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Photoelectrochemical water splitting offers a promising approach for carbon neutrality, but its commercial prospects are still hampered by a lack of efficient and stable photoelectrodes with earth-abundant materials. Here, we report a strategy to construct an efficient photoanode with a coaxial nanobelt structure, comprising a buried-ZrS3/ZrOS n-p junction, for photoelectrochemical water splitting. The p-type ZrOS layer, formed on the surface of the n-type ZrS3 nanobelt through a pulsed-ozone-treatment method, acts as a hole collection layer for hole extraction and a protective layer to shield the photoanode from photocorrosion. The resulting ZrS3/ZrOS photoanode exhibits light harvesting with good photo-to-current efficiencies across the whole visible region to over 650 nm. By further employing NiOOH/FeOOH as the oxygen evolution reaction cocatalyst, the ZrS3/ZrOS/NiOOH/FeOOH photoanode yields a photocurrent density of ~9.3 mA cm-2 at 1.23 V versus the reversible hydrogen electrode with an applied bias photon-to-current efficiency of ~3.2% under simulated sunlight irradiation in an alkaline solution (pH = 13.6). The conformal ZrOS layer enables ZrS3/ZrOS/NiOOH/FeOOH photoanode operation over 1000 hours in an alkaline solution without obvious performance degradation. This study, offering a promising approach to fabricate efficient and durable photoelectrodes with earth-abundant materials, advances the frontiers of photoelectrochemical water splitting.
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In this research, the impact of the different zinc (Zn) concentrations on the physical and optoelectronic properties of Bi2S3 nanorods as self-powered and photodiode applications was investigated. The performance of P-N junction photodiodes has been for decades since they are crucial in energy applications. The structure, degree of crystallinity, and shape of Zn-doped Bi2S3 nanorods of various doping percentages formed onto the indium tin oxide (ITO) substrates by the dip coating technique are investigated using X-ray powder diffraction (XRD) and SEM. With increasing illumination time, the current-voltage (I-V) graphs demonstrate a rise in photocurrent. The diode's idealist factor was estimated using the I-V technique under 30 min of light illumination.
Asunto(s)
Bismuto , Nanotubos , Sulfuros , Zinc , Bismuto/química , Zinc/química , Nanotubos/química , Sulfuros/química , Compuestos de Estaño/química , Tamaño de la Partícula , Difracción de Rayos X , LuzRESUMEN
High-performance semiconductor devices capable of multiple functions are pivotal in meeting the challenges of miniaturization and integration in advanced technologies. Despite the inherent difficulties of incorporating dual functionality within a single device, a high-performance, dual-mode device is reported. This device integrates an ultra-thin Al2O3 passivation layer with a PbS/Si hybrid heterojunction, which can simultaneously enable optoelectronic detection and neuromorphic operation. In mode 1, the device efficiently separates photo-generated electron-hole pairs, exhibiting an ultra-wide spectral response from ultraviolet (265 nm) to near-infrared (1650 nm) wavelengths. It also reproduces high-quality images of 256 × 256 pixels, achieving a Q-value as low as 0.00437 µW cm- 2 at a light intensity of 8.58 µW cm- 2. Meanwhile, when in mode 2, the as-assembled device with typical persistent photoconductivity (PPC) behavior can act as a neuromorphic device, which can achieve 96.5% accuracy in classifying standard digits underscoring its efficacy in temporal information processing. It is believed that the present dual-function devices potentially advance the multifunctionality and miniaturization of chips for intelligence applications.
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The photoconductive gain theory demonstrates that the photoconductive gain is related to the ratio of carrier lifetime to carrier transit time. Theoretically, to achieve higher gain, one can either prolong the carrier lifetime or select materials with high mobility to shorten the transit time. However, the former slows the response speed of the device, while the latter increases the dark current and degrades device sensitivity. To address this challenge, a horizontal p-n-p junction-based photoconductor is proposed in this work. This device utilizes the n-region as the charge transport channel, with the charge transport direction perpendicular to the p-n-p junction. This design offers two advantages: (i) the channel is depleted by the space charge layer generated by the p and n regions, enabling the device to maintain a low dark current. (ii) The photovoltage generated in the p-n junction upon light absorption can compress the space charge layer and expand the conductive path in the n-region, enabling the device to achieve high gain and responsivity without relying on long carrier lifetimes. By adopting this device structure design, a balance between responsivity, dark current, and response speed is achieved, offering a new approach to designing high-performance photodetectors based on both traditional materials and emerging nanomaterials.
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Heterostructure engineering offers a powerful approach to creating innovative electrocatalysts. By combining different materials, it can achieve synergistic effects that enhance both charge storage and electrocatalytic activity. In this work, it is capitalized on this concept by designing a 1D/3D CoWO4(OH)2·H2O/molybdenum disulfide (CTH/MoS2) heterostructure. It is achieved this by in situ depositing 3D MoS2 nanoflowers on 1D CTH nanorods. To explore the impact of precursor choice, various sulfur (S) sources is investigated. Interestingly, the S precursor influenced the dimensionality of the MoS2 component. For example, L-cysteine (L-cys), and glutathione (GSH) resulted in 0D morphologies, thiourea (TU) led to a 2D structure, and thioacetamide (TAA) yielded a desirable 3D architecture. Notably, the 1D/3D CTH/MoS2-TAA heterostructure exhibited exceptional performance in both supercapacitors (SCs) and quantum dot-sensitized solar cells (QDSSCs). This achievement can be attributed to several factors: the synergetic effect between 1D CTH and 3D MoS2, improved accessibility due to the multi-dimensional structure, and a tailored electronic structure facilitated by the Mott-Schottky (M-S) interaction arising from the different material Fermi levels. This interaction further enhances conductivity, ultimately leading to the observed high specific capacity in SCs (154.44 mAh g-1 at 3 mA cm-2) and remarkable photovoltaic efficiency in QDSSCs (6.48%).
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The p- or n-type property of semiconductor materials directly determine the final performance of photoelectronic devices. Generally, perovskite deposited on p-type substrate tends to be p-type, while perovskite deposited on n-type substrate tends to be n-type. Motived by this, a substrate-induced re-growth strategy is reported to induce p- to n-transition of perovskite surface in inverted perovskite solar cells (PSCs). p-type perovskite film is obtained and crystallized on p-type substrate first. Then an n-type ITO/SnO2 substrate with saturated perovskite solution is pressed onto the perovskite film and annealed to induce the secondary re-growth of perovskite surface region. As a result, p- to n-type transition happens and induces an extra junction at perovskite surface region, thus enhancing the built-in potential and promoting carrier extraction in PSCs. Resulting inverted PSCs exhibit high efficiency of over 25% with good operational stability, retaining 90% of initial efficiency after maximum power point (MPP) tracking for 800 h at 65 °C with ISOS-L-2 protocol.
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A promising strategy to boost electrocatalytic performance is via assembly of hetero-nanostructured electrocatalysts that delivers the essential specific surface area and also active sites by lowering the reaction barrier. However, the challenges associated with the intricate designs and mechanisms remain underexplored. Therefore, the present study constructs a p-n junction in a free-standing MnCo2O4.5@Ni3S2 on Ni-Foam. The space-charge region's electrical characteristics is dramatically altered by the formed p-n junction, which enhances the electron transfer process for urea-assisted electrocatalytic water splitting (UOR). The optimal MnCo2O4.5@Ni3S2 electrocatalyst results in greater oxygen evolution reactivity (OER) than pure systems, delivering an overpotential of only 240 mV. Remarkably, upon employing as UOR electrode the required potential decreases to 30 mV. The impressive performance of the designed catalyst is attributed to the enhanced electrical conductivity, greater number of electrochemical active sites, and improved redox activity due to the junction interface formed between p-MnCo2O4.5 and n-Ni3S2. There are strong indications that the in situ formed extreme-surface NiOOH, starting from Ni3S2, boosts the electrocatalytic activity, i.e., the electrochemical surface reconstruction generates the active species. In conclusion, this work presents a high-performance p-n junction design for broad use, together with a viable and affordable UOR electrocatalyst.
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Intermolecular charge-transfer (CT) states are extended excitons with a charge separation on the nanometer scale. Through absorption and emission processes, they couple to the ground state. This property is employed both in light-emitting and light-absorbing devices. Their conception often relies on donor-acceptor (D-A) interfaces, so-called type-II heterojunctions, which usually generate significant electric fields. Several recent studies claim that these fields alter the energetic configuration of the CT states at the interface, an idea holding prospects like multicolor emission from a single emissive interface or shifting the absorption characteristics of a photodetector. Here, we test this hypothesis and contribute to the discussion by presenting a new model system. Through the fabrication of planar organic p-(i-)n junctions, we generate an ensemble of oriented CT states that allows the systematic assessment of electric field impacts. By increasing the thickness of the intrinsic layer at the D-A interface from 0 to 20 nm and by applying external voltages up to 6 V, we realize two different scenarios that controllably tune the intrinsic and extrinsic electric interface fields. By this, we obtain significant shifts of the CT-state peak emission of about 0.5 eV (170 nm from red to green color) from the same D-A material combination. This effect can be explained in a classical electrostatic picture, as the interface electric field alters the potential energy of the electric CT-state dipole. This study illustrates that CT-state energies can be tuned significantly if their electric dipoles are aligned to the interface electric field.
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This study involved direct doping of In2O3 into silicon carbide (SiC) powder, resulting in 8.0 at% In-doped SiC powder. Subsequently, heating at 500 °C was performed to form a target, followed by the utilization of electron beam (e-beam) technology to deposit the In-doped SiC thin films with the thickness of approximately 189.8 nm. The first breakthrough of this research was the successful deposition of using e-beam technology. The second breakthrough involved utilizing various tools to analyze the physical and electrical properties of In-doped SiC thin films. Hall effect measurement was used to measure the resistivity, mobility, and carrier concentration and confirm its n-type semiconductor nature. The uniform dispersion of In ions in SiC was as confirmed by electron microscopy energy-dispersive spectroscopy and secondary ion mass spectrometry analyses. The Tauc Plot method was employed to determine the Eg values of pure SiC and In-doped SiC thin films. Semiconductor parameter analyzer was used to measure the conductivity and the I-V characteristics of devices in In-doped SiC thin films. Furthermore, the third finding demonstrated that In2O3-doped SiC thin films exhibited remarkable current density. X-ray photoelectron spectroscopy and Gaussian-resolved spectra further confirmed a significant relationship between conductivity and oxygen vacancy concentration. Lastly, depositing these In-doped SiC thin films onto p-type silicon substrates etched with buffered oxide etchant resulted in the formation of heterojunction p-n junction. This junction exhibited the rectifying characteristics of a diode, with sample current values in the vicinity of 102 mA, breakdown voltage at approximately -5.23 V, and open-circuit voltage around 1.56 V. This underscores the potential of In-doped SiC thin films for various semiconductor devices.
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The removal of antibiotics from aquatic solutions remains a global environmental challenge. In this work, the photocatalytic removal of a typical antibiotic-tetracycline (TC) using hydroxyapatite (HAp) as a catalyst was investigated. It was impressive that TC could be efficiently degraded by HAp under visible light irradiation, even though both HAp and TC exhibited poor harvesting in visible light region. The experimental and theoretical explorations were undertaken to thoroughly investigate the underlying mechanism of visible light degradation of TC over HAp. The results indicated that the formed TC-HAp complexes via surface coordination played an important role as photosensitizers for the visible light response. Together with the formation of a quasi p-n junction via band alignment, the photogenerated electrons in the highest unoccupied molecular orbital (HOMO) of TC-HAp were excited to the lowest unoccupied molecular orbital (LUMO) and subsequently migrated to the conduction band of HAp to achieve the efficient charge separation. Superoxide radicals and holes were found to be the major active species for TC degradation. The toxicity evaluation showed that TC could be transferred to the lower toxic intermediates, and deep oxidation with prolonged reaction time was necessary to eliminate the toxicity of TC. This work demonstrates the surface coordination with subsequent quasi p-n junction mechanism of TC degradation over HAp under visible light, which will stimulate us to explore new efficient photocatalytic systems for the degradation of various contaminants.
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Two-dimensional (2D) materials with atomic-scale thickness are promising candidates to develop next-generation electronic and optoelectronic devices with multiple functions due to their widely tunable physical properties by various stimuli. The surface acoustic wave (SAW) produced at the surface of the piezoelectrical substrate can generate electrical and strain fields simultaneously with micro/nanometer resolution during propagation. It provides a stable and wireless platform to manipulate the rich and fascinating properties of 2D materials. However, the interaction mechanisms between the SAW and 2D materials remain unclear, preventing further development and potential applications of SAW-integrated 2D devices. This work studied the acoustoelectric (AE) charge transport mechanism in 2D materials thoroughly by characterizing the performances of the n-type MoS2 and p-type MoTe2 field effect transistors (FETs) and the MoS2/MoTe2 p-n junction driven by the SAW. As compared to the case driven by the static electrical field alone, the SAW drove the electron and hole transport along the same direction as its propagation, and the generated AE current always had the opposite direction to the AE voltage. In the device level, the 2D FETs showed a significantly reduced subthreshold swing up to around 67% when the SAW was used to drive the channel carriers, indicating that the SAW enhanced the on/off switching speed. Moreover, the MoTe2/MoS2 p-n junction showed a tunable photoresponsivity by the power and propagation direction of the SAW. These findings provide a solid foundation to promote future research and potential applications of SAW-driven multifunctional devices based on 2D materials.
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In recent years, antimony sulfide (Sb2S3) has been investigated as a photovoltaic absorber material due to its suitable absorber coefficient, direct band gap, extinction coefficient, earth-abundant, and environmentally friendly constituents. Therefore, this work proposes Sb2S3 film preparation by an effective two-step process using a new graphite box design and sulfur distribution, which has a high repeatability level and can be scalable. First, an Sb thin film was deposited using the RF-Sputtering technique, and after that, the samples were annealed with elemental sulfur into a graphite box, varying the sulfurization time from 20 to 50 min. The structural, optical, morphological, and chemical characteristics of the resulting thin films were analyzed. Results reveal the method's effectivity and the best properties were obtained for the sample sulfurized during 40 min. This Sb2S3 thin film presents an orthorhombic crystalline structure, elongated grains, a band gap of 1.69 eV, a crystallite size of 15.25 Å, and a nearly stoichiometric composition. In addition, the formation of a p-n junction was achieved by depositing silver back contact on the Glass/FTO/CdS/Sb2S3 structure. Therefore, the graphite box design has been demonstrated to be functional to obtain Sb2S3 by a two-step process.
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As a highly regarded superconducting material with a concise layered structure, MgB2 has attracted significant scientific attention and holds vast potential for applications. However, its limited current-carrying capacity under high magnetic fields has greatly hindered its practical use. To address this issue, we have enhanced the superconducting performance of MgB2 by incorporating inhomogeneous phase nanostructures of p-n junctions with electroluminescent properties. Through temperature-dependent measurements of magnetization, electronic specific heat, and Hall coefficient under various magnetic fields, we have confirmed the crucial role of inhomogeneous phase electroluminescent nanostructures in improving the properties of MgB2. Experimental results demonstrate that the introduction of electroluminescent inhomogeneous phases effectively enhances the superconducting performance of MgB2. Moreover, by controlling the size of the electroluminescent inhomogeneous phases and optimizing grain connectivity, density, and microstructural uniformity, we can further improve the critical temperature (TC) and flux-pinning capability of MgB2 superconducting materials. Comprehensive studies on the physical properties of MgB2 superconducting structures added with p-n junction electroluminescent inhomogeneous phases also confirm the general effectiveness of electroluminescent inhomogeneous phases in enhancing the performance of superconducting materials.
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Heterojunctions in electrode materials offer diverse improvements during the cycling process of energy storage devices, such as volume change buffering, accelerated ion/electron transfer, and better electrode structure integrity, however, obtaining optimal heterostructures with nanoscale domains remains challenging within constrained materials. A novel in situ electrochemical method is introduced to develop a reversible CuSe/PSe p-n heterojunction (CPS-h) from Cu3PSe4 as starting material, targeting maximum stability in potassium ion storage. The CPS-h formation is thermodynamically favorable, characterized by its superior reversibility, minimized diffusion barriers, and enhanced conversion post K+ interaction. Within CPS-h, the synergy of the intrinsic electric field and P-Se bonds enhance electrode stability, effectively countering the Se shuttling phenomenon. The specific orientation between CuSe and PSe leads to a 35° lattice mismatch generates large space at the interface, promoting efficient K ion migration. The Mott-Schottky analysis validates the consistent reversibility of CPS-h, underlining its electrochemical reliability. Notably, CPS-h demonstrates a negligible 0.005% capacity reduction over 10,000 half-cell cycles and remains stable through 2,000 and 4,000 cycles in full cells and hybrid capacitors, respectively. This study emphasizes the pivotal role of electrochemical dynamics in formulating highly stable p-n heterojunctions, representing a significant advancement in potassium-ion battery (PIB) electrode engineering.
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DPC in Scanning Transmission Electron Microscopy (STEM) is a valuable method for mapping the electric fields in semiconductor materials. However, optimising the experimental conditions can be challenging. In this paper, we test and compare critical experimental parameters, including the convergence angle, camera length, acceleration voltage, sample configuration, and orientation using a four-quadrant segmented detector and a Si specimen containing layers of different As concentrations. The DPC measurements show a roughly linear correlation with the estimated electric fields, until the field gets close to the detection limitation, which is â¼0.5 mV/nm with a sample thickness of â¼145 nm. These results can help inform which technique to use for different user cases: When the electric field at a planar junction is above â¼0.5 mV/nm, DPC with a segmented detector is practical for electric field mapping. With a planar junction, the DPC signal-to-noise ratio can be increased by increasing the specimen thickness. However, for semiconductor devices with electric fields smaller than â¼0.5 mV/nm, or for devices containing curved junctions, DPC is unreliable and techniques with higher sensitivity will need to be explored, such as 4D STEM using a pixelated detector.
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Understanding "efficiency roll-off" (i.e., the drop in emission efficiency with increasing current) is critical if efficient and bright emissive technologies are to be rationally designed. Emerging light-emitting electrochemical cells (LECs) can be cost- and energy-efficiently fabricated by ambient-air printing by virtue of the in situ formation of a p-n junction doping structure. However, this in situ doping transformation renders a meaningful efficiency analysis challenging. Herein, a method for separation and quantification of major LEC loss factors, notably the outcoupling efficiency and exciton quenching, is presented. Specifically, the position of the emissive p-n junction in common singlet-exciton emitting LECs is measured to shift markedly with increasing current, and the influence of this shift on the outcoupling efficiency is quantified. It is further verified that the LEC-characteristic high electrochemical-doping concentration renders singlet-polaron quenching (SPQ) significant already at low drive current density, but also that SPQ increases super-linearly with increasing current, because of increasing polaron density in the p-n junction region. This results in that SPQ dominates singlet-singlet quenching for relevant current densities, and significantly contributes to the efficiency roll-off. This method for deciphering the LEC efficiency roll-off can contribute to a rational realization of all-printed LEC devices that are efficient at highluminance.
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We present a novel approach to achieve n-type doping in graphene and create graphene p-n junctions through a photoinduced electron doping method using photobase generators (PBGs). The unique properties of PBGs allow us to spatially and temporally control the doping process via light activation. The selective irradiation of specific regions on the graphene film enables switching their doping from p- to n-type, as confirmed by changes in the electromotive force and Seebeck and Hall coefficients. We demonstrate a stable (over 2 months) high electron mobility exceeding 1000 cm2 V-1s-1 using Hall effect measurements. The precise control of doping and the creation of p-n junctions in graphene offer exciting possibilities for various electronic, optoelectronic, and thermoelectric applications. Furthermore, we fabricate transparent graphene thermocouples with a high electromotive force of approximately ca. 80 µV/K, which validates the reliability and effectiveness of our approach for temperature sensing applications. This work paves the way for high-performance graphene-based electronic devices via controlled doping and patterning techniques. These findings provide valuable insights for the practical implementation of graphene in various fields.
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Superconducting materials exhibit unique physical properties and have great scientific value and vast industrial application prospects. However, due to limitations, such as the critical temperature (TC) and critical current density (JC), the large-scale application of superconducting materials remains challenging. Chemical doping has been a commonly used method to enhance the superconductivity of B(P)SCCO. However, satisfactory enhancement results have been difficult to achieve. In this study, we introduce green-light GaN p-n junction particles as inhomogeneous phases into B(P)SCCO polycrystalline particles to form a smart meta-superconductor (SMSC) structure. Based on the electroluminescence properties of the p-n junction, the Cooper pairs were stimulated and strengthened to enhance the superconductivity of B(P)SCCO. The experimental results demonstrate that the introduction of inhomogeneous phases can indeed enhance the critical temperature TC, critical current density JC, and complete diamagnetism (Meissner effect) of B(P)SCCO superconductors. Moreover, when the particle size of the raw material of B(P)SCCO is reduced from 30 to 5 µm, the grain size of the sintered samples also decreases, and the optimal doping concentration of the inhomogeneous phases increases from 0.15 wt.% to 0.2 wt.%, further improving the superconductivity.
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The electrostatic potential distribution in materials and devices plays an important role in controlling the behaviors of charge carriers. Kelvin probe force microscopy (KPFM) is a powerful technique for measuring the surface potential at a high spatial resolution. However, the measured surface potential often deviates from the potential deep in the bulk owing to certain factors. Here, we performed KPFM measurements across the p-n junction, in which such factors were eliminated as much as possible by selecting the sample, force sensor, and measurement mode. The measured surface potential distribution agrees well with the line shape of the simulated bulk potential. Our results demonstrate that KPFM is capable of quantitatively characterizing potential distributions whose changes occur on the order of 10 nm.
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In this paper, diamond-based vertical p-n junction diodes with step edge termination are investigated using a Silvaco simulation (Version 5.0.10.R). Compared with the conventional p-n junction diode without termination, the step edge termination shows weak influences on the forward characteristics and helps to suppress the electric field crowding. However, the breakdown voltage of the diode with simple step edge termination is still lower than that of the ideal parallel-plane one. To further enhance the breakdown voltage, we combine a p-n junction-based junction termination extension on the step edge termination. After optimizing the structure parameters of the device, the depletion regions formed by the junction termination extension overlap with that of the p-n junction on the top mesa, resulting in a more uniform electric field distribution and higher device performance.