We report a high resolution resonant inelastic x-ray scattering investigation of the bilayer manganites La$_{2-2x}$Sr$_{1+2x}$Mn$_2$O$_7$ with $x = 0.36$ and $0.5$. The momentum dependence along the crystallographic $(110)$ direction for energy losses $1\,\rm{eV} \leq ΔE \leq 15\,\rm{eV}$ has been measured in detail with the data analysis focusing on the energy loss region $1\,\rm{eV} \leq ΔE \leq 5\,\rm{eV}$, which includes a strong peak located at $ΔE \approx 2\,\rm{eV}$. We observe a clear dispersion of up to $0.5\,\rm{eV}$ in the measured $\textbf{q}$ range, which is direct evidence of the non-local character of this excitation. Further, we found that the intensity in this low energy region strongly depends on both the reduced wave vector $\textbf{q} = (h, h, 0)$, $h = 0.1 - 0.5$, and temperature, i.e. different ordered phases. Results can be explained via an intersite $d-d$ charge transfer excitation, proposed for pseudo-cubic manganites, where the hopping rate is strongly increased (decreased) by ferromagnetic (antiferromagnetic) alignment of neighboring in-plane Mn ion core spins.
We have examined magnetic ordering of the two-dimensional (2D) bilayer manganite La$_{1.1}$Sr$_{1.9}$Mn$_2$O$_7$ with neutron diffraction technique. Due to the two-dimensionality, there appears intense 2D ridge scattering along the tetragonal $(00l)$ direction, and the analyses of such scattering leads to a conclusion that the low temperature spin structure is a canted antiferromagnetic ordering.
Half-metallicity in materials has been a subject of extensive research due to its potential for applications in spintronics. Ferromagnetic manganites have been seen as a good candidate, and aside from a small minority-spin pocket observed in La$_{2-2x}$Sr$_{1+2x}$Mn$_{2}$O$_{7}$ $(x=0.38)$, transport measurements show that ferromagnetic manganites essentially behave like half metals. Here we develop robust tight-binding models to describe the electronic band structure of the majority as well as minority spin states of ferromagnetic, spin-canted antiferromagnetic, and fully antiferromagnetic bi…
We report the measurement of spin waves in the bilayer colossal magnetoresistive manganites La(2-2x)Sr(1+2x)Mn2O7 with x=0.30, 0.35 and 0.40. For x=0.35 and 0.40 the entire acoustic and optic dispersion relations are reasonably well described by those for a bilayer Heisenberg Hamiltonian with nearest neighbour exchange only. The in-plane coupling is only weakly dependent on x, but the coupling between the planes of a bilayer changes by a factor of four. The results directly reveal the change from mixed and character of the orbitals to mostly character with increasing hole concentration.
We have investigated the time dependence of remanent magnetostriction in a (La,Pr)$_{1.2}$Sr$_{1.8}$Mn$_{2}$O$_{7}$ single crystal, in order to examine the slow dynamics of lattice distortion in bilayered manganites. A competition between double exchange and Jahn-Teller type orbital-lattice interactions results in the observed lattice profile following a stretched exponential function. This finding suggests that spatial growth of the local lattice distortions coupled with e$_{g}$-electron orbital strongly correlates with the appearance of the field-induced CMR effect.
We have performed a muon spin rotation study on polycrystalline samples of electron-doped layered manganites, La$_{2-2x}$Sr$_{1+2x}$Mn$_2$O$_7$ (0.4< x<1), in order to investigate the local magnetic structure and spin dynamics. Our results provide evidence for phase separation into A-type antiferromagnetic and charge-ordered phases for x=0.52 and spin freezing at low temperatures (T<100K) for 0.52<x<0.75. A new phase diagram which includes this spin freezing region is proposed.
A novel frequency dependence of anomaly in dielectric constant versus temperature plot, around the Neel temperature T_N (~150 K), has been observed in a single crystal of bilayer manganite Pr(Sr0.1Ca0.9)2Mn2O7. The anomaly in the permittivity (epsilon'||c) occurs at a temperature T_f which moves within a temperature window (delT_f) of ~40 K around T_N for a frequency range 50 kHz-5 MHz. The capacitive component Cp of the dielectric response exhibits a clear yet broad feature around T_N which establishes the intrinsic capacitive nature of the anomaly.
We report an inelastic neutron scattering study of acoustic phonons in the charge and orbitally ordered bilayer manganite LaSr$_2$Mn$_2$O$_7$. For excitation energies less than $15\,\rm{meV}$, we observe an abrupt increase (decrease) of the phonon energies (linewidths) of a transverse acoustic phonon branch at $\mathbf{q} = (h, h, 0)$, $h\le0.3$, upon entering the low temperature charge and orbital ordered state ($T_{COO} = 225\,\rm{K}$). This indicates a reduced electron-phonon coupling due to a decrease of electronic states at the Fermi level leading to a partial removal of the Fermi surface…
Photoemission data taken with hard x-ray radiation on cleaved single crystals of the bilayered, colossal magnetoresistant manganite La_(2-2x)Sr_(1+2x)Mn_2O_7 (LSMO) with 0.30<x<0.50 are presented. Making use of the increased bulk-sensitivity upon hard x-ray excitation it is shown that the core level footprint of the electronic structure of the LSMO cleavage surface is identical to that of the bulk. Furthermore, by comparing the core level shift of the different elements as a function of doping level x, it is shown that microscopic phase separation is unlikely to occur for this particular manga…
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 …
We demonstrate that the half-doped bilayer manganite La_{1}Sr_{2}Mn_{2}O_{7} exhibits CE-type charge-ordered and spin-ordered states below $T_{N, CO}^A = 210$ K and below $T_{N}^{CE} \sim 145$ K, respectively. However, the volume fraction of the CE-type ordering is relatively small, and the system is dominated by the A-type spin ordering. The coexistence of the two types of ordering is essential to understand its transport properties, and we argue that it can be viewed as an effective phase separation between the metallic $d(x^{2}-y^{2})$ orbital ordering and the charge-localized $d(3x^{2}-r^{…
Recently, an intriguing doping dependence of the exchange energies in the bilayer manganites $La_{2-2x}Sr_{1+2x}Mn_2O_7$ has been observed in the neutron scattering experiments. The intra-layer exchange only weakly changed with doping while the inter-layer one drastically decreased. Here we propose a theory which accounts for these experimental findings. We argue, that the observed striking doping dependence of the exchange energies can be attributed to the evaluation of the orbital level splitting with doping. The latter is handled by the interplay between Jahn-Teller effect (supporting an ax…
We have undertaken a systematic study of thermal conductivity as a function of temperature and magnetic field of single crystals of the compound (La$_{1-z}$Pr$_{z}$)$_{1.2}$Sr$_{1.8}$Mn$_{2}$O$_{7}$ for $z$(Pr) =0.2,0.4. and 0.6. The lattice distortion due to Pr-substitution and anisotropic thermal conductivity in bilayer manganites are discussed on the basis of different relaxation models of local lattice distortions in metal and insulating states proposed by Maderda et al. The giant magnetothermal effect is scaled as a function of magnetization and discussed on the basis of a systematic vari…
The charge ordering in the bilayer manganite system La$_{2-2x}$Sr$_{1+2x}$Mn$_{2}$O$_{7}$ with $0.30 \le x \le 0.50$ has been studied by neutron diffraction. The charge order is characterized by the propagation vector parallel to the [1 0 0] direction (MnO$_2$ direction), but the correlation length is short-ranged and extremely anisotropic, being $\sim 0.02a^{*}$ and $\sim 0.2a^{*}$ parallel and perpendicular to the modulation direction, respectively. The observed charge order can be viewed as a quasi-bi-stripe order, and accounts well for the $x$ dependence of the resistivity. The quasi-bistr…
$^{139}$La- and $^{55}$Mn-NMR spectra demonstrate that the ground state of the A-site ordered perovskite manganite LaBaMn$_2$O$_6$ is a spatial mixture of the ferromagnetic (FM) and antiferromagnetic (AFI(CE)) regions, which are assigned to the metallic and the insulating charge ordered state, respectively. This exotic coexisting state appears below 200 K via a first-order-like formation of the AFI(CE) state inside the FM one. Mn spin-spin relaxation rate indicates that the FM region coexisting with the AFI(CE) one in LaBaMn$_2$O$_6$ is identical to the bulk FM phase of the disordered form La$…
By performing angle-resolved photoemission spectroscopy of the bilayer colossal magnetoresistive (CMR) manganite, $La_{2-2x}Sr_{1+2x}Mn_{2}O_{7}$, we provide the complete mapping of the Fermi level spectral weight topology. Clear and unambiguous bilayer splitting of the in-plane 3d$_{x^2-y^2}$ band, mapped throughout the Brillouin zone, and the full mapping of the 3d$_{3z^2-r^2}$ band are reported. Peculiar doping and temperature dependencies of these bands imply that as transition from the ferromagnetic metallic phase approaches, either as a function of doping or temperature, coherence along …
The exact nature of the low temperature electronic phase of the manganite materials family, and hence the origin of their colossal magnetoresistant (CMR) effect, is still under heavy debate. By combining new photoemission and tunneling data, we show that in La{2-2x}Sr{1+2x}Mn2O7 the polaronic degrees of freedom win out across the CMR region of the phase diagram. This means that the generic ground state is that of a system in which strong electron-lattice interactions result in vanishing coherent quasi-particle spectral weight at the Fermi level for all locations in k-space. The incoherence of …
The ground state of half-doped manganites involves intricate spin, charge and orbital orderings, which are difficult to discern experimentally. In this work, we resort to the theoretical analysis of the spin fluctuation spectrum of the half-doped bilayer Pr(Ca$_{0.9}$Sr$_{0.1}$)$_2$ Mn$_2$O$_7$ in order to get an insight of its electronic ground state. By means of the linear spin wave approximation, we compute the magnon dispersion for a family of localized spin models, which can describe several phases proposed for the ground state of half-doped manganites, like the intermediate one proposed …
We report a magnetic force microscopy study of the magnetic domain evolution in the layered manganite La$_{2-2x}$Sr$_{1+2x}$Mn$_2$O$_7$ (with $x=0.32$). This strongly correlated electron compound is known to exhibit a wide range of magnetic phases, including a recently uncovered biskyrmion phase. We observe a continuous transition from dendritic to stripe-like domains, followed by the formation of magnetic bubbles due to a field- and temperature dependent competition between in-plane and out-of-plane spin alignments. The magnetic bubble phase appears at comparable field- and temperature ranges…
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…
We present high resolution high energy and resonant x-ray diffraction results from La2-2xSr1+2xMn2O7 for x=0.55,0.575 and 0.60. These compounds show superlattice reflections at wavevectors of (h+-δ,k+-δ,l) and (h+-2δ,k+-2δ,l), arising from orbital ordering with associated Jahn-Teller distortions and charge ordering respectively. We observe a phase transition between the x=0.55 and x=0.575 doping levels. Samples with x=0.55 display structural characteristics similar to those previously reported for x=0.5. Compared to this, the long range order in samples with x=0.55 and x=0.6 have a distinct ch…
The magnetic and orbital orders for the bilayer manganites in the doping region $0.5 < x <1.0$ have been investigated from a model that incorporates the two $e_g$ orbitals at each Mn site, the inter-orbital Coulomb interaction and lattice distortions. The usual double exchange operates via the $e_g$ orbitals. It is shown that such a model reproduces much of the phase diagram recently obtained for the bilayer systems in this range of doping. The C-type phase with ($π,0,π$) spin order seen by Ling et al. appears as a natural consequence of the layered geometry and is stabilised by the static dis…
We have investigated the resistive relaxation of a (La$_{0.4}$Pr$_{0.6}$)$_{1.2}$Sr$_{1.8}$Mn$_{2}$O$_{7}$ single crystal, in order to examine the slow dynamics of the field-induced insulator to metal transition of bilayered manganites. The temporal profiles observed in remanent resistance follow a stretched exponential function accompanied by a slow relaxation similar to that obtained in magnetization and magnetostriction data. We demonstrate that the remanent relaxation in magnetotransport has a close relationship with magnetic relaxation that can be understood in the framework of an effecti…
Exchange bias has been studied in a series of La2/3Ca1/3MnO3 / La1/3Ca2/3MnO3 bilayers grown on (001) SrTiO3 substrates by ozone-assisted molecular beam epitaxy. The high crystalline quality of the samples and interfaces has been verified using high-resolution X-ray diffractometry and Z-contrast scanning transmission electron microscopy with electron energy loss spectroscopy. The dependence of exchange bias on the thickness of the antiferromagnetic layer has been investigated. A critical value for the onset of the hysteresis loop shift has been determined. An antiferromagnetic anisotropy const…
We report measurements of in-plane $ρ_{ab}$ and out-of-plane $ρ_{c}$ resistivities on a single crystal of the half-doped bilayer manganite LaSr$_{2}$Mn$_{2}$O$_{7}$. In the temperature $T$ range 220 to 300 K, the resistive anisotropy $ρ_{c}/ρ_{ab}=A+B/T$ ($A$ and $B$ constants), which provides evidence for the variable-range-hopping conduction in the presence of a Coulomb gap. This hopping mechanism also accounts for the quadratic magnetic field $H$ and $\sin^{2}ϕ$ dependences of the negative magnetoresistivity $\ln [ρ_{i}(T,H,ϕ)/ρ_{i}(T,H=0)]$ ($i=ab,c$), where $ϕ$ is the in-plane angle betwe…
In correlated electron systems such as cuprate superconductors and colossal magnetoresistive (CMR) oxides there is often a tendency for a nanoscale self-organization of electrons that can give rise to exotic properties and to extreme non-linear responses. The driving mechanisms for this self-organization are highly debated, especially in the CMR oxides in which two types of self-organized stripes of charge and orbital order coexist with each other. By utilizing angle-resolved photoemission spectroscopy measurements over a wide doping range, we show that one type of stripe is exclusively linked…
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 suppressio…
An oxide heterostructure made of manganite bilayers and ferroelectric perovskites is predicted to lead to the full control of magnetism when switching the ferroelectric polarizations. By using asymmetric polar interfaces in the superlattices, more electrons occupy the Mn layer at the $n$-type interface side than at the $p$-type side. This charge disproportionation can be enhanced or suppressed by the ferroelectric polarization. Quantum model and density functional theory calculations reach the same conclusion: a ferromagnetic-ferrimagnetic phase transition with maximal change $>90%$ of the tot…
We measured the magneto-optical response of (La$_{0.4}$Pr$_{0.6}$)$_{1.2}$Sr$_{1.8}$Mn$_2$O$_7$ in order to investigate the microscopic aspects of the magnetic field driven spin-glass insulator to ferromagnetic metal transition. Application of a magnetic field recovers the ferromagnetic state with an overall redshift of the electronic structure, growth of the bound carrier localization associated with ferromagnetic domains, development of a pseudogap, and softening of the Mn-O stretching and bending modes that indicate a structural change. We discuss field- and temperature-induced trends withi…
We report anisotropic resistivity measurements on a La$_{1.2}$Sr$_{1.8}$Mn$_{2}$O$_{7}$ single crystal over a temperature $T$ range from 2 to 400 K and in magnetic fields $H$ up to 14 T. For $T\geq 218$ K, the temperature dependence of the zero-field in-plane $ρ_{ab}(T)$ resistivity obeys the adiabatic small polaron hopping mechanism, while the out-of-plane $ρ_{c}(T)$ resistivity can be ascribed by an Arrhenius law with the same activation energy. Considering the magnetic character of the polarons and the close correlation between the resistivity and magnetization, we developed a model which a…
There have been recent reports of charge ordering around $x=0.5$ in the bilayer manganites. At $x=0.5$, there appears to be a coexistence region of layered A-type antiferromagnetc and charge order. There are also reports of orbital order in this region without any Jahn-Teller effect. Based on physical grounds, this region is investigated from a model that incorporates the two $e_g$ orbitals at each Mn site and a near-neighbour Coulomb repulsion. It is shown that there indeed is both charge and orbital order close to the half-doped region coincident with a layered magnetic structure. Although t…
The influence of the grain size in the magnetic properties of phase separated manganites is an important issue evidenced more than a decade ago. The formation of long range ordered phases is suppressed as the grain size decreases giving place to a metastable state instead of the ground state. In this work we present a study of the magnetocaloric effect in the prototypical manganite La0.5Ca0.5MnO3 as function of the grain size. The differences obtained using direct and indirect methods are discussed in the framework of domain walls in the ferromagnetic phase of the system.
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 …
Memristive switching serves as the basis for a new generation of electronic devices. Memristors are two-terminal devices in which the current is turned on and off by redistributing point defects, e.g., vacancies, which is difficult to control. Memristors based on alternative mechanisms have been explored, but achieving both the high On/Off ratio and the low switching energy desirable for use in electronics remains a challenge. Here we report memristive switching in a La0.7Ca0.3MnO3/PrBa2Cu3O7 bilayer with an On/Off ratio greater than 10^3 and demonstrate that the phenomenon originates from a n…
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 patter…
The temperature $T$ and magnetic field $H$ dependence of anisotropic in-plane $ρ_{ab}$ and out-of-plane $ρ_{c}$ resistivities have been investigated in single crystals of the bilayer manganite La$_{1.2}$Sr$_{1.8}$Mn$_{2}$O$_{7}$. Below the Curie transition temperature $T_c=$ 125 K, $ρ_{ab}$ and $ρ_{c}$ display almost the same temperature dependence with an up-turn around 50 K. In the metallic regime (50 K $\leq T \leq$ 110 K), both $ρ_{ab}(T)$ and $ρ_{c}(T)$ follow a $T^{9/2}$ dependence, consistent with the two-magnon scattering. We found that the value of the proportionality coefficient $B_{…
The atomic pair distribution function (PDF) technique is employed to probe the atomic local structural responses in naturally double layered manganites \lsmo in the doping range $0.54 \leq x \leq 0.80$. Our low temperature neutron powder diffraction measurements suggest the coexistence of two different Jahn-Teller (JT) distorted MnO$_6$ octahedra when its ordered magnetic structure crosses over from type A ($0.54 \leq x \leq 0.66$) to type C/C$^*$ ($0.74 \leq x \leq 0.90$) ordering. At all doping levels at low temperature the doped holes reside predominantly in the plane of the bilayer. In the…
We present angle-resolved photoemission studies of (La1-zPrz)2-2xSr1+2xMn2O7 with x=0.4 and z=0.1,0.2 and 0.4 along with density functional theory calculations and x-ray scattering data. Our results show that the bilayer splitting in the ferromagnetic metallic phase of these materials is small, if not completely absent. The charge carriers are therefore confined to a single MnO2-layer, which in turn results in a strongly nested Fermi surface. In addition to this, the spectral function also displays clear signatures of an electronic ordering instability well below the Fermi level. The increase …
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 $d_{x^2-y^2}$…
Using inelastic neutron scattering we measured the microscopic magnetic coupling associated with the ferromagnetic (FM) clusters of the ``colossal magnetoresistance'' (CMR) compound Pr$_{0.70}$Ca$_{0.30}$MnO$_3$. When the insulating to metal (I-M) transition is induced by an external magnetic field there is a discontinuous change in the spin-wave stiffness constant. This result indicates that the probed regions undergo a first-order transition from an insulating to a metallic state, and that there are no FM metallic domains in the insulating region. We argue that the I-M transition in the CMR …
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 …
The spin correlations of the bilayer manganite $La_{1.2}Sr_{1.8}Mn_{2}O_{7}$ have been studied using neutron scattering. On cooling within the paramagnetic state, we observe purely two-dimensional behavior with a crossover to three-dimensional scaling close to the ferromagnetic transition. Below $T_C$, an effective finite size behavior is observed. The quantitative agreement of these observations with the conventional quasi two-dimensional Kosterlitz-Thouless model indicates that the phase transition is driven by the growth of magnetic correlations, which are only weakly coupled to polarons ab…
The layered manganese oxides LnBaMn1.96Fe0.04Oy (Ln=Y, Gd, Sm, Nd, Pr, La) have been synthesized for y=5, 5.5 and 6. In the oxygen-saturated state (y=6) they exhibit the charge and orbital order at ambient temperature for Ln=Y, Gd, Sm, but unordered eg-electronic system for Ln=La,Pr,Nd. Fourfold increase of quadrupole splitting was observed owing to the charge and orbital ordering. This is in agreement with the jumplike increase in distortion of the reduced perovskite-like cell for the charge and orbitally ordered manganites compared to the unordered ones. Substitution of 2 percents of Mn by F…
We have observed a sizable positive magnetocapacitance ($\sim$$5-90\%$) in perovskite Pr$_{0.55}$Ca$_{0.45}$MnO$_3$ and bilayer Pr(Sr$_{0.1}$Ca$_{0.9}$)$_2$Mn$_2$O$_7$ system under 5T magnetic field across 20-100 K below the magnetic transition point T$_N$. The magnetodielectric effect, on the other hand, exhibits a crossover: (a) from positive to negative for the perovskite system and (b) from negative to positive for the bilayer system over the same temperature range. The bilayer Pr(Sr$_{0.1}$Ca$_{0.9}$)$_2$Mn$_2$O$_7$ system exhibits a sizable anisotropy as well. We have also noticed the in…
We have studied the low-temperature behavior of the magnetization and the specific heat of the bilayered perovskite system $% La_{2-2x}Sr_{1+2x}Mn_{2}O_{7}$, for $0.30\leq x\leq 0.50$. Our analysis reveals that below 30 K the temperature dependence of the magnetization of the ferromagnetic samples, $x=0.30$, 0.32, and 0.36, in a field of 1T can be interpreted in terms of the thermal excitations of a two-dimensional gas of ferromagnetic magnons. The specific heat in zero field for these samples as for the $x=0.50$ antiferromagnetic one, is linear with temperature between the range of 1.8K $\leq…
We construct a theory of spin wave excitations in the bilayer manganite La(1.2)Sr(1.8)Mn2O7 based on the simplest possible double-exchange model, but including leading quantum corrections to the spin wave dispersion and damping. Comparison is made with recent inelastic neutron scattering experiments. We find that quantum effects account for some part of the measured damping of spin waves, but cannot by themselves explain the observed softening of spin waves at the zone boundary. Furthermore a doping dependence of the total spin wave dispersion and the optical spin wave gap is predicted.
Neutron scattering measurements on a bilayer manganite near optimal doping show that the short-range polarons correlations are completely dynamic at high T, but then freeze upon cooling to a temperature T* 310 K. This glass transition suggests that the paramagnetic/insulating state arises from an inherent orbital frustration that inhibits the formation of a long range orbital- and charge-ordered state. Upon further cooling into the ferromagnetic-metallic state (Tc=114 K), where the polarons melt, the diffuse scattering quickly develops into a propagating, transverse optic phonon.
Neutron scattering investigations of the paramagnetic correlations in the layered manganite La$_{1.2}$Sr$_{1.8}$Mn$_{2}$O$_{7}$, which exhibits colossal magnetoresistance above the Curie transition at T$_C$ = 112 K, show that spins in neighboring layers within each bilayer are strongly canted at an average angle that is dependent on both the magnetic field and temperature, as predicted by de Gennes. The in-plane correlation length does not diverge at T$_C$, although the magnetic Bragg intensity obeys critical scaling below T$_C$, with the same temperature dependence as the zero-field electrica…
Microscopic evidence for spin-spinless stripe order with reduced Ni moments within $ab$ plane for bilayer nickelate La$_3$Ni$_2$O$_7$ probed by $^{139}$La-NQR
We have measured the spin-wave spectrum of the half-doped bilayer manganite Pr(Ca,Sr)2Mn2O7 in its spin, charge, and orbital ordered phase. The measurements, which extend throughout the Brillouin zone and cover the entire one-magnon spectrum, are compared critically with spin-wave calculations for different models of the electronic ground state. The data are described very well by the Goodenough model, which has weakly interacting ferromagnetic zig-zag chains in the CE-type arrangement. A model that allows ferromagnetic dimers to form within the zigzags is inconsistent with the data. The analy…
In correlated electron materials, electrons often self-organize and form a variety of patterns with potential ordering of charges, spins, and orbitals, which are believed to be closely connected to many novel properties of these materials including superconductivity, metal-insulator transitions, and the CMR effect. How these real-space patterns affect the conductivity and other properties of materials (which are usually described in momentum space) is one of the major challenges of modern condensed matter physics. Moreover, although the presence of static stripes is indisputable, the existence…
In this contribution to the special issue on multiferroics we focus on multiferroicity driven by different forms of charge ordering. We will present the generic mechanisms by which charge ordering can induce ferroelectricity in magnetic systems. There is a number of specific classes of materials for which this is relevant. We will discuss in some detail $(i)$ perovskite manganites of the type (PrCa)MnO$_3$, $(ii)$ the complex and interesting situation in magnetite Fe$_3$O$_4$, $(iii)$ strongly ferroelectric frustrated LuFe$_2$O$_4$, $(iv)$ an example of a quasi one-dimensional organic system. …
We present a low-energy muon-spin-rotation study of the magnetic and superconducting properties of YBa2Cu3O7/PrBa2Cu3O7 trilayer and bilayer heterostructures. By determining the magnetic-field profiles throughout these structures we show that a finite superfluid density can be induced in otherwise semiconducting PrBa2Cu3O7 layers when juxtaposed to YBa2Cu3O7 "electrodes" while the intrinsic antiferromagnetic order is unaffected.
This article reports a detailed x-ray resonant scattering study of the bilayer iridate compound, Sr3Ir2O7, at the Ir L2 and L3 edges. Resonant scattering at the Ir L3 edge has been used to determine that Sr3Ir2O7 is a long-range ordered antiferromagnet below TN 230K with an ordering wavevector, q=(1/2,1/2,0). The energy resonance at the L3 edge was found to be a factor of ~30 times larger than that at the L2. This remarkable effect has been seen in the single layer compound Sr2IrO4 and has been linked to the observation of a Jeff=1/2 spin-orbit insulator. Our result shows that despite the modi…
Recent experiments by Larson et al. demonstrate the feasibility of measuring local $dd$ excitations using nonresonant inelastic X-ray scattering (IXS). We establish a general framework for the interpretation where the $dd$ transitions created in the scattering process are expressed in effective one-particle operators that follow a simple selection rule. The different operators can be selectively probed by employing their different dependence on the direction and magnitude of the transferred momentum. We use the operators to explain the presence of nodal directions and the nonresonant IXS in sp…
We have studied the [100]-[110] anisotropy of the Compton profile in the bilayer manganite. Quantitative agreement is found between theory and experiment with respect to the anisotropy in the two metallic phases (i.e. the low temperature ferromagnetic and the colossal magnetoresistant phase under a magnetic field of 7 T). Robust signatures of the metal-insulator transition are identified in the momentum density for the paramagnetic phase above the Curie temperature. We interpret our results as providing direct evidence for the transition from the metallic-like to the admixed ionic-covalent bon…
Distinguishing Electronic Band Structure of Single-layer and Bilayer Ruddlesden-Popper Nickelates Probed by in-situ High Pressure X-ray Absorption Near-edge Spectroscopy
Surface magnetic properties of perovskite manganites have been a recurrent topic during last years since they play a major role in the implementation of magnetoelectronic devices. Magneto-optical techniques, such as X-ray magnetic circular dichroism, turn out to be a very efficient tool to study surface magnetism due to their sensitivity to magnetic and chemical variations across the sample depth. Nevertheless, the application of the sum rules for the determination of the spin magnetic moment might lead to uncertainties as large as 40% in case of Mn ions. To overcome this problem we present an…
Neutron elastic, inelastic and high energy x-ray scattering techniques are used to explore the nature of the polaron order and dynamics in La0.7Ca0.3MnO3. Static polaron correlations develop within a narrow temperature regime as the Curie temperature is approached from low temperatures, with a nanoscale correlation length that is only weakly temperature dependent. The static nature of these short-range polaron correlations indicates the presence of a glass-like state, similar to the observations for the bilayer manganite in the metallic-ferromagnetic doping region. In addition to this elastic …
