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We derive the kinetic equations for polaron hopping in organics that explicitly take into account the double occupation possibility and pair intersite correlations. The equations include simplified phenomenological spin dynamics and provide a self-consistent framework for the description of the bipolaron mechanism of the organic magnetoresistance. At low applied voltages the equations can be reduced to effective resistor network that generalizes the Miller-Abrahams network and includes the effect of spin relaxation on the system resistivity. Our theory discloses the close relationship between the organic magnetoresistance and the intersite correlations. Moreover, in the absence of correlations, as in ordered system with zero Hubbard energy, the magnetoresistance vanishes., Comment: 17 pages 10 figures accepted for publication in Physical Review B

The quest for a spin-polarized organic light emitting diode (spin-OLED) is a common goal in the emerging fields of molecular electronics and spintronics. In this device two ferromagnetic electrodes are used to enhance the electroluminescence intensity of the OLED through a magnetic control of the spin polarization of the injected carriers. The major difficulty is that the driving voltage of an OLED device exceeds of a few volts, while spin injection in organic materials is only efficient at low voltages. We report here the fabrication of a spin-OLED that uses a conjugated polymer as bipolar spin collector layer and ferromagnetic electrodes. Through a careful engineering of the organic/inorganic interfaces we have succeeded in obtaining a light-emitting device showing spin-valve effects at high voltages (up to 14 V). This has allowed us to detect a magneto-electroluminescence enhancement on the order of a 2.4 % at 9 V for the antiparallel configuration of the magnetic electrodes. This observation provides evidence for the long-standing fundamental issue of injecting spins from magnetic electrodes into the frontier levels of a molecular semiconductor. Our finding opens the way for the design of multifunctional devices coupling the light and the spin degrees of freedom.

We derive kinetic equations describing injection and transport of spin polarized carriers in organic semiconductors with hopping conductivity via an impurity level. The model predicts a strongly voltage dependent magnetoresistance, defined as resistance variation between devices with parallel and antiparallel electrode magnetizations (spin valve effect). The voltage dependence of the magnetoresistance splits into three distinct regimes. The first regime matches well known inorganic spintronic regimes, corresponding to barrier controlled spin injection or the well known conductivity mismatch case. The second regime at intermediate voltages corresponds to strongly suppressed magnetoresistance. The third regime develops at higher voltages and accounts for a novel paradigm. It is promoted by the strong non-linearity in the charge transport which strength is characterized by the dimensionless parameter $eU/k_BT$. This nonlinearity, depending on device conditions, can lead to both significant enhancement or to exponential suppression of the spin valve effect in organic devices. We believe that these predictions are valid beyond the case of organic semiconductors and should be considered for any material characterized by strongly non-linear charge transport., Comment: 7 pages, 5 figures

Highly-anisotropic in-plane magneto-resistance (MR) in graphite (HOPG) samples has been recently observed (Y. Kopelevich et al., arXiv:1202.5642) which is negative and linear in low fields in some current direction while it is giant, super-linear and positive in the perpendicular direction. In the framework of the hopping conductance theory via non-zero angular momentum orbitals we link extraordinary MRs in graphite and in organic insulators (OMAR) observed in about the same magnetic fields. The theory predicts quadratic negative MR (NMR) when there is a time-reversal symmetry (TRS), and linear NMR if TRS is broken. We argue that the observed linear NMR could be a unique signature of the broken TRS both in graphite and organic compounds. While some local paramagnetic centers are responsible for the broken TRS in organic insulators, a large diamagnetism of our HOPG samples may involve a more intriguing scenario of TRS breaking., Comment: 7 pages, 7 figures. arXiv admin note: substantial text overlap with arXiv:1202.5642

The effect of the AlOx barrier thickness on magnetic and morphological properties of Ta/Co/(AlOx)/Alq3/Si hybrid structures was systematically studied by means of atomic force microscopy, SQUID magnetometry and nuclear magnetic resonance (NMR). All used techniques pointed out that the barrier thickness of 2 nm is required to obtain a magnetically good cobalt layer on top of Alq3. 59Co NMR measurements revealed that the AlOx barrier gives rise to the formation of an interface layer with "defective" cobalt favouring growth of "bulk" cobalt with good magnetic properties., Comment: 4 pages, Accepted for publication in Applied Physics Letters

The surface spin polarization in the epitaxial films of a prototype manganite, La0.7Sr0.3MnO3, has been investigated by Scanning Tunneling Spectroscopy with ferromagnetic SP tips at room temperature. The manganite surface splits into ferromagnetic (FM) and paramagnetic(PM) regions characterized by metallic and insulating like behavior respectively. Spin polarized spectroscopy with Ni tips has been performed separately for the two phases, and the results compared with standard W and Pt tips. While PM exhibits featureless tunneling characteristics, the FM regions exhibit at room temperature strongly nonlinear behavior with a band-gap like behavior. The spin resolved density of states of the FM regions of the manganite has been extracted by the deconvolution of the spectroscopic curves. It indicates very high spin polarization (nearly halfmetallic behavior) with the spin down band separated from Fermi level by 0.4 eV. This value corresponds exactly to the gap value measured for the whole surface of this manganite at low temperatures. Thus the surface of the La0.7Sr0.3MnO3 films maintain even at room temperature nano- and micrometric islands of very high spin polarization, while the total polarization is given by the coverage of the surface by FM regions. This result is extremely important for spintronic applications of this material and indicates possible roots for the realization of manganite nanosized devices with extremely high spin polarization., Comment: 15 pages, 5 figures

The electronic structure of the interface between Tris (8-hydroxyquinolino)-aluminum (Alq3) and La0.7Sr0.3MnO3 manganite (LSMO) was investigated by means of photoelectron spectroscopy. As demonstrated recently this interface is characterized by efficient spin injection in organic spintronic devices. We detected a strong interface dipole of about 0.9 eV that shifts down the whole energy diagram of the Alq3 with respect to the vacuum level. This modifies the height of the barriers for the holes injection to 1.7 eV, indicating that hole injection from LSMO into Alq3 is more difficult than it was expected as the energy level matched by vacuum levels. We believe the interface dipole is due to the intrinsic dipole moment characteristic for Alq3 layer. An additional weak interaction is observed between the two materials influencing the N 1s core levels of the organic semiconductor. The presented data are of greatest importance for both qualitative and quantitative description of the organic spin valves., Comment: 17 pages, 4 figures

We report detailed investigations of hybrid organic-inorganic vertical spin valves. Spin polarized injection in tris(8-hydroxyquinoline) aluminum (Alq3) organic semiconductor (OS) was performed using La0.7Sr0.3MnO3 manganite as the bottom electrode and Co as the top electrode. While manganite was directly connected to the organic semiconductor layer, a thin tunnel barrier was placed between the OS and the Co electrode. A clear negative spin valve effect - low resistance for antiparallel electrodes configuration - was observed below 210 K in various devices using two different tunnel barriers: LiF and Al2O3. The magnetoresistance effect was found to be strongly asymmetric with respect to the bias voltage. Photoelectron Spectroscopy (PES) investigation of the interface between manganite and Alq3 revealed a strong interface dipole, which leads to a better matching of the metal Fermi level with Alq3 LUMO (1.1 eV) rather than with HOMO level (1.7 eV). This unequivocally indicates that the current in these devices is dominated by the electron channel, and not by holes as previously suggested. The knowledge of the energy diagram at the bottom interface allowed us to work out a semi- quantitative model explaining both negative spin valve effect and strong voltage asymmetry. This model involves a sharp energy selection of the moving charges by the very narrow LUMO level of the organic material leading to peculiar resonant effects.

The ferromagnetic phase in La0.7Sr0.3MnO3 manganite is completely spin polarized (100%) at room temperature. This is demonstrated on high quality epitaxial films by Spin-Polarized Scanning Tunneling Microscopy. The films consist of a highly homogeneous ferromagnetic (FM) phase in which minority paramagnetic (PM) defects are embedded (less than 1% for best films). PM defects exhibit featureless tunneling spectroscopic characteristics and an insulating-like conductance. FM phase exhibit metallic behavior and strongly nonlinear characteristics. Deconvolution of the spectroscopic curves for the FM phase reveals the totally spin-splitted egt2g manganite bands whose shape and width are in an excellent agreement with optical and photoemission spectroscopy data. These results promote the manganites as efficient spin polarized injectors at ambient conditions., Comment: 12 pages, 4 figures

Electroluminescence in organic semiconductors strongly depends on the relative population of excited singlet and triplet excitonic states resulting from recombination of injected carriers. In conventional organic light-emitting diodes (OLED) optical emission is usually based on fluorescence from excited singlet states1, although phosphorescence from triplets is also investigated2. Governing the spin statistics of the injected carriers would open the way to amplify a chosen electronic transition increasing therefore the OLED efficiency. Direct injection of carriers with high degree of spin polarisation along a given axis should lead to preferential population of either singlet or triplet excited states, depending on the relative electrodes polarisation. Here we report a first experimental evidence of direct spin polarised (SP) injection in sexithienyl (T6), a prototypical organic semiconductor, from half-metallic manganites. The spin penetration depth in T6 is about 250-300 nm at room temperature. The results are discussed taking into account possible spin-flip mechanisms in organic material and interface effects., Comment: 6pages, 2 figures

We report a study of polycrystalline samples of the family La1-xCdxMnO3+dwith different percentage of Mn4+ ions. X-rays diffraction, Iodometric titration, Raman, Magnetic and Electrical Resistivity measurements provide a general characterisation of the physical properties. Results are qualitatively similar to the ones found in Ca doped manganese perovskites. Key words: Cd, manganese perovskites, magnetoresistance, Raman, magnetic, resistivity, Comment: 7 pages including 3 figures

The Channel-Spark method was used for deposition of highly oriented ferromagnetic La0.7Sr0.3MnO3 films on NdGaO3 substrates. It was found that additional oxygen decreases the film quality suppressing the Curie temperature and metal-insulator transition below the room temperature. To achieve the best quality of the films the samples were either annealed in high vacuum at deposition temperature or even deposited in argon atmosphere with no oxygen annealing. For such films the resistive measurements showed a metallic behaviour in the interval 10-300 K in accordance with the high Curie point (Tc 350 K). Micro-Raman analysis indicate that the La0.7Sr0.3MnO3 films are well ordered, while some outgrowths show stoichiometrical deviations., Comment: 7 pages, 4 figures