Search for: All records

Using molecular beam epitaxy (MBE) to grow multielemental oxides (MEOs) is generally challenging, partly due to difficulty in stoichiometry control. Occasionally, if one of the elements is volatile at the growth temperature, stoichiometry control can be greatly simplified using adsorption-controlled growth mode. Otherwise, stoichiometry control remains one of the main hurdles to achieving high-quality MEO film growths. Here, we report another kind of self-limited growth mode, dubbed diffusion-assisted epitaxy, in which excess species diffuses into the substrate and leads to the desired stoichiometry, in a manner similar to the conventional adsorption-controlled epitaxy. Specifically, we demonstrate that using diffusion-assisted epitaxy, high-quality epitaxial CuCrO2 films can be grown over a wide growth window without precise flux control using MBE.

 

High entropy oxides are emerging as an exciting new avenue to design highly tailored functional behaviors that have no traditional counterparts. Study and application of these materials are bringing together scientists and engineers from physics, chemistry, and materials science. The diversity of each of these disciplines comes with perspectives and jargon that may be confusing to those outside of the individual fields, which can result in miscommunication of important aspects of research. In this Perspective, we provide examples of research and characterization taken from these different fields to provide a framework for classifying the differences between compositionally complex oxides, high entropy oxides, and entropy stabilized oxides, which is intended to bring a common language to this emerging area. We highlight the critical importance of understanding a material’s crystallinity, composition, and mixing length scales in determining its true definition. 

Abstract When a three-dimensional material is constructed by stacking different two-dimensional layers into an ordered structure, new and unique physical properties can emerge. An example is the delafossite PdCoO 2 , which consists of alternating layers of metallic Pd and Mott-insulating CoO 2 sheets. To understand the nature of the electronic coupling between the layers that gives rise to the unique properties of PdCoO 2 , we revealed its layer-resolved electronic structure combining standing-wave X-ray photoemission spectroscopy and ab initio many-body calculations. Experimentally, we have decomposed the measured VB spectrum into contributions from Pd and CoO 2 layers. Computationally, we find that many-body interactions in Pd and CoO 2 layers are highly different. Holes in the CoO 2 layer interact strongly with charge-transfer excitons in the same layer, whereas holes in the Pd layer couple to plasmons in the Pd layer. Interestingly, we find that holes in states hybridized across both layers couple to both types of excitations (charge-transfer excitons or plasmons), with the intensity of photoemission satellites being proportional to the projection of the state onto a given layer. This establishes satellites as a sensitive probe for inter-layer hybridization. These findings pave the way towards a better understanding of complex many-electron interactions in layered quantum materials. 

The interface between 2D topological Dirac states and ans‐wave superconductor is expected to support Majorana‐bound states (MBS) that can be used for quantum computing applications. Realizing these novel states of matter and their applications requires control over superconductivity and spin‐orbit coupling to achieve spin‐momentum‐locked topological interface states (TIS) which are simultaneously superconducting. While signatures of MBS have been observed in the magnetic vortex cores of bulk FeTe_0.55Se_0.45, inhomogeneity and disorder from doping make these signatures unclear and inconsistent between vortices. Here superconductivity is reported in monolayer (ML) FeTe_1–ySe_y(Fe(Te,Se)) grown on Bi₂Te₃by molecular beam epitaxy (MBE). Spin and angle‐resolved photoemission spectroscopy (SARPES) directly resolve the interfacial spin and electronic structure of Fe(Te,Se)/Bi₂Te₃heterostructures. Fory = 0.25, the Fe(Te,Se) electronic structure is found to overlap with the Bi₂Te₃TIS and the desired spin‐momentum locking is not observed. In contrast, fory = 0.1, reduced inhomogeneity measured by scanning tunneling microscopy (STM) and a smaller Fe(Te,Se) Fermi surface with clear spin‐momentum locking in the topological states are found. Hence, it is demonstrated that the Fe(Te,Se)/Bi₂Te₃system is a highly tunable platform for realizing MBS where reduced doping can improve characteristics important for Majorana interrogation and potential applications.

 

The availability of native substrates is a cornerstone in the development of microelectronic technologies relying on epitaxial films. If native substrates are not available, virtual substrates - crystalline buffer layers epitaxially grown on a structurally dissimilar substrate - offer a solution. Realizing commercially viable virtual substrates requires the growth of high-quality films at high growth rates for large-scale production. We report the stoichiometric growth of SrTiO₃exceeding 600 nm hr⁻¹. This tenfold increase in growth rate compared to SrTiO₃grown on silicon by conventional methods is enabled by a self-regulated growth window accessible in hybrid molecular beam epitaxy. Overcoming the materials integration challenge for complex oxides on silicon using virtual substrates opens a path to develop new electronic devices in the More than Moore era and silicon integrated quantum computation hardware.