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High-harmonic generation (HHG) is a typical high-order nonlinear optical phenomenon and can be used to probe electronic structures of solids. Here, we investigate the temperature dependence of HHG from Pr_{0.6}Ca_{0.4}MnO_{3} in the range of 7 K to 294 K including the charge ordering (CO) transition and magnetic transition temperatures. The high-harmonic intensity remains almost constant in the high-temperature charge-disordered phase. However, as the temperature is lowered, it starts to gradually increase near the CO transition temperature where an optical gap related to the CO phase appears. The anomalous gap energy dependence resembles the one recently reported in a Mott insulator. We attribute the HHG suppression at high temperatures to the destructive interference among high-harmonic emissions from thermally activated multiple CO configurations. Our results suggest that HHG is a promising tool for probing the fluctuation of local order in strongly correlated systems., Comment: 16 pages, 8 figures

Electric quadrupolar state in a frustrated quantum magnet $\rm Tb_{2+\it \delta}Ti_{2-\it \delta}O_7$ has been studied by means of ultrasonic and magnetostriction measurements. A single crystal showed elastic anomaly at about 0.4 K, manifesting a long-range quadrupole ordering. By investigating anisotropy of the magnetoelastic responses, we found a crossover temperature for the strongly correlated quadrupole state, below which the experimental data of elastic constant and magnetostriction become qualitatively different from their calculations based on a single-ion model. We suppose that relatively high onset temperature of the quadrupole correlation compared with the transition temperature is ascribed to the geometrical frustration effect, and this correlated state seems to be responsible for the unusual properties in the paramagentic state of $\rm Tb_2Ti_2O_7$., Comment: 9 pages, 9 figures

We report the direct observation of a "resonance" mode in the lowest-energy optic phonon very near the zone center around (111) in the multiferroic BiFeO$_3$ using neutron scattering methods. The phonon scattering intensity is enhanced when antiferromagnetic (AFM) order sets in at T$_N = 640$~K, and it increases on cooling. This "resonance" is confined to a very narrow region in energy-momentum space where no spin-wave excitation intensity is expected, and it can be modified by an external magnetic field. Our results suggest the existence of a novel coupling between the lattice and spin fluctuations in this multiferroic system in which the spin-wave excitations are mapped onto the lattice vibrations via the Dzyaloshinskii-Moriya (DM) interaction.

We use spatially-resolved transport techniques to investigate the superconducting properties of single crystals La$_{2-x}$Ba$_x$CuO$_4$. We find a new superconducting transition temperature $T_{cs}$ associated with the ab-plane surface region which is considerably higher than the bulk $T_c$. The effect is pronounced in the region of charge carrier doping $x$ with strong spin-charge stripe correlations, reaching $T_{cs}=36$ K or 1.64$T_c$.

We report on a thermoelectric investigation of the stripe and superconducting phases of the cuprate La$_{2-x}$Ba$_{x}$CuO$_{4}$ near the $x=1/8$ doping known to host stable stripes. We use the doping and magnetic field dependence of field-symmetric Nernst effect features to delineate the phenomenology of these phases. Our measurements are consistent with prior reports of time-reversal symmetry breaking signatures above the superconducting $T_{{\rm c}}$, and crucially detect a sharp, robust, field-invariant peak at the stripe charge order temperature, $T_{{\rm {\scriptscriptstyle CO}}}$. Our observations suggest the onset of a nontrivial charge ordered phase at $T_{{\rm {\scriptscriptstyle CO}}}$, and the subsequent presence of spontaneously generated vortices over a broad temperature range before the emergence of bulk superconductivity in LBCO.

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., Comment: 14 pages, 11 figures

We present neutron inelastic scattering measurements of the low-energy phonons in single crystal BiFeO3. The dispersions of the three acoustic phonon modes (LA along [100], TA1 along [010] and TA2 along [110]) and two low energy optic phonon modes (LO and TO1) have been mapped out between 300 K and 700 K. Elastic constants are extracted from the phonon measurements. The energy linewidths of both TA phonons at the zone boundary clearly broaden when the system is warmed toward the magnetic ordering temperature TN = 640 K. This suggests that the magnetic and low-energy lattice dynamics in this multiferroic material are coupled.

We have performed an angle-resolved photoemission spectroscopy (ARPES) study of BaNi$_2$P$_2$ which shows a superconducting transition at $T_c$ $\sim$ 2.5 K. We observed hole and electron Fermi surfaces (FSs) around the Brillouin zone center and corner, respectively, and the shapes of the hole FSs dramatically changed with photon energy, indicating strong three-dimensionality. The observed FSs are consistent with band-structure calculation and de Haas-van Alphen measurements. The mass enhancement factors estimated in the normal state were $m^*$/$m_b$ $\leq$ 2, indicating weak electron correlation compared to typical iron-pnictide superconductors. An electron-like Fermi surface around the Z point was observed in contrast with BaNi$_2$As$_2$ and may be related to the higher $T_c$ of BaNi$_2$P$_2$., Comment: 6 figures

We carried out a comparative study of the in-plane resistivity and optical spectrum of doped BaFe2As2 and investigated the doping evolution of the charge dynamics. For BaFe2As2, charge dynamics is incoherent at high temperatures. Electron (Co) and isovalent (P) doping into BaFe2As2 increase coherence of the system and transform the incoherent charge dynamics into highly coherent one. On the other hand, charge dynamics remains incoherent for hole (K) doping. It is found in common with any type of doping that superconductivity with high transition temperature emerges when the normal-state charge dynamics maintains incoherence and when the resistivity associated with the coherent channel exhibits dominant temperature-linear dependence., Comment: 8 pages, 5 figures

We carried out combined transport and optical measurements for BaFe2As2 and five isostructural transition-metal (TM) pnictides. The low-energy optical conductivity spectra of these compounds are, to a good approximation, decomposed into a narrow Drude (coherent) component and an incoherent component. The iron arsenides, BaFe2As2 and KFe2As2, are distinct from other pnictides in their highly incoherent charge dynamics or bad metallic behavior with the coherent Drude component occupying a tiny fraction of the low-energy spectral weight. The fraction of the coherent spectral weight or the degree of coherence is shown to be well correlated with the TM-pnictogen bond angle and the electron filling of TM 3d orbitals, which are measures of the strength of electronic correlations. The iron arsenides are thus strongly correlated systems, and the doping into BaFe2As2 controls the strength of electronic correlations. This naturally explains a remarkable asymmetry in the charge dynamics of electron- and hole-doped systems, and the unconventional superconductivity appears to emerge when the correlations are fairly strong., Comment: 6 pages, 4 figures

The nature of the pseudogap in high transition temperature (high-Tc) superconducting cuprates has been a major issue in condensed matter physics. It is still unclear whether the high-Tc superconductivity can be universally associated with the pseudogap formation. Here we provide direct evidence of the existence of the pseudogap phase via angle-resolved photoemission spectroscopy in another family of high-Tc superconductor, iron-pnictides. Our results reveal a composition dependent pseudogap formation in the multi-band electronic structure of BaFe2(As1-xPx)2. The pseudogap develops well above the magnetostructural transition for low x, persists above the nonmagnetic superconducting dome for optimal x and is destroyed for x ~ 0.6, thus showing a notable similarity with cuprates. In addition, the pseudogap formation is accompanied by inequivalent energy shifts in xz/yz orbitals of iron atoms, indicative of a peculiar iron orbital ordering which breaks the four-fold rotational symmetry., Comment: 14 pages, 10 figures

In Fe-based superconductors, electron doping is often realized by the substitution of transition-metal atoms for Fe. In order to investigate how the electronic structure of the parent compound is influenced by Zn substitution, which supplies nominally four extra electrons per substituted atom but is expected to induce the strongest impurity potential among the transition-metal atoms, we have performed an angle-resolved photoemission spectroscopy measurements on Ba(Fe_{1-x}Zn_x)_2As_2 (Zn-122). In Zn-122, the temperature dependence of the resistivity shows a kink around T~135 K, indicating antiferromagnetic order below the Neel temperature of T_N ~ 135 K. In fact, folded Fermi surfaces (FSs) similar to those of the parent compound have been observed below T_N. The hole and electron FS volumes are, therefore, different from those expected from the rigid-band model. The results can be understood if all the extra electrons occupy the Zn 3d state ~10 eV below the Fermi level and do not participate in the formation of the FSs., Comment: 6 pages, 8 figures

In the iron pnictide superconductors, two distinct unconventional mechanisms of superconductivity have been put forth: One is mediated by spin fluctuations leading to the s+- state with sign change of superconducting gap between the hole and electron bands, and the other is orbital fluctuations which favor the s++ state without sign reversal. Here we report direct observation of peculiar momentum-dependent anisotropy in the superconducting gap from angle-resolved photoemission spectroscopy (ARPES) in BaFe2(As1-xPx)2 (Tc=30 K). The large anisotropy found only in the electron Fermi surface (FS) and the nearly isotropic gap on the entire hole FSs are together consistent with modified s+- gap with nodal loops, which can be theoretically reproduced by considering both spin and orbital fluctuations whose competition generates the gap modulation. This indicates that these two fluctuations are nearly equally important to the high-Tc superconductivity in this system.

Electronic orderings of charges, orbitals and spins are observed in many strongly correlated electron materials, and revealing their dynamics is a critical step toward understanding the underlying physics of important emergent phenomena. Here we use time-resolved resonant soft x-ray scattering spectroscopy to probe the dynamics of antiferromagnetic spin ordering in the manganite Pr$_{0.7}$Ca$_{0.3}$MnO$_3$ following ultrafast photo-exitation. Our studies reveal a glass-like recovery of the spin ordering and a crossover in the dimensionality of the restoring interaction from quasi-1D at low pump fluence to 3D at high pump fluence. This behavior arises from the metastable state created by photo-excitation, a state characterized by spin disordered metallic droplets within the larger charge- and spin-ordered insulating domains. Comparison with time-resolved resistivity measurements suggests that the collapse of spin ordering is correlated with the insulator-to-metal transition, but the recovery of the insulating phase does not depend on the re-establishment of the spin ordering., Comment: Scientific Reports, in press

We investigated the anisotropy in the in-plane optical spectra of detwinned Ba(Fe1-xCox)2As2. The optical conductivity spectrum of BaFe2As2 shows appreciable anisotropy in the magnetostructural ordered phase, whereas the dc resistivity is almost isotropic at low temperatures. Upon Co doping, the resistivity becomes highly anisotropic, while the finite-energy intrinsic anisotropy is suppressed. It is found that anisotropy in resistivity arises from anisotropic impurity scattering from doped Co atoms, extrinsic in origin. Intensity of a specific optical phonon mode is also found to show striking anisotropy in the ordered phase. The anisotropy induced by Co impurity and that observed in the optical phonon mode are hallmarks of the highly polarizable electronic state in the ordered phase., Comment: 5 pages, 4 figures

We investigated the in-plane resistivity anisotropy for underdoped Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$ single crystals with improved quality. We demonstrate that the anisotropy in resistivity in the magnetostructural ordered phase arises from the anisotropy in the residual component which increases in proportion to the Co concentration $x$. This gives evidence that the anisotropy originates from the impurity scattering by Co atoms substituted for the Fe sites, rather than so far proposed mechanism such as the anisotropy of Fermi velocities of reconstructed Fermi surface pockets. As doping proceeds to the paramagnetic-tetragonal phase, a Co impurity transforms to a weak and isotropic scattering center., Comment: 12 pages, 3figures, published in PRL 110, 207001 (2013)

In order to examine to what extent the rigid-band-like electron doping scenario is applicable to the transition metal-substituted Fe-based superconductors, we have performed angle-resolved photoemission spectroscopy studies of Ba(Fe$_{1-x}$Ni$_{x}$)$_2$As$_2$ (Ni-122) and Ba(Fe$_{1-x}$Cu$_{x}$)$_2$As$_2$ (Cu-122), and compared the results with Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$ (Co-122). We find that Ni 3$\it{d}$-derived features are formed below the Fe 3$\it{d}$ band and that Cu 3$\it{d}$-derived ones further below it. The electron and hole Fermi surface (FS) volumes are found to increase and decrease with substitution, respectively, qualitatively consistent with the rigid-band model. However, the total extra electron number estimated from the FS volumes (the total electron FS volume minus the total hole FS volume) is found to decrease in going from Co-, Ni-, to Cu-122 for a fixed nominal extra electron number, that is, the number of electrons that participate in the formation of FS decreases with increasing impurity potential. We find that the N$\acute{\rm{e}}$el temperature $T_{\rm{N}}$ and the critical temperature $T_{\it{c}}$ maximum are determined by the FS volumes rather than the nominal extra electron concentration nor the substituted atom concentration., Comment: Total: 9 pages, 10 figures

We have determined the full magnetic dispersion relations of multiferroic BiFeO3. In particular, two excitation gaps originating from magnetic anisotropies have been clearly observed. The direct observation of the gaps enables us to accurately determine the Dzyaloshinskii-Moriya (DM) interaction and the single ion anisotropy. The DM interaction supports a strong magneto-electric coupling in this compound., Comment: 5 pages, 5 figures

We investigated the transport properties of BaFe$_2$As$_2$ single crystals before and after annealing with BaAs powder. The annealing remarkably improves transport properties, in particular the magnitude of residual resistivity which decreases by a factor of more than 10. From the resistivity measurement on detwinned crystals we found that the anisotropy of the in-plane resistivity is remarkably diminished after annealing, indicative of dominant contributions to the charge transport from the carriers with isotropic and high mobility below magnetostructural transition temperature $T_{\rm s}$ and the absence of nematic state above $T_{\rm s}$. We found that the Hall resistivity shows strong non-linearity against magnetic field and the magnetoresistance becomes very large at low temperatures. These results give evidence for the manifestation of multiple carriers with distinct characters in the ordered phase below $T_{\rm s}$. By analyzing the magnetic field dependences, we found that at least three carriers equally contribute to the charge transport in the ordered phase, which is in good agreement with the results of recent quantum oscillation measurements., Comment: 20 pages, 8 figures, 2 tables, Published in Physical Review B

An ordered phase showing remarkable electronic anisotropy in proximity to the superconducting phase is now a hot issue in the field of high-transition-temperature superconductivity. As in the case of copper oxides, superconductivity in iron arsenides competes or coexists with such an ordered phase. Undoped and underdoped iron arsenides have a magnetostructural ordered phase exhibiting stripe-like antiferromagnetic spin order accompanied by an orthorhombic lattice distortion; both the spin order and lattice distortion break the tetragonal symmetry of crystals of these compounds. In this ordered state, anisotropy of in-plane electrical resistivity is anomalous and difficult to attribute simply to the spin order and/or the lattice distortion. Here, we present the anisotropic optical spectra measured on detwinned BaFe2As2 crystals with light polarization parallel to the Fe planes. Pronounced anisotropy is observed in the spectra, persisting up to an unexpectedly high photon energy of about 2 eV. Such anisotropy arises from an anisotropic energy gap opening below and slightly above the onset of the order. Detailed analysis of the optical spectra reveals an unprecedented electronic state in the ordered phase., Comment: 7 pages, 7 figures, accepted to PNAS

We present resonant soft X-ray scattering (RSXS) results from small band width manganites (Pr,Ca)MnO$_3$, which show that the CE-type spin ordering (SO) at the phase boundary is stabilized only below the canted antiferromagnetic transition temperature and enhanced by ferromagnetism in the macroscopically insulating state (FM-I). Our results reveal the fragility of the CE-type ordering that underpins the colossal magnetoresistance (CMR) effect in this system, as well as an unexpected cooperative interplay between FM-I and CE-type SO which is in contrast to the competitive interplay between the ferromagnetic metallic (FM-M) state and CE-type ordering., Comment: Accepted for publication in Phys. Rev. Lett

We investigated the optical spectrum of Ba(Fe1-xCox)2As2 single crystals with various doping levels. It is found that the low-energy optical conductivity spectrum of this system can be decomposed into two components: a sharp Drude term and a broad "incoherent" term. For the compounds showing magnetic order, a gap appears predominantly in the "incoherent" component, while an s-wave like superconducting gap opens in both components for highly doped compounds. The Drude weight steadily increases as doping proceeds, consistent with electron doping in this system. On the other hand, the "incoherent" spectral weight is almost doping independent, but its spectral feature is intimately connected with the magnetism. We demonstrate that the presence of two distinct components in the optical spectrum well explains the doping and temperature dependences of the dc resistivity., Comment: 10 pages, 10 figures, to be published in Phys. Rev. B

Characteristic normal-state charge transport is found in the oxygen-deficient iron-arsenides LnFeAsO1-y (Ln: La and Nd) with the highest Tc's among known Fe-based superconductors. The effect of "doping" in this system is mainly on the carrier scattering, quite distinct from that in high-Tc cuprates. In the superconducting regime of the La system with maximum Tc = 28 K, the low-temperature resistivity is dominated by a T^2 term. On the other hand, in the Nd system with Tc higher than 40 K, the carriers are subject to stronger scattering showing T-linear resistivity and small magnetoresistance. Such strong scattering appears crucial for high-Tc superconductivity in the iron-based system., Comment: 7 pages, 6 figures

We report that the incorporation of hydroxide ions (OH)- significantly enhances the superconducting transition temperature (Tc) in the LnFeAsO-based superconductors (Ln1111: Ln = La, Ce and Pr). For La1111, Tc of the (OH)- incorporated sample synthesized using high-pressure technique becomes 35 K, which is higher by 7 K than the typical optimally-doped La1111 superconductors. Similar enhancement in Tc is also observed for Ce1111 and Pr1111. 1H-NMR measurement have confirmed the existence of hydrogen atoms in the samples. Accompanying the (OH)- incorporation, the lattice parameters are largely contracted, down to the values which have never been attained by any other dopings/substitutions., Comment: 8 pages, 5 figures, 1 table, Appl. Phys. Lett. to be published

We have studied the effects of band filling and bandwidth control on the chemical potential in perovskite manganites $R_{1-x}A_x$MnO$_3$ ($R$ : rare earth, $A$ : alkaline earth) by measurements of core-level photoemission spectra. A suppression of the doping-dependent chemical potential shift was observed in and around the CE-type charge-ordered composition range, indicating that there is charge self-organization such as stripe formation or its fluctuations. As a function of bandwidth, we observed a downward chemical potential shift with increasing bandwidth due to the reduction of the orthorhombic distortion. After subtracting the latter contribution, we found an upward chemical potential shift in the ferromagnetic metallic region $0.3

Neutron scattering has been used to investigate the evolution of the long- and short-range charge-ordered (CO), ferromagnetic (FM), and antiferromagnetic (AF) correlations in single crystals of Pr1-xCaxMnO3. The existence and population of spin clusters as refected by short-range correlations are found to drastically depend on the doping (x) and temperature (T). Concentrated spin clusters coexist with long-range canted AF order in a wide temperature range in x = 0.3 while clusters do not appear in x = 0.4 crystal. In contrast, both CO and AF order parameters in the x = 0.35 crystal show a precipitous decrease below ~ 35 K where spin clusters form. These results provide direct evidence of magnetic phase separation and indicate that there is a critical doping x_c (close to x = 0.35) that divides the phase-separated site-centered from the homogeneous bond-centered or charge-disproportionated CO ground state., Comment: 4 pages, 4 figures, submitted to Phys. Rev. Letters

A detailed study of the electric field gradient (EFG) across the Pr1-xCaxMnO3 phase diagram and its temperature dependence is given. Clearly, distinct EFG behaviours for samples outside/inside the charge order (CO) region are observed. The EFG temperature dependence evidences a new phase transition occurring over the broad CO region of the phase diagram. This transition is discontinuous and occurs at temperatures between the charge ordering and the Neel temperatures. The features observed in the EFG are associated with polar atomic vibrations which eventually lead to a spontaneous local electric polarization below CO transition., Comment: 8 pages, 4 figures

We have studied the bandwidth-temperature-magnetic field phase diagram of RE(0.55)Sr(0.45)MnO(3) colossal magnetoresistance manganites with ferromagnetic metallic (FM) ground state. The bandwidth (or equivalently the double exchange interaction) was controlled both via chemical substitution and hydrostatic pressure with a focus on the vicinity of the critical pressure p* where the character of the zero-field FM transition changes from first to second order. Below p* the first-order FM transition extends up to a critical magnetic field, H_cr. It is suppressed by pressure and approaches zero on the larger bandwidth side where the surface of the first-order FM phase boundary is terminated by a multicritical end-point (p*~32 kbar, T*~188 K, H*=0). The change in the character of the transition and the decrease of the CMR effect is attributed to the reduced CO/OO fluctuations., Comment: 4 pages, 4 figures

We have studied the chemical potential shift as a function of temperature in Nd$_{1-x}$Sr$_x$MnO$_3$ (NSMO) by measurements of core-level photoemission spectra. For ferromagnetic samples ($x=0.4$ and 0.45), we observed an unusually large upward chemical potential shift with decreasing temperature in the low-temperature region of the ferromagnetic metallic (FM) phase. This can be explained by the double-exchange (DE) mechanism if the $e_g$ band is split by dynamical/local Jahn-Teller effect. The shift was suppressed near the Curie temperature ($T_C$), which we attribute to the crossover from the DE to lattice-polaron regimes., Comment: 5 pages, 6 figures

We present a systematic optical study for a bandwidth-controlled series of nearly half doped colossal magnetoresistive manganites RE$_{0.55}$AE$_{0.45}$MnO$_3$ (RE and AE being rare earth and alkaline earth ions, respectively) under the presence of quenched disorder over a broad temperature region $T=10-800$ K. The ground state of the compounds ranges from the charge and orbital ordered insulator through the spin glass to the ferromagnetic metal. The enhanced phase fluctuations, namely the short-range charge and orbital correlations dominate the paramagnetic region of the phase diagram above all the ground-state phases. This paramagnetic region is characterized by a full-gap to pseudo-gap crossover towards elevated temperatures where a broad low-energy electronic structure appears in the conductivity spectra over a large variation of the bandwidth. This pseudo-gap state with local correlations is robust against thermal fluctuations at least up to T=800 K. For small bandwidth the onset of the long-range charge order is accompanied by an instantaneous increase of the gap. The emergence of the ferromagnetic state is manifested in the optical spectra as a first-order insulator to metal transition for compounds with moderate bandwidth while it becomes a second-order transition on the larger bandwidth side. Unusually large scattering rate of the metallic carriers is observed in the ferromagnetic state which is attributed to orbital correlation with probably rod-like ($3z^2-r^2$-like) character.

The coupling of multiple degrees of freedom - charge, spin, and lattice - in manganites has mostly been considered at the microscopic level. However, on larger length scales, these correlations may be affected by strain and disorder, which can lead to short range order in these phases and affect the coupling between them. To better understand these effects, we explore the dynamics of orbitally ordered domains in a half-doped manganite near the orbital ordering phase transition. Our results suggest that the domains are largely static, and exhibit only slow fluctuations near domain boundaries., Comment: 10 pages, 4 figures

We have studied the temperature dependence of the photoemission spectra of Pr$_{1-x}$Ca$_x$MnO$_3$ (PCMO) with $x=0.25$, 0.3 and 0.5. For $x=0.3$ and 0.5, we observed a gap in the low-temperature CE-type charge-ordered (CO) phase and a pseudogap with a finite intensity at the Fermi level ($E_F$) in the high-temperature paramagnetic insulating (PI) phase. Within the CO phase, the spectral intensity near $E_F$ gradually increased with temperature. These observations are consistent with the results of Monte Carlo simulations on a model including charge ordering and ferromagnetic fluctuations [H. Aliaga {\it et al.} Phys. Rev. B {\bf 68}, 104405 (2003)]. For $x=0.25$, on the other hand, little temperature dependence was observed within the low-temperature ferromagnetic insulating (FI) phase and the intensity at $E_F$ remained low in the high-temperature PI phase. We attribute the difference in the temperature dependence near $E_F$ between the CO and FI phases to the different correlation lengths of orbital order between both phases. Furthermore, we observed a chemical potential shift with temperature due to the opening of the gap in the FI and CO phases. The doping dependent chemical potential shift was recovered at low temperatures, corresponding to the disappearance of the doping dependent change of the modulation wave vector. Spectral weight transfer with hole concentration was clearly observed at high temperatures but was suppressed at low temperatures. We attribute this observation to the fixed periodicity with hole doping in PCMO at low temperatures., Comment: 5pages, 7figures

Using time-of-flight and triple-axis inelastic neutron spectroscopy, we determine spin wave excitations throughout the Brillouin zone for ferromagnetic manganites La$_{1-x}$Ca$_x$MnO$_3$ ($x=0.25,0.3$) in their low temperature metallic states. While spin wave excitations in the long wavelength limit (spin stiffness $D$) have similar values for both compounds, the excitations near the Brillouin zone boundary of La$_{0.7}$Ca$_{0.3}$MnO$_3$ are considerable softened in all symmetry directions compared to that of La$_{0.75}$Ca$_{0.25}$MnO$_3$. A Heisenberg model with the nearest neighbor and the fourth neighbor exchange interactions can describe the overall dispersion curves fairly well. We compare the data with various theoretical models describing the spin excitations of ferromagnetic manganites., Comment: to be published in Phys. Rev. B

Phase diagrams in the plane of $r_A$ (the average ionic radius, related to one-electron bandwidth $W$) and $\sigma^2$ (the ionic radius variance, measuring the quenched disorder), or ``bandwidth-disorder phase diagrams'', have been established for perovskite manganites, with three-dimensional (3$D$) Mn-O network. Here we establish the intrinsic bandwidth-disorder phase diagram of half-doped layered manganites with the two-dimensional (2$D$) Mn-O network, examining in detail the ``mother state'' of the colossal magnetoresistance (CMR) phenomenon in crystals without ferromagnetic instability. The consequences of the reduced dimensionality, from 3$D$ to 2$D$, on the order-disorder phenomena in the charge-orbital sectors are also highlighted., Comment: REVTeX 4 style; 5 pages, 4 figures

We have studied the chemical potential shift and changes in the electronic density of states near the Fermi level ($E_F$) as a function of carrier concentration in Pr$_{1-x}$Ca$_x$MnO$_3$ (PCMO, $0.2 \le x \le 0.65$) through the measurements of photoemission spectra. The results showed that the chemical potential shift was suppressed for $x \agt 0.3$, where the charge exchange (CE)-type antiferromagnetic charge-ordered state appears at low temperatures. We consider this observation to be related to charge self-organization such as stripe formation on a microscopic scale in this composition range. Together with the previous observation of monotonous chemical potential shift in La$_{1-x}$Sr$_x$MnO$_3$, we conclude that the tendency toward the charge self-organization increases with decreasing bandwidth. In the valence band, spectral weight of the Mn 3$d$ $e_g$ electrons in PCMO was transferred from $\sim$ 1 eV below $E_F$ to the region near $E_F$ with hole doping, leading to a finite intensity at $E_F$ even in the paramagnetic insulating phase for $x \agt 0.3$, probably related with the tendency toward charge self-organization. The finite intensity at $E_F$ in spite of the insulating transport behavior is consistent with fluctuations involving ferromagnetic metallic states., Comment: 6 pages, 5 figures

Neutron scattering results are presented for spin-wave excitations of three ferromagnetic metallic $A_{1-x}A^{\prime}_{x}$MnO$_3$ manganites (where $A$ and $A^\prime$ are rare- and alkaline-earth ions), which when combined with previous work elucidate systematics of the interactions as a function of carrier concentration $x$, on-site disorder, and strength of the lattice distortion. The long wavelength spin dynamics show only a very weak dependence across the series. The ratio of fourth to first neighbor exchange ($J_4/J_1$) that controls the zone boundary magnon softening changes systematically with $x$, but does not depend on the other parameters. None of the prevailing models can account for these behaviors., Comment: Submitted to Phys. Rev. Lett

We use neutron scattering to study the spin and charge/orbital ordering (CO-OO) in the nearly half-doped perovskite manganite $Pr_{0.55}(Ca_{0.8}Sr_{0.2})_{0.45}MnO_3$ (PCSMO). On cooling from room temperature, PCSMO first enters into a CO-OO state below $T_{CO}$ and then becomes a CE-type long-range ordered antiferromagnet below $T_N$. At temperatures above $T_N$ but below $T_{CO}$ ($T_N

The temperature dependence of the O K-edge pre-edge structure in the x-ray absorption spectra of the perovskites La(1-x)A(x)MnO(3), (A = Ca, Sr; x = 0.3, 0.4) reveals a correlation between the disappearance of the splitting in the pre-edge region and the presence of Jahn-Teller distortions. The different magnitudes of the distortions for different compounds is proposed to explain some dissimilarity in the line shape of the spectra taken above the Curie temperature., Comment: To appear in Phys. Rev. B, 5 pages, 3 figures

We report the observation of temperature dependent electronic excitations in various manganites utilizing resonant inelastic x-ray scattering (RIXS) at the Mn K-edge. Excitations were observed between 1.5 and 16 eV with temperature dependence found as high as 10 eV. The change in spectral weight between 1.5 and 5 eV was found to be related to the magnetic order and independent of the conductivity. On the basis of LDA+U and Wannier function calculations, this dependence is associated with intersite d-d excitations. Finally, the connection between the RIXS cross-section and the loss function is addressed., Comment: 5 pages, 5 figures

The magnetic and electrical properties of high quality single crystals of $A$-site disordered (solid solution) Ln$_{0.5}$Ba$_{0.5}$MnO$_3$ are investigated near the phase boundary between the spin glass insulator and colossal-magnetoresistive ferromagnetic metal, locating near Ln = Sm. The temperature dependence of the ac-susceptibility and the x-ray diffuse scattering of Eu$_{0.5}$Ba$_{0.5}$MnO$_3$ are analyzed in detail. The uniformity of the random potential perturbation in Ln$_{0.5}$Ba$_{0.5}$MnO$_3$ crystals with small bandwidth yields, rather than the phase separation, an homogeneous short ranged charge/orbital order which gives rise to a nearly-atomic spin glass state. Remarkably, this microscopically disordered ``CE-glass'' state alone is able to bring forth the colossal magnetoresistance., Comment: REVTeX 4 style; 4 pages, 4 figures; revised 4/9 and accepted for publication

The temperature dependence of the electronic and atomic structure of the colossal magnetoresistive oxides $La_{1-x}Sr_{x}MnO_{3}$ (x = 0.3, 0.4) has been studied using core and valence level photoemission, x-ray absorption and emission, and extended x-ray absorption fine structure spectroscopy. A dramatic and reversible change of the electronic structure is observed on crossing the Curie temperature, including charge localization and spin moment increase of Mn, together with Jahn-Teller distortions, both signatures of polaron formation. Our data are also consistent with a phase-separation scenario., Comment: 5 pages, 4 figures, revtex