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Register a new userSuppression of Magnetic Phase Separation in Epitaxial SrCoOx Films
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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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Using real-time spectroscopic ellipsometry, we directly observed a reversible lattice and electronic structure evolution in SrCoOx (x = 2.5 - 3) epitaxial thin films. Drastically different electronic ground states, which are extremely susceptible to the oxygen content x, are found in the two topotactic phases, i.e. the brownmillerite SrCoO2.5 and the perovskite SrCoO3. First principles calculations confirmed substantial differences in the electronic structure, including a metal-insulator transition, which originates from the modification in the Co valence states and crystallographic structures. More interestingly, the two phases can be reversibly controlled by changing the ambient pressure at greatly reduced temperatures. Our finding provides an important pathway to understanding the novel oxygen-content-dependent phase transition uniquely found in multivalent transition metal oxides.
Control of oxygen stoichiometry in complex oxides via topotactic phase transition is an interesting avenue to not only modifying the physical properties, but utilizing in many energy technologies, such as energy storage and catalysts. However, detailed structural evolution in the close proximity of the topotactic phase transition in multivalent oxides has not been much studied. In this work, we used strontium cobaltites (SrCoOx) epitaxially grown by pulsed laser epitaxy (PLE) as a model system to study the oxidation-driven evolution of the structure, electronic, and magnetic properties. We grew coherently strained SrCoO2.5 thin films and performed post-annealing at various temperatures for topotactic conversion into the perovskite phase (SrCoO3-{delta}). We clearly observed significant changes in electronic transport, magnetism, and microstructure near the critical temperature for the topotactic transformation from the brownmillerite to the perovskite phase. Nevertheless, the overall crystallinity was well maintained without much structural degradation, indicating that topotactic phase control can be a useful tool to control the physical properties repeatedly via redox reactions.
We have successfully grown epitaxial La$_{1.67}$Sr$_{0.33}$NiO$_4$ films with a small crystalline mosaic using pulsed laser deposition. With synchrotron radiation, the x-ray diffraction peaks associated with charge stripes have been successfully observed for relatively thick films. Anomalies due to the charge-ordering transition have been examined using four-point probe resistivity measurements. X-ray scattering provides direct evidence for suppression of the stripe phase in thin samples; the phase disappears for film thicknesses $leqslant$ 2600 ~AA{}. The suppression appears to be a result of shrinking the stripe phase domains. This may reflect the stripe phase progressing from nematic to isotropic.
We have explored the magnetism in the non-geometrically frustrated spin-chain system $gamma$-CoV$_{2}$O$_{6}$ which possesses a complex magnetic exchange network. Our neutron diffraction patterns at low temperatures ($T$ $leqslant$ $T_{mathrm{N}}$ = 6.6 K) are best described by a model in which two magnetic phases coexist in a volume ratio 65(1) : 35(1), with each phase consisting of a single spin modulation. This model fits previous studies and our observations better than the model proposed by Lenertz $et$ $al$ in J. Phys. Chem. C 118, 13981 (2014), which consisted of one phase with two spin modulations. By decreasing the temperature from $T_{mathrm{N}}$, the minority phase of our model undergoes an incommensurate-commensurate lock-in transition at $T^{*}$ = 5.6 K. Based on these results, we propose that phase separation is an alternative approach for degeneracy-lifting in frustrated magnets.
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.
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