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1.
Photoacoustics ; 38: 100612, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38711869

RESUMEN

A miniaturized photoacoustic spectroscopy-based gas sensor is proposed for the purpose of detecting sub-ppm-level carbonyl sulfide (OCS) using a tunable mid-infrared interband cascade laser (ICL) and a Helmholtz photoacoustic cell. The tuning characteristics of the tunable ICL with a center wavelength of 4823.3 nm were investigated to achieve the optimal driving parameters. A Helmholtz photoacoustic cell with a volume of ∼2.45 mL was designed and optimized to miniaturize the measurement system. By optimizing the modulation parameters and signal processing, the system was verified to have a good linear response to OCS concentration. With a lock-in amplifier integration time of 10 s, the 1σ noise standard deviation in differential mode was 0.84 mV and a minimum detection limit (MDL) of 409.2 ppbV was achieved at atmospheric pressure and room temperature.

2.
Adv Mater ; : e2313570, 2024 May 02.
Artículo en Inglés | MEDLINE | ID: mdl-38693828

RESUMEN

Ternary copper (Cu) halides are promising candidates for replacing toxic lead halides in the field of perovskite light-emitting diodes (LEDs) toward practical applications. However, the electroluminescent performance of Cu halide-based LEDs remains a great challenge due to the presence of serious nonradiative recombination and inefficient charge transport in Cu halide emitters. Here, the rational design of host-guest [dppb]2Cu2I2 (dppb denotes 1,2-bis[diphenylphosphino]benzene) emitters and its utility in fabricating efficient Cu halide-based green LEDs that show a high external quantum efficiency (EQE) of 13.39% are reported. The host-guest [dppb]2Cu2I2 emitters with mCP (1,3-bis(N-carbazolyl)benzene) host demonstrate a significant improvement of carrier radiative recombination efficiency, with the photoluminescence quantum yield increased by nearly ten times, which is rooted in the efficient energy transfer and type-I energy level alignment between [dppb]2Cu2I2 and mCP. Moreover, the charge-transporting mCP host can raise the carrier mobility of [dppb]2Cu2I2 films, thereby enhancing the charge transport and recombination. More importantly, this strategy enables a large-area prototype LED with a record-breaking area up to 81 cm2, along with a decent EQE of 10.02% and uniform luminance. It is believed these results represent an encouraging stepping stone to bring Cu halide-based LEDs from the laboratory toward commercial lighting and display panels.

3.
ACS Appl Mater Interfaces ; 16(20): 26643-26652, 2024 May 22.
Artículo en Inglés | MEDLINE | ID: mdl-38716902

RESUMEN

A scene that contains both old and instant events with a clear motion trail is visually intriguing and dynamic, which can convey a sense of change, transition, or evolution. Developing an eco-friendly delay display system offers a powerful tool for fusing old and instant events, which can be used for visualizing motion trails. Herein, we brighten triplet excitons of carbon nanodots (CNDs) and increase their emission yield by a multidimensional confinement strategy, and the CND-based delay display array is demonstrated. The intense confinement effects via multidimensional confinement strategy suppress nonradiative transitions, and 240% enhancement in the phosphorescence efficiency and 260% enhancement in the lifetime of the CNDs are thus realized. Considering their distinctive phosphorescence performances, a delay display array containing a 4 × 4 CND-based delay lighting device is demonstrated, which can provide ultralong phosphorescence over 7 s, and the motion that occurred in different timelines is recorded clearly. This finding will motivate the investigation of phosphorescent CNDs in motion trail recognition.

4.
Small ; : e2312218, 2024 May 08.
Artículo en Inglés | MEDLINE | ID: mdl-38716754

RESUMEN

Room-temperature phosphorescent materials, renowned for their long luminescence lifetimes, have garnered significant attention in the field of optical materials. However, the challenges posed by thermally induced quenching have significantly hindered the advancement of luminescence efficiency and stability. In this study, thermally enhanced phosphorescent carbon nanodots (CND) are developed by incorporating them into fiber matrices. Remarkably, the phosphorescence lifetime of the thermally enhanced CND exhibits a twofold enhancement, increasing from 326 to 753 ms, while the phosphorescence intensity experienced a tenfold enhancement, increasing from 25 to 245 as the temperature increased to 373 K. Rigid fiber matrices can effectively suppress the non-radiative transition rate of triplet excitons, while high temperatures can desorb oxygen adsorbed on the surface of the CND, disrupting the interaction between the CND and oxygen. Consequently, a thermally enhanced phosphorescence is obtained. In addition, benefiting from the thermally enhanced phosphorescence property of CND, a warning indicator with an anti-counterfeiting function for monitoring cold-chain logistics is demonstrated based on CND.

5.
Opt Lett ; 49(8): 2101-2104, 2024 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-38621086

RESUMEN

The introduction of cantilever-based fiber-optic microphones (FOMs) has proven to be effective in acoustic sensing. Further improvements in cantilevers face two key constraints: the challenge of achieving minimal sizes with sufficient reflective area and the trade-off between sensitivity and response bandwidth. Herein, we present a geometry optimization framework for a cantilever-based FOM that addresses this issue. Employing drumstick-shaped cantilevers housed within a Fabry-Perot (F-P) interferometric structure, we showcase a heightened sensitivity of 302.8 mV/Pa at 1 kHz and a minimum detectable acoustic pressure (MDP) of 2.35 µPa/H z. Notably, these metrics outperform those of the original rectangular cantilever with identical dimensions. Furthermore, our proposed cantilever effectively mitigates the reduction in resonance frequencies, thereby improving the response bandwidth. This geometry optimization framework offers considerable design flexibility and scalability, making it especially suitable for high-performance acoustic sensing applications.

6.
Adv Sci (Weinh) ; : e2308337, 2024 Apr 04.
Artículo en Inglés | MEDLINE | ID: mdl-38572504

RESUMEN

Physical unclonable functions (PUFs) have emerged as a promising encryption technology, utilizing intrinsic physical identifiers that offer enhanced security and tamper resistance. Multi-level PUFs boost system complexity, thereby improving system reliability and fault tolerance. However, crosstalk-free multi-level PUFs remain a persistent challenge. In this study, a hierarchical PUF system that harnesses the spontaneous phase separation of silk fibroin /PVA blend and the random distribution of silicon-vacancy diamonds within the blend is presented. The thermodynamic instability of phase separation and inherent unpredictability of diamond dispersion gives rise to intricate random patterns at two distinct scales, enabling time-efficient hierarchical authentication for cryptographic keys. These patterns are complementary yet independent, inherently resistant to replication and damage thus affording robust security and reliability to the proposed system. Furthermore, customized authentication algorithms are constructed: visual PUFs authentication utilizes neural network combined structural similarity index measure, while spectral PUFs authentication employs Hamming distance and cross-correlation bit operation. This hierarchical PUF system attains a high recognition rate without interscale crosstalk. Additionally, the coding capacity is exponentially enhanced using M-ary encoding to reinforce multi-level encryption. Hierarchical PUFs hold significant potential for immediate application, offering unprecedented data protection and cryptographic key authentication capabilities.

7.
Adv Sci (Weinh) ; : e2309126, 2024 Mar 13.
Artículo en Inglés | MEDLINE | ID: mdl-38477425

RESUMEN

Along with the increasing integration density and decreased feature size of current semiconductor technology, heterointegration of the Si-based devices with diamond has acted as a promising strategy to relieve the existing heat dissipation problem. As one of the heterointegration methods, the microwave plasma chemical vapor deposition (MPCVD) method is utilized to synthesize large-scale diamond films on a Si substrate, while distinct structures appear at the Si-diamond interface. Investigation of the formation mechanisms and modulation strategies of the interface is crucial to optimize the heat dissipation behaviors. By taking advantage of electron microscopy, the formation of the epitaxial ß-SiC interlayer is found to be caused by the interaction between the anisotropically sputtered Si and the deposited amorphous carbon. Compared with the randomly oriented ß-SiC interlayer, larger diamond grain sizes can be obtained on the epitaxial ß-SiC interlayer under the same synthesis condition. Moreover, due to the competitive interfacial reactions, the epitaxial ß-SiC interlayer thickness can be reduced by increasing the CH4 /H2 ratio (from 3% to 10%), while further increase in the ratio (to 20%) can lead to the broken of the epitaxial relationship. The above findings are expected to provide interfacial design strategies for multiple large-scale diamond applications.

8.
Nat Commun ; 15(1): 2365, 2024 Mar 15.
Artículo en Inglés | MEDLINE | ID: mdl-38491012

RESUMEN

It remains a challenge to obtain biocompatible afterglow materials with long emission wavelengths, durable lifetimes, and good water solubility. Herein we develop a photooxidation strategy to construct near-infrared afterglow carbon nanodots with an extra-long lifetime of up to 5.9 h, comparable to that of the well-known rare-earth or organic long-persistent luminescent materials. Intriguingly, size-dependent afterglow lifetime evolution from 3.4 to 5.9 h has been observed from the carbon nanodots systems in aqueous solution. With structural/ultrafast dynamics analysis and density functional theory simulations, we reveal that the persistent luminescence in carbon nanodots is activated by a photooxidation-induced dioxetane intermediate, which can slowly release and convert energy into luminous emission via the steric hindrance effect of nanoparticles. With the persistent near-infrared luminescence, tissue penetration depth of 20 mm can be achieved. Thanks to the high signal-to-background ratio, biological safety and cancer-specific targeting ability of carbon nanodots, ultralong-afterglow guided surgery has been successfully performed on mice model to remove tumor tissues accurately, demonstrating potential clinical applications. These results may facilitate the development of long-lasting luminescent materials for precision tumor resection.


Asunto(s)
Nanopartículas , Neoplasias , Animales , Ratones , Luminiscencia
9.
ACS Nano ; 18(10): 7610-7617, 2024 Mar 12.
Artículo en Inglés | MEDLINE | ID: mdl-38426715

RESUMEN

The quest for solar-blind photodetectors (SBPDs) with exceptional optoelectronic properties for imaging applications has prompted the investigation of SBPD arrays. Ga2O3, characterized by its ultrawide bandgap and low growth cost, has emerged as a promising material for solar-blind detection. In this study, SBPD arrays were fabricated by weaving Sn-doped ß-Ga2O3 microbelts (MBs). These MBs, which have a conductive core surrounded by a high-resistivity depletion surface layer resulting from the segregation of Sn and oxygen, are woven into a grid structure. Each intersection of the MBs functions as a photodetector pixel, with the intersecting MBs serving as the output electrodes of the pixel. This design simplifies the readout circuit for the photodetector array. The solar-blind photodetector array demonstrates superior solar-blind detection performance, including a dark current of 0.5 pA, a response time of 38.8 µs, a light/dark current ratio of 108, and a responsivity of 300 A/W. This research may provide a feasible strategy for the fabrication of photodetector arrays, thus pushing forward the application of photodetectors in imaging.

10.
Proc Natl Acad Sci U S A ; 121(9): e2316580121, 2024 Feb 27.
Artículo en Inglés | MEDLINE | ID: mdl-38377204

RESUMEN

Achieving high-performance materials with superior mechanical properties and electrical conductivity, especially in large-sized bulk forms, has always been the goal. However, it remains a grand challenge due to the inherent trade-off between these properties. Herein, by employing nanodiamonds as precursors, centimeter-sized diamond/graphene composites were synthesized under moderate pressure and temperature conditions (12 GPa and 1,300 to 1,500 °C), and the composites consisted of ultrafine diamond grains and few-layer graphene domains interconnected through covalently bonded interfaces. The composites exhibit a remarkable electrical conductivity of 2.0 × 104 S m-1 at room temperature, a Vickers hardness of up to ~55.8 GPa, and a toughness of 10.8 to 19.8 MPa m1/2. Theoretical calculations indicate that the transformation energy barrier for the graphitization of diamond surface is lower than that for diamond growth directly from conventional sp2 carbon materials, allowing the synthesis of such diamond composites under mild conditions. The above results pave the way for realizing large-sized diamond-based materials with ultrahigh electrical conductivity and superior mechanical properties simultaneously under moderate synthesis conditions, which will facilitate their large-scale applications in a variety of fields.

11.
ACS Appl Mater Interfaces ; 16(7): 8321-8332, 2024 Feb 21.
Artículo en Inglés | MEDLINE | ID: mdl-38330195

RESUMEN

Long-lasting and highly efficient antibacterial fabrics play a key role in public health occurrences caused by bacterial and viral infections. However, the production of antibacterial fabrics with a large size, highly efficient, and broad-spectrum antibacterial performance remains a great challenge due to the complex processes. Herein, we demonstrate sizable and highly efficient antibacterial fabrics through hydrogen bonding interaction and electrostatic interaction between surface groups of ZnO nanoparticles and fabric fibers. The production process can be carried out at room temperature and achieve a production rate of 300 × 1 m2 within 1 h. Under both visible light and dark conditions, the bactericidal rate against Gram-positive (S. aureus), Gram-negative (E. coli), and multidrug-resistant (MRSA) bacteria can reach an impressive 99.99%. Furthermore, the fabricated ZnO nanoparticle-decorated antibacterial fabrics (ZnO@fabric) show high stability and long-lasting antibacterial performance, making them easy to develop into variable antibacterial blocks for protection suits.


Asunto(s)
Escherichia coli , Óxido de Zinc , Staphylococcus aureus , Óxido de Zinc/farmacología , Enlace de Hidrógeno , Electricidad Estática , Antibacterianos/farmacología
12.
Nano Lett ; 23(24): 11755-11762, 2023 Dec 27.
Artículo en Inglés | MEDLINE | ID: mdl-38091579

RESUMEN

The issues of fruit waste and safety resulting from rot have spurred a demand for improved packaging systems. Herein, we present highly antibacterial and antioxidative carbon nanodot/silk fibroin (CD/SF) films for fruit preservation. The films are composed of CDs and SF together with a small amount of glycerol via hydrogen bonding, exhibiting outstanding biosafety, transparency, and stretchability. The films effectively integrate key functionalities (atmosphere control, resistance to food-borne pathogens, and antioxidation properties) and can be manufactured in large sizes (about 20 × 30 cm), boasting a transmission rate of 13 183 cm3/m2·day for oxygen and 2860 g/m2·day for water vapor, favoring the preservation of fresh fruits. A convenient dip-coating method enables in situ fabrication of films with a thickness of approximately 14 µm directly on the fruits' surface providing comprehensive protection. Importantly, the films are washable and biodegradable. This work presents a promising technology to produce multifunctional and eco-friendly antibacterial packaging systems.


Asunto(s)
Fibroínas , Frutas/microbiología , Antioxidantes/farmacología , Antibacterianos/farmacología
13.
Nano Lett ; 23(24): 11669-11677, 2023 Dec 27.
Artículo en Inglés | MEDLINE | ID: mdl-38060996

RESUMEN

Supramolecular aggregation has provided the archetype concept to understand the variants in an emerging systems property. Herein, we have achieved the supramolecular assembly of carbon nanodots (CDs) for the first time and employ supramolecular aggregation to understand their alteration in photophysical properties. In detail, we have employed the CDs as a block to construct the supramolecular assembly of aggregates in the CDs' antisolvent of ethanol. The CD-based aggregates exhibit complex and organized morphologies with another long-wavelength excitation-dependent emission band. The experimental results and density functional theoretical calculations reveal that the supramolecular assembly of CDs can decrease the energy gap between the ground and excited states, contributing to the new long-wavelength excitation-dependent emission. The supramolecular aggregation can be employed as one universal strategy to manipulate and understand the luminescence of CDs. These findings cast new light to build the emerging systems and understand the light emission of CDs through supramolecular chemistry.

14.
Adv Mater ; 35(44): e2305495, 2023 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-37603794

RESUMEN

Fluorescence thermometry has been propelled to the forefront of scientific attention due to its high spatial resolution and remote non-invasive detection. However, recent generations of thermometers still suffer from limited thermal sensitivity (Sr ) below 10% change per Kelvin. Herein, this work presents an ideal temperature-responsive fluorescence material through Te4+ -doped 0D Cs2 ScCl5 ·H2 O, in which isolated polyhedrons endow highly localized electronic structures, and the strong electron-phonon coupling facilitates the formation of self-trapped excitons (STEs). With rising temperature, the dramatic asymmetric expansion of the soft lattice induces increased defects, strong exciton-phonon coupling, and low thermal activation energy, which evokes a rapid de-trapping process of STEs, enabling several orders of magnitude changes in the fluorescence lifetime over a narrow temperature range. After regulating the de-trapping process with different Te4+ doping, a record-high Sr (27.36% K-1 ) of fluorescence lifetime-based detection is achieved at 325 K. The robust stability against multiple heating/cooling cycles and long-term measurements enables a low temperature uncertainty of 0.067 K. Further, the developed thermometers are demonstrated for the remote local monitoring of operating temperature on internal electronic components. It is believed that this work constitutes a solid step towards building the next generation of ultrasensitive thermometers based on low-dimensional metal halides.

15.
Nano Lett ; 23(17): 8241-8248, 2023 Sep 13.
Artículo en Inglés | MEDLINE | ID: mdl-37594857

RESUMEN

Next-generation mid-infrared (MIR) imaging chips demand free-cooling capability and high-level integration. The rising two-dimensional (2D) semimetals with excellent infrared (IR) photoresponses are compliant with these requirements. However, challenges remain in scalable growth and substrate-dependence for on-chip integration. Here, we demonstrate the inch-level 2D palladium ditelluride (PdTe2) Dirac semimetal using a low-temperature self-stitched epitaxy (SSE) approach. The low formation energy between two precursors facilitates low-temperature multiple-point nucleation (∼300 °C), growing up, and merging, resulting in self-stitching of PdTe2 domains into a continuous film, which is highly compatible with back-end-of-line (BEOL) technology. The uncooled on-chip PdTe2/Si Schottky junction-based photodetector exhibits an ultrabroadband photoresponse of up to 10.6 µm with a large specific detectivity. Furthermore, the highly integrated device array demonstrates high-resolution room-temperature imaging capability, and the device can serve as an optical data receiver for IR optical communication. This study paves the way toward low-temperature growth of 2D semimetals for uncooled MIR sensing.

16.
Materials (Basel) ; 16(13)2023 Jun 30.
Artículo en Inglés | MEDLINE | ID: mdl-37445057

RESUMEN

X-ray detectors have numerous applications in medical imaging, industrial inspection, and crystal structure analysis. Gallium oxide (Ga2O3) shows potential as a material for high-performance X-ray detectors due to its wide bandgap, relatively high mass attenuation coefficient, and resistance to radiation damage. In this study, we present Sn-doped Ga2O3 microwire detectors for solar-blind and X-ray detection. The developed detectors exhibit a switching ratio of 1.66 × 102 under X-ray irradiation and can operate stably from room temperature to 623 K, which is one of the highest reported operating temperatures for Ga2O3 X-ray detectors to date. These findings offer a promising new direction for the design of Ga2O3-based X-ray detectors.

18.
Adv Mater ; : e2305044, 2023 Jul 24.
Artículo en Inglés | MEDLINE | ID: mdl-37486859

RESUMEN

The emerging nonvolatile memory technologies based on ferroic materials are promising for producing high-speed, low-power, and high-density memory in the field of integrated circuits. Long-range ferroic orders observed in 2D materials have triggered extensive research interest in 2D magnets, 2D ferroelectrics, 2D multiferroics, and their device applications. Devices based on 2D ferroic materials and heterostructures with an atomically smooth interface and ultrathin thickness have exhibited impressive properties and significant potential for developing advanced nonvolatile memory. In this context, a systematic review of emergent 2D ferroic materials is conducted here, emphasizing their recent research on nonvolatile memory applications, with a view to proposing brighter prospects for 2D magnetic materials, 2D ferroelectric materials, 2D multiferroic materials, and their relevant devices.

19.
Small ; 19(31): e2302504, 2023 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-37282771

RESUMEN

Phosphorescent materials as block elements to build artwork incorporating the time and emission, enable them with spectacular lighting effects. In this work, enhanced phosphorescence of carbon nanodots (CNDs) is demonstrated via double confinement strategy, which silica and epoxy resin are used as the first and the second order confinement layer. The multi-confined CNDs show an enhanced phosphorescence quantum yield up to 16.4%, with enduring emission lifetime up to 1.44 s. Delicately, the plasticity of the epoxy resin enables them easily to be designed for 3D artworks with long emission lifetimes in different shapes. The efficient and eco-friendly phosphorescent CNDs may arouse intense interest both in the academic community and markets.

20.
Opt Express ; 31(13): 21796-21805, 2023 Jun 19.
Artículo en Inglés | MEDLINE | ID: mdl-37381268

RESUMEN

Transducer components are crucial in optimizing the sensitivity of microphones. Cantilever structure is commonly used as a structural optimization technique. Here, we present a novel Fabry-Perot (F-P) interferometric fiber-optic microphone (FOM) using a hollow cantilever structure. The proposed hollow cantilever aims to reduce the effective mass and spring constant of the cantilever, thereby enhancing the sensitivity of the FOM. Experimental results demonstrate that the proposed structure outperforms the original cantilever design in terms of sensitivity. The sensitivity and minimum detectable acoustic pressure level (MDP) can reach 91.40 mV/Pa and 6.20 µPa/Hz at 1.7 kHz, respectively. Notably, the hollow cantilever provides an optimization framework for highly sensitive FOMs.

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