Synthesis Of Epitaxial Thin Films Research Articles

Synthesis of antiferromagnetic Weyl semimetal Mn3Ge on insulating substrates by electron beam assisted molecular beam epitaxy

The antiferromagnetic kagome semimetals Mn3X (X = Ge, Sn, Ga) are of great interest due to properties arising from their Berry curvature, such as large anomalous Nernst and anomalous Hall coefficients, and spin to charge conversion efficiencies at ambient temperatures. However, the synthesis of epitaxial thin films of Mn3Ge in the desired hexagonal phase has been challenging because they do not wet insulating substrates, necessitating the use of a metallic buffer layer. Furthermore, a ferrimagnetic tetragonal phase also forms readily under typical growth conditions, interfering with hexagonal phase properties. We have synthesized atomically smooth and continuous epitaxial thin films of hexagonal Mn3Ge directly on insulating LaAlO3 (111) substrates using electron beam assisted molecular beam epitaxy, using a three-step process that mitigates the formation of the tetragonal phase. The anomalous Nernst coefficient is found to be more than six times larger in our films than in sputtered thin films of Mn3Ge and significantly larger than that of Fe. Our approach can be used to grow thin layers of kagome materials, without interference from a buffer layer in transport properties, and may be applicable to a broader range of materials with large surface energies that do not grow readily on insulating substrates.

Single-Crystal Alkali Antimonide Photocathodes: High Efficiency in the Ultrathin Limit.

The properties of photoemission electron sources determine the ultimate performance of a wide class of electron accelerators and photon detectors. To date, all high-efficiency visible-light photocathode materials are either polycrystalline or exhibit intrinsic surface disorder, both of which limit emitted electron beam brightness. In this Letter, we demonstrate the synthesis of epitaxial thin films of Cs_{3}Sb on 3C-SiC (001) using molecular-beam epitaxy. Films as thin as 4nm have quantum efficiencies exceeding 2% at 532nm. We also find that epitaxial films have an order of magnitude larger quantum efficiency at 650nm than comparable polycrystalline films on Si. Additionally, these films permit angle-resolved photoemission spectroscopy measurements of the electronic structure, which are found to be in good agreement with theory. Epitaxial films open the door to dramatic brightness enhancements via increased efficiency near threshold, reduced surface disorder, and the possibility of engineering new photoemission functionality at the level of single atomic layers.

Crystallization engineering as a route to epitaxial strain control

The controlled synthesis of epitaxial thin films offers opportunities for tuning their functional properties via enabling or suppressing strain relaxation. Examining differences in the epitaxial crystallization of amorphous oxide films, we report on an alternate, low-temperature route for strain engineering. Thin films of amorphous Bi–Fe–O were grown on (001)SrTiO3 and (001)LaAlO3 substrates via atomic layer deposition. In situ X-ray diffraction and X-ray photoelectron spectroscopy studies of the crystallization of the amorphous films into the epitaxial (001)BiFeO3 phase reveal distinct evolution profiles of crystallinity with temperature. While growth on (001)SrTiO3 results in a coherently strained film, the same films obtained on (001)LaAlO3 showed an unstrained, dislocation-rich interface, with an even lower temperature onset of the perovskite phase crystallization than in the case of (001)SrTiO3. Our results demonstrate how the strain control in an epitaxial film can be accomplished via its crystallization from the amorphous state.

Rapid Solid-State Synthesis of Oxides by Means of Irradiation with Light

A novel kind of synthesis for oxide materials, especially complex ones, has been developed. The process involves the intense irradiation of the powder mixture of the starting oxides by light at elevated temperature. The spectral range tested extends from infrared to ultraviolet with sufficient intensity for the solid-state reaction between the reagents to take place. The resulting reaction speed exceeds the conventional thermal one by up to two orders of magnitude. This method should be applicable for the synthesis of epitaxial thin films of high-TC superconductors used in RABITS or IBAD technologies, high-Q filters, and magnetic oxide films for magnetoelectronics.

Optical band gap of NpO2 and PuO2 from optical absorbance of epitaxial films

We report a solution based synthesis of epitaxial thin films of neptunium oxide and plutonium oxide. Actinides represent a challenge to first principle calculations due to features that arise from f orbital interactions. Conventional semi-local density functional theory predicts NpO2 and PuO2 to be metallic, when they are well known insulators. Improvements in theory are dependent on comparison with accurate measurements of material properties, which in turn demand high-quality samples. The high melting point of actinide oxides and their inherent radioactivity makes single crystal and epitaxial film formation challenging. We report on the preparation of high quality epitaxial actinide films. The films have been characterized through a combination of X-ray diffraction and X-ray absorption fine structure (XANES and EXAFS) measurements. We report band gaps of 2.80 ± 0.1 eV and 2.85 ± 0.1 eV at room temperature for PuO2 and NpO2, respectively, and compare our measurements with state-of-the-art calculations.

Chemical epitaxy of semiconductor thin films

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