron pocket around the $Γ$ point. A comparison with first-principles spin-polarized band-structure calculations shows that the extra electron pocket arises from $t_{2g}$ electrons of minority-spin character, indicating this compound is not a complete half-metallic ferromagnet, with similar expectations for lightly-doped cubic manganites. However, our data suggest that a complete half-metallic state is likely to be reached as long as the bandwidth is mildly reduced. Moreover, the band-resolved capability of ARPES enables us to investigate the band structure effects on spin polarization for different experimental conditions.

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arXiv2013

Gigantic magnetic field polarization and magnetoelectric coupling in a ferrimagnetic oxide CaBaCo4O7

The single crystal study of CaBaCo4O7, a non collinear ferrimagnet (TC=64K), with a polar orthorhombic space group (Pbn21) between 4 K and 293 K, shows the appearance below TC of a large electric polarization along its c axis, reaching 17mC.m-2 at 10K. At 62.5K, a magnetic field driven giant variation of polarization, P(9T)-P(0T)=8mC.m-2, is observed. Moreover, the present magnetoelectric measurements, are fully consistent with the m'm2' magnetic point group, strongly supporting that this oxide is also ferrotoroidic. This ferrimagnetic oxide, which belongs to the '114' structural family, opens an avenue for the search of new magnetoelectrics.

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arXiv2013

Local Structural Evidence for Strong Electronic Correlations in LiRh$_2$O$_4$ Spinel

The local structure of the spinel LiRh$_2$O$_4$ has been studied using atomic pair distribution function (PDF) analysis of powder x-ray diffraction data. This measurement is sensitive to the presence of short Rh-Rh bonds that form due to dimerization of Rh$^{4+}$ ions on the pyrochlore sublattice, independent of the existence of long range order. We show that structural dimers exist in the low-temperature phase, as previously supposed, with a bond shortening of $Δr \sim 0.15$ Å. The dimers persist up to 350 K, well above the insulator-metal transition, with $Δr$ decreasing in magnitude on warming. Such behavior is inconsistent with the Fermi surface nesting-driven Peierls transition model. Instead, we argue that LiRh$_2$O$_4$ should properly be described as a strongly correlated system.

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arXiv2013

Observation of electronic inhomogeneity and charge density wave in a bilayer La$_{1.36}$Sr$_{1.64}$Mn$_2$O$_7$ single crystal

We employed a scanning tunneling microscope to image the (001) surface topography and local density of states (LDOS) in La$_{2-2x}$Sr$_{1+2x}$Mn$_2$O$_7$ (x=0.32, LSMO) single crystals below the Curie temperature (T$_C$ = 120 K). The LDOS maps revealed a stripe-like modulation propagating along the tetragonal a axis with a wavelength of about 1.6 Å, which is indicative of a charge density wave (CDW). The observed CDW in the x=0.32 sample is far from the Fermi surface nesting instability as compared with the data of angle resolved photoemission spectroscopy in an x=0.40 sample. The stripe model developed previously for cuprates can explain the observed CDW in our LSMO sample, indicating that competing interactions between localized and itinerant phases are the origin of the spatial modulations present intrinsically in cuprates and manganites.

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arXiv2013

Antiferromagnetic Domain Structure in Bilayer Manganite

We report a novel soft x-ray nanodiffraction study of antiferromagnetic domains in the strongly correlated bylayer manganite La$_{0.96}$Sr$_{2.04}$Mn$_{2}$O$_{7}$. We find that the antiferromagnetic domains are quenched, forming a unique domain pattern with each domain having an intrinsic memory of its spin direction, and with associated domain walls running along crystallographic directions. This can be explained by the presence of crystallographic or magnetic imperfections locked in during the crystal growth process which pin the antiferromagnetic domains. The antiferromagnetic domain pattern shows two distinct types of domain. We observe, in one type only, a periodic ripple in the manganese spin direction with a period of approximately 4 \micro\meter. We propose that the loss of inversion symmetry within a bilayer is responsible for this ripple structure through a Dzyaloshinskii-Moriya-type interaction.

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arXiv2012

Evolution of magnetic oxygen states in Sr-doped LaCoO$_3$

Magnetism in La$_{1-x}$Sr$_x$CoO$_3$ as a function of doping is investigated with X-ray absorption spectroscopy and X-ray magnetic circular dichroism at the O K edge, and corresponding first principles electronic structure calculations. For small x, the spectra are consistent with the formation of ferromagnetic clusters occurring within a nonmagnetic insulating matrix. Sr-induced, magnetic O-hole states form just above E$_F$ and grow with increasing Sr doping. Density functional calculations for x = 0 yield a nonmagnetic ground state with the observed rhombohedral distortion and indicates that doping introduces holes at the Fermi level in magnetic states with significant O 2p and Co t$_{2g}$ character for the undistorted pseudocubic structure. Supercell calculations show stronger magnetism on oxygen atoms having more Sr neighbors.

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arXiv2012

A cascade of magnetic field induced spin transitions in LaCoO3

We present magnetization and magnetostriction studies of the insulating perovskite LaCoO3 in magnetic fields approaching 100 T. In marked contrast with expectations from single-ion models, the data reveal two distinct first-order spin transitions and well-defined magnetization plateaux. The magnetization at the higher plateau is only about half the saturation value expected for spin-1 Co3+ ions. These findings strongly suggest collective behavior induced by strong interactions between different electronic -- and therefore spin -- configurations of Co3+ ions. We propose a model of these interactions that predicts crystalline spin textures and a cascade of four magnetic phase transitions at high fields, of which the first two account for the experimental data.

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arXiv2012

Dimensionality Driven Spin-Flop Transition in Layered Iridates

Using resonant x-ray diffraction, we observe an easy c-axis collinear antiferromagnetic structure for the bilayer Sr$_3$Ir$_2$O$_7$, a significant contrast to the single layer Sr$_2$IrO$_4$ with in-plane canted moments. Based on a microscopic model Hamiltonian, we show that the observed spin-flop transition as a function of number of IrO$_2$ layers is due to strong competition among intra- and inter-layer bond-directional pseudo-dipolar interactions of the spin-orbit entangled $J_{eff}$=1/2 moments. With this we unravel the origin of anisotropic exchange interactions in a Mott insulator in the strong spin-orbit coupling regime, which holds the key to the various types of unconventional magnetism proposed in 5$d$ transition metal oxides.

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