Multilevel Conductance States of Vapor-Transport-Deposited Sb2S3 Memristors Achieved via Electrical and Optical Modulation.

The pursuit of advanced brain-inspired electronic devices and memory technologies has led to explore novel materials by processing multimodal and multilevel tailored conductive properties as the next generation of semiconductor platforms, due to von Neumann architecture limits. Among such materials, antimony sulfide (Sb2S3) thin films exhibit outstanding optical and electronic properties, and therefore, they are ideal for applications such as thin-film solar cells and nonvolatile memory systems. This study investigates the conduction modulation and memory functionalities of Sb2S3 thin films deposited via the vapor transport deposition technique. Experimental results indicate that the Ag/Sb2S3/Pt device possesses properties suitable for memory applications, including low operational voltages, robust endurance, and reliable switching behavior. Further, the reproducibility and stability of these properties across different device batches validate the reliability of these devices for practical implementation. Moreover, Sb2S3-based memristors exhibit artificial neuroplasticity with prolonged stability, promising considerable advancements in neuromorphic computing. Leveraging the photosensitivity of Sb2S3 enables the Ag/Sb2S3/Pt device to exhibit significant low operating potential and conductivity modulation under optical stimulation for memory applications. This research highlights the potential applications of Sb2S3 in future memory devices and optoelectronics and in shaping electronics with versatility.

Scanning Tunneling Spectroscopy Method for the Prediction of Semiconductor Heterojunction Performance as a Prequel for Device Development.

The prediction of semiconductor device performance is a persistent challenge in materials science, and the ability to anticipate useful specifications prior to construction is crucial for enhancing the overall efficiency. In this study, we investigate the constituents of a solar cell by employing scanning tunneling microscopy (STM) and spectroscopy (STS). Through our observations, we identify a spatial distribution of the dopant type in thin films of materials that were designed to present major p-doping for germanium sulfide (GeS) and dominant n-doping for tin disulfide (SnS2). By generating separate STS maps for each semiconductor film and conducting a statistical analysis of the gap and doping distribution, we determine intrinsic limitations for the solar cell efficiency that must be understood prior to processing. Subsequently, we fabricate a solar cell utilizing these materials (GeS and SnS2) via vapor phase deposition and carry out a characterization using standard J-V curves under both dark/illuminated irradiance conditions. Our devices corroborate the expected reduced efficiency due to doping fluctuation but exhibit stable photocurrent responses. As originally planned, quantum efficiency measurements reveal that the peak efficiency of our solar cell coincides with the range where the standard silicon solar cells sharply decline. Our STS method is suggested as a prequel to device development in novel material junctions or deposition processes where fluctuations of doping levels are retrieved due to intrinsic material characteristics such as the occurrence of defects, roughness, local chemical segregation, and faceting or step bunching.

Substrate Morphology Directs (001) Sb2 Se3 Thin Film Growth by Crystallographic Orientation Filtering.

Antimony chalcogenide, Sb2 X3 (X = S, Se), applications greatly benefit from efficient charge transport along covalently bonded (001) oriented (Sb4 X6 )n ribbons, making thin film orientation control highly desirable - although particularly hard to achieve experimentally. Here, it is shown for the first time that substrate nanostructure plays a key role in driving the growth of (001) oriented antimony chalcogenide thin films. Vapor Transport Deposition of Sb2 Se3 thin films is conducted on ZnO substrates whose morphology is tuned between highly nanostructured and flat. The extent of Sb2 Se3 (001) orientation is directly correlated to the degree of substrate nanostructure. These data showcase that nanostructuring a substrate is an effective tool to control the orientation and morphology of Sb2 Se3 films. The optimized samples demonstrate high (001) crystallographic orientation. A growth mechanism for these films is proposed, wherein the substrate physically restricts the development of undesirable crystallographic orientations. It is shown that the surface chemistry of the nanostructured substrates can be altered and still drive the growth of (001) Sb2 Se3 thin films - not limiting this phenomenon to a particular substrate type. Insights from this work are expected to guide the rational design of Sb2 X3 thin film devices and other low-dimensional crystal-structured materials wherein performance is intrinsically linked to morphology and orientation.

HTL-Free Sb2(S, Se)3 Solar Cells with an Optimal Detailed Balance Band Gap.

Antimony chalcogenides are widely studied as a light-absorbing material due to their merits of low toxicity, efficient cost, and excellent photovoltaic properties. However, the band gaps of antimony selenide (approximately 1.1 eV) and antimony sulfide (approximately 1.7 eV) both deviate from the optimal detailed balance band gap (∼1.3 eV) for terrestrial single-junction solar cells. Notably, the band gap of Sb2(S, Se)3 can be tunable in the range from 1.1 to 1.7 eV, which can cover the detailed balance band gap. In this work, the vapor transport deposition method with two independent evaporation sources is used to deposit Sb2(S, Se)3 thin films. By carefully optimizing the evaporation temperature and the start evaporation time of the Sb2Se3 and Sb2S3 sources, a suitable band gap of 1.33 eV is obtained. Finally, on the basis of the optimal Sb2(S, Se)3 films, Sb2(S, Se)3 solar cells without a hole transport layer achieved an efficiency of 7.03%.

High-Crystallinity Epitaxial Sb2Se3 Thin Films on Mica for Flexible Near-Infrared Photodetectors.

The V-VI binary chalcogenide, Sb2Se3, has attracted considerable attention for its applications in thin film optoelectronic devices because of its unique 1D structure and remarkable optoelectronic properties. Herein, we report an Sb2Se3 thin film epitaxially grown on a flexible mica substrate through a relatively weak (van der Waals) interaction by vapor transport deposition. The epitaxial Sb2Se3 thin films exhibit a single (120) out-of-plane orientation and a 0.25° full width at half-maximum of (120) rocking curve in X-ray diffraction, confirming the high crystallinity of the epitaxial films. The Sb2Se3(120) plane is epitaxially aligned on mica(001) surface with the in-plane relationship of Sb2Se3[2̅10]//mica[010] and Sb2Se3[001]//mica[100]. Compared to the photodetector made of a nonepitaxial Sb2Se3 film, the photocurrent of the epitaxial Sb2Se3 film photodetector is almost doubled. Furthermore, because of the flexibility and high sensitivity of the epitaxial Sb2Se3 film photodetector on mica, it has been successfully employed to detect the heart rate of a person. These encouraging results will facilitate the development of epitaxial Sb2Se3 film-based devices and potential applications in wearable electronics.

Quasi-Vertically-Orientated Antimony Sulfide Inorganic Thin-Film Solar Cells Achieved by Vapor Transport Deposition.

The one-dimensional photovoltaic absorber material Sb2S3 requires crystal orientation engineering to enable efficient carrier transport. In this work, we adopted the vapor transport deposition (VTD) method to fabricate vertically aligned Sb2S3 on a CdS buffer layer. Our work shows that such a preferential vertical orientation arises from the sulfur deficit of the CdS surface, which creates a beneficial bonding environment between exposed Cd2+ dangling bonds and S atoms in the Sb2S3 molecules. The CdS/VTD-Sb2S3 interface recombination is suppressed by such properly aligned ribbons at the interface. Compared to typical [120]-oriented Sb2S3 films deposited on CdS by the rapid thermal evaporation (RTE) method, the VTD-Sb2S3 thin film is highly [211]- and [121]-oriented and the performance of the solar cell is increased considerably. Without using any hole transportation layer, a conversion efficiency of 4.73% is achieved with device structure of indium tin oxide (ITO)/CdS/Sb2S3/Au. This work provides a potential way to obtain vertically aligned thin films on different buffer layers.