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Register a new userStructural evolution of epitaxial SrCoOx films near topotactic phase transition
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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.
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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.
We report a Raman scattering investigation of multiferroic bismuth ferrite BiFeO3 epitaxial (c-axis oriented) thin films from -192 to 1000C. Phonon anomalies have been observed in three temperature regions: in the gamma-phase from 930C to 950C; at ~370C, Neel temperature (TN), and at ~123C, due to a phase transition of unknown type (magnetic or structural). An attempt has been made to understand the origin of the weak phonon-magnon coupling and the dynamics of the phase sequence. The disappearance of several Raman modes at ~820C (Tc) is compatible with the known structural phase transition and the Pbnm orthoferrite space group assigned by Arnold {it et al.} cite{arnold:09}. The spectra also revealed a {it non-cubic} $beta$-phase from 820-930dc and the same {it non-cubic} phase extends through the $gamma$-phase between 930-950dc, in agreement with Arnold {it et al.} cite{arnold2:09}, and an evidence of a cubic $delta$-phase around 1000dc in thin films that is not stable in powder and bulk. Such a cubic phase has been theoretically predicted in cite{vasquez:prb09}. Micro-Raman scattering and X-ray diffraction showed no structural decomposition in thin films during the thermal cycling from 22-1000dc.
Three different film systems have been systematically investigated to understand the effects of strain and substrate constraint on the phase transitions of perovskite films. In SrTiO$_3$ films, the phase transition temperature T$_C$ was determined by monitoring the superlattice peaks associated with rotations of TiO$_6$ octahedra. It is found that T$_C$ depends on both SrTiO$_3$ film thickness and SrRuO$_3$ buffer layer thickness. However, lattice parameter measurements showed no sign of the phase transitions, indicating that the tetragonality of the SrTiO$_3$ unit cells was no longer a good order parameter. This signals a change in the nature of this phase transition, the internal degree of freedom is decoupled from the external degree of freedom. The phase transitions occur even without lattice relaxation through domain formation. In NdNiO$_3$ thin films, it is found that the in-plane lattice parameters were clamped by the substrate, while out-of-plane lattice constant varied to accommodate the volume change across the phase transition. This shows that substrate constraint is an important parameter for epitaxial film systems, and is responsible for the suppression of external structural change in SrTiO$_3$ and NdNiO$_3$ films. However, in SrRuO$_3$ films we observed domain formation at elevated temperature through x-ray reciprocal space mapping. This indicated that internal strain energy within films also played an important role, and may dominate in some film systems. The final strain states within epitaxial films were the result of competition between multiple mechanisms and may not be described by a single parameter.
In multiferroic BiFeO3 thin films grown on highly mismatched LaAlO3 substrates, we reveal the coexistence of two differently distorted polymorphs that leads to striking features in the temperature dependence of the structural and multiferroic properties. Notably, the highly distorted phase quasi-concomitantly presents an abrupt structural change, transforms from a hard to a soft ferroelectric and transitions from antiferromagnetic to paramagnetic at 360+/-20 K. These coupled ferroic transitions just above room temperature hold promises of giant piezoelectric, magnetoelectric and piezomagnetic responses, with potential in many applications fields.
The electronic and magnetic properties of transition metal dichalcogenides are known to be extremely sensitive to their structure. In this paper we study the effect of structure on the electronic and magnetic properties of mono- and bilayer $VSe_2$ films grown using molecular beam epitaxy. $VSe_2$ has recently attracted much attention due to reports of emergent ferromagnetism in the 2D limit. To understand this important compound, high quality 1T and distorted 1T films were grown at temperatures of 200 $^text{o}$C and 450 $^text{o}$C respectively and studied using 4K Scanning Tunneling Microscopy/Spectroscopy. The measured density of states and the charge density wave (CDW) patterns were compared to band structure and phonon dispersion calculations. Films in the 1T phase reveal different CDW patterns in the first layer compared to the second. Interestingly, we find the second layer of the 1T-film shows a CDW pattern with 4a $times$ 4a periodicity which is the 2D version of the bulk CDW observed in this compound. Our phonon dispersion calculations confirm the presence of a soft phonon at the correct wavevector that leads to this CDW. In contrast, the first layer of distorted 1T phase films shows a strong stripe feature with varying periodicities, while the second layer displays no observable CDW pattern. Finally, we find that the monolayer 1T $VSe_2$ film is weakly ferromagnetic, with ~ $3.5 {mu}_B$ per unit similar to previous reports.
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