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Register a new userEnhanced electrocatalytic activity via phase transitions in strongly correlated SrRuO3 thin films
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Transition metal oxides have been extensively studied and utilized as efficient catalysts. However, the strongly correlated behavior which often results in intriguing emergent phenomena in these materials has been mostly overlooked in understanding the electrochemical activities. Here, we demonstrate a close correlation between the phase transitions and oxygen evolution reaction (OER) in a strongly correlated SrRuO3. By systematically introducing Ru-O vacancies into the single-crystalline SrRuO3 epitaxial thin films, we induced phase transition in crystalline symmetry which resulted in corresponding modification in the electronic structure. The modified electronic structure significantly affect the electrochemical activities, so a 30% decrease in the overpotential for the OER activity was achieved. Our study suggests that a substantial enhancement in the OER activity can be realized even within single material systems, by rational design and engineering of their crystal and electronic structures.
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For generation of sustainable, clean and highly efficient energy, the electrocatalytic oxygen evolution reaction represents an attractive platform, thus inviting immense research activities in recent years. However, designing the catalyst with enhanced electrocatalytic activity remains one of the major challenges. Here, we examined the oxygen evolution reaction activities of geometrically designed (with and without step-textured morphology) thin films of an electrocatalytically active correlated metallic SrRuO3 perovskite grown on c- and r-plane sapphire substrates. On c-plane sapphire, as compared to the uniform surface, the step-textured films endowed with active Ru-sites show remarkable decrease in the overpotential (25 mV). Interestingly, the behavior is opposite for the r-plane case, highlighting the significance of the active sites, in addition with the polar surface termination of selective crystal facets. Density functional theory calculation confirms the favorable energy reaction pathway for the active site dependent enhancement in OER. Our strategy might pave the way towards designing the surfaces of various oxide thin films for high performance energy conversion based devices.
Enhanced magnetic moment and coercivity in SrRuO3 thin films are significant issues for advanced technological usages and hence are researched extensively in recent times. Most of the previous reports on thin films with enhanced magnetic moment attributed the high spin state for the enhancement. Our magnetization results show high magnetic moment of 3.3 Bohr-magnetron/Ru ion in the epitaxial thin films grown on LSAT substrate against 1.2 Bohr-magnetron/Ru ion observed in bulk compound. Contrary to the expectation the Ru ions are found to be in low spin state and the orbital moment is shown to be contributing significantly in the enhancement of magnetic moment. We employed x-ray absorption spectroscopy and resonant valance band spectroscopy to probe the spin state and orbital contributions in these films. The existence of strong spin-orbit coupling responsible for the de-quenching of the 4d orbitals is confirmed by the observation of the non-statistical large branching ratio at the Ru M2,3 absorption edges. The relaxation of orbital quenching by strain engineering provides a new tool for enhancing magnetic moment. Strain disorder is shown to be an efficient mean to control the spin-orbit coupling.
Nickelates are known for their metal to insulator transition (MIT) and an unusual magnetic ordering, occurring at T=T_Neel. Here, we investigate thin films of SmNiO_3 subjected to different levels of epitaxial strain. We find that the original bulk behavior (T_Neel<T_MI) is strongly affected by applying compressive strain to the films. For small compressive strains, a regime where T_Neel=T_MI is achieved, the paramagnetic insulating phase characteristic of the bulk compound is suppressed and the MIT becomes 1st order. Further increasing the in-plane compression of the SmNiO_3 lattice leads to the stabilization of a single metallic paramagnetic phase.
We highlight recent advances in the theory, materials fabrication, and experimental characterization of strongly correlated and topological states in [111] oriented transition metal oxide thin films and heterostructures, which are notoriously difficult to realize compared to their [001] oriented counterparts. We focus on two classes of complex oxides, with the chemical formula ABO3 and A2B2O7, where the B sites are occupied by an open-shell transition metal ion with a local moment, and the A sites are typically a rare earth. The [111] oriented quasi-two-dimensional lattices derived from these parent compound lattices can exhibit peculiar geometries and symmetries, namely, a buckled honeycomb lattice, as well as kagome and triangular lattices. These lattice motifs form the basis for emergent strongly correlated and topological states expressed in exotic magnetism, various forms of orbital ordering, topological insulators, topological semimetals, quantum anomalous Hall insulators, and quantum spin liquids. For transition metal ions with high atomic number, spin-orbit coupling plays a significant role and may give rise to additional topological features in the electronic band structure and in the spectrum of magnetic excitations. We conclude the Perspective by articulating open challenges and opportunities in this actively developing field.
V2O3 thin films about 10 nm thick were grown on Al2O3 (0001) by pulsed laser deposition. The XRD analysis is in agreement with R-3c space group. Some of them exhibit the metal / insulator transition characteristic of V2O3 bulk material and others samples exhibit a metallic behavior. For the latter, the XPS analysis indicates an oxidation state of +III for vanadium. There is no metal / insulator transition around 150 K in this sample and a strongly correlated Fermi liquid rho = AT2 behavior of the resistivity at low temperature is observed, with a value of A of 1.2 10-4 ohm cm, 3 times larger than the bulk value at 25 kbar.
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