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Register a new userSuppression of the ferromagnetic state in LaCoO3 films by rhombohedral distortion
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Epitaxially strained LaCoO3 (LCO) thin films were grown with different film thickness, t, on (001) oriented (LaAlO3)0.3(SrAl0.5Ta0.5O3)0.7 (LSAT) substrates. After initial pseudomorphic growth the films start to relieve their strain partly by the formation of periodic nano-twins with twin planes predominantly along the <100> direction. Nano-twinning occurs already at the initial stage of growth, albeit in a more moderate way. Pseudomorphic grains, on the other hand, still grow up to a thickness of at least several tenths of nanometers. The twinning is attributed to the symmetry lowering of the epitaxially strained pseudo-tetragonal structure towards the relaxed rhombohedral structure of bulk LCO. However, the unit-cell volume of the pseudo-tetragonal structure is found to be nearly constant over a very large range of t. Only films with t > 130 nm show a significant relaxation of the lattice parameters towards values comparable to those of bulk LCO.
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We investigate the structure and magnetic properties of thin films of the LaCoO$_{3}$ compound. Thin films are deposited by pulsed laser deposition on various substrates in order to tune the strain from compressive to tensile. Single-phase (001) oriented LaCoO$_{3}$ layers were grown on all substrates despite large misfits. The tetragonal distortion of the films covers a wide range from -2% to 2.8%. Our LaCoO$_{3}$ films are ferromagnetic with Curie temperature around 85 K, contrary to the bulk. The total magnetic moment is below $1mu_{B}$/Co$^{3+}$, a value relatively small for an exited spin-state of the Co$^{3+}$ ions, but comparable to values reported in literature. A correlation of strain states and magnetic moment of Co$^{3+}$ ions in LaCoO$_{3}$ thin films is observed.
We investigate the spin state of LaCoO3 using state-of-the-art photoemission spectroscopy and ab initio band structure calculations. The GGA+U calculations provide a good description of the ground state for the experimentally estimated value of electron correlation strength, U. In addition to the correlation effect, spin-orbit interaction is observed to play a significant role in the case of intermediate spin and high spin configurations. The comparison of the calculated Co 3d and O 2p partial density of states with the experimental valence band spectra indicates that at room temperature, Co has dominant intermediate spin state configuration and that the high spin configuration may not be significant at this temperature. The lineshape of the La 5p and O 2s core level spectra could be reproduced well within these ab initio calculations.
Electronic structure of the three-dimensional colossal magnetoresistive perovskite La1-xSrxMnO3 has been established using soft-X-ray ARPES with its intrinsically sharp definition of three-dimensional electron momentum. The experimental results show much weaker polaronic coupling compared to the bilayer manganites and are consistent with the GGA+U band structure. The experimental Fermi surface unveils the canonical topology of alternating three-dimensional electron spheres and hole cubes, with their shadow contours manifesting the rhombohedral lattice distortion. This picture has been confirmed by one-step photoemission calculations including displacement of the apical oxygen atoms. The rhombohedral distortion is neutral to the Jahn-Teller effect and thus polaronic coupling, but affects the double-exchange electron hopping and thus the colossal magnetoresistance effect.
LaCoO3 (LCO) nanoparticles were synthesized and their magnetic and structural properties were examined using SQUID magnetometery and neutron diffraction. The nanoparticles exhibit ferromagnetic long-range order beginning at T_C approximately 87K that persists to low temperatures. This behavior is contrasted with the ferromagnetism of bulk LCO, which also starts at T_C approximately 87K but is suppressed below a second transition at T_o approximately 37K, due to a structural phase transition. The ferromagnetism in both systems is attributed to the tensile stress from particle surfaces and impurity phase interfaces. This stress locally increases the Co-O-Co bond angle gamma, and competes with the thermal contraction of the lattice. It has recently been shown that LCO loses long-range ferromagnetic order when gamma decreases below the critical value gamma_c = 162.8 degrees. Consistent with this model, we show that gamma in nanoparticles remains larger than gamma_c at low temperatures, likely a consequence of all spins being in close proximity to surfaces or interfaces.
Using pulsed laser deposition and a unique fast quenching method, we have prepared SrCoOx epitaxial films on SiTiO3 substrates. As electrochemical oxidation increases the oxygen content from x = 2.75 to 3.0, the films tend to favor the discrete magnetic phases seen in bulk samples for the homologous series SrCoO(3-n/8) (n = 0, 1, 2). Unlike bulk samples, 200nm thick films remain single phase throughout the oxidation cycle. 300 nm films can show two simultaneous phases during deoxidation. These results are attributed to finite thickness effects and imply the formation of ordered regions larger than approximately 300 nm.
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