Min-Ju Choi, Krishna P. Koirala, Hua Zhou, Mark E. Bowden, Hyoju Park, Christie Nelson, Raul Acevedo-Esteves, Jinhui Tao, Peter V. Sushko, Yingge Du
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Orientation Control in Epitaxial PdO Thin Films Grown on MgO (001) – Role of Oxygen Chemical Potential
Control of crystal orientations in thin films of functional materials allowsedictive tuning of their strain states, electronic properties, and surface chemical reactivity. Here, conditions for orientation control in epitaxial PdO films are investigated. Due to its tetragonal structure, PdO can form two orientational relationships with the MgO (001). It is shown that, under an oxygen-rich environment provided by oxygen-plasma-assisted molecular beam epitaxy, both (00l)- and (100)-oriented PdO domains form on MgO (001). Subsequent thermal annealing in a vacuum promotes film restructuring to a predominantly (100)-oriented PdO with improved crystallinity. Ab initio calculations reveal that the (001) orientation has lower strain energy but weaker interfacial interactions and serves as an oxygen vacancy sink, whereas the (100) orientation benefits from significantly stronger MgO─PdO bonding. Consequently (100)-oriented domains become favored under oxygen-poor conditions. A mechanism is proposed whereby vacuum annealing drives orientation transformation by generating oxygen vacancies that destabilize the (001) domains and promote (100) ordering. These findings deepen the understanding of how oxygen content impacts interfacial stability and reorganization, thereby offering a route to tune domain orientations in oxide thin films.
期刊介绍:
Advanced Materials Interfaces publishes top-level research on interface technologies and effects. Considering any interface formed between solids, liquids, and gases, the journal ensures an interdisciplinary blend of physics, chemistry, materials science, and life sciences. Advanced Materials Interfaces was launched in 2014 and received an Impact Factor of 4.834 in 2018.
The scope of Advanced Materials Interfaces is dedicated to interfaces and surfaces that play an essential role in virtually all materials and devices. Physics, chemistry, materials science and life sciences blend to encourage new, cross-pollinating ideas, which will drive forward our understanding of the processes at the interface.
Advanced Materials Interfaces covers all topics in interface-related research:
Oil / water separation,
Applications of nanostructured materials,
2D materials and heterostructures,
Surfaces and interfaces in organic electronic devices,
Catalysis and membranes,
Self-assembly and nanopatterned surfaces,
Composite and coating materials,
Biointerfaces for technical and medical applications.
Advanced Materials Interfaces provides a forum for topics on surface and interface science with a wide choice of formats: Reviews, Full Papers, and Communications, as well as Progress Reports and Research News.