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N. B. Brookes

Publications and source records attributed to N. B. Brookes.

At least 73 records · Page 4Linked to original sources

Direct observation of a highly spin-polarized organic spinterface at room temperature

The design of large-scale electronic circuits that are entirely spintronics-driven requires a current source that is highly spin-polarised at and beyond room temperature, cheap to build, efficient at the nanoscale and straightforward to integrate with semiconductors. Yet despite research within several subfields spanning nearly two decades, this key building block is still lacking. We experimentally and theoretically show how the interface between Co and phthalocyanine molecules constitutes a promising candidate. Spin-polarised direct and inverse photoemission experiments reveal a high degree of spin polarisation at room temperature at this interface. We measured a magnetic moment on the molecules's nitrogen pi orbitals, which substantiates an ab-initio theoretical description of highly spin-polarised charge conduction across the interface due to differing spinterface formation mechanims in each spin channel. We propose, through this example, a recipe to engineer simple organic-inorganic interfaces with remarkable spintronic properties that can endure well above room temperature.

cond-mat.mtrl-sci↗

Long-range incommensurate charge fluctuations in (Y,Nd)Ba2Cu3O(6+x)

There are increasing indications that superconductivity competes with other orders in cuprate superconductors, but obtaining direct evidence with bulk-sensitive probes is challenging. We have used resonant soft x-ray scattering to identify two-dimensional charge fluctuations with an incommensurate periodicity of $\bf \sim 3.2$ lattice units in the copper-oxide planes of the superconductors (Y,Nd)Ba$_2$Cu$_3$O$_{6+x}$ with hole concentrations $0.09 \leq p \leq 0.13$ per planar Cu ion. The intensity and correlation length of the fluctuation signal increase strongly upon cooling down to the superconducting transition temperature, $T_c$; further cooling below $T_c$ abruptly reverses the divergence of the charge correlations. In combination with prior observations of a large gap in the spin excitation spectrum, these data indicate an incipient charge-density-wave instability that competes with superconductivity.

cond-mat.str-el↗

Bimagnon studies in cuprates with Resonant Inelastic X-ray Scattering at the O K edge. I - An assessment on La2CuO4 and a comparison with the excitation at Cu L3 and Cu K edges

We assess the capabilities of magnetic Resonant Inelastic X-ray Scattering (RIXS) at the O $K$ edge in undoped cuprates by taking La_{2}CuO_{4} as a benchmark case, based on a series of RIXS measurements that we present here. By combining the experimental results with basic theory we point out the fingerprints of bimagnon in the O $K$ edge RIXS spectra. These are a dominant peak around 450 meV, the almost complete absence of dispersion both with $π$ and $σ$ polarization and the almost constant intensity vs. the transferred momentum with $σ$ polarization. This behavior is quite different from Cu $L_3$ edge RIXS giving a strongly dispersing bimagnon tending to zero at the center of the Brillouin zone. This is clearly shown by RIXS measurements at the Cu $L_3$ edge that we present. The Cu $L_3$ bimagnon spectra and those at Cu $K$ edge - both from the literature and from our data - however, have the same shape. These similarities and differences are understood in terms of different sampling of the bimagnon continuum. This panorama points out the unique possibilities offered by O $K$ RIXS in the study of magnetic excitations in cuprates near the center of the BZ.

cond-mat.supr-con↗

Bimagnon studies in cuprates with Resonant Inelastic X-ray Scattering at the O K edge. II - The doping effect in La2-xSrxCuO4

We present RIXS data at O K edge from La2-xSrxCuO4 vs. doping between x=0.10 and x=0.22 with attention to the magnetic excitations in the Mid-Infrared region. The sampling done by RIXS is the same as in the undoped cuprates provided the excitation is at the first pre-peak induced by doping. Note that this excitation energy is about 1.5 eV lower than that needed to see bimagnons in the parent compound. This approach allows the study of the upper region of the bimagnon continuum around 450 meV within about one third of the Brilluoin Zone around Γ. The results show the presence of damped bimagnons and of higher even order spin excitations with almost constant spectral weight at all the dopings explored here. The implications on high Tc studies are briefly addressed.

cond-mat.supr-con↗

Electronic and magnetic structure of carbon nanotubes using x-ray absorption and magnetic circular dichroism spectroscopy

Carbon nanotubes are a fraction of the size of transistors used in today's best microchips, as it could reduce power demands and heating in next electronics revolution. Present study investigates the electronic and magnetic structure of multi walled carbon nanotubes (MWCNT) synthesized by chemical vapor deposition technique using near edge x-ray absorption spectroscopy (NEXAFS) measurement at C K-edge and x-ray magnetic circular dichroism (XMCD) at Co and Fe $L_{3,2}$ -edges. NEXAFS at C K-edge shows significant $π$-bonding, and Fe(Co) L-edge proves the presence of Co$^{2+}$ and Fe$^{2+}$ in octahedral symmetry, and embedded in C-matrix of MWCNT. Element specific hystersis loops and XMCD spectra clearly shows that these MWCNTs exhibits room temperature ferromagnetism. These measurements elucidated the electronic structure of CNTs and presence of magnetic interactions at room temperature.

cond-mat.mtrl-sci↗

BaVS$_3$ probed by V L edge X-ray absorption spectroscopy

Polarization dependent vanadium L edge X-ray absorption spectra of BaVS$_3$ single crystals are measured in the four phases of the compound. The difference between signals with the polarization \textbf{E}$\perp$\textbf{c} and \textbf{E}$\parallel$\textbf{c} (linear dichroism) changes with temperature. Besides increasing intensity of one of the maxima, a new structure appears in the pre-edge region below the metal-insulator transition. More careful examination brings to light that the changes start already with pretransitional charge density wave fluctuations. Simple symmetry analysis suggests that the effect is related to rearrangements in $E_{g}$ and $A_{1g}$ states, and is compatible with the formation of four inequivalent V sites along the V-S chain.

cond-mat.str-el↗

Hole-depletion of ladders in Sr$_{14}$Cu$_{24}$O$_{41}$ induced by correlation effects

The hole distribution in Sr$_{14}$Cu$_{24}$O$_{41}$ is studied by low temperature polarization dependent O K Near-Edge X-ray Absorption Fine Structure measurements and state of the art electronic structure calculations that include core-hole and correlation effects in a mean-field approach. Contrary to all previous analysis, based on semi-empirical models, we show that correlations and antiferromagnetic ordering favor the strong chain hole-attraction. For the remaining small number of holes accommodated on ladders, leg-sites are preferred to rung-sites. The small hole affinity of rung-sites explains naturally the 1D - 2D cross-over in the phase diagram of (La,Y,Sr,Ca)$_{14}$Cu$_{24}$O$_{41}$

cond-mat.str-el↗

Orbital order in La0.5Sr1.5MnO4: beyond a common local Jahn-Teller picture

The standard way to find the orbital occupation of Jahn-Teller (JT) ions is to use structural data, with the assumption of a one-to-one correspondence between the orbital occupation and the associated JT distortion, e.g. in O6 octahedron. We show, however, that this approach in principle does not work for layered systems. Specifically, using the layered manganite La0.5Sr1.5MnO4 as an example, we found from our x-ray absorption measurements and theoretical calculations, that the type of orbital ordering strongly contradicts the standard local distortion approach for the Mn3+O6 octahedra, and that the generally ignored long-range crystal field effect and anisotropic hopping integrals are actually crucial to determine the orbital occupation. Our findings may open a pathway to control of the orbital state in multilayer systems and thus of their physical properties.

cond-mat.str-el↗

Orbital occupation and magnetic moments of tetrahedrally coordinated iron in CaBaFe4O7

CaBaFe4O7 is a mixed-valent transition metal oxide having both Fe2+ and Fe3+ ions in tetrahedral coordination. Here we characterize its magnetic properties by magnetization measurements and investigate its local electronic structure using soft x-ray absorption spectroscopy at the Fe L2,3 edges, in combination with multiplet cluster and spin-resolved band structure calculations. We found that the Fe2+ ion in the unusual tetrahedral coordination is Jahn-Teller active with the high-spin e^2 (up) t2^3 (up) e^1 (down) configuration having a x^2-y^2-like electron for the minority spin. We deduce that there is an appreciable orbital moment of about L_z=0.36 caused by multiplet interactions, thereby explaining the observed magnetic anisotropy. CaBaFe4O7, a member of the '114' oxide family, offers new opportunities to explore charge, orbital and spin physics in transition metal oxides.

cond-mat.str-el↗

Energy and symmetry of $dd$ excitations in undoped layered cuprates measured by Cu $L_3$ resonant inelastic x-ray scattering

We measured high resolution Cu $L_3$ edge resonant inelastic x-ray scattering (RIXS) of the undoped cuprates La$_2$CuO$_4$, Sr$_2$CuO$_2$Cl$_2$, CaCuO$_2$ and NdBa$_2$Cu$_3$O$_6$. The dominant spectral features were assigned to $dd$ excitations and we extensively studied their polarization and scattering geometry dependence. In a pure ionic picture, we calculated the theoretical cross sections for those excitations and used them to fit the experimental data with excellent agreement. By doing so, we were able to determine the energy and symmetry of Cu-3$d$ states for the four systems with unprecedented accuracy and confidence. The values of the effective parameters could be obtained for the single ion crystal field model but not for a simple two-dimensional cluster model. The firm experimental assessment of $dd$ excitation energies carries important consequences for the physics of high $T_c$ superconductors. On one hand, having found that the minimum energy of orbital excitation is always $\geq 1.4$ eV, i.e., well above the mid-infrared spectral range, leaves to magnetic excitations (up to 300 meV) a major role in Cooper pairing in cuprates. On the other hand, it has become possible to study quantitatively the effective influence of $dd$ excitations on the superconducting gap in cuprates.

cond-mat.supr-con↗

Multiple double-exchange mechanism by Mn$^{2+}$-doping in manganite compounds

Double-exchange mechanisms in RE$_{1-x}$AE$_{x}$MnO$_{3}$ manganites (where RE is a trivalent rare-earth ion and AE is a divalent alkali-earth ion) relies on the strong exchange interaction between two Mn$^{3+}$ and Mn$^{4+}$ ions through interfiling oxygen 2p states. Nevertheless, the role of RE and AE ions has ever been considered "silent" with respect to the DE conducting mechanisms. Here we show that a new path for DE-mechanism is indeed possible by partially replacing the RE-AE elements by Mn$^{2+}$-ions, in La-deficient La$_{x}$MnO$_{3-δ}$ thin films. X-ray absorption spectroscopy demonstrated the relevant presence of Mn$^{2+}$ ions, which is unambiguously proved to be substituted at La-site by Resonant Inelastic X-ray Scattering. Mn$^{2+}$ is proved to be directly correlated to the enhanced magneto-transport properties because of an additional hopping mechanism trough interfiling Mn$^{2+}$-ions, theoretically confirmed by calculations within the effective single band model. The very idea to use Mn$^{2+}$ both as a doping element and an ions electronically involved in the conduction mechanism, has never been foreseen, revealing a new phenomena in transport properties of manganites. More important, such a strategy might be also pursed in other strongly correlated materials.

cond-mat.str-el↗

Exchange bias in GeMn nanocolumns: the role of surface oxidation

We report on the exchange biasing of self-assembled ferromagnetic GeMn nanocolumns by GeMn-oxide caps. The x-ray absorption spectroscopy analysis of this surface oxide shows a multiplet fine structure that is typical of the Mn2+ valence state in MnO. A magnetization hysteresis shift |HE|~100 Oe and a coercivity enhancement of about 70 Oe have been obtained upon cooling (300-5 K) in a magnetic field as low as 0.25 T. This exchange bias is attributed to the interface coupling between the ferromagnetic nanocolumns and the antiferromagnetic MnO-like caps. The effect enhancement is achieved by depositing a MnO layer on the GeMn nanocolumns.

cond-mat.mtrl-sci↗

Evidence for Dynamic Phase Separation and High Energy Spin Dynamics in underdoped La$_{2-x}$Sr$_x$CuO$_4$ from Resonant Inelastic X-Ray Scattering

We probe the collective magnetic modes of La$_2$CuO$_4$ (LCO) and underdoped La$_{2-x}$Sr$_x$CuO$_4$ (LSCO) by momentum resolved Resonant Inelastic X-ray Scattering (RIXS) at the Cu $L_3$ edge. In LCO the single magnon dispersion measured by RIXS coincides with the one determined by inelastic neutron scattering. For LSCO the spin dynamics shows a branch dispersing up to $\sim$400 meV coexisting with a branch at lower energy. Only the latter has been observed with neutrons so far and is considered a key signature of doped cuprates. The presence of the high-energy branch indicates that LSCO is in a dynamic inhomogeneous spin state.

cond-mat.supr-con↗

Evolution of magnetic phases and orbital occupation in (SrMnO3)n/(LaMnO3)2n superlattices

The magnetic and electronic modifications induced at the interfaces in (SrMnO$_{3}$)$_{n}$/(LaMnO$_{3}$)$_{2n}$ superlattices have been investigated by linear and circular magnetic dichroism in the Mn L$_{2,3}$ x-ray absorption spectra. Together with theoretical calculations, our data demonstrate that the charge redistribution across interfaces favors in-plane ferromagnetic (FM) order and $e_{g}(x^{2}-y^{2})$ orbital occupation, in agreement with the average strain. Far from interfaces, inside LaMnO$_3$, electron localization and local strain favor antiferromagnetism (AFM) and $e_{g}(3z^{2}-r^{2})$ orbital occupation. For $n=1$ the high density of interfacial planes ultimately leads to dominant FM order forcing the residual AFM phase to be in-plane too, while for $n \geq 5$ the FM layers are separated by AFM regions having out-of-plane spin orientation.

cond-mat.str-el↗

Orbital occupation, atomic moments and magnetic ordering at interfaces of manganite thin films

We have performed x-ray linear and circular magnetic dichroism experiments at the Mn L2,3-edge of the La0.7Sr0.3MnO3 ultra thin films. Our measurements show that the antiferromagnetic (AF) insulating phase is stabilized by the interfacial rearrangement of the Mn 3d orbitals, despite the relevant magnetostriction anisotropic effect on the double-exchange ferromagnetic (FM) metallic phase. As a consequence, the Mn atomic magnetic moment orientation and how it reacts to strain differ in the FM and AF phases. In some cases a FM insulating (FMI) phase adds to the AF and FM. Its peculiar magnetic properties include in-plane magnetic anisotropy and partial release of the orbital moment quenching. Nevertheless the FMI phase appears little coupled to the other ones.

cond-mat.str-el↗

Valence band electronic structure of V2O3: identification of V and O bands

We present a comprehensive study of the photon energy dependence of the valence band photoemission yield in the prototype Mott-Hubbard oxide V2O3. The analysis of our experimental results, covering an extended photon energy range (20-6000 eV) and combined with GW calculations, allow us to identify the nature of the orbitals contributing to the total spectral weight at different binding energies, and in particular to locate the V 4s at about 8 eV binding energy. From this comparative analysis we can conclude that the intensity of the quasiparticle photoemission peak, observed close to the Fermi level in the paramagnetic metallic phase upon increasing photon energy, does not have a significant correlation with the intensity variation of the O 2p and V 3d yield, thus confirming that bulk sensitivity is an essential requirement for the detection of this coherent low energy excitation.

cond-mat.str-el↗

Orbital reconstruction and two-dimensional electron gas at the LaAlO3/SrTiO3 interface

Conventional two-dimensional electron gases are realized by engineering the interfaces between semiconducting compounds. In 2004, Ohtomo and Hwang discovered that an electron gas can be also realized at the interface between large gap insulators made of transition metal oxides [1]. This finding has generated considerable efforts to clarify the underlying microscopic mechanism. Of particular interest is the LaAlO3/SrTiO3 system, because it features especially striking properties. High carrier mobility [1], electric field tuneable superconductivity [2] and magnetic effects [3], have been found. Here we show that an orbital reconstruction is underlying the generation of the electron gas at the LaAlO3/SrTiO3 n-type interface. Our results are based on extensive investigations of the electronic properties and of the orbital structure of the interface using X-ray Absorption Spectroscopy. In particular we find that the degeneracy of the Ti 3d states is fully removed, and that the Ti 3dxy levels become the first available states for conducting electrons.

cond-mat.mtrl-sci↗

Ising magnetism and ferroelectricity in Ca$_3$CoMnO$_6$

The origin of both the Ising chain magnetism and ferroelectricity in Ca$_3$CoMnO$_6$ is studied by $ab$ $initio$ electronic structure calculations and x-ray absorption spectroscopy. We find that Ca$_3$CoMnO$_6$ has the alternate trigonal prismatic Co$^{2+}$ and octahedral Mn$^{4+}$ sites in the spin chain. Both the Co$^{2+}$ and Mn$^{4+}$ are in the high spin state. In addition, the Co$^{2+}$ has a huge orbital moment of 1.7 $μ_B$ which is responsible for the significant Ising magnetism. The centrosymmetric crystal structure known so far is calculated to be unstable with respect to exchange striction in the experimentally observed $\uparrow\uparrow\downarrow\downarrow$ antiferromagnetic structure for the Ising chain. The calculated inequivalence of the Co-Mn distances accounts for the ferroelectricity.

cond-mat.mtrl-sci↗