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1.
Cell ; 186(13): 2853-2864.e8, 2023 06 22.
Artigo em Inglês | MEDLINE | ID: mdl-37290436

RESUMO

Electrically conductive appendages from the anaerobic bacterium Geobacter sulfurreducens, recently identified as extracellular cytochrome nanowires (ECNs), have received wide attention due to numerous potential applications. However, whether other organisms employ similar ECNs for electron transfer remains unknown. Here, using cryoelectron microscopy, we describe the atomic structures of two ECNs from two major orders of hyperthermophilic archaea present in deep-sea hydrothermal vents and terrestrial hot springs. Homologs of Archaeoglobus veneficus ECN are widespread among mesophilic methane-oxidizing Methanoperedenaceae, alkane-degrading Syntrophoarchaeales archaea, and in the recently described megaplasmids called Borgs. The ECN protein subunits lack similarities in their folds; however, they share a common heme arrangement, suggesting an evolutionarily optimized heme packing for efficient electron transfer. The detection of ECNs in archaea suggests that filaments containing closely stacked hemes may be a common and widespread mechanism for long-range electron transfer in both prokaryotic domains of life.


Assuntos
Nanofios , Microscopia Crioeletrônica , Composição de Bases , Filogenia , RNA Ribossômico 16S , Análise de Sequência de DNA , Transporte de Elétrons , Citocromos , Archaea , Heme
2.
Cell ; 177(2): 361-369.e10, 2019 04 04.
Artigo em Inglês | MEDLINE | ID: mdl-30951668

RESUMO

Long-range (>10 µm) transport of electrons along networks of Geobacter sulfurreducens protein filaments, known as microbial nanowires, has been invoked to explain a wide range of globally important redox phenomena. These nanowires were previously thought to be type IV pili composed of PilA protein. Here, we report a 3.7 Å resolution cryoelectron microscopy structure, which surprisingly reveals that, rather than PilA, G. sulfurreducens nanowires are assembled by micrometer-long polymerization of the hexaheme cytochrome OmcS, with hemes packed within ∼3.5-6 Å of each other. The inter-subunit interfaces show unique structural elements such as inter-subunit parallel-stacked hemes and axial coordination of heme by histidines from neighboring subunits. Wild-type OmcS filaments show 100-fold greater conductivity than other filaments from a ΔomcS strain, highlighting the importance of OmcS to conductivity in these nanowires. This structure explains the remarkable capacity of soil bacteria to transport electrons to remote electron acceptors for respiration and energy sharing.


Assuntos
Transporte de Elétrons/fisiologia , Geobacter/metabolismo , Heme/metabolismo , Biofilmes , Condutividade Elétrica , Elétrons , Proteínas de Fímbrias/química , Fímbrias Bacterianas/química , Nanofios , Oxirredução
3.
Proc Natl Acad Sci U S A ; 121(27): e2406884121, 2024 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-38935562

RESUMO

Degeneracy and symmetry have a profound relation in quantum systems. Here, we report gate-tunable subband degeneracy in PbTe nanowires with a nearly symmetric cross-sectional shape. The degeneracy is revealed in electron transport by the absence of a quantized plateau. Utilizing a dual gate design, we can apply an electric field to lift the degeneracy, reflected as emergence of the plateau. This degeneracy and its tunable lifting were challenging to observe in previous nanowire experiments, possibly due to disorder. Numerical simulations can qualitatively capture our observation, shedding light on device parameters for future applications.

4.
Proc Natl Acad Sci U S A ; 119(19): e2119964119, 2022 05 10.
Artigo em Inglês | MEDLINE | ID: mdl-35503913

RESUMO

Using a series of multiheme cytochromes, the metal-reducing bacterium Shewanella oneidensis MR-1 can perform extracellular electron transfer (EET) to respire redox-active surfaces, including minerals and electrodes outside the cell. While the role of multiheme cytochromes in transporting electrons across the cell wall is well established, these cytochromes were also recently found to facilitate long-distance (micrometer-scale) redox conduction along outer membranes and across multiple cells bridging electrodes. Recent studies proposed that long-distance conduction arises from the interplay of electron hopping and cytochrome diffusion, which allows collisions and electron exchange between cytochromes along membranes. However, the diffusive dynamics of the multiheme cytochromes have never been observed or quantified in vivo, making it difficult to assess their hypothesized contribution to the collision-exchange mechanism. Here, we use quantum dot labeling, total internal reflection fluorescence microscopy, and single-particle tracking to quantify the lateral diffusive dynamics of the outer membrane-associated decaheme cytochromes MtrC and OmcA, two key components of EET in S. oneidensis. We observe confined diffusion behavior for both quantum dot-labeled MtrC and OmcA along cell surfaces (diffusion coefficients DMtrC = 0.0192 ± 0.0018 µm2/s, DOmcA = 0.0125 ± 0.0024 µm2/s) and the membrane extensions thought to function as bacterial nanowires. We find that these dynamics can trace a path for electron transport via overlap of cytochrome trajectories, consistent with the long-distance conduction mechanism. The measured dynamics inform kinetic Monte Carlo simulations that combine direct electron hopping and redox molecule diffusion, revealing significant electron transport rates along cells and membrane nanowires.


Assuntos
Shewanella , Imagem Individual de Molécula , Membrana Celular/metabolismo , Citocromos/metabolismo , Transporte de Elétrons , Oxirredução , Shewanella/metabolismo
5.
Nano Lett ; 24(22): 6553-6559, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38775731

RESUMO

New approaches such as selective area growth (SAG), where crystal growth is lithographically controlled, allow the integration of bottom-up grown semiconductor nanomaterials in large-scale classical and quantum nanoelectronics. This calls for assessment and optimization of the reproducibility between individual components. We quantify the structural and electronic statistical reproducibility within large arrays of nominally identical selective area growth InAs nanowires. The distribution of structural parameters is acquired through comprehensive atomic force microscopy studies and transmission electron microscopy. These are compared to the statistical distributions of the cryogenic electrical properties of 256 individual SAG nanowire field effect transistors addressed using cryogenic multiplexer circuits. Correlating measurements between successive thermal cycles allows distinguishing between the contributions of surface impurity scattering and fixed structural properties to device reproducibility. The results confirm the potential of SAG nanomaterials, and the methodologies for quantifying statistical metrics are essential for further optimization of reproducibility.

6.
Nano Lett ; 24(27): 8394-8401, 2024 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-38865258

RESUMO

Hybrid semiconductor-superconductor nanowires have emerged as a cornerstone in modern quantum devices. Integrating such nanowires into hybrid devices typically requires extensive postgrowth processing which may affect device performance unfavorably. Here, we present a technique for in situ shadowing superconductors on nanowires and compare the structural and electronic properties of Al junctions formed by shadowing versus etching. Based on transmission electron microscopy, we find that typical etching procedures lead to atomic-scale surface roughening. This surface perturbation may cause a reduction of the electron mobility as demonstrated in transport measurements. Further, we display advanced shadowing geometries aiding in the pursuit of bringing fabrication of hybrid devices in situ. Finally, we give examples of shadowed junctions exploited in various device geometries that exhibit high-quality quantum transport signatures.

7.
Nano Lett ; 24(5): 1660-1666, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38266180

RESUMO

Scalable and addressable integrated manipulation of qubits is crucial for practical quantum information applications. Different waveguides have been used to transport the optical and electrical driving pulses, which are usually required for qubit manipulation. However, the separated multifields may limit the compactness and efficiency of manipulation and introduce unwanted perturbation. Here, we develop a tapered fiber-nanowire-electrode hybrid structure to realize integrated optical and microwave manipulation of solid-state spins at nanoscale. Visible light and microwave driving pulses are simultaneously transported and concentrated along an Ag nanowire. Studied with spin defects in diamond, the results show that the different driving fields are aligned with high accuracy. The spatially selective spin manipulation is realized. And the frequency-scanning optically detected magnetic resonance (ODMR) of spin qubits is measured, illustrating the potential for portable quantum sensing. Our work provides a new scheme for developing compact, miniaturized quantum sensors and quantum information processing devices.

8.
Nano Lett ; 24(14): 4132-4140, 2024 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-38534013

RESUMO

Inspired by the retina, artificial optoelectronic synapses have groundbreaking potential for machine vision. The field-effect transistor is a crucial platform for optoelectronic synapses that is highly sensitive to external stimuli and can modulate conductivity. On the basis of the decent optical absorption, perovskite materials have been widely employed for constructing optoelectronic synaptic transistors. However, the reported optoelectronic synaptic transistors focus on the static processing of independent stimuli at different moments, while the natural visual information consists of temporal signals. Here, we report CsPbBrI2 nanowire-based optoelectronic synaptic transistors to study the dynamic responses of artificial synaptic transistors to time-varying visual information for the first time. Moreover, on the basis of the dynamic synaptic behavior, a hardware system with an accuracy of 85% is built to the trajectory of moving objects. This work offers a new way to develop artificial optoelectronic synapses for the construction of dynamic machine vision systems.

9.
Nano Lett ; 2024 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-38608187

RESUMO

Germanium-tin (Ge1-xSnx) semiconductors are a front-runner platform for compact mid-infrared devices due to their tunable narrow bandgap and compatibility with silicon processing. However, their large lattice parameter has been a major hurdle, limiting the quality of epitaxial layers grown on silicon or germanium substrates. Herein, we demonstrate that 20 nm Ge nanowires (NWs) act as effective compliant substrates to grow extended defect-free Ge1-xSnx alloys with a composition uniformity over several micrometers along the NW growth axis without significant buildup of the compressive strain. Ge/Ge1-xSnx core/shell NWs with Sn content spanning the 6-18 at. % range are achieved and processed into photoconductors exhibiting a high signal-to-noise ratio at room temperature with a cutoff wavelength in the 2.0-3.9 µm range. The processed NW devices are integrated in an uncooled imaging setup enabling the acquisition of high-quality images under both broadband and laser illuminations at 1550 and 2330 nm without the lock-in amplifier technique.

10.
Nano Lett ; 24(22): 6488-6495, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38771151

RESUMO

Understanding heating and cooling mechanisms in mesoscopic superconductor-semiconductor devices is crucial for their application in quantum technologies. Owing to their poor thermal conductivity, heating effects can drive superconducting-to-normal transitions even at low bias, observed as sharp conductance dips through the loss of Andreev excess currents. Tracking such dips across magnetic field, cryostat temperature, and applied microwave power allows us to uncover cooling bottlenecks in different parts of a device. By applying this "Joule spectroscopy" technique, we analyze heat dissipation in devices based on InAs-Al nanowires and reveal that cooling of superconducting islands is limited by the rather inefficient electron-phonon coupling, as opposed to grounded superconductors that primarily cool by quasiparticle diffusion. We show that powers as low as 50-150 pW are able to suppress superconductivity on the islands. Applied microwaves lead to similar heating effects but are affected by the interplay of the microwave frequency and the effective electron-phonon relaxation time.

11.
Nano Lett ; 24(19): 5904-5912, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38700588

RESUMO

Stretchable electroluminescent devices represent an emerging optoelectronic technology for future wearables. However, their typical construction on sub-millimeter-thick elastomers has limited moisture permeability, leading to discomfort during long-term skin attachment. Although breathable textile displays may partially address this issue, they often have distinct visual appearances with discrete emissions from fibers or fiber junctions. This study introduces a convenient procedure to create stretchable, permeable displays with continuous luminous patterns. The design utilizes ultrathin nanocomposite devices embedded in a porous elastomeric microfoam to achieve high moisture permeability. These displays also exhibit excellent deformability, low-voltage operation, and excellent durability. Additionally, the device is decorated with fluorinated silica nanoparticles to achieve self-cleaning and washable capabilities. The practical implementation of these nanocomposite devices is demonstrated by creating an epidermal counter display that allows intimate integration with the human body. These developments provide an effective design of stretchable and breathable displays for comfortable wearing.

12.
Nano Lett ; 24(23): 6897-6905, 2024 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-38805366

RESUMO

Aluminum nanocrystals created by catalyst-driven colloidal synthesis support excellent plasmonic properties, due to their high level of elemental purity, monocrystallinity, and controlled size and shape. Reduction in the rate of nanocrystal growth enables the synthesis of highly anisotropic Al nanowires, nanobars, and singly twinned "nanomoustaches". Electron energy loss spectroscopy was used to study the plasmonic properties of these nanocrystals, spanning the broad energy range needed to map their plasmonic modes. The coupling between these nanocrystals and other plasmonic metal nanostructures, specifically Ag nanocubes and Au films of controlled nanoscale thickness, was investigated. Al nanocrystals show excellent long-term stability under atmospheric conditions, providing a practical alternative to coinage metal-based nanowires in assembled nanoscale devices.

13.
Nano Lett ; 24(22): 6644-6650, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38767455

RESUMO

Phase separation is an intriguing phenomenon often found in III-V nanostructures, but its effect on the atomic and electronic structures of III-V nanomaterials is still not fully understood. Here we study the variations in atomic arrangement and band structure due to the coexistence of wurtzite (WZ) and zinc blende (ZB) phases in single GaAs nanowires by using scanning transmission electron microscopy and monochromated electron energy loss spectroscopy. The WZ lattice distances are found to be larger (by ∼1%), along both the nanowire length direction and the perpendicular direction, than the ZB lattice. The band gap of the WZ phase is ∼20 meV smaller than that of the ZB phase. A shift of ∼70 meV in the conduction band edge between the two phases is also found. The direct and local measurements in single GaAs nanowires reveal important effects of phase separation on the properties of individual III-V nanostructures.

14.
Nano Lett ; 24(4): 1309-1315, 2024 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-38258741

RESUMO

Electrically percolating nanowire networks are among the most promising candidates for next-generation transparent electrodes. Scientific interest in these materials stems from their intrinsic current distribution heterogeneity, leading to phenomena like percolating pathway rerouting and localized self-heating, which can cause irreversible damage. Without an experimental technique to resolve the current distribution and an underpinning nonlinear percolation model, one relies on empirical rules and safety factors to engineer materials. We introduce Bose-Einstein condensate microscopy to address the longstanding problem of imaging active current flow in 2D materials. We report on performance improvement of this technique whereby observation of dynamic redistribution of current pathways becomes feasible. We show how this, combined with existing thermal imaging methods, eliminates the need for assumptions between electrical and thermal properties. This will enable testing and modeling individual junction behavior and hot-spot formation. Investigating both reversible and irreversible mechanisms will contribute to improved performance and reliability of devices.

15.
Nano Lett ; 24(3): 790-796, 2024 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-38189790

RESUMO

We experimentally and computationally investigate the magneto-conductance across the radial heterojunction of InAs-GaSb core-shell nanowires under a magnetic field, B, up to 30 T and at temperatures in the range 4.2-200 K. The observed double-peak negative differential conductance markedly blue-shifts with increasing B. The doublet accounts for spin-polarized currents through the Zeeman split channels of the InAs (GaSb) conduction (valence) band and exhibits strong anisotropy with respect to B orientation and marked temperature dependence. Envelope function approximation and a semiclassical (WKB) approach allow to compute the magnetic quantum states of InAs and GaSb sections of the nanowire and to estimate the B-dependent tunneling current across the broken-gap interface. Disentangling different magneto-transport channels and a thermally activated valence-to-valence band transport current, we extract the g-factor from the spin-up and spin-down dI/dV branch dispersion, revealing a giant, strongly anisotropic g-factor in excess of 60 (100) for the radial (tilted) field configurations.

16.
Nano Lett ; 24(21): 6233-6239, 2024 May 29.
Artigo em Inglês | MEDLINE | ID: mdl-38758973

RESUMO

We study the molecular beam epitaxy of rock-salt ScN on the wurtzite GaN(11̅00) surface. To this end, ScN is grown on freestanding GaN(11̅00) substrates and self-assembled GaN nanowires exhibiting (11̅00) sidewalls. On both substrates, ScN crystallizes twin-free thanks to a specific epitaxial relationship, namely ScN(110)[001]∥GaN(11̅00)[0001], providing a congruent, low-symmetry interface. The 13.1% uniaxial lattice mismatch occurring in this orientation mostly relaxes within the first few monolayers of growth by forming a near-coincidence site lattice, where 7 GaN planes coincide with 8 ScN planes, leaving the ScN surface nearly free of extended defects. Overgrowth of the ScN with GaN leads to a kinetic stabilization of the zinc blende phase, that rapidly develops wurtzite inclusions nucleating on {111} nanofacets, commonly observed during zinc blende GaN growth. Our ScN/GaN(11̅00) platform opens a new route for the epitaxy of twin-free metal-semiconductor heterostructures including closely lattice-matched GaN, ScN, HfN, and ZrN compounds.

17.
Small ; : e2400784, 2024 Jun 04.
Artigo em Inglês | MEDLINE | ID: mdl-38837286

RESUMO

Marine biofouling is a complex and dynamic process that significantly increases the carbon emissions from the maritime industry by increasing drag losses. However, there are no existing non-toxic marine paints that can achieve both effective fouling reduction and efficient fouling release. Inspired by antifouling strategies in nature, herein, a superoleophobic zwitterionic nanowire coating with a nanostructured hydration layer is introduced, which exhibits simultaneous fouling reduction and release performance. The zwitterionic nanowires demonstrate >25% improvement in fouling reduction compared to state-of-the-art antifouling nanostructures, and four times higher fouling-release compared to conventional zwitterionic coatings. Fouling release is successfully achieved under a wall shear force that is four orders of magnitude lower than regular water jet cleaning. The mechanism of this simultaneous fouling reduction and release behavior is explored, and it is found that a combination of 1) a mechanical biocidal effect from the nanowire geometry, and 2) low interfacial adhesion resulting from the nanostructured hydration layer, are the major contributing factors. These findings provide insights into the design of nanostructured coatings with simultaneous fouling reduction and release. The newly established synthesis procedure for the zwitterionic nanowires opens new pathways for implementation as antifouling coatings in the maritime industry and biomedical devices.

18.
Small ; 20(27): e2308796, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38363026

RESUMO

A race to achieve a crossover from positive to negative magnetoresistance is intense in the field of nanostructured materials to reduce the size of memory devices. Here, the unusual complex magnetoresistance in nonmagnetic sulfur-doped Sb2Se3 nanowires is demonstrated. Intentionally, sulfur is doped in such a way to nearly achieve the charge neutrality point that is evident from switching of carrier type from p-type to n-type at 13 K as inferred from the low-temperature thermoelectric power measurements. A change from 3D variable range hopping (VRH) to power law transport with α = 0.18  in resistivity measurement signifies a Luttinger liquid transport with weak links through the nanowires. Interestingly, high magnetic field induced negative magnetoresistance (NMR) occurring in hole dominated temperature regimes can only be explained by invoking the concept of charge puddles. Spot energy dispersive spectroscopy (EDS), magnetic force microscopy (MFM) measurements, Tmott and Regel plot indicate an enhanced disorder in these sulfurized nanowires that are found to be the precursor for the formation of these charge puddles. Tunability of conducting states in these nanowires is investigated in the light of interplay of carrier type, magnetic field, temperature, and intricate intra-inter wire transport that makes this nanowires potential for large scale spintronic devices.

19.
Small ; 20(1): e2304614, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37670206

RESUMO

Nanowires (NWs) are among the most studied nanostructures as they have numerous promising applications thanks to their various unique properties. Furthermore, the properties of NWs can be tailored during synthesis by introducing structural defects such as nano-twins, periodic polytypes, and kinks, i.e., abrupt changes in their axial direction. Here, this work reports for the first time the postsynthesis formation of such defects, achieved by exploiting a peculiar plasticity that may occur in nanosized covalent materials. Specifically, in this work the authors found that single-crystal CuO NWs can form double kinks when subjected to external mechanical loading. Both the microscopy and atomistic modeling suggest that deformation-induced twinning along the ( 1 ¯ 10 ) $( {\bar{1}10} )$ plane is the mechanism behind this effect. In a single case the authors are able to unkink a NW back to its initial straight profile, indicating the possibility of reversible plasticity in CuO NWs, which is supported by the atomistic simulations. The phenomenon reported here provides novel insights into the mechanisms of plastic deformation in covalent NWs and offers potential avenues for developing techniques to customize the shape of NWs postsynthesis and introduce new functionalities.

20.
Small ; 20(6): e2305366, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37792210

RESUMO

Metal nanoclusters (NCs) with atomic precision are growing into a fascinating class of building blocks for supramolecular chemistry. What makes it more interesting is the enhanced optical properties of the ordered structures, including aggregation-induced emission (AIE). However, algorithm dictating the self-assembly of metal NCs in multicomponent environment remains largely unknown, and effective means to manipulate the self-assembly is still lacking, especially under kinetic control. Herein, nanofibers which contain sub-1 nm nanowires and exhibit circularly polarized phosphorescence (CPP) are obtained from crystallization-induced self-assembly (CISA) of water-soluble, negatively charged silver NCs (Ag9 -NCs) in the presence of glutamic acid (Glu). By the introduction of a positively-charged additive (choline chloride, CC), the structure of the nanowires is modulated and the lateral interaction between adjacent nanofibers is adjusted, leading to simultaneous improvement of the phosphorescence and chirality which finally enhances CPP. Importantly, changing the time at which CC is introduced altered the kinetic pathway of the CISA, which enables to effectively manipulate both the final structures of the self-assembled Ag9 -NCs and the output of the optical signals.

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