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

ABSTRACT

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.
Article in English | MEDLINE | ID: mdl-35727969

ABSTRACT

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.
Article in English | MEDLINE | ID: mdl-38848282

ABSTRACT

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.
Article in English | MEDLINE | ID: mdl-39115248

ABSTRACT

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(37): 11661-11668, 2024 Sep 18.
Article in English | MEDLINE | ID: mdl-39250914

ABSTRACT

Fluorescent nanodiamonds (FNDs) with nitrogen-vacancy centers are pivotal for advancing quantum photonics and imaging through deterministic quantum state manipulation. However, deterministic integration of quantum emitters into photonic devices remains a challenge due to the need for high coupling efficiency and Purcell enhancement. We report a deterministic FND-integrated nanofocusing device achieved by assembling FNDs at a plasmonic waveguide tip through plasmonic-enhanced optical trapping. This technique not only increases the emission rate by 58.6 times compared to isolated FNDs but also preferentially directs radiation into the waveguide at a rate 5.3 times higher than that into free space, achieving an exceptional figure-of-merit of ∼3000 for efficient energy transfer. Our findings represent a significant step toward deterministic integration in quantum imaging and communication, opening new avenues for quantum technology advancements.

6.
Nano Lett ; 24(17): 5189-5196, 2024 May 01.
Article in English | MEDLINE | ID: mdl-38636084

ABSTRACT

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.

7.
Nano Lett ; 24(44): 14012-14019, 2024 Nov 06.
Article in English | MEDLINE | ID: mdl-39467266

ABSTRACT

We report an experimental study of a 1D quintuple-quantum-dot array integrated with two charge sensors in an InAs nanowire. The device is studied by measuring double quantum dots formed consecutively in the array, and corresponding charge stability diagrams are revealed with both direct current measurements and charge sensor signals. The one-dimensional quintuple-quantum-dot array is then tuned up, and its charge configurations are fully mapped out with the two charge sensors. The energy level of each dot in the array can be controlled individually using virtual gates. After that, four dots in the array are selected to form two double quantum dots, and ultrastrong inter-double-dot interaction is obtained. A theoretical simulation confirms the strong coupling strength between the two double quantum dots. The highly controllable one-dimensional quantum dot array is expected to be valuable for employing InAs nanowires to construct advanced quantum hardware in the future.

8.
Nano Lett ; 24(12): 3750-3758, 2024 Mar 27.
Article in English | MEDLINE | ID: mdl-38488747

ABSTRACT

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.

9.
Nano Lett ; 24(19): 5799-5807, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38701332

ABSTRACT

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.

10.
Nano Lett ; 2024 Nov 04.
Article in English | MEDLINE | ID: mdl-39495491

ABSTRACT

Predicting the optical properties of large-scale ensembles of luminescent nanowire arrays that host active quantum heterostructures is of paramount interest for on-chip integrated photonic and quantum photonic devices. However, this has remained challenging due to the vast geometrical parameter space and variations at the single object level. Here, we demonstrate high-throughput spectroscopy on 16800 individual InGaAs quantum heterostructures grown by site-selective epitaxy on silicon, with varying geometrical parameters to assess uniformity/yield in luminescence efficiency, and emission energy trends. The luminescence uniformity/yield enhances significantly at prepatterned array mask opening diameters (d0) greater than 50 nm. Additionally, the emission energy exhibits anomalous behavior with respect to d0, which is notably attributed to rotational twinning within the InGaAs region, inducing significant energy shifts due to quantum confinement effects. These findings provide useful insights for mapping and optimizing the interdependencies between geometrical parameters and electronic/optical properties of widely tunable sets of quantum nanowire heterostructures.

11.
Nano Lett ; 24(4): 1223-1230, 2024 Jan 31.
Article in English | MEDLINE | ID: mdl-38232153

ABSTRACT

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.

12.
Nano Lett ; 24(26): 7825-7832, 2024 Jul 03.
Article in English | MEDLINE | ID: mdl-38885473

ABSTRACT

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.

13.
Nano Lett ; 24(37): 11403-11410, 2024 Sep 18.
Article in English | MEDLINE | ID: mdl-39083658

ABSTRACT

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.

14.
Nano Lett ; 24(18): 5656-5661, 2024 May 08.
Article in English | MEDLINE | ID: mdl-38657275

ABSTRACT

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.

15.
Nano Lett ; 24(20): 6158-6164, 2024 May 22.
Article in English | MEDLINE | ID: mdl-38723204

ABSTRACT

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.

16.
Nano Lett ; 24(42): 13388-13396, 2024 Oct 23.
Article in English | MEDLINE | ID: mdl-39383340

ABSTRACT

Polarization-sensitive optoelectronic detection has been achieved by an all-Si detector in the NIR range, based on plasmon hot electron generation/internal photoemission effect. An advanced architecture with a specially designed anisotropic metasurface was developed and structurally optimized for maximizing the internal quantum efficiency (IQE). Assisted by finite difference time domain (FDTD) simulations, the well-designed device exhibits a maximum optical absorption of 80% around 1.45 µm, corresponding to an optical discrimination ratio of 120. Optoelectronic measurements show the peak responsivity and detectivity of 51.2 mA/W and 8.05 × 1010 cm Hz1/2/W, respectively, at 1.45 µm. A high polarization photocurrent ratio of 35 nm is also achieved at 1.55 µm. Moreover, the optoelectronic response can be tuned by a back-gate bias. Last but not least, we built up a model for theoretically estimating the IQE, which provides instructive guidance for further enhancing the optoelectronic performance of hot electron detectors.

17.
Nano Lett ; 24(44): 13903-13910, 2024 Nov 06.
Article in English | MEDLINE | ID: mdl-39437837

ABSTRACT

Josephson junctions are typically characterized by a single phase difference across two superconductors. This conventional two-terminal Josephson junction can be generalized to a multiterminal device where the Josephson energy contains terms with contributions from multiple independent phase variables. Such multiterminal Josephson junctions (MTJJs) are being considered as platforms for engineering effective Hamiltonians with nontrivial topologies, such as Weyl crossings and higher-order Chern numbers. These prospects rely on the ability to create MTJJs with nonclassical multiterminal couplings in which only a few quantum modes are populated. Here, we demonstrate these requirements in a three-terminal Josephson junction fabricated on selective-area-grown (SAG) PbTe nanowires. We observe signatures of a π-shifted Josephson effect, consistent with interterminal couplings mediated by four-particle quantum states called Cooper quartets. We further observe a supercurrent coexistent with a non-monotonic evolution of the conductance with gate voltage, indicating transport mediated by a few quantum modes in both two- and three-terminal devices.

18.
Nano Lett ; 24(15): 4336-4345, 2024 Apr 17.
Article in English | MEDLINE | ID: mdl-38567915

ABSTRACT

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.


Subject(s)
Nanowires , Synapses
19.
BMC Genomics ; 25(1): 982, 2024 Oct 20.
Article in English | MEDLINE | ID: mdl-39428470

ABSTRACT

BACKGROUND: Multiheme cytochromes c (MHC) provide prokaryotes with a broad metabolic versatility that contributes to their role in the biogeochemical cycling of the elements and in energy production in bioelectrochemical systems. However, MHC have only been isolated and studied in detail from a limited number of species. Among these, Desulfuromonadia spp. are particularly MHC-rich. To obtain a broad view of the diversity of MHC, we employed bioinformatic tools to study the cytochromome encoded in the genomes of the Desulfuromonadia class. RESULTS: We found that the distribution of the MHC families follows a different pattern between the two orders of the Desulfuromonadia class and that there is great diversity in the number of heme-binding motifs in MHC. However, the vast majority of MHC have up to 12 heme-binding motifs. MHC predicted to be extracellular are the least conserved and show high diversity, whereas inner membrane MHC are well conserved and show lower diversity. Although the most prevalent MHC have homologues already characterized, nearly half of the MHC families in the Desulforomonadia class have no known characterized homologues. AlphaFold2 was employed to predict their 3D structures. This provides an atlas of novel MHC, including examples with high beta-sheet content and nanowire MHC with unprecedented high numbers of putative heme cofactors per polypeptide. CONCLUSIONS: This work illuminates for the first time the universe of experimentally uncharacterized cytochromes that are likely to contribute to the metabolic versatility and to the fitness of Desulfuromonadia in diverse environmental conditions and to drive biotechnological applications of these organisms.


Subject(s)
Heme , Heme/metabolism , Heme/chemistry , Phylogeny , Genetic Variation , Computational Biology/methods , Models, Molecular , Cytochromes c/metabolism , Cytochromes c/genetics , Cytochromes c/chemistry , Amino Acid Motifs
20.
Small ; 20(10): e2307458, 2024 Mar.
Article in English | MEDLINE | ID: mdl-38145355

ABSTRACT

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.

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