arXiv subjects

J. P. Hill

Publications and source records attributed to J. P. Hill.

At least 73 records · Page 4Linked to original sources

arXiv2004

Resonant x-ray diffraction study of the magnetoresistant perovskite Pr0.6Ca0.4MnO3

We report a x-ray resonant diffraction study of the perovskite Pr0.6Ca0.4MnO3. At the Mn K-edge, this technique is sensitive to details of the electronic structure of the Mn atoms. We discuss the resonant x-ray spectra measured above and below the charge and orbital ordering phase transition temperature (TCOO = 232 K), and present a detailed analysis of the energy and polarization dependence of the resonant scattering. The analysis confirms that the structural transition is a transition to an orbitally ordered phase in which inequivalent Mn atoms are ordered in a CE-type pattern. The Mn atoms differ mostly by their 3d orbital occupation. We find that the charge disproportionation is incomplete, 3d^{3.5-δ} and 3d^{3.5+δ} with δ\ll0.5 . A revised CE-type model is considered in which there are two Mn sublattices, each with partial e_{g} occupancy. One sublattice consists of Mn atoms with the 3x^{2}-r^{2} or 3y^{2}-r^{2} orbitals partially occupied, the other sublattice with the x^{2}-y^{2} orbital partially occupied.

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arXiv2003

Soft x-ray resonant diffraction study of magnetic and orbital correlations in a manganite near half-doping

We have utilized the resonant x-ray diffraction technique at the Mn L-edge in order to directly compare magnetic and orbital correlations in the Mn sub-lattice of Pr0.6Ca0.4MnO3. The resonant line shape is measured below T_OO ~ 240 K at the orbital ordering wave vector (0,1/2,0), and below T_N ~ 175 K at the antiferromagnetic wave vector (1/2,0,0). Comparing the width of the super-lattice peaks at the two wavevectors, we find that the correlation length of the magnetism exceeds that of the orbital order by nearly a factor of two. Furthermore, we observe a large (~ 3 eV) shift in spectral weight between the magnetic and orbital line shapes, which cannot be explained within the classic Goodenough picture of a charge-ordered ground state. To explain the large shift, we calculate the resonant line shapes for orbital and magnetic diffraction based on a relaxed charge-ordered model.

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arXiv2003

Charge and orbital excitations in Li2CuO2

We report a resonant inelastic x-ray scattering study of electronic excitations in Li_2CuO_2, an insulating compound comprised of ribbons of edge-sharing copper-oxygen chains. Three excitations, which show little dependence on momentum transfer, are observed in our measurements. The lowest energy excitation at ~2.1 eV is dispersionless and is attributed to a localized d-d orbital excitation. We also observe two excitations at ~5.4 eV and ~7.6 eV which we assign to charge-transfer excitations. These high-energy excitations are also dispersionless along the copper-oxygen chain direction. However, in each case we observe a small energy dispersion along the direction perpendicular to the copper-oxygen ribbons, suggesting a significant interchain coupling in this system. We also discuss the possible implications of ferromagnetic nearest-neighbor intrachain coupling on the charge excitation spectra.

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arXiv2003

Substrate-induced strain effects on Pr_{0.6}Ca_{0.4}MnO_{3} films

We report the characterization of the crystal structure, low-temperature charge and orbital ordering, transport, and magnetization of Pr_{0.6}Ca_{0.4}MnO_{3} films grown on LaAlO_{3}, NdGaO_{3}, and SrTiO_{3} substrates, which provide compressive (LaAlO_{3}) and tensile (NdGaO_{3} and SrTiO_{3}) strain. The films are observed to exhibit different crystallographic symmetries than the bulk material, and the low-temperature ordering is found to be more robust under compressive-- as opposed to tensile-- strain. In fact, bulk-like charge and orbital ordering is not observed in the film grown on NdGaO_{3}, which is the substrate that provides the least amount of nominal and measured, but tensile, strain. This result suggests the importance of the role played by the Mn--O--Mn bond angles in the formation of charge and orbital ordering at low temperatures. Finally, in the film grown on LaAlO_{3}, a connection between the lattice distortion associated with orbital ordering and the onset of antiferromagnetism is reported.

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arXiv2003

Average Lattice Symmetry and Nanoscale Structural Correlations in Magnetoresistive Manganites

We report x-ray scattering studies of nanoscale structural correlations in the paramagnetic phases of the perovskite manganites La$_{0.75}$(Ca$_{0.45}$Sr$_{0.55}$)$_{0.25}$MnO$_3$, La$_{0.625}$Sr$_{0.375}$MnO$_3$, and Nd$_{0.45}$Sr$_{0.55}$MnO$_3$. We find that these correlations are present in the orthorhombic $O$ phase in La$_{0.75}$(Ca$_{0.45}$Sr$_{0.55}$)$_{0.25}$MnO$_3$, but they disappear abruptly at the orthorhombic-to-rhombohedral transition in this compound. The orthorhombic phase exhibits increased electrical resistivity and reduced ferromagnetic coupling, in agreement with the association of the nanoscale correlations with insulating regions. In contrast, the correlations were not detected in the two other compounds, which exhibit rhombohedral and tetragonal phases. Based on these results, as well as on previously published work, we propose that the local structure of the paramagnetic phase correlates strongly with the average lattice symmetry, and that the nanoscale correlations are an important factor distinguishing the insulating and the metallic phases in these compounds.

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arXiv2002

Resonant inelastic x-ray scattering study of charge excitations in La2CuO4

We report a resonant inelastic x-ray scattering study of the dispersion relations of charge transfer excitations in insulating La$_2$CuO$_4$. These data reveal two peaks, both of which show two-dimensional characteristics. The lowest energy excitation has a gap energy of $\sim 2.2$ eV at the zone center, and a dispersion of $\sim 1$ eV. The spectral weight of this mode becomes dramatically smaller around ($π$, $π$). The second peak shows a smaller dispersion ($\sim 0.5$ eV) with a zone-center energy of $\sim 3.9$ eV. We argue that these are both highly dispersive exciton modes damped by the presence of the electron-hole continuum.

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arXiv2002

Coherent X-ray Scattering from Manganite Charge and Orbital Domains

We report coherent x-ray scattering studies of charge and orbital domains in manganite systems. The experiments were carried out on LaMnO_3 and Pr_{0.6}Ca_{0.4}MnO_3, with the incident photon energy tuned near the Mn K edge. At room temperature, the orbital speckle pattern of LaMnO_3 was observed to be constant over a timescale of at least minutes, which is indicative of static orbital domains on this timescale. For Pr_{0.6}Ca_{0.4}MnO_3, both charge and orbital speckle patterns were observed. The observation of the latter rules out the presence of fast orbital fluctuations, while long time series data-- on the order of several minutes-- were suggestive of slow dynamic behavior. In contrast, the charge order speckle patterns were static.

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arXiv2002

Complex Quantum Phenomena in a Bilayered Calcium Ruthenate

Ca$_3$Ru$_2$O$_7$ undergoes an antiferromagnetic transition at $T_{\text{N}}=56 $K, followed by a Mott-like (MI) transition at $T_{\text{MI}}=48$ K. This nonmetallic ground state, with a charge gap of 0.1 eV, is suppressed by a highly anisotropic metamagnetic transition that leads to a fully spin-polarized metallic state. We report the observation of Shubnikov-de Haas oscillations in the \textit{gapped} state, colossal magnetoresistance in the inter-plane resistivity with a large anisotropy different from that observed in the magnetization, and non-Fermi liquid behavior in the metallic state at high magnetic fields.

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arXiv2001

Common features of nanoscale structural correlations in magnetoresistive manganites with ferromagnetic low-temperature state

We report x-ray scattering studies of nanoscale structural correlations in Nd$_{1-x}$Sr$_x$MnO$_3$ and La$_{1-x}$(Ca,Sr)$_x$MnO$_3$, $x$=0.2--0.5. We find that the correlated regions possess a temperature-independent correlation length of 2-3 lattice constants which is the same in all samples. The period of the lattice modulation of the correlated regions is proportional to the Ca/Sr doping concentration $x$. Remarkably, the lattice modulation periods of these and several other manganites with a ferromagnetic ground state fall on the same curve when plotted as a function of $x$. Thus, the structure of the correlated regions in these materials appears to be determined by a single parameter, $x$. We argue that these observations provide important clues for understanding the Colossal Magnetoresistance phenomenon in manganites.

cond-mat↗

arXiv2001

Magnetic-field-induced collapse of charge-ordered nanoclusters and the Colossal Magnetoresistance effect in Nd(0.3)Sr(0.3)MnO(3)

We report synchrotron x-ray scattering studies of charge/orbitally ordered (COO) nanoclusters in Nd$_{0.7}$Sr$_{0.3}$MnO$_3$. We find that the COO nanoclusters are strongly suppressed in an applied magnetic field, and that their decreasing concentration follows the field-induced decrease of the sample electrical resistivity. The COO nanoclusters, however, do not completely disappear in the conducting state, suggesting that this state is inhomogeneous and contains an admixture of an insulating phase. Similar results were also obtained for the zero-field insulator-metal transition that occurs as temperature is reduced. These observations suggest that these correlated lattice distortions play a key role in the Colossal Magnetoresistance effect in this prototypical manganite.

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arXiv2001

Orbital Correlations in Doped Manganites

We review our recent x-ray scattering studies of charge and orbital order in doped manganites, with specific emphasis on the role of orbital correlations in Pr_1-xCa_xMnO_3. For x=0.25, we find an orbital structure indistinguishable from the undoped structure with long range orbital order at low temperatures. For dopings 0.3<x<0.5, we find scattering consistent with a charge and orbitally ordered CE-type structure. While in each case the charge order peaks are resolution limited, the orbital order exhibits only short range correlations. We report the doping dependence of the correlation length and discuss the connection between the orbital correlations and the finite magnetic correlation length observed on the Mn^3+ sublattice with neutron scattering techniques. The physical origin of these domains, which appear to be isotropic, remains unclear. We find that weak orbital correlations persist well above the phase transitions, with a correlation length of 1-2 lattice constants at high temperatures. Significantly, we observe similar correlations at high temperatures in La_0.7Ca_0.3MnO_3, which does not have an orbitally ordered ground state, and we conclude that such correlations are robust to variations in the relative strength of the electron-phonon coupling.

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arXiv2001

A Resonant X-ray Scattering Study of Octahedral Tilt Ordering in LaMnO$_3$ and Pr$_{1-x}$Ca$_x$MnO$_3$

We report an x-ray scattering study of octahedral tilt ordering in the manganite series Pr$_{1-x}$Ca$_x$MnO$_3$ with x=0.4 and 0.25 and in LaMnO$_3$. The sensitivity to tilt ordering is achieved by tuning the incident x-ray energy to the L$_I$, L$_{II}$ and L$_{III}$ absorption edges of Pr and La, respectively. The resulting energy-dependent profiles are characterized by a dipole-resonant peak and higher energy fine structure. The polarization dependence is predominantly $σ$-to-$π$ and the azimuthal dependence follows a sin-squared behavior. These results are similar to those obtained in recent x-ray scattering studies of orbital ordering carried out in these same materials at the Mn K edge. They lead to a description of the cross-section in terms of Templeton scattering in which the tilt ordering breaks the symmetry at the rare earth site. The most interesting result of the present work is our observation that octahedral tilt ordering persists above the orbital ordering transition temperatures in all three samples. Indeed, we identify separate structural transitions which may be associated with the onset of orbital and tilt ordering, respectively, and characterize the loss of tilt ordering versus temperature in LaMnO$_3$.

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arXiv2001

Nanoscale anisotropic structural correlations in the paramagnetic and ferromagnetic phases of Nd0.5Sr0.5 MnO3

We report x-ray scattering studies of short-range structural correlations and diffuse scattering in Nd0.5Sr0.5MnO3. On cooling, this material undergoes a series of transitions, first from a paramagnetic insulating (PI) to a ferromagnetic metallic (FM) phase, and then to a charge-ordered (CO) insulating state. Highly anisotropic structural correlations were found in both the PI and FM states. The correlations increase with decreasing temperature, reaching a maximum at the CO transition temperature. Below this temperature, they abruptly collapsed. Single-polaron diffuse scattering was also observed in both the PI and FM states suggesting that substantial local lattice distortions are present in these phases. We argue that our measurements indicate that nanoscale regions exhibiting layered orbital order exist in the paramagnetic and ferromagnetic phases of Nd0.5Sr0.5MnO3.

cond-mat↗

arXiv2000

Correlated Polarons in Dissimilar Perovskite Manganites

We report x-ray scattering studies of broad peaks located at a (0.5 0 0)/(0 0.5 0)-type wavevector in the paramagnetic insulating phases of La_{0.7}Ca_{0.3}MnO_{3} and Pr_{0.7}Ca_{0.3}MnO_{3}. We interpret the scattering in terms of correlated polarons and measure isotropic correlation lengths of 1-2 lattice constants in both samples. Based on the wavevector and correlation lengths, the correlated polarons are found to be consistent with CE-type bipolarons. Differences in behavior between the samples arise as they are cooled through their respective transition temperatures and become ferromagnetic metallic (La_{0.7}Ca_{0.3}MnO_{3}) or charge and orbitally ordered insulating (Pr_{0.7}Ca_{0.3}MnO_{3}). Since the primary difference between the two samples is the trivalent cation size, these results illustrate the robust nature of the correlated polarons to variations in the relative strength of the electron-phonon coupling, and the sensitivity of the low-temperature ground state to such variations.

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arXiv2000

Spin Dynamics and Orbital State in LaTiO_3

A neutron scattering study of the Mott-Hubbard insulator LaTiO$_{3}$ (T$_{\rm N}=132$ K) reveals a spin wave spectrum that is well described by a nearest-neighbor superexchange constant $J=15.5$ meV and a small Dzyaloshinskii-Moriya interaction ($D=1.1$ meV). The nearly isotropic spin wave spectrum is surprising in view of the absence of a static Jahn-Teller distortion that could quench the orbital angular momentum, and it may indicate strong orbital fluctuations. A resonant x-ray scattering study has uncovered no evidence of orbital order in LaTiO$_{3}$.

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arXiv2000

X-ray Anomalous Scattering Study of a Charge-Ordered State in NaV2O5

Charge ordering of V4+ and V5+ in NaV2O5 has been studied by an X-ray diffraction technique using anomalous scattering near a vanadium K-absorption edge to critically enhance a contrast between the two ions. A dramatic energy dependence of the superlattice intensities is observed below Tc=35 K. Consequently, the charge ordering pattern is the zigzag-type ladders with the unit cell 2a*2b*4c, but not the chain-type originally proposed for the spin-Peierls state. Charge disproportionation suggested in our model as the average valence V^{4.5+-delta_c/2} is observed below T_C, showing continuous variation of delta_c as a function of temperature.

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arXiv2000

Multiphase segregation and metal-insulator transition in single crystal La(5/8-y)Pr(y)Ca(3/8)MnO3

The insulator-metal transition in single crystal La(5/8-y)Pr(y)Ca(3/8)MnO3 with y=0.35 was studied using synchrotron x-ray diffraction, electric resistivity, magnetic susceptibility, and specific heat measurements. Despite the dramatic drop in the resistivity at the insulator-metal transition temperature Tmi, the charge-ordering (CO) peaks exhibit no anomaly at this temperature and continue to grow below Tmi. Our data suggest then, that in addition to the CO phase, another insulating phase is present below Tco. In this picture, the insulator-metal transition is due to the changes within this latter phase. The CO phase does not appear to play a major role in this transition. We propose that a percolation-like insulator-metal transition occurs via the growth of ferromagnetic metallic domains within the parts of the sample that do not exhibit charge ordering. Finally, we find that the low-temperature phase-separated state is unstable against x-ray irradiation, which destroys the CO phase at low temperatures.

cond-mat↗

arXiv2000

X-ray Resonant Scattering Studies of Orbital and Charge Ordering in Pr$_{1-x}$Ca$_x$MnO$_3$

We present the results of a systematic x-ray scattering study of the charge and orbital ordering in the manganite series Pr$_{1-x}$Ca$_x$MnO$_3$ with $x$=0.25, 0.4 and 0.5. The temperature dependence of the scattering at the charge and orbital wavevectors, and of the lattice constants, was characterized throughout the ordered phase of each sample. It was found that the charge and orbital order wavevectors are commensurate with the lattice, in striking contrast to the results of earlier electron diffraction studies of samples with $x$=0.5. High momentum-transfer resolution studies of the x=0.4 and 0.5 samples further revealed that while long-range charge order is present, long-range orbital order is never established. Above the charge/orbital ordering temperature T$_o$, the charge order fluctuations are more highly correlated than the orbital fluctuations. This suggests that charge order drives orbital order in these samples. In addition, a longitudinal modulation of the lattice with the same periodicity as the charge and orbital ordering was discovered in the x=0.4 and 0.5 samples. For x=0.25, only long-range orbital order was observed with no indication of charge ordering, nor of an additional lattice modulation. We also report the results of a preliminary investigation of the loss of charge and orbital ordering in the x=0.4 sample by application of a magnetic field. Finally, the polarization and azimuthal dependence of the charge and orbital ordering in these compounds is characterized both in the resonant and nonresonant limits, and compared with the predictions of current theories. The results are qualitatively consistent with both cluster and LDA+U calculations of the electronic structure.

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