bulk-thin-film-synthesis-compositionally-variant-entropy-stabilized

Bulk and Thin Film Synthesis of Compositionally Variant Entropy-stabilized Oxides

Here, we present a procedure for the synthesis of bulk and thin film multicomponent (Mg0.25(1-x)CoxNi0.25(1-x)Cu0.25(1-x)Zn0.25(1-x))O (Co variant) and ...

Materials that exhibit simultaneous order in their electric and magnetic ground states hold promise for use in next-generation memory devices in which electric fields control magnetism. Such materials are exceedingly rare, however, owing to competing requirements for displacive ferroelectricity and magnetism. Despite the recent identification of several new multiferroic materials and magnetoelectric coupling mechanisms, known single-phase multiferroics remain limited by antiferromagnetic or weak ferromagnetic alignments, by a lack of coupling between the order parameters, or by having properties that emerge only well below room temperature, precluding device applications. Here we present a methodology for constructing single-phase multiferroic materials in which ferroelectricity and strong magnetic ordering are coupled near room temperature. Starting with hexagonal LuFeO3-the geometric ferroelectric with the greatest known planar rumpling-we introduce individual monolayers of FeO during growth to construct formula-unit-thick syntactic layers of ferrimagnetic LuFe2O4 (refs 17, 18) within the LuFeO3 matrix, that is, (LuFeO3)m/(LuFe2O4)1 superlattices. The severe rumpling imposed by the neighbouring LuFeO3 drives the ferrimagnetic LuFe2O4 into a simultaneously ferroelectric state, while also reducing the LuFe2O4 spin frustration. This increases the magnetic transition temperature substantially-from 240 kelvin for LuFe2O4 (ref. 18) to 281 kelvin for (LuFeO3)9/(LuFe2O4)1. Moreover, the ferroelectric order couples to the ferrimagnetism, enabling direct electric-field control of magnetism at 200 kelvin. Our results demonstrate a design methodology for creating higher-temperature magnetoelectric multiferroics by exploiting a combination of geometric frustration, lattice distortions and epitaxial engineering.

Atomically engineered ferroic layers yield a room-temperature magnetoelectric multiferroic.

Entropy-stabilized materials are stabilized by the configurational entropy of the constituents, rather than the enthalpy of formation of the compound. A unique benefit to entropy-stabilized materials is the increased solubility of elements, which opens a broad compositional space, with subsequent local chemical and structural disorder resulting from different atomic sizes and preferred coordinations of the constituents. Known entropy-stabilized oxides contain magnetically interesting constituents, however, the magnetic properties of the multi-component oxide have yet to be investigated. Here we examine the role of disorder and composition on the exchange anisotropy of permalloy/(MgCoNiCuZn)O heterostructures. Anisotropic magnetic exchange and the presence of a critical blocking temperature indicates that the magnetic order of the entropy-stabilized oxides considered here is antiferromagnetic. Changing the composition of the oxide tunes the disorder, exchange field and magnetic anisotropy. Here, we exploit this tunability to enhance the strength of the exchange field by a factor of 10x at low temperatures, when compared to a permalloy/CoO heterostructure. Significant deviations from the rule of mixtures are observed in the structural and magnetic parameters, indicating that the crystal is dominated by configurational entropy. Our results reveal that the unique characteristics of entropy-stabilized materials can be utilized and tailored to engineer magnetic functional phenomena in oxide thin films.

Article	Year
Atomically engineered ferroic layers yield a room-temperature magnetoelectric multiferroic. Nature\| PubMed ID: 27652564	2016
Giant Enhancement of Exchange Coupling in Entropy-Stabilized Oxide Heterostructures. Scientific reports\| PubMed ID: 29042610	2017

John T. Heron

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