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J. F. Mitchell

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

At least 109 records · Page 6Linked to original sources

Reentrant Orbital Order and the True Ground State of LaSr2Mn2O7

Contrary to conventional wisdom, our purified La2-2xSr1+2xMn2O7 crystals exhibit CE-type orbital and charge order as the low-temperature ground state for a hole doping level h = 0.5. For small deviations from h = 0.5, the high temperature CE phase is replaced at low temperatures by an A-type antiferromagnet without coexistence. Larger deviations result in a lack of CE order at any temperature. Thus, small inhomogeneities in cation or oxygen composition could explain why others commonly see this reentrance with coexistence.

cond-mat.str-el↗

Magnetic momentum density, Fermi surface and directional magnetic Compton profiles in LaSr$_{2}$Mn$_{2}$O$_{7}$ and La$_{1.2}$Sr$_{1.8}$Mn$_2$O$_7$

We have carried out first principles, all-electron computations of the magnetic momentum density $ρ_{mag}({\mathbf p})$ and magnetic Compton profiles (MCPs) for momentum transfer along the [100], [001], and [110] directions in LaSr$_2$Mn$_2$O$_7$ and La$_{1.2}$Sr$_{1.8}$Mn$_2$O$_7$ within the local spin density approximation (LSDA) based band theory framework. Parallel measurements of these three MCPs from a single crystal of La$_{1.2}$Sr$_{1.8}$Mn$_2$O$_7$ at 5 K in a magnetic field of 7 T are also reported. $ρ_{mag}({\mathbf p})$ is shown to contain distinct peaks arising from the occupied majority-spin $t_{2g}$ electrons and to display images of the Fermi surface (FS) in the first and higher Brillouin zones (BZs). The overall shape of the MCPs, $J_{mag}(p_z)$, obtained by integrating $ρ_{mag}({\mathbf p})$ over $p_x$ and $p_y$, is found to be dominated by the majority-spin $t_{2g}$ states. The FS-related fine structure in the MCPs is however substantial only in the [100] MCP, which contains features arising from the large majority-spin hole sheets. The overall shapes and widths of the experimental MCPs along all three directions investigated are in reasonably good accord with theoretical predictions, although some discrepancies indicating inadequacy of the LSDA in treating the magnetic states can be identified. We discuss details of the FS-related signatures in the first and higher BZs in the [100] MCP and show that high resolution magnetic Compton scattering experiments with a momentum resolution of 0.1 a.u. FWHM (full-width-at-half-maximum) or better will be necessary to observe this fine structure. We comment also on the feasibility of using positron annihilation spectroscopy in this connection.

cond-mat.str-el↗

A local metallic state in globally insulating $La_{1.24}Sr_{1.76}Mn_2O_7$ well above the metal-insulator transition

Angle-resolved photoemission spectroscopy was used to investigate the evolution of the electronic structure across the metal-insulator transition in bi-layer manganite $La_{1.24}Sr_{1.76}Mn_2O_7$. We found that this system is a metal for $T T^*$. These results indicate the critical role of electronic phase separation and percolation effects for the metal-insulator transition in $La_{1.24}Sr_{1.76}Mn_2O_7$.

cond-mat.str-el↗

Understanding the insulating phase in CMR manganites: Shortening of the Jahn-Teller long-bond across the phase diagram of La_{1-x} Ca_x Mn O_3

The detailed evolution of the magnitude of the local Jahn-Teller (JT) distortion in La_{1-x} Ca_x Mn O_3 is obtained across the phase diagram for 0 < x < 0.5 from high quality neutron diffraction data using the atomic pair distribution function (PDF) method. A local JT distortion is observed in the insulating phase for all Ca concentrations studied. However, in contrast with earlier local structure studies its magnitude is not constant, but decreases continuously with increasing Ca content. This observation is at odds with a simple small-polaron picture for the insulating state.

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Suppressed Magnetization at the Surfaces and Interfaces of Ferromagnetic Metallic Manganites

What happens to ferromagnetism at the surfaces and interfaces of manganites? With the competition between charge, spin, and orbital degrees of freedom, it is not surprising that the surface behavior may be profoundly different than that of the bulk. Using a powerful combination of two surface probes, tunneling and polarized x-ray interactions, this paper reviews our work on the nature of the electronic and magnetic states at manganite surfaces and interfaces. The general observation is that ferromagnetism is not the lowest energy state at the surface or interface, which results in a suppression or even loss of ferromagnetic order at the surface. Two cases will be discussed ranging from the surface of the quasi-2D bilayer manganite (La$_{2-2x}$Sr$_{1+2x}$Mn$_2$O$_7$) to the 3D Perovskite (La$_{2/3}$Sr$_{1/3}$MnO$_3$)/SrTiO$_3$ interface. For the bilayer manganite, that is, ferromagnetic and conducting in the bulk, these probes present clear evidence for an intrinsic insulating non-ferromagnetic surface layer atop adjacent subsurface layers that display the full bulk magnetization. This abrupt intrinsic magnetic interface is attributed to the weak inter-bilayer coupling native to these quasi-two-dimensional materials. This is in marked contrast to the non-layered manganite system (La$_{2/3}$Sr$_{1/3}$MnO$_3$/SrTiO$_3$), whose magnetization near the interface is less than half the bulk value at low temperatures and decreases with increasing temperature at a faster rate than the bulk.

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Non-collinear long-range magnetic ordering in HgCr2S4

The low-temperature magnetic structure of \HG has been studied by high-resolution powder neutron diffraction. Long-range incommensurate magnetic order sets in at T$_N\sim$22K with propagation vector \textbf{k}=(0,0,$\sim$0.18). On cooling below T$_N$, the propagation vector increases and saturates at the commensurate value \textbf{k}=(0,0,0.25). The magnetic structure below T$_N$ consists of ferromagnetic layers in the \textit{ab}-plane stacked in a spiral arrangement along the \textit{c}-axis. Symmetry analysis using corepresentations theory reveals a point group symmetry in the ordered magnetic phase of 422 (D$_4$), which is incompatible with macroscopic ferroelectricity. This finding indicates that the spontaneous electric polarization observed experimentally cannot be coupled to the magnetic order parameter.

cond-mat.mtrl-sci↗

Evidence of Orbital Ordering in Jahn-Teller Undistorted LaSr$_{2}$Mn$_{2}$O$_{7}$

Resonant soft x-ray diffraction has been used to probe the temperature dependent orbital and magnetic structure of $\mathrm{LaSr_{2}Mn_{2}O_7}$. Previous crystallographic studies have shown that this material has almost no MnO$_{6}$ oxygen displacement due to Jahn-Teller distortions at low temperatures. Within the low-temperature A-type antiferromagnetic phase, we found strong intensity at the $({1/4},{1/4},0)$ orbital and $LaSr_{2}Mn_{2}O_7$ magnetic reflections. This shows that even in the near absence of Jahn-Teller distortion, this compound is strongly orbitally ordered. A fit to the Mn $L$-edge resonance spectra demonstrates the presence of orbital ordering of the Mn$^{3+}$ ions with virtually no Jahn-Teller crystal field in addition to possible Mn$^{3+}$ and Mn$^{2+}$~like valence fluctuations.

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Competing magnetic interactions in the extended Kagome system YBaCo4O7

YBaCo4O7 belongs to a new class of geometrically frustrated magnets like the pyrochlores, in which Co-spins occupy corners of tetrahedra. The structure can be viewed as an alternating stacking of Kagome and triangular layers. Exactly half of the triangular units of the Kagome plane are capped by Co ions to form columns running perpendicular to the Kagome sheets. Neutron powder diffraction reveals a broad temperature range of diffuse magnetic scattering, followed by long range magnetic ordering below 110K. A unique low-temperature magnetic structure simultaneously satisfies an S=0 arrangement in the uncapped triangular units and antiferromagnetic coupling along the columns. A spin reorientation above 30K tracks the relative strengths of the in-plane and out-of-plane interactions.

cond-mat.mtrl-sci↗

Nano-magnetic droplets and implications to orbital ordering in La1-xSrxCoO3

Inelastic cold neutron scattering on LaCoO3 provided evidence for a distinct low energy excitation at 0.6 meV coincident with the thermally induced magnetic transition. Coexisting strong ferromagnetic (FM) and weaker antiferromagnetic (AFM) correlations that are dynamic follow the activation to the excited state, identified as the intermediate S=1 spin triplet. This is indicative of dynamical orbital ordering favoring the observed magnetic interactions. With hole doping as in La1-xSrxCoO3, the FM correlations between Co spins become static and isotropically distributed due to the formation of FM droplets. The correlation length and condensation temperature of these droplets increase rapidly with metallicity due to the double exchange mechanism.

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Nodal quasiparticle in pseudogapped colossal magnetoresistive manganites

A characteristic feature of the copper oxide high-temperature superconductors is the dichotomy between the electronic excitations along the nodal (diagonal) and antinodal (parallel to the Cu-O bonds) directions in momentum space, generally assumed to be linked to the "d-wave" symmetry of the superconducting state. Angle-resolved photoemission measurements in the superconducting state have revealed a quasiparticle spectrum with a d-wave gap structure that exhibits a maximum along the antinodal direction and vanishes along the nodal direction. Subsequent measurements have shown that, at low doping levels, this gap structure persists even in the high-temperature metallic state, although the nodal points of the superconducting state spread out in finite "Fermi arcs". This is the so-called pseudogap phase, and it has been assumed that it is closely linked to the superconducting state, either by assigning it to fluctuating superconductivity or by invoking orders which are natural competitors of d-wave superconductors. Here we report experimental evidence that a very similar pseudogap state with a nodal-antinodal dichotomous character exists in a system that is markedly different from a superconductor: the ferromagnetic metallic groundstate of the colossal magnetoresistive bilayer manganite La1.2Sr1.8Mn2O7. Our findings therefore cast doubt on the assumption that the pseudogap state in the copper oxides and the nodal-antinodal dichotomy are hallmarks of the superconductivity state.

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Quasiparticle-like peaks, kinks, and electron-phonon coupling at the ($π$,0) regions in the CMR oxide La$_{2-2x}$Sr$_{1+2x}$Mn$_{2}$O$_{7}$

Using Angle-Resolved Photoemission (ARPES), we present the first observation of sharp quasiparticle-like peaks in a CMR manganite. We focus on the ($π$,0) regions of k-space and study their electronic scattering rates and dispersion kinks, uncovering the critical energy scales, momentum scales, and strengths of the interactions that renormalize the electrons. To identify these bosons we measured phonon dispersions in the energy range of the kink by inelastic neutron scattering (INS), finding a good match in both energy and momentum to the oxygen bond-stretching phonons.

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Magnetodielectric consequences of phase separation in the colossal magnetoresistance manganite Pr0.7Ca0.3MnO3

We have studied the low-frequency dielectric properties of the phase-separated manganite Pr0.7Ca0.3MnO3 as a function of applied magnetic field in the low temperature phase-separated state. The dielectric constant is strongly field dependent and also depends on the magnetic field history of the sample. The dielectric behavior appears to be associated with the hopping of polaronic charge carriers, and we can derive the field dependent hopping energy barrier from the frequency dependence of the dielectric constant. This analysis allows us to associate the metal-insulator transition observed in this material with the field-induced suppression of the polaron activation energy.

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Extracting d-orbital occupancy from magnetic Compton scattering in bilayer manganites

We consider the shape of the magnetic Compton profile (MCP), $J_{mag}(p_z)$, in La$_{1.2}$Sr$_{1.8}$Mn$_2$O$_7$ for momentum transfer $p_z$ along the [110] direction and the associated reciprocal form factor $B(r)$ defined by taking the one-dimensional Fourier transform of $J_{mag}(p_z)$. $B(r)$ is shown to contain a prominent dip at $r\approx$ 1 $Å$, where the minimum value $B_{min}$ of $B(r)$ can be related to the occupancies of the $e_g$ orbitals of $d_{x^2-y^2}$ and $d_{3z^2-r^2}$ symmetry in the system. We illustrate our procedure in detail by analyzing the measured MCP at 5K and the MCP computed within the framework of the local spin density approximation (LSDA) and comment on the differences between the measured and computed $e_g$ occupancies as a reflection of the limitations of the LSDA in treating electron correlation effects.

cond-mat.str-el↗

Full Bulk Spin Polarization and Intrinsic Tunnel Barriers at the Surface of Layered Manganites

Transmission of information using the spin of the electron as well as its charge requires a high degree of spin polarization at surfaces. At surfaces however this degree of polarization can be quenched by competing interactions. Using a combination of surface sensitive x-ray and tunneling probes, we show for the quasi-two-dimensional bilayer manganites that the outermost Mn-O bilayer, alone, is affected: it is a 1-nm thick insulator that exhibits no long-range ferromagnetic order while the next bilayer displays the full spin polarization of the bulk. Such an abrupt localization of the surface effects is due to the two-dimensional nature of the layered manganite while the loss of ferromagnetism is attributed to weakened double exchange in the reconstructed surface bilayer and a resultant antiferromagnetic phase. The creation of a well-defined surface insulator demonstrates the ability to naturally self-assemble two of the most demanding components of an ideal magnetic tunnel junction.

cond-mat.str-el↗

Neutron diffraction study of average and local structure in La0.5Ca0.5MnO3

We used neutron powder diffraction to obtain the local and long-range structure of La0.5Ca0.5MnO3 at room temperature and 20K. By combining Rietveld and pair distribution function analysis of the total neutron scattering data, we have analyzed the structure of the compound using two competing models describing the low temperature phase: first the charge ordered/orbital ordered model and second the Mn-Mn dimer model. These structural models fit the 20K neutron powder diffraction pattern equally well using Rietveld analysis. Therefore, pair distribution function analysis is used to probe the local and medium-range structure revealing a system with two distinctly distorted Mn octahedra and Mn ions with non-integral valence states. The distorted octahedra differ with the structural model for the Zener polaron type Mn-Mn dimer picture proposed for Pr0.6Ca0.4MnO3 and order in a similar checkerboard configuration associated with the CE-type anti-ferromagnetic structure. Therefore, locally the charge difference and structural ordering between the two Mn is appreciable enough to describe the system at 20K as "partially charge ordered".

cond-mat.str-el↗

Temperature dependent orbital degree of freedom in a bilayer manganite by magnetic Compton scattering

We have measured temperature-dependent magnetic Compton profiles (MCPs) from a single crystal of La$_{1.2}$Sr$_{1.8}$Mn$_2$O$_7$. The MCPs, which involved the scattering of circularly polarized x-rays, are in general related to the momentum density of all the unpaired spins in the system. Nevertheless, we show that when the x-ray scattering vector lies along the [110] direction, the number of magnetic electrons of a specific symmetry, i.e. $d$-electrons of $x^2-y^2$ symmetry, yield a distinct signature in the MCP, allowing us to monitor substantial changes in the occupancy of the $d_{x^2-y^2}$ states over the investigated temperature range of 5-200K. This study indicates that magnetic Compton scattering can provide a powerful window on the properties of specific magnetic electrons in complex materials.

cond-mat.str-el↗

Orbital correlations in the pseudo-cubic \emph{O} and rhombohedral ${R}$-phases of LaMnO$_3$

The local and intermediate structure of stoichiometric LaMnO$_3$ has been studied in the pseudocubic and rhombohedral phases at high temperatures (300 to 1150 K). Neutron powder diffraction data were collected and a combined Rietveld and high real space resolution atomic pair distribution function analysis carried out. The nature of the Jahn-Teller (JT) transition around 750 K is confirmed to be orbital order to disorder. In the high temperature orthorhombic ($O$) and rhombohedral ($R$) phases the MnO$_6$ octahedra are still fully distorted locally. The data suggest the presence of local orbitally ordered clusters of diameter $\sim 16$ Å($\sim$four MnO$_6$ octahedra) implying strong nearest neighbor JT anti-ferrodistortive coupling.

cond-mat.str-el↗

Field-induced avalanche to the ferromagnetic state in the phase-separated ground state of manganites

Perovskite manganite compounds such as Pr_(1-x)(Ca_(1-y)Sr_y)_xMn3 can be tuned to exhibit a metastable ground state where two magnetic/crystallographic phases coexist in zero magnetic field. Field-dependent neutron diffraction measurements on both poly- and single-crystal samples with a range of Pr, Ca, and Sr dopings(0.3<x<0.35 and y<0.30) reveal that the charge-ordered, antiferromagnetic phase of the ground state suddenly and irreversibly jumps to the ferromagnetic state. The transition occurs spontaneously at some time after the field is set above a threshold field, indicating that once the transition is initiated an avalanche occurs that drives it to completion.

cond-mat.str-el↗