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1.
ACS Nano ; 15(7): 12019-12033, 2021 Jul 27.
Artículo en Inglés | MEDLINE | ID: mdl-34157222

RESUMEN

In order to reduce medical facility overload due to the rise of the elderly population, modern lifestyle diseases, or pandemics, the medical industry is currently developing point-of-care and home medical device systems. Diabetes is an incurable and lifetime disease, accountable for a significant mortality and socio-economic public health burden. Thus, tight glucose control in diabetic patients, which can prevent the onset of its late complications, is of enormous importance. Despite recent advances, the current best achievable management of glucose control is still inadequate, due to several key limitations in the system components, mainly related to the reliability of sensing components, both temporally and chemically, and the integration of sensing and delivery components in a single wearable platform, which is yet to be achieved. Thus, advanced closed-loop artificial pancreas systems able to modulate insulin delivery according to the measured sensor glucose levels, independently of patient supervision, represent a key requirement of development efforts. Here, we demonstrate a minimally invasive, transdermal, multiplex, and versatile continuous metabolites monitoring system in the subcutaneous interstitial fluid space based on a chemically modified SiNW-FET nanosensor array on microneedle elements. Using this technology, ISF-borne metabolites require no extraction and are measured directly and continuously by the nanosensors. Due to their chemical sensing mechanism, the nanosensor response is only influenced by the specific metabolite of interest, and no response is observed in the presence of potential exogenous and endogenous interferents known to seriously affect the response of current electrochemical glucose detection approaches. The 2D architecture of this platform, using a single SOI substrate as a top-down multipurpose material, resulted in a standard fabricated chip with 3D functionality. After proving the ability of the system to act as a selective multimetabolites sensor, we have implemented our platform to reach our main goal for in vivo continuous glucose monitoring of healthy human subjects. Furthermore, minor adjustments to the fabrication technique allow the on-chip integration of microinjection needle elements, which can ideally be used as a drug delivery system. Preliminary experiments on a mice animal model successfully demonstrated the single-chip capability to both monitor glucose levels as well as deliver insulin. By that, we hope to provide in the future a cost-effective and reliable wearable personalized clinical tool for patients and a strong tool for research, which will be able to perform direct monitoring of clinical biomarkers in the ISF as well as synchronized transdermal drug delivery by this single-chip multifunctional platform.


Asunto(s)
Páncreas Artificial , Dispositivos Electrónicos Vestibles , Anciano , Humanos , Ratones , Animales , Automonitorización de la Glucosa Sanguínea , Glucemia , Reproducibilidad de los Resultados , Insulina
2.
J Nanobiotechnology ; 19(1): 51, 2021 Feb 17.
Artículo en Inglés | MEDLINE | ID: mdl-33596905

RESUMEN

Programmable nano-bio interfaces driven by tuneable vertically configured nanostructures have recently emerged as a powerful tool for cellular manipulations and interrogations. Such interfaces have strong potential for ground-breaking advances, particularly in cellular nanobiotechnology and mechanobiology. However, the opaque nature of many nanostructured surfaces makes non-destructive, live-cell characterization of cellular behavior on vertically aligned nanostructures challenging to observe. Here, a new nanofabrication route is proposed that enables harvesting of vertically aligned silicon (Si) nanowires and their subsequent transfer onto an optically transparent substrate, with high efficiency and without artefacts. We demonstrate the potential of this route for efficient live-cell phase contrast imaging and subsequent characterization of cells growing on vertically aligned Si nanowires. This approach provides the first opportunity to understand dynamic cellular responses to a cell-nanowire interface, and thus has the potential to inform the design of future nanoscale cellular manipulation technologies.


Asunto(s)
Nanotecnología/métodos , Nanocables/química , Óptica y Fotónica , Silicio/química , Instalación Eléctrica , Ensayo de Materiales , Nanoestructuras/química
3.
Langmuir ; 36(16): 4556-4562, 2020 04 28.
Artículo en Inglés | MEDLINE | ID: mdl-32239960

RESUMEN

In biological systems, membrane proteins play major roles in energy conversion, transport, sensing, and signal transduction. Of special interest are the photosynthetic reaction centers involved in the initial process of light energy conversion to electrical and chemical energies. The oriented binding of membrane proteins to solid surfaces is important for biotechnological applications. In some cases, novel properties are generated as a result of the interaction between proteins and solid surfaces. We developed a novel approach for the oriented tagging of membrane proteins. In this unique process, bifunctional molecules are used to chemically tag the exposed surfaces of membrane proteins at selected sides of membrane vesicles. The isolated tagged membrane proteins were self-assembled on solid surfaces, leading to the fabrication of dens-oriented layers on metal and glass surfaces, as seen from the atomic force microscopy (AFM) images. In this work, we used chromatophores and membrane vesicles containing protein chlorophyll complexes for the isolation of the bacterial reaction center and photosystem I, from photosynthetic bacteria and cyanobacteria, respectively. The oriented layers, which were fabricated on metal surfaces, were functional and generated light-induced photovoltage that was measured by the Kalvin probe apparatus. The polarity of the photovoltage depended on the orientation of proteins in the layers. Other membrane proteins can be tagged by the same method. However, we preferred the use of reaction centers because their orientation can be easily detected by the polarity of their photovoltages.


Asunto(s)
Proteínas Bacterianas/química , Proteínas Inmovilizadas/química , Complejo de Proteína del Fotosistema I/química , Proteínas Bacterianas/efectos de la radiación , Reactivos de Enlaces Cruzados/química , Electroquímica , Oro/química , Proteínas Inmovilizadas/efectos de la radiación , Luz , Liposomas/química , Complejo de Proteína del Fotosistema I/efectos de la radiación , Rhodobacter/enzimología , Succinimidas/química , Synechocystis/enzimología
4.
Nano Lett ; 19(9): 5868-5878, 2019 09 11.
Artículo en Inglés | MEDLINE | ID: mdl-31381354

RESUMEN

The analysis of biosamples, e.g., blood, is a ubiquitous task of proteomics, genomics, and biosensing fields; yet, it still faces multiple challenges, one of the greatest being the selective separation and detection of target proteins from these complex biosamples. Here, we demonstrate the development of an on-chip light-triggered reusable nanostructured selective and quantitative protein separation and preconcentration platform for the direct analysis of complex biosamples. The on-chip selective separation of required protein analytes from raw biosamples is performed using antibody-photoacid-modified Si nanopillars vertical arrays (SiNPs) of ultralarge binding surface area and enormously high binding affinity, followed by the light-controlled rapid release of the tightly bound target proteins in a controlled liquid media. Two important experimental observations are presented: (1) the first demonstration on the control of biological reaction binding affinity by the nanostructuring of the capturing surface, leading to highly efficient protein collection capabilities, and (2) the light-triggered switching of the highly sticky binding surfaces into highly reflective nonbinding surfaces, leading to the rapid and quantitative release of the originally tightly bound protein species. Both of these two novel behaviors were theoretically and experimentally investigated. Importantly, this is the first demonstration of a three-dimensional (3D) SiNPs on-chip filter with ultralarge binding surface area and reversible light-controlled quantitative release of adsorbed biomolecules for direct purification of blood samples, able to selectively collect and separate specific low abundant proteins, while easily removing unwanted blood components (proteins, cells) and achieving desalting results, without the requirement of time-consuming centrifugation steps, the use of desalting membranes, or affinity columns.


Asunto(s)
Proteínas Sanguíneas/aislamiento & purificación , Dispositivos Laboratorio en un Chip , Nanoestructuras/química , Proteínas Sanguíneas/química , Humanos , Luz , Unión Proteica/efectos de la radiación , Silicio/química , Propiedades de Superficie
5.
Nano Lett ; 18(1): 190-201, 2018 01 10.
Artículo en Inglés | MEDLINE | ID: mdl-29202247

RESUMEN

Silicon-based photodetectors cannot distinguish between different wavelengths. Therefore, these detectors relay on color-specific filters to achieve color separation. Color filters add complexity to color sensitive device fabrication, and hinder miniaturization of such devices. Here, we report an ultrasmall (as small as ∼20 nm by 300 nm), red-green-blue-violet (RGBV) filter-free spectrally gated field effect transistor (SGFET) detectors. These photodetectors are based on organic-silicon nanowire hybrid FET devices, capable of detecting specific visible wavelength spectrum with full width at half-maxima (fwhm) under 100 nm. Each SGFET is controlled by a distinctive RGBV spectral range, according to its specific organic fluorophore functionalization. The spectral-specific RGBV detection is accomplished via covalent attachment of different fluorophores. The fluorophore molecules inject electrons into the nanowire structure as a result of light absorption at the appropriate RGBV spectral range. These photoinduced electrons modify the occupancies of the oxide's surface states, shifting the device threshold voltage, thus changing its conductivity, and functioning as a negative stress bias in a p-type SiNW FETs. A positive biasing can be achieved via UV light-induced ionization, which leads to detrapping and translocation of electrons at the oxide layer. Furthermore, a novel theoretical model on the mechanism of action of these devices was developed. Also, we show that suspended SGFETs can function as nonvolatile memory elements, which unlike fast-relaxing on-surface SGFETs, can store discrete "on" (RGBV illumination) and "off" (UV illumination) states for several days at ambient conditions. We also demonstrate a unique single-nanowire multicolor photodetector, enabling in principle a broad spectral detection over a single silicon nanowire element. These highly compact, spectral-controlled nanodevices have the potential to serve in various future novel optoelectric applications.

6.
Nano Lett ; 16(11): 6960-6966, 2016 11 09.
Artículo en Inglés | MEDLINE | ID: mdl-27753499

RESUMEN

Here, we demonstrate a novel method for the production of single-crystal Si nanowire arrays based on the top-down carving of Si-nanowall structures from a donor substrate, and their subsequent controlled and selective harvesting into a sacrificial solid material block. Nanosectioning of the nanostructures-embedding block by ultramicrotome leads to the formation of size, shape, and orientation-controlled high quality nanowire arrays. Additionally, we introduce a novel approach that enables transferring the nanowire arrays to any acceptor substrate, while preserving their orientation, and placing them on defined locations. Furthermore, crystallographic analysis and electrical measurements were performed, proving that the quality of the sectioned nanowires, which derive from their original crystalline donor substrate, are remarkably preserved.

7.
Nat Commun ; 6: 7334, 2015 Jun 09.
Artículo en Inglés | MEDLINE | ID: mdl-26055942

RESUMEN

Molecule-plasmon interactions have been shown to have a definite role in light propagation through optical microcavities due to strong coupling between molecular excitations and surface plasmons. This coupling can lead to macroscopic extended coherent states exhibiting increment in temporal and spatial coherency and a large Rabi splitting. Here, we demonstrate spatial modulation of light transmission through a single microcavity patterned on a free-standing Au film, strongly coupled to one of the most efficient energy transfer photosynthetic proteins in nature, photosystem I. Here we observe a clear correlation between the appearance of spatial modulation of light and molecular photon absorption, accompanied by a 13-fold enhancement in light transmission and the emergence of a distinct electromagnetic standing wave pattern in the cavity. This study provides the path for engineering various types of bio-photonic devices based on the vast diversity of biological molecules in nature.

8.
Angew Chem Int Ed Engl ; 53(34): 8953-8, 2014 Aug 18.
Artículo en Inglés | MEDLINE | ID: mdl-24989350

RESUMEN

Photosystem I (PSI) is one of the most studied electron transfer (ET) systems in nature; it is found in plants, algae, and bacteria. The effect of the system structure and its electronic properties on the electron transfer rate and yield was investigated for years in details. In this work we show that not only those system properties affect the ET efficiency, but also the electrons' spin. Using a newly developed spintronic device and a technique which enables control over the orientation of the PSI monolayer relative to the device (silver) surface, it was possible to evaluate the degree and direction of the spin polarization in ET in PSI. We find high-spin selectivity throughout the entire ET path and establish that the spins of the electrons being transferred are aligned parallel to their momenta. The spin selectivity peaks at 300 K and vanishes at temperatures below about 150 K. A mechanism is suggested in which the chiral structure of the protein complex plays an important role in determining the high-spin selectivity and its temperature dependence. Our observation of high light induced spin dependent ET in PSI introduces the possibility that spin may play an important role in ET in biology.


Asunto(s)
Transporte de Electrón , Complejo de Proteína del Fotosistema I/química
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