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1.
Proc Natl Acad Sci U S A ; 121(35): e2408183121, 2024 Aug 27.
Artigo em Inglês | MEDLINE | ID: mdl-39172778

RESUMO

The conversion of CO2 into liquid fuels, using only sunlight and water, offers a promising path to carbon neutrality. An outstanding challenge is to achieve high efficiency and product selectivity. Here, we introduce a wireless photocatalytic architecture for conversion of CO2 and water into methanol and oxygen. The catalytic material consists of semiconducting nanowires decorated with core-shell nanoparticles, with a copper-rhodium core and a chromium oxide shell. The Rh/CrOOH interface provides a unidirectional channel for proton reduction, enabling hydrogen spillover at the core-shell interface. The vectorial transfer of protons, electrons, and hydrogen atoms allows for switching the mechanism of CO2 reduction from a proton-coupled electron transfer pathway in aqueous solution to hydrogenation of CO2 with a solar-to-methanol efficiency of 0.22%. The reported findings demonstrate a highly efficient, stable, and scalable wireless system for synthesis of methanol from CO2 that could provide a viable path toward carbon neutrality and environmental sustainability.

2.
Proc Natl Acad Sci U S A ; 119(26): e2121174119, 2022 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-35727969

RESUMO

The carbon-neutral synthesis of syngas from CO2 and H2O powered by solar energy holds grand promise for solving critical issues such as global warming and the energy crisis. Here we report photochemical reduction of CO2 with H2O into syngas using core/shell Au@Cr2O3 dual cocatalyst-decorated multistacked InGaN/GaN nanowires (NWs) with sunlight as the only energy input. First-principle density functional theory calculations revealed that Au and Cr2O3 are synergetic in deforming the linear CO2 molecule to a bent state with an O-C-O angle of 116.5°, thus significantly reducing the energy barrier of CO2RR compared with that over a single component of Au or Cr2O3. Hydrogen evolution reaction was promoted by the same cocatalyst simultaneously. By combining the cooperative catalytic properties of Au@Cr2O3 with the distinguished optoelectronic virtues of the multistacked InGaN NW semiconductor, the developed photocatalyst demonstrated high syngas activity of 1.08 mol/gcat/h with widely tunable H2/CO ratios between 1.6 and 9.2 under concentrated solar light illumination. Nearly stoichiometric oxygen was evolved from water splitting at a rate of 0.57 mol/gcat/h, and isotopic testing confirmed that syngas originated from CO2RR. The solar-to-syngas energy efficiency approached 0.89% during overall CO2 reduction coupled with water splitting. The work paves a way for carbon-neutral synthesis of syngas with the sole inputs of CO2, H2O, and solar light.

3.
Nano Lett ; 2024 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-38848282

RESUMO

Gatemon qubits are the electrically tunable cousins of superconducting transmon qubits. In this work, we demonstrate the full coherent control of a gatemon qubit based on hole carriers in a Ge/Si core/shell nanowire, with the longest coherence times in group IV material gatemons to date. The key to these results is a high-quality Josephson junction obtained using a straightforward and reproducible annealing technique. We demonstrate that the transport through the narrow junction is dominated by only two quantum channels, with transparencies up to unity. This novel qubit platform holds great promise for quantum information applications, not only because it incorporates technologically relevant materials, but also because it provides new opportunities, like an ultrastrong spin-orbit coupling in the few-channel regime of Josephson junctions.

4.
Nano Lett ; 24(33): 10313-10321, 2024 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-39115248

RESUMO

Lightweight porous ceramics with a unique combination of superior mechanical strength and damage tolerance are in significant demand in many fields such as energy absorption, aerospace vehicles, and chemical engineering; however, it is difficult to meet these mechanical requirements with conventional porous ceramics. Here, we report a graded structure design strategy to fabricate porous ceramic nanowire networks that simultaneously possess excellent mechanical strength and energy absorption capacity. Our optimized graded nanowire networks show a compressive strength of up to 35.6 MPa at a low density of 540 mg·cm-3, giving rise to a high specific compressive strength of 65.7 kN·m·kg-1 and a high energy absorption capacity of 17.1 kJ·kg-1, owing to a homogeneous distribution of stress upon loading. These values are top performance compared to other porous ceramics, giving our materials significant potential in various engineering fields.

5.
Nano Lett ; 24(12): 3750-3758, 2024 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-38488747

RESUMO

Semiconductor planar nanowire arrays (PNAs) are essential for achieving large-scale device integration. Direct heteroepitaxy of PNAs on a flat substrate is constrained by the mismatch in crystalline symmetry and lattice parameters between the substrate and epitaxial nanowires. This study presents a novel approach termed "self-competitive growth" for heteroepitaxy of CsPbBr3 PNAs on mica. The key to inducing the self-competitive growth of CsPbBr3 PNAs on mica involves restricting the nucleation of CsPbBr3 nanowires in a high-adsorption region, which is accomplished by overlaying graphite sheets on the mica surface. Theoretical calculations and experimental results demonstrate that CsPbBr3 nanowires oriented perpendicular to the boundary of the high-adsorption area exhibit greater competitiveness in intercepting the growth of nanowires in the other two directions, resulting in PNAs with a consistent orientation. Moreover, these PNAs exhibit low-threshold and stable amplified spontaneous emission under one-, two-, and three-photon excitation, indicating their potential for an integrated laser array.

6.
Nano Lett ; 24(19): 5799-5807, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38701332

RESUMO

Controlled growth of semiconductor nanowires with atomic precision offers the potential to tune the material properties for integration into scalable functional devices. Despite significant progress in understanding the nanowire growth mechanism, definitive control over atomic positions of its constituents, structure, and morphology via self-assembly remains challenging. Here, we demonstrate an exquisite control over synthesis of cation-ordered nanoscale superstructures in Ge-Sb-Te nanowires with the ability to deterministically vary the nanowire growth direction, crystal facets, and periodicity of cation ordering by tuning the relative precursor flux during synthesis. Furthermore, the role of anisotropy on material properties in cation-ordered nanowire superstructures is illustrated by fabricating phase-change memory (PCM) devices, which show significantly different growth direction dependent amorphization current density. This level of control in synthesizing chemically ordered nanoscale superstructures holds potential to precisely modulate fundamental material properties such as the electronic and thermal transport, which may have implications for PCM, thermoelectrics, and other nanoelectronic devices.

7.
Nano Lett ; 24(17): 5189-5196, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38636084

RESUMO

The development of large-scale, high-quality ferroelectric semiconductor nanowire arrays with interesting light-emitting properties can address limitations in traditional wide-bandgap ferroelectrics, thus serving as building blocks for innovative device architectures and next-generation high-density optoelectronics. Here, we investigate the optical properties of ferroelectric CsGeX3 (X = Br, I) halide perovskite nanowires that are epitaxially grown on muscovite mica substrates by vapor phase deposition. Detailed structural characterizations reveal an incommensurate heteroepitaxial relationship with the mica substrate. Furthermore, photoluminescence that can be tuned from yellow-green to red emissions by varying the halide composition demonstrates that these nanowire networks can serve as platforms for future optoelectronic applications. In addition, the room-temperature ferroelectricity and ferroelectric domain structures of these nanowires are characterized using second harmonic generation (SHG) polarimetry. The combination of room-temperature ferroelectricity with photoluminescence in these nanowire arrays unlocks new avenues for the design of novel multifunctional materials.

8.
Nano Lett ; 24(4): 1223-1230, 2024 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-38232153

RESUMO

Hybridizing a microwave mode with a quantum state requires precise frequency matching of a superconducting microwave resonator and the corresponding quantum object. However, fabrication always brings imperfections in geometry and material properties, causing deviations from the desired operating frequencies. An effective and universal strategy for their resonant coupling is to tune the frequency of a resonator, as quantum states like phonons are hardly tunable. Here, we demonstrate gate-tunable, titanium-nitride (TiN)-based superconducting resonators by implementing a nanowire inductor whose kinetic inductance is tuned via the gate-controlled supercurrent (GCS) effect. We investigate their responses for different gate biases and observe 4% (∼150 MHz) frequency tuning with decreasing internal quality factors. We also perform temperature-controlled experiments to support phonon-related mechanisms in the GCS effect and the resonance tuning. The GCS effect-based method proposed in this study provides an effective route for locally tunable resonators that can be employed in various hybrid quantum devices.

9.
Nano Lett ; 24(26): 7825-7832, 2024 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-38885473

RESUMO

Vertical gate-all-around (V-GAA) represents the ultimate configuration in the forthcoming transistor industry, but it still encounters challenges in the semiconductor community. This paper introduces, for the first time, a dual-input logic gate circuit achieved using 3D vertical transistors with nanoscale sub-20-nm GAA, employing a novel technique for creating contacts and patterning metallic lines at the bottom level without the conventional lift-off process. This involves a two-step oxidation process: patterning the first field oxide to form bottom metal lines and then creating the gate oxide layer on nanowires (NWs), followed by selective removal from the top and bottom of the nanostructures. VGAA-NW transistors, fabricated using the lift-off-free approach, exhibit improved yield and reduced access resistance, leading to an enhanced drive current while maintaining good immunity against short-channel effects. Finally, elementary two-input logic gates within a single cell, using VNW transistors, demonstrate novel possibilities in advanced logic circuitry design and routing options in 3D.

10.
Nano Lett ; 2024 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-39083658

RESUMO

The high operating voltage of conventional nanoelectromechanical switches, typically tens of volts, is much higher than the driving voltage of the complementary metal oxide semiconductor integrated circuit (∼1 V). Though the operating voltage can be reduced by adopting a narrow air gap, down to several nanometers, this leads to formidable manufacturing challenges and occasionally irreversible switch failures due to the surface adhesive force. Here, we demonstrate a new nanowire-morphed nanoelectromechanical (NW-NEM) switch structure with ultralow operation voltages. In contrast to conventional nanoelectromechanical switches actuated by unidirectional electrostatic attraction, the NW-NEM switch is bidirectionally driven by Lorentz force to allow the use of a large air gap for excellent electrical isolation, while achieving a record-low driving voltage of <0.2 V. Furthermore, the introduction of the Lorentz force allows the NW-NEM switch to effectively overcome the adhesion force to recover to the turn-off state.

11.
Nano Lett ; 24(15): 4336-4345, 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38567915

RESUMO

This study demonstrates the conceptual design and fabrication of a vertically integrated monolithic (VIM) neuromorphic device. The device comprises an n-type SnO2 nanowire bottom channel connected by a shared gate to a p-type P3HT nanowire top channel. This architecture establishes two distinct neural pathways with different response behaviors. The device generates excitatory and inhibitory postsynaptic currents, mimicking the corelease mechanism of bilingual synapses. To enhance the signal processing efficiency, we employed a bipolar spike encoding strategy to convert fluctuating sensory signals to spike trains containing positive and negative pulses. Utilizing the neuromorphic platform for synaptic processing, physiological signals featuring bidirectional fluctuations, including electrocardiogram and breathing signals, can be classified with an accuracy of over 90%. The VIM device holds considerable promise as a solution for developing highly integrated neuromorphic hardware for healthcare and edge intelligence applications.


Assuntos
Nanofios , Sinapses
12.
Nano Lett ; 24(18): 5656-5661, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38657275

RESUMO

A physical platform for nodes of the envisioned quantum Internet is long-sought. Here we propose such a platform, along with a conceptually simple and experimentally uncomplicated quantum information processing scheme, realized in a system of multiple crystal-phase quantum dots. We introduce novel location qubits, describe a method to construct a universal set of all-optical quantum gates, and simulate their performance in realistic structures, including decoherence sources. Our results show that location qubits are robust against the main decoherence mechanisms, and realistic single-qubit gate fidelities exceed 99.9%. Our scheme paves a clear way toward constructing multiqubit solid-state quantum registers with a built-in photonic interface─a key building block of the forthcoming quantum Internet.

13.
Nano Lett ; 24(20): 6158-6164, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38723204

RESUMO

The gate-all-around (GAA) field-effect transistor (FET) holds great potential to support next-generation integrated circuits. Nanowires such as carbon nanotubes (CNTs) are one important category of channel materials in GAA FETs. Based on first-principles investigations, we propose that SiX2 (X = S, Se) nanowires are promising channel materials that can significantly elevate the performance of GAA FETs. The sub-5 nm SiX2 (X = S, Se) nanowire GAA FETs exhibit excellent ballistic transport properties that meet the requirements of the 2013 International Technology Roadmap for Semiconductors (ITRS). Compared to CNTs, they are also advantageous or at least comparable in terms of gate controllability, device dimensions, etc. Importantly, SiSe2 GAA FETs show superb gate controllability due to the ultralow minimum subthreshold swing (SSmin) that breaks "Boltzmann's tyranny". Moreover, the energy-delay product (EDP) of SiX2 GAA FETs is significantly lower than that of the CNT FETs. These features make SiX2 nanowires ideal channel material in the sub-5 nm GAA FET devices.

14.
Small ; 20(29): e2311661, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38597694

RESUMO

Electronically conductive protein-based materials can enable the creation of bioelectronic components and devices from sustainable and nontoxic materials, while also being well-suited to interface with biological systems, such as living cells, for biosensor applications. However, as proteins are generally electrical insulators, the ability to render protein assemblies electroactive in a tailorable manner can usher in a plethora of useful materials. Here, an approach to fabricate electronically conductive protein nanowires is presented by aligning heme molecules in proximity along protein filaments, with these nanowires also possessing charge transfer abilities that enable energy harvesting from ambient humidity. The heme-incorporated protein nanowires demonstrate electron transfer over micrometer distances, with conductive atomic force microscopy showing individual nanowires having comparable conductance to other previously characterized heme-based bacterial nanowires. Exposure of multilayer nanowire films to humidity produces an electrical current, presumably through water molecules ionizing carboxyl groups in the filament and creating an unbalanced total charge distribution that is enhanced by the heme. Incorporation of heme and potentially other metal-center porphyrin molecules into protein nanostructures could pave the way for structurally- and electrically-defined protein-based bioelectronic devices.


Assuntos
Condutividade Elétrica , Heme , Nanofios , Nanofios/química , Heme/química , Microscopia de Força Atômica , Proteínas/química
15.
Small ; : e2402682, 2024 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-39058237

RESUMO

Low-dimensional photoconductors have extraordinarily high photoresponse and gain, which can be modulated by gate voltages as shown in literature. However, the physics of gate modulation remains elusive. In this work, the physics of gate modulation in silicon nanowire photoconductors with the analytical photoresponse equations is investigated. It is found that the impact of gate voltage varies vastly for nanowires with different size. For the wide nanowires that cannot be pinched off by high gate voltage, it is found that the photoresponses are enhanced by at least one order of magnitude due to the gate-induced electric passivation. For narrow nanowires that starts with a pinched-off channel, the gate voltage has no electric passivation effect but increases the potential barrier between source and drain, resulting in a decrease in dark and photocurrent. For the nanowires with an intermediate size, the channel is continuous but can be pinched off by a high gate voltage. The photoresponsivity and photodetectivity is maximized during the transition from the continuous channel to the pinched-off one. This work provides important insights on how to design high-performance photoconductors.

16.
Small ; 20(10): e2307458, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38145355

RESUMO

Low-dimensional semiconductor nanostructures, particularly in the form of nanowire configurations with large surface-to-volume-ratio, offer intriguing optoelectronic properties for the advancement of integrated photonic technologies. Here, a bias-controlled, superior dual-functional broadband light detecting/emitting diode enabled by constructing the aluminum-gallium-nitride-based nanowire on the silicon-platform is reported. Strikingly, the diode exhibits a stable and high responsivity (R) of over 200 mAW-1 covering an extremely wide operation band under reverse bias conditions, ranging from deep ultraviolet (DUV: 254 nm) to near-infrared (NIR: 1000 nm) spectrum region. While at zero bias, it still possesses superior DUV light selectivity with a high off-rejection ratio of 106. When it comes to the operation of the light-emitting mode under forward bias, it can achieve large spectral changes from UV to red simply by coating colloid quantum dots on the nanowires. Based on the multifunctional features of the diodes, this study further employs them in various optoelectronic systems, demonstrating outstanding applications in multicolor imaging, filterless color discrimination, and DUV/NIR visualization. Such highly responsive broadband photodetector with a tunable emitter enabled by III-V nanowire on silicon provides a new avenue toward the realization of integrated photonics and holds great promise for future applications in communication, sensing, imaging, and visualization.

17.
Small ; 20(3): e2304327, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37699748

RESUMO

Flexible composite films have attracted considerable attention due to great potential for healthcare, telecommunication, and aerospace. However, it is still challenging to achieve high conductivity and multifunctional integration, mainly due to poorly designed composite structures of these films. Herein, a novel sandwich-structured assembly strategy is proposed to fabricate flexible composite thin films made of Ag nanowire (AgNW) core and MXene layers by combination of spray coating and vacuum filtration process. In this case, ultrathin MXene layers play crucial roles in constructing compact composite structures strongly anchored to substrate with extensive hydrogen-bonding interactions. The resultant sandwich-structured MXene/AgNW composite thin films (SMAFs) exhibit ultrahigh electrical conductivity (up to 27193 S cm-1 ), resulting in exceptional electromagnetic interference shielding effectiveness of 16 223.3 dB cm2 g-1 and impressive Joule heating performance with rapid heating rate of 10.4 °C s-1 . Moreover, the uniform SMAFs can also be facilely cut into kirigami-patterned interconnects, which indicate superior strain-insensitive conductance even after long-term exposure to extreme temperatures. The demonstrated strategy offers a significant paradigm to construct multifunctional composite thin films for next-generation integrated flexible electronics with practical applications.

18.
Small ; 20(16): e2305831, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38088536

RESUMO

A novel combined setup, with a scanning thermal microscope (SThM) embedded in a scanning electron microscope (SEM), is used to characterize a suspended silicon rough nanowire (NW), which is epitaxially clamped at both sides and therefore monolithically integrated in a microfabricated device. The rough nature of the NW surface, which prohibits vacuum-SThM due to loose contact for heat dissipation, is circumvented by decorating the NW with periodic platinum dots. Reproducible approaches over these dots, enabled by the live feedback image provided by the SEM, yield a strong improvement in thermal contact resistance and a higher accuracy in its estimation. The results-thermal resistance at the tip-sample contact of 188±3.7K µW-1 and thermal conductivity of the NW of 13.7±1.6W m-1 K-1-are obtained by performing a series of approach curves on the dots. Noteworthy, the technique allows measuring elastic properties at the same time-the moment of inertia of the NW is found to be (6.1±1.0) × 10-30m4-which permits to correlate the respective effects of the rough shell on heat dissipation and on the NW stiffness. The work highlights the capabilities of the dual SThM/SEM instrument, in particular the interest of systematic approach curves with well-positioned and monitored tip motion.

19.
Small ; 20(34): e2400458, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38607289

RESUMO

1D nanowire networks, sharing similarities of structure, information transfer, and computation with biological neural networks, have emerged as a promising platform for neuromorphic systems. Based on brain-like structures of 1D nanowire networks, neuromorphic synaptic devices can overcome the von Neumann bottleneck, achieving intelligent high-efficient sensing and computing function with high information processing rates and low power consumption. Here, high-temperature neuromorphic synaptic devices based on SiC@NiO core-shell nanowire networks optoelectronic memristors (NNOMs) are developed. Experimental results demonstrate that NNOMs attain synaptic short/long-term plasticity and modulation plasticity under both electrical and optical stimulation, and exhibit advanced functions such as short/long-term memory and "learning-forgetting-relearning" under optical stimulation at both room temperature and 200 °C. Based on the advanced functions under light stimulus, the constructed 5 × 3 optoelectronic synaptic array devices exhibit a stable visual memory function up to 200 °C, which can be utilized to develop artificial visual systems. Additionally, when exposed to multiple electronic or optical stimuli, the NNOMs effectively replicate the principles of Pavlovian classical conditioning, achieving visual heterologous synaptic functionality and refining neural networks. Overall, with abundant synaptic characteristics and high-temperature thermal stability, these neuromorphic synaptic devices offer a promising route for advancing neuromorphic computing and visual systems.

20.
Small ; 20(22): e2310036, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38126916

RESUMO

Strain effect in the structurally defective materials can contribute to the catalysis optimization. However, it is challenging to achieve the performance improvement by strain modulation with the help of geometrical structure because strain is spatially dependent. Here, a new class of compressively strained platinum-iridium-metal zigzag-like nanowires (PtIrM ZNWs, M = nickel (Ni), cobalt (Co), iron (Fe), zinc (Zn) and gallium (Ga)) is reported as the efficient alkaline hydrogen evolution reaction (HER) and hydrogen oxidation reaction (HOR) catalysts. Particularly, the optimized PtIrNi ZNWs with 3% compressive strain (cs-PtIrNi ZNWs) can achieve the highest HER/HOR performances among all the catalysts investigate. Their HOR mass and specific activities are 3.2/14.4 and 2.6/32.7 times larger than those of PtIrNi NWs and commercial Pt/C, respectively. Simultaneously, they can exhibit the superior stability and high CO resistance for HOR. Further, experimental and theoretical studies collectively reveal that the compressive strain in cs-PtIrNi ZNWs effectively weakens the adsorption of hydroxyl intermediate and modulates the electronic structure, resulting in the weakened hydrogen binding energy (HBE) and moderate hydroxide binding energy (OHBE), beneficial for the improvement of HOR performance. This work highlights the importance of strain tuning in enhancing Pt-based nanomaterials for hydrogen catalysis and beyond.

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