Solid-phase heteroepitaxy of oriented Sb2Se3 on GaAs for birefringent thin films
We investigate the amorphous-to-crystalline transformation of antimony selenide (Sb2Se3) on UHV-prepared GaAs (001) substrates. In the bulk orthorhombic form, Sb2Se3 is a layered quasi-1D semiconductor with highly anisotropic properties of interest for optical and electronic devices. We find that an amorphous layer deposited by molecular beam epitaxy annealed at or above 230 °C yields a textured-epitaxial structure among some randomly oriented domains. The textured-epitaxial Sb2Se3 grains are oriented with the covalently bonded “1D axis” constrained in-plane to GaAs [110] and with multiple van der Waals (hk0) orientations out-of-plane. The same texture was achieved exclusively without randomly oriented grains using continuous-wave laser radiation, highlighting the use of thermal and optical methods to yield anisotropic crystalline Sb2Se3 films directly from the amorphous phase. Polarized reflectance and polarized microscopy confirm the unique state of in-plane birefringence in the crystallized thin film. Overall, we show that solid-phase heteroepitaxy provides additional pathways to the integration of low-symmetry chalcogenide semiconductors for demanding applications where the inherent anisotropy needs to be preserved.
more »
« less
- Award ID(s):
- 2036520
- PAR ID:
- 10672305
- Publisher / Repository:
- AVS
- Date Published:
- Journal Name:
- Journal of Vacuum Science & Technology A
- Volume:
- 44
- Issue:
- 2
- ISSN:
- 0734-2101
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
Beta-phase gallium oxide ([Formula: see text]-Ga 2 O 3 ) is a promising semiconductor for high frequency, high temperature, and high voltage applications. In addition to the [Formula: see text]-phase, numerous other polymorphs exist and understanding the competition between phases is critical to control practical devices. The phase formation sequence of Ga 2 O 3 , starting from amorphous thin films, was determined using lateral-gradient laser spike annealing at peak temperatures of 500–1400 °C on 400 μs to 10 ms timescales, with transformations characterized by optical microscopy, x-ray diffraction, and transmission electron microscopy (TEM). The resulting phase processing map showed the [Formula: see text]-phase, a defect-spinel structure, first nucleating under all annealing times for temperatures from 650 to 800 °C. The cross-sectional TEM at the onset of the [Formula: see text]-phase formation showed nucleation near the film center with no evidence of heterogeneous nucleation at the interfaces. For temperatures above 850 °C, the thermodynamically stable [Formula: see text]-phase was observed. For anneals of 1–4 ms and temperatures below 1200 °C, small randomly oriented grains were observed. Large grains were observed for anneals below 1 ms and above 1200 °C, with anneals above 4 ms and 1200 °C resulting in textured films. The formation of the [Formula: see text]-phase prior to [Formula: see text]-phase, coupled with the observed grain structure, suggests that the [Formula: see text]-phase is kinetically preferred during thermal annealing of amorphous films, with [Formula: see text]-phase subsequently forming by nucleation at higher temperatures. The low surface energy of the [Formula: see text]-phase implied by these results suggests an explanation for the widely observed [Formula: see text]-phase inclusions in [Formula: see text]-phase Ga 2 O 3 films grown by a variety of synthesis methods.more » « less
-
Flexible electronics and mechanically bendable devices based on Group III-N semiconductor materials are emerging; however, there are several challenges in manufacturing, such as cost reduction, device stability and flexibility, and device-performance improvement. To overcome these limitations, it is necessary to replace the brittle and expensive semiconductor wafers with single-crystalline flexible templates for a new-bandgap semiconductor platform. The substrates in the new concept of semiconductor materials have a hybrid structure consisting of a single-crystalline III-N thin film on a flexible metal tape substrate which provides a convenient and scalable roll-to-roll deposition process. We present a detailed study of a unique and simple direct epitaxial growth technique for crystallinity transformation to deliver single-crystalline GaN thin film with highly oriented grains along both a -axis and c -axis directions on a flexible and polycrystalline copper tape. A 2-dimensional (2D) graphene having the same atomic configuration as the (0001) basal plane of wurtzite structure is employed as a seed layer which plays a key role in following the III-N epitaxy growth. The DC reactive magnetron sputtering method is then applied to deposit an AlN layer under optimized conditions to achieve preferred-orientation growth. Finally, single-crystalline GaN layers (∼1 μm) are epitaxially grown using metal organic chemical vapor deposition (MOCVD) on the biaxially-textured buffer layer. The flexible single-crystalline GaN film obtained using this method provides a new way for a wide-bandgap semiconductor platform pursuing flexible, high-performance, and versatile device technology.more » « less
-
Sb thin films have attracted wide interest due to their tunable band structure, topological phases, high electron mobility, and thermoelectric properties. We successfully grow epitaxial Sb thin films on a closely lattice-matched GaSb(001) surface by molecular beam epitaxy. We find a novel anisotropic directional dependence on their structural, morphological, and electronic properties. The origin of the anisotropic features is elucidated using first-principles density functional theory (DFT) calculations. The growth regime of crystalline and amorphous Sb thin films was determined by mapping the surface reconstruction phase diagram of the GaSb(001) surface under Sb2 flux, with confirmation of structural characterizations. Crystalline Sb thin films show a rhombohedral crystal structure along the rhombohedral (211) surface orientation parallel to the cubic (001) surface orientation of the GaSb substrate. At this coherent interface, Sb atoms are aligned with the GaSb lattice along the [1̄10] crystallographic direction but are not aligned well along the [110] crystallographic direction, which results in anisotropic features in reflection of high-energy electron diffraction patterns, misfit dislocation formation, surface morphology, and transport properties. Our DFT calculations show that the preferential orientation of the rhombohedral Sb (211) plane may originate from the GaSb surface, where Sb atoms align with the Ga and Sb atoms on the reconstructed surface. The formation energy calculations confirm the stability of the experimentally observed structures. Our results provide optimal film growth conditions for further studies of novel properties of Bi1−xSbx thin films with similar lattice parameters and an identical crystal structure, as well as functional heterostructures of them with III–V semiconductor layers along the (001) surface orientation, supported by a theoretical understanding of the anisotropic film orientation.more » « less
-
The antimony selenide (Sb2Se3) thin film solar cells technology become promising due to its excellent anisotropic charge transport and brilliant light absorption capability. Especially, the device performance heavily relies on the vertically oriented Sb2Se3 grain to promote photoexcited carrier transport. However, crystalline orientation control has been a major issue in Sb2Se3 thin film solar cells. In this work, a new strategy has been developed to tailor the crystal growth of Sb2Se3 ribbons perpendicular to the substrate by using the structural heterostructured CdS buffer layer. The heterostructured CdS buffer layer was formed by a dual layer of CdS nanorods and nanoparticles. The hexagonal CdS nanorods passivated by a thin cubic CdS nanoparticle layer can promote [211] and [221] directional growth of Sb2Se3 ribbons using a close space sublimation approach. The improved buffer/absorber interface, reduced interface defects, and recombination loss contribute to the improved device efficiency of 7.16%. This new structural heterostructured CdS buffer layer can regulate Sb2Se3 nanoribbons crystal growth and pave the way to further improve the low-dimensional chalcogenide thin film solar cell efficiency.more » « less
An official website of the United States government

