The making of BaZrS3thin films by molecular beam epitaxy (MBE) is demonstrated. BaZrS3forms in the orthorhombic distorted‐perovskite structure with corner‐sharing ZrS6octahedra. The single‐step MBE process results in films smooth on the atomic scale, with near‐perfect BaZrS3stoichiometry and an atomically sharp interface with the LaAlO3substrate. The films grow epitaxially via two competing growth modes: buffered epitaxy, with a self‐assembled interface layer that relieves the epitaxial strain, and direct epitaxy, with rotated‐cube‐on‐cube growth that accommodates the large lattice constant mismatch between the oxide and the sulfide perovskites. This work sets the stage for developing chalcogenide perovskites as a family of semiconductor alloys with properties that can be tuned with strain and composition in high‐quality epitaxial thin films, as has been long‐established for other systems including Si‐Ge, III‐Vs, and II‐VIs. The methods demonstrated here also represent a revival of gas‐source chalcogenide MBE.
Topological materials are derived from the interplay between symmetry and topology. Advances in topological band theories have led to the prediction that the antiperovskite oxide Sr3SnO is a topological crystalline insulator, a new electronic phase of matter where the conductivity in its (001) crystallographic planes is protected by crystallographic point group symmetries. Realization of this material, however, is challenging. Guided by thermodynamic calculations, a deposition approach is designed and implemented to achieve the adsorption‐controlled growth of epitaxial Sr3SnO single‐crystal films by molecular‐beam epitaxy (MBE). In situ transport and angle‐resolved photoemission spectroscopy measurements reveal the metallic and electronic structure of the as‐grown samples. Compared with conventional MBE, the used synthesis route results in superior sample quality and is readily adapted to other topological systems with antiperovskite structures. The successful realization of thin films of Sr3SnO opens opportunities to manipulate topological states by tuning symmetries via strain engineering and heterostructuring.
more » « less- PAR ID:
- 10456783
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 32
- Issue:
- 34
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
more » « less
Abstract -
more » « less
Abstract The interface between 2D topological Dirac states and an
s ‐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 FeTe0.55Se0.45, inhomogeneity and disorder from doping make these signatures unclear and inconsistent between vortices. Here superconductivity is reported in monolayer (ML) FeTe1–ySey(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. -
more » « less
Abstract Chirality and polarity are the two most important and representative symmetry‐dependent properties. For polar structures, all the twofold axes perpendicular to the principal axis of symmetry should be removed. For chiral structures, all the mirror‐related symmetries and inversion axes should be removed. Especially for duality (polarity and chirality), all of the above symmetries should be broken and that also represents the highest‐level challenge. Herein, a new symmetry‐breaking strategy that employs heteroanionic groups to construct hourglass‐like [Sr3OGeS3]2+and [Sr3SGeS3]2+groups to design and synthesize a new oxychalcogenide Sr18Ge9O5S31with chiral‐polar duality is proposed. The presence of two enantiomers of Sr18Ge9O5S31is confirmed by the single‐crystal X‐ray diffraction. Its optical activity and ferroelectricity are also studied by solid‐state circular dichroism spectroscopy and piezoresponse force microscopy, respectively. Further property measurements show that Sr18Ge9O5S31possesses excellent nonlinear optical properties, including the strong second harmonic generation efficiency (≈2.5 × AGS), large bandgap (3.61 eV), and wide mid‐infrared transparent region (≈15.3 µm). These indicate that the unique microstructure groups of heteroanionic materials are conducive to realizing symmetry‐breaking and are able to provide some inspiration for exploring the chiral‐polar duality materials.
-
more » « less
Abstract We have investigated the collective electronic and magnetic orderings of a series of La1−
x Srx MnO3thin films grown epitaxially strained to (001) oriented strontium titanate substrates as a function of doping,x , for 0 ≤x ≤ 0.4. We find that the ground states of these crystalline thin films are, in general, consistent with that observed in bulk crystals and thin film samples synthesized under a multitude of techniques. Our systematic study, however, reveal subtle features in the temperature dependent electronic transport and magnetization measurements, which presumably arise due to Jahn-Teller type distortions in the lattice for particular doping levels. For the parent compound LaMnO3(x = 0), we report evidence of a strain-induced ferromagnetic ordering in contrast to the antiferromagnetic ground state found in bulk crystals. -
more » « less
Abstract This work characterizes the structural, magnetic, and ferroelectric properties of epitaxial LuFeO3orthoferrite thin films with different Lu/Fe ratios. LuFeO3thin films are grown by pulsed laser deposition on SrTiO3substrates with Lu/Fe ratio ranging from 0.6 to 1.5. LuFeO3is antiferromagnetic with a weak canted moment perpendicular to the film plane. Piezoresponse force microscopy imaging and switching spectroscopy reveal room temperature ferroelectricity in Lu‐rich and Fe‐rich films, whereas the stoichiometric film shows little polarization. Ferroelectricity in Lu‐rich films is present for a range of deposition conditions and crystallographic orientations. Positive‐up‐negative‐down ferroelectric measurements on a Lu‐rich film yield ≈13 µC cm−2of switchable polarization, although the film also shows electrical leakage. The ferroelectric response is attributed to antisite defects analogous to that of Y‐rich YFeO3, yielding multiferroicity via defect engineering in a rare earth orthoferrite.
