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1.
Nano Lett ; 24(31): 9583-9590, 2024 Aug 07.
Artículo en Inglés | MEDLINE | ID: mdl-39041791

RESUMEN

Thanks to their tunable infrared absorption, solution processability, and low fabrication costs, HgTe colloidal quantum dots (CQDs) are promising for optoelectronic devices. Despite advancements in device design, their potential for imaging applications remains underexplored. For integration with Si-based readout integrated circuits (ROICs), top illumination is necessary for simultaneous light absorption and signal acquisition. However, most high-performing traditional HgTe CQD photodiodes are p-on-n stack and bottom-illuminated. Herein, we report top-illuminated inverted n-on-p HgTe CQD photodiodes using a robust p-type CQD layer and a thermally evaporated Bi2S3 electron transport layer. The p-type CQD solid is achieved by exploring the synergism in binary HgTe and Ag2Te CQDs. These photodetectors show a room-temperature detectivity of 3.4 × 1011 jones and an EQE of ∼44% at ∼1.7 µm wavelength, comparable to the p-on-n HgTe CQD photodiodes. A top-illuminated HgTe CQD short-wave infrared imager (640 × 512 pixels) was fabricated, demonstrating successful infrared imaging.

2.
Inorg Chem ; 63(17): 7714-7724, 2024 Apr 29.
Artículo en Inglés | MEDLINE | ID: mdl-38630017

RESUMEN

Modulating the band gap of two-dimensional (2D) transition metal dichalcogenide (TMDC) semiconductors is critical for their application in a wider spectral range. Alloying has been demonstrated as an effective method for regulating the band gap of 2D TMDC semiconductors. The fabrication of large-area 2D TMDC alloy films with centimeter-scale uniformity is fundamental to the application of integrated devices. Herein, we report a liquid-phase precursor one-step chemical vapor deposition (CVD) method for fabricating a MoxW1-xS2 alloy monolayer with a large size and an adjustable band gap. Good crystalline quality and high uniformity on a wafer scale enable the continuous adjustment of its band gap in the range of 1.8-2.0 eV. Density functional theory calculations provided a deep understanding of the Raman-active vibration modes of the MoxW1-xS2 alloy monolayer and the change in the conductivity of the alloy with photon energy. The synthesis of large-area MoxW1-xS2 alloy monolayers is a critical step toward the application of 2D layered semiconductors in practical optoelectronic devices.

3.
Phys Chem Chem Phys ; 26(5): 3880-3889, 2024 Jan 31.
Artículo en Inglés | MEDLINE | ID: mdl-38226853

RESUMEN

The development of efficient electrocatalysts for the hydrogen evolution reaction (HER) holds immense importance in the context of large-scale hydrogen production from water. Nevertheless, the practical application of such catalysts still relies on precious platinum-based materials. There is a pressing need to design high-performing, non-precious metal electrocatalysts capable of generating hydrogen at substantial current levels. We report here a stable monolith catalyst of Te-doped-WSe2 directly supported by a highly conductive W mesh. This catalyst demonstrates outstanding electrocatalytic performance and stability in acidic electrolytes, especially under high current conditions, surpassing the capabilities of commercial 5% Pt/C catalysts. Specifically, at current densities of 10 and 1200 mA cm-2, it exhibits a minimal overpotential of 79 and 232 mV, along with a small Tafel slope of 55 mV dec-1, respectively. The remarkable catalytic activity of Te-WSe2 can be attributed to the exceptional electron transfer facilitated by the stable monolithic structure, as well as the abundant and efficient active sites in the material. In addition, density functional theory calculations further indicate that Te doping adjusts H atom adsorption on various positions of WSe2, making it closer to thermal neutrality compared to the original material. This study presents an innovative approach to develop cost-effective HER electrocatalysts that perform optimally under high current density conditions.

4.
J Chem Theory Comput ; 20(13): 5717-5731, 2024 Jul 09.
Artículo en Inglés | MEDLINE | ID: mdl-38898771

RESUMEN

Rapid advancements in machine-learning methods have led to the emergence of machine-learning-based interatomic potentials as a new cutting-edge tool for simulating large systems with ab initio accuracy. Still, the community awaits universal interatomic models that can be applied to a wide range of materials without tuning neural network parameters. We develop a unified deep-learning interatomic potential (the DPA-Semi model) for 19 semiconductors ranging from group IIB to VIA, including Si, Ge, SiC, BAs, BN, AlN, AlP, AlAs, InP, InAs, InSb, GaN, GaP, GaAs, CdTe, InTe, CdSe, ZnS, and CdS. In addition, independent deep potential models for each semiconductor are prepared for detailed comparison. The training data are obtained by performing density functional theory calculations with numerical atomic orbitals basis sets to reduce the computational costs. We systematically compare various properties of the solid and liquid phases of semiconductors between different machine-learning models. We conclude that the DPA-Semi model achieves GGA exchange-correlation functional quality accuracy and can be regarded as a pretrained model toward a universal model to study group IIB to VIA semiconductors.

5.
Adv Mater ; 36(27): e2311830, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38501495

RESUMEN

Colloidal Quantum Dots (CQDs) of mercury telluride (HgTe) hold particular appeal for infrared photodetection due to their widely tunable infrared absorption and good compatibility with silicon electronics. While advances in surface chemistry have led to improved CQD solids, the chemical stability of HgTe material is not fully emphasized. In this study, it is aimed to address this issue and identifies a Se-stabilization strategy based on the surface coating of Se on HgTe CQDs via engineering in the precursor reactivity. The presence of Se-coating enables HgTe CQDs with improved colloidal stability, passivation, and enhanced degree of freedom in doping tuning. This enables the construction of optimized p-i-n HgTe CQD infrared photodetectors with an ultra-low dark current 3.26 × 10-6 A cm⁻2 at -0.4 V and room-temperature specific detectivity of 5.17 × 1011 Jones at wavelength ≈2 um, approximately one order of magnitude improvement compared to that of the control device. The stabilizing effect of Se is well preserved in the thin film state, contributing to much improved device stability. The in-synthesis Se-stabilization strategy highlights the importance of the chemical stability of materials for the construction of semiconductor-grade CQD solids and may have important implications for other high-performance CQD optoelectronic devices.

6.
Adv Sci (Weinh) ; 11(29): e2400636, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38778554

RESUMEN

Over the past years, the application potential of ferroelectric nanomaterials with unique physical properties for modern electronics is highlighted to a large extent. However, it is relatively challenging to fabricate inorganic ferroelectric nanomaterials, which is a process depending on a vacuum atmosphere at high temperatures. As significant complements to inorganic ferroelectric nanomaterials, the nanomaterials of molecular ferroelectrics are rarely reported. Here a low-cost room-temperature antisolvent method is used to synthesize free-standing 2D organic-inorganic hybrid perovskite (OIHP) ferroelectric nanosheets (NSs), that is, (CHA)2PbBr4 NSs (CHA = cyclohexylammonium), with an average lateral size of 357.59 nm and a thickness ranging from 10 to 70 nm. This method shows high repeatability and produces NSs with excellent crystallinity. Moreover, ferroelectric domains in single NSs can be clearly visualized and manipulated using piezoresponse force microscopy (PFM). The domain switching and PFM-switching spectroscopy indicate the robust in-plane ferroelectricity of the NSs. This work not only introduces a feasible, low-cost, and scalable method for preparing molecular ferroelectric NSs but also promotes the research on molecular ferroelectric nanomaterials.

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