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Antimony selenide (Sb2Se3) has sparked significant interest in high-efficiency photovoltaic applications due to its advantageous material and optoelectronic properties. In recent years, there has been considerable development in this area. Nonetheless, defects and suboptimal [hk0] crystal orientation expressively limit further device efficiency enhancement. This study used Zinc (Zn) to adjust the interfacial energy band and strengthen carrier transport. For the first time, it is discovered that the diffusion of Zn in the cadmium sulfide (CdS) buffer layer can affect the crystalline orientation of the Sb2Se3 thin films in the superstrate structure. The effect of Zn diffusion on the morphology of Sb2Se3 thin films with CdxZn1-xS buffer layer has been investigated in detail. Additionally, Zn doping promotes forming Sb2Se3 thin films with the desired [hk1] orientation, resulting in denser and larger grain sizes which will eventually regulate the defect density. Finally, based on the energy band structure and high-quality Sb2Se3 thin films, this study achieves a champion power conversion efficiency (PCE) of 8.76%, with a VOC of 458 mV, a JSC of 28.13 mA cm-2, and an FF of 67.85%. Overall, this study explores the growth mechanism of Sb2Se3 thin films, which can lead to further improvements in the efficiency of Sb2Se3 solar cells.
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Antimony selenide (Sb2 Se3 ) is a highly promising photovoltaic material thanks to its outstanding optoelectronic properties, as well as its cost-effective and eco-friendly merits. However, toxic CdS is widely used as an electron transport layer (ETL) in efficient Sb2 Se3 solar cells, which largely limit their development toward market commercialization. Herein, an effective green Cd-free ETL of SnOx is introduced and deposited by atomic layer deposition method. Additionally, an important post-annealing treatment is designed to further optimize the functional layers and the heterojunction interface properties. Such engineering strategy can optimize SnOx ETL with higher nano-crystallinity, higher carrier density, and less defect groups, modify Sb2 Se3 /SnOx heterojunction with better interface performance and much desirable "spike-like" band alignment, and also improve the Sb2 Se3 light absorber layer quality with passivated bulk defects and prolonged carrier lifetime, and therefore to enhance carrier separation and transport while suppressing non-radiative recombination. Finally, the as-fabricated Cd-free Mo/Sb2 Se3 /SnOx /ITO/Ag thin-film solar cell exhibits a stimulating efficiency of 7.39%, contributing a record value for Cd-free substrate structured Sb2 Se3 solar cells reported to date. This work provides a viable strategy for developing and broadening practical applications of environmental-friendly Sb2 Se3 photovoltaic devices.
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Antimony selenide (Sb2Se3) is a promising semiconductor for photodetector applications due to its unique photovoltaic properties. Achieving optimal carrier transport in (001)-Sb2Se3 by the material of contacting substrate requires in-depth study. In this paper, the induced growth of Sb2Se3 films from (hk0) to (hk1) planes is achieved on digenite (Cu9S5) films by post-annealing treatment. The flake-like and flower-like morphologies on the surface of Sb2Se3 films are caused by different thicknesses of the Cu9S5 films, which are related to the (hk0) and (hk1) planes of Sb2Se3 surface. The epitaxial growth of Sb2Se3 films on (105)-Cu9S5 surfaces exhibits thickness dependence. The results inform research into the controlled induced growth of low-dimensional materials. The device of Sb2Se3/Cu9S5/Si has good broadband response (visible to near-infrared), self-powered characteristics, and stability. As the crystalline quality of the Sb2Se3 film increases along the (hk1) plane, the carrier transport is enhanced correspondingly. Under the 980 nm light irradiation, the device has an excellent switching ratio of 2 × 104 at 0 bias, with responsivity, detectivity, and response time up to 17 µA W-1, 1.48 × 107 Jones, and 355/490 µs, respectively. This suggests that Sb2Se3 is suitable for self-powered photodetectors and related optical and optoelectronic devices.
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Short-wavelength infrared photodetectors play a significant role in various fields such as autonomous driving, military security, and biological medicine. However, state-of-the-art short-wavelength infrared photodetectors, such as InGaAs, require high-temperature fabrication and heterogenous integration with complementary metal-oxide-semiconductor (CMOS) readout circuits (ROIC), resulting in a high cost and low imaging resolution. Herein, for the first time, a low-cost, high-performance, high-stable, and thin-film transistor (TFT) ROIC monolithic-integrated (Bi,Sb)2 Se3 alloy thin-film short-wavelength infrared photodetector is reported. The (Bi,Sb)2 Se3 alloy thin-film short-wavelength infrared photodetectors demonstrate a high external quantum efficiency (EQE) of 21.1% (light intensity of 0.76 µW cm-2 ) and a fast response time (3.24 µs). The highest EQE is about two magnitudes than that of the extrinsic photoconduction of Sb2 Se3 (0.051%). In addition, the unpackaged devices demonstrate high electric and thermal stability (almost no attenuation at 120 °C for 312 h), showing potential for in-vehicle applications that may experient such a high temperature. Finally, both the (Bi,Sb)2 Se3 alloy thin film and n-type CdSe buffer layer are directly deposited on the TFT ROIC (with a 64 × 64-pixel array) with a low-temperature process and the material identification and imaging applications are presented. This work is a significant breakthrough in ROIC monolithic-integrated short-wavelength infrared imaging chips.
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Ammonia (NH3 ) is recognized as a transportable carrier for renewable energy fuels. Photoelectrochemical nitrate reduction reaction (PEC NO3 RR) offers a sustainable solution for nitrate-rich wastewater treatment by directly converting solar energy to ammonia. In this study, we demonstrate the highly selective PEC ammonia production from NO3 RR by constructing a CoCu/TiO2 /Sb2 Se3 photocathode. The constructed CoCu/TiO2 /Sb2 Se3 photocathode achieves an ammonia Faraday efficiency (FE) of 88.01 % at -0.2â VRHE and an ammonia yield as high as 15.91â µmol h-1 cm-2 at -0.3â VRHE with an excellent onset potential of 0.43â VRHE . Dynamics experiments and theoretical calculations have demonstrated that the CoCu/TiO2 /Sb2 Se3 photocathode possesses high light absorption capacity, excellent carrier transfer capability, and high charge separation and transfer efficiencies. The photocathode can effectively adsorb the reactant NO3 - and intermediate, and the CoCu co-catalyst increases the maximum Gibbs free energy difference between NO3 RR and HER. Meanwhile, the Co species enhances the spin density of Cu, and increases the density of states near the Fermi level in pdos, which results in a high PEC NO3 RR activity on CoCu/TiO2 /Sb2 Se3 . This work provides a new avenue for the feasibility of efficient PEC ammonia synthesis from nitrate-rich wastewater.
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Copper-doped antimony selenide (Cu-doped Sb2Se3) thin films were deposited as absorber layers in photovoltaic solar cells using the low-temperature pulsed electron deposition (LT-PED) technique, starting from Sb2Se3 targets where part of the Sb was replaced with Cu. From a crystalline point of view, the best results were achieved for thin films with about Sb1.75Cu0.25Se3 composition. In order to compare the results with those previously obtained on undoped thin films, Cu-doped Sb2Se3 films were deposited both on Mo- and Fluorine-doped Tin Oxide (FTO) substrates, which have different influences on the film crystallization and grain orientation. From the current-voltage analysis it was determined that the introduction of Cu in the Sb2Se3 absorber enhanced the open circuit voltage (VOC) up to remarkable values higher than 500 mV, while the free carrier density became two orders of magnitude higher than in pure Sb2Se3-based solar cells.
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As a promising candidate for large-scale energy storage, sodium-ion batteries (SIBs) have superiority due to their low cost and abundance as a resource. Herein, homogeneous Sb2 Se3 nanocrystallites embedded in carbon nanofibers (Sb2 Se3 /CNFs) by electrospinning and selenization treatment are prepared. The obtained Sb2 Se3 /CNFs exhibit good cycling performance, high reversible capacity, and excellent rate capability as anodes for SIBs. The outstanding performances are attributed to a combination of Na+ intercalation, conversion reaction, and alloying with Sb2 Se3 , disclosed through in-situ X-ray diffraction. Meanwhile, unique nanostructures provide large contact surface and tolerant accommodation to volume expansion which bring high reversibility and long cycle durability. This distinctive material shows prospective applications of SIBs especially under high current density.
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It was believed that the Se-rich synthesis condition can suppress the formation of deep-level donor defect VSe (selenium vacancy) in Sb2 Se3 and is thus critical for fabricating high-efficiency Sb2 Se3 solar cells. However, here it is shown that by first-principles calculations the density of VSe increases unexpectedly to 1016 cm-3 when the Se chemical potential increases, so Se-rich condition promotes rather than suppresses the formation of VSe . Therefore, high density of VSe is thermodynamically inevitable, no matter under Se-poor or Se-rich conditions. This abnormal behavior can be explained by a physical concept "defect-correlation", i.e., when donor and acceptor defects compensate each other, all defects become correlated with each other due to the formation energy dependence on Fermi level which is determined by densities of all ionized defects. In quasi-1D Sb2 Se3 , there are many defects and the complicated defect-correlation can give rise to abnormal behaviors, e.g., lowering Fermi level and thus decreasing the formation energy of ionized donor VSe 2+ in Se-rich Sb2 Se3 . Such behavior exists also in Sb2 S3 . It explains the recent experiments that the extremely Se-rich condition causes the efficiency drop of Sb2 Se3 solar cells, and demonstrates that the common chemical intuition and defect engineering strategies may be invalid in compensated semiconductors.
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Low-dimensional semiconductors have attracted considerable attention due to their unique structures and remarkable properties, which makes them promising materials for a wide range of applications related to electronics and optoelectronics. Herein, the preparation of 1D Sb2 Se3 nanowires (NWs) with high crystal quality via chemical vapor deposition growth is reported. The obtained Sb2 Se3 NWs have triangular prism morphology with aspect ratio range from 2 to 200, and three primary lattice orientations can be achieved on the sixfold symmetry mica substrate. Angle-resolved polarized Raman spectroscopy measurement reveals strong anisotropic properties of the Sb2 Se3 NWs, which is also developed to identify its crystal orientation. Furthermore, photodetectors based on Sb2 Se3 NW exhibit a wide spectral photoresponse range from visible to NIR (400-900 nm). Owing to the high crystallinity of Sb2 Se3 NW, the photodetector acquires a photocurrent on/off ratio of about 405, a responsivity of 5100 mA W-1 , and fast rise and fall times of about 32 and 5 ms, respectively. Additionally, owing to the anisotropic structure of Sb2 Se3 NW, the device exhibits polarization-dependent photoresponse. The high crystallinity and superior anisotropy of Sb2 Se3 NW, combined with controllable preparation endows it with great potential for constructing multifunctional optoelectronic devices.
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Antimony-based electrode materials with high specific capacity have aroused considerable interest as anode materials for sodium-ion batteries (SIBs). Herein, we develop a template-engaged ion-exchange method to synthesize Sb2 Se3 microclips, and the as-obtained Sb2 Se3 microclips are further inâ situ coated with polypyrrole (PPy). Benefiting from the structural and compositional merits, these PPy-coated Sb2 Se3 microclips exhibit enhanced sodium-storage properties in terms of high reversible capacity, superior rate capability, and stable cycling performance.
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The unique 1D crystal structure of Antimony Triselenide (Sb2Se3) offers notable potential for use in flexible, lightweight devices due to its excellent bending characteristics. However, fabricating high-efficiency flexible Sb2Se3 solar cells is challenging, primarily due to the suboptimal contact interface between the embedded Sb2Se3 layer and the molybdenum back-contact, compounded by complex intrinsic defects. This study introduces a novel Molybdenum Trioxide (MoO3) interlayer to address the back contact interface issues in flexible Sb2Se3 devices. Further investigations indicate that incorporating a MoO3 interlayer not only enhances the crystalline quality but also promotes a favorable [hk1] growth orientation in the Sb2Se3 absorber layer. It also reduces the barrier height at the back contact interface and effectively passivates harmful defects. As a result, the flexible Sb2Se3 solar cell, featuring a Mo-foil/Mo/MoO3/Sb2Se3/CdS/ITO/Ag substrate structure, demonstrates exceptional flexibility and durability, enduring large bending radii and multiple bending cycles while achieving an impressive efficiency of 8.23%. This research offers a straightforward approach to enhancing the performance of flexible Sb2Se3 devices, thereby expanding their application scope in the field of photovoltaics.
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Photodetectors (PDs) rapidly capture optical signals and convert them into electrical signals, making them indispensable in a variety of applications including imaging, optical communication, remote sensing, and biological detection. Recently, antimony selenide (Sb2Se3) has achieved remarkable progress due to its earth-abundant, low toxicity, low price, suitable bandgap width, high absorption coefficient, and unique structural characteristics. Sb2Se3 has been extensively studied in solar cells, but there's a lack of timely updates in the field of PDs. A literature review based on Sb2Se3 PDs is urgently warranted. This review aims to provide a concise understanding of the latest progress in Sb2Se3 PDs, with a focus on the basic characteristics and the performance optimization for Sb2Se3 photoconductive-type and photodiode-type detectors, including nanostructure regulation, process optimization, and stability improvement of flexible devices. Furthermore, the application progresses of Sb2Se3 PDs in heart rate monitoring, and monolithic-integrated matrix images are introduced. Finally, this review presents various strategies with potential and feasibility to address challenges for the rapid development and commercial application of Sb2Se3 PDs.
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Sb2 Se3 solar cells deposited by rapid thermal evaporation (RTE) have drawn extensive attention owing to their compatibility with the commercial production line of CdTe solar cells and can be used to fabricate high-quality Sb2 Se3 films with high reproducibility. However, the deposition pressure during the RTE process has not been clearly explored, although it has a significant effect on the Sb2 Se3 film quality. A novel two-step deposition strategy is proposed that finely regulates the deposition pressure to improve the quality of Sb2 Se3 absorber layers, thereby improving the device performance of Sb2 Se3 solar cells. This novel method includes a rapid deposition process under a low pressure (5 mTorr) and an in situ annealing process under a relatively high pressure (200 Torr). The maximum power conversion efficiency (PCE) of Sb2 Se3 solar cells fabricated by two-step deposited approach is up to 8.12%. The PCE enhancement is attributed to the increased grain size, reduced grain boundaries, modified surface Fermi level gradient of the absorber layer, and improved defect performance. This innovative deposition technique is expected to benefit other low-melting-point metal sulfoselenides for solar cell applications.
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Antimony selenide (Sb2Se3) consists of 1D (Sb4Se6)n ribbons, along which the carriers exhibit high transport efficiency. By adjusting the deposition parameters of vacuum-deposited methods, such as evaporation temperature, chamber pressure, and vapor concentration, it is possible to grow the (Sb4Se6)n ribbons vertically or highly inclined towards the substrate, resulting in films with [hk1] orientation. However, the specific mechanisms by which these deposition parameters affect the orientation of thin films require a deeper understanding. Herein, a molecular beam epitaxy technique is developed for the preparation of highly [hk1]-oriented Sb2Se3 films, and the effect of evaporation parameters on the film orientation is investigated. It is found that the evaporation temperature can affect the decomposition degree of Sb2Se3, which in turn determines the vapor composition and film orientation. Additionally, the decomposition of Sb2Se3 related to evaporation temperature leads to significant changes in the elemental composition of the film, thereby passivating deep-level defects under Se-rich conditions. Consequently, the Sb2Se3 films with highly [hk1] orientation achieve a power conversion efficiency of 8.42% for the solar cells. This study provides new insights into the control of orientation in antimony-based chalcogenide films and points out new directions for improving the photovoltaic performance of solar cells.
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The photogenerated charge carrier separation and transportation of inside photocathodes can greatly influence the performance of photoelectrochemical (PEC) H2 production devices. Coupling TiO2 with p-type semiconductors to construct heterojunction structures is one of the most widely used strategies to facilitate charge separation and transportation. However, the band position of TiO2 could not perfectly match with all p-type semiconductors. Here, taking antimony selenide (Sb2Se3) as an example, a rational strategy was developed by introducing a viologen electron transfer mediator (ETM) containing polymeric film (poly-1,1'-dially-[4,4'-bipyridine]-1,1'-diium, denoted as PV2+) at the interface between Sb2Se3 and TiO2 to regulate the energy band alignment, which could inhibit the recombination of photogenerated charge carriers of interfaces. With Pt as a catalyst, the constructed Sb2Se3/PV2+/TiO2/Pt photocathode showed a superior PEC hydrogen generation activity with a photocurrent density of -18.6 mA cm-2 vs. a reversible hydrogen electrode (RHE) and a half-cell solar-to-hydrogen efficiency (HC-STH) of 1.54% at 0.17 V vs. RHE, which was much better than that of the related Sb2Se3/TiO2/Pt photocathode without PV2+ (-9.8 mA cm-2, 0.51% at 0.10 V vs. RHE).
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Optical logic devices are essential functional devices for achieving optical signal processing. In this study, we design an ultra-compact (4.92 × 2.52 µm2) reconfigurable optical logic gate by using inverse design method with DBS algorithm based on Sb2Se3-SOI integrated platform. By selecting different amorphous/crystalline distributions of Sb2Se3 via programmable electrical triggers, the designed structure can switch between OR, XOR, NOT or AND logic gate. This structure works well for all four logic functions in the wavelength range of 1540-1560 nm. Especially at the wavelength of 1550 nm, the Contrast Ratios for XOR, NOT and AND logic gate are 13.77 dB, 11.69 dB and 3.01 dB, respectively, indicating good logical judgment ability of the device. Our design is robust to a certain range of fabrication imperfections. Even if performance weakens due to deviations, improvements can be obtained by rearranging the configurations of Sb2Se3 without reproducing the whole device.
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Interfacial regions play a key role in determining the overall power conversion efficiency of thin film solar cells. However, the nanoscale investigation of thin film interfaces using conventional analytical tools is challenging due to a lack of required sensitivity and spatial resolution. Here, we surmount these obstacles using tip-enhanced Raman spectroscopy (TERS) and apply it to investigate the absorber (Sb2Se3) and buffer (CdS) layers interface in a Sb2Se3-based thin film solar cell. Hyperspectral TERS imaging with 10 nm spatial resolution reveals that the investigated interface between the absorber and buffer layers is far from uniform, as TERS analysis detects an intermixing of chemical compounds instead of a sharp demarcation between the CdS and Sb2Se3 layers. Intriguingly, this interface, comprising both Sb2Se3 and CdS compounds, exhibits an unexpectedly large thickness of 295 ± 70 nm attributable to the roughness of the Sb2Se3 layer. Furthermore, TERS measurements provide compelling evidence of CdS penetration into the Sb2Se3 layer, likely resulting from unwanted reactions on the absorber surface during chemical bath deposition. Notably, the coexistence of ZnO, which serves as the uppermost conducting layer, and CdS within the Sb2Se3-rich region has been experimentally confirmed for the first time. This study underscores TERS as a promising nanoscale technique to investigate thin film inorganic solar cell interfaces, offering novel insights into intricate interface structures and compound intermixing.
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Antimony triselenide (Sb2 Se3 ) has possessed excellent optoelectronic properties and has gained interest as a light-harvesting material for photovoltaic technology over the past several years. However, the severe interfacial and bulk recombination obviously contribute to significant carrier transport loss thus leading to the deterioration of power conversion efficiency (PCE). In this work, buried interface and heterojunction engineering are synergistically employed to regulate the film growth kinetic and optimize the band alignment. Through this approach, the orientation of the precursor films is successfully controlled, promoting the preferred orientational growth of the (hk1) of the Sb2 Se3 films. Besides, interfacial trap-assisted nonradiative recombination loss and heterojunction band alignment are successfully minimized and optimized. As a result, the champion device presents a PCE of 9.24% with short-circuit density (JSC ) and fill factor (FF) of 29.47 mA cm-2 and 63.65%, respectively, representing the highest efficiency in sputtered-derived Sb2 Se3 solar cells. This work provides an insightful prescription for fabricating high-quality Sb2 Se3 thin film and enhancing the performance of Sb2 Se3 solar cells.
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Atomic layer deposition (ALD) is an effective technique for depositing thin films with precise control of layer thickness and functional properties. In this work, Sb2Te3-Sb2Se3 nanostructures were synthesized using thermal ALD. A decrease in the Sb2Te3 layer thickness led to the emergence of distinct peaks from the Laue rings, indicative of a highly textured film structure with optimized crystallinity. Density functional theory simulations revealed that carrier redistribution occurs at the interface to establish charge equilibrium. By carefully optimizing the layer thicknesses, we achieved an obvious enhancement in the Seebeck coefficient, reaching a peak figure of merit (zT) value of 0.38 at room temperature. These investigations not only provide strong evidence for the potential of ALD manipulation to improve the electrical performance of metal chalcogenides but also offer valuable insights into achieving high performance in two-dimensional materials.
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The development of imaging technology and optical communication demands a photodetector with high responsiveness. As demonstrated by microfabrication and nanofabrication technology advancements, recent progress in plasmonic sensor technologies can address this need. However, these photodetectors have low optical absorption and ineffective charge carrier transport efficiency. Sb2Se3 is light-sensitive material with a high absorption coefficient, making it suitable for photodetector applications. We developed an efficient, scalable, low-cost near-infrared (NIR) photodetector based on a nanostructured Sb2Se3 film deposited on p-type micropyramidal Si (made via the wet chemical etching process), working on photoconductive phenomena. Our results proved that, at the optimized thickness of the Sb2Se3 layer, the proposed Si micropyramidal substrate enhanced the responsivity nearly two times, compared with that of the Sb2Se3 deposited on a flat Si reference sample and a glass/Sb2Se3 sample at 1064 nm (power density = 15 mW/cm2). More interestingly, the micropyramidal silicon-based device worked at 0 V bias, paving a path for self-bias devices. The highest specific detectivity of 2.25 × 1015 Jones was achieved at 15 mW/cm2 power density at a bias voltage of 0.5 V. It is demonstrated that the enhanced responsivity was closely linked with field enhancement due to the Kretschmann configuration of Si pyramids, which acts as hot spots for Si/Sb2Se3 junction. A high responsivity of 47.8 A W-1 proved it suitable for scalable and cost-effective plasmonic-based NIR photodetectors.