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1.
Nano Lett ; 2020 May 11.
Artigo em Inglês | MEDLINE | ID: mdl-32364741

RESUMO

Herein, plasmonic metal tripod nanoframes with three-fold symmetry were synthesized in a high yield (∼83%), and their electric field distribution and single-particle surface-enhanced Raman scattering (SERS) were studied. We realized such complex frame morphology by synthesizing analogous tripod nanoframes through multiple transformations. The precise control of the Au growth pattern led to uniform tripod nanoframes embedded with circle or line-shaped hot spots. The linear-shaped nanogaps ("Y"-shaped hot-zone) of the frame structures can strongly and efficiently confine the electric field, allowing for strong SERS signals. Coupled with a high synthetic yield of the targeted frame structure, strong and uniform SERS signals were obtained inside the nanoframe gaps. Remarkably, quite reproducible SERS signals were obtained with these structures-the SERS enhancement factors with an average value of 7.9 × 107 with a distribution of enhancement factors from 2.2 × 107 to 2.2 × 108 for 45 measured individual particles.

2.
Adv Mater ; : e2001360, 2020 May 25.
Artigo em Inglês | MEDLINE | ID: mdl-32449217

RESUMO

Since infectious diseases, particularly viral infections, have threatened human health and caused huge economical losses globally, a rapid, sensitive, and selective virus detection platform is highly demanded. Enzyme-linked immunosorbent assay (ELISA) with flat solid substrates has been dominantly used in detecting whole viruses for its straightforwardness and simplicity in assay protocols, but it often suffers from limited sensitivity, poor quantification range, and a time-consuming assay procedure. Here, a lipid-nanopillar-array-based immunosorbent assay (LNAIA) is developed with a nanopillar-supported lipid bilayer substrate with fluorophore-modified antibodies for rapid, sensitive, and quantitative detection of viruses. 3D nanopillar array structures and fluid antibodies with fluorophores facilitate faster and efficient target binding and rapid fluorophore localization for quick, reliable analysis on binding events with a conventional fluorescence microscopy setup. LNAIA enables quantification of H1N1 virus that targets down to 150 virus particles with 5-orders-of-magnitude dynamic range within 25 min, which cannot be achieved with conventional ELISA platforms.

3.
Nat Nanotechnol ; 15(4): 321-330, 2020 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-32042163

RESUMO

Extracellular potassium concentration affects the membrane potential of neurons, and, thus, neuronal activity. Indeed, alterations of potassium levels can be related to neurological disorders, such as epilepsy and Alzheimer's disease, and, therefore, selectively detecting extracellular potassium would allow the monitoring of disease. However, currently available optical reporters are not capable of detecting small changes in potassium, in particular, in freely moving animals. Furthermore, they are susceptible to interference from sodium ions. Here, we report a highly sensitive and specific potassium nanosensor that can monitor potassium changes in the brain of freely moving mice undergoing epileptic seizures. An optical potassium indicator is embedded in mesoporous silica nanoparticles, which are shielded by an ultrathin layer of a potassium-permeable membrane, which prevents diffusion of other cations and allows the specific capturing of potassium ions. The shielded nanosensor enables the spatial mapping of potassium ion release in the hippocampus of freely moving mice.

4.
ACS Nano ; 14(1): 28-117, 2020 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-31478375

RESUMO

The discovery of the enhancement of Raman scattering by molecules adsorbed on nanostructured metal surfaces is a landmark in the history of spectroscopic and analytical techniques. Significant experimental and theoretical effort has been directed toward understanding the surface-enhanced Raman scattering (SERS) effect and demonstrating its potential in various types of ultrasensitive sensing applications in a wide variety of fields. In the 45 years since its discovery, SERS has blossomed into a rich area of research and technology, but additional efforts are still needed before it can be routinely used analytically and in commercial products. In this Review, prominent authors from around the world joined together to summarize the state of the art in understanding and using SERS and to predict what can be expected in the near future in terms of research, applications, and technological development. This Review is dedicated to SERS pioneer and our coauthor, the late Prof. Richard Van Duyne, whom we lost during the preparation of this article.

5.
Chem Rev ; 119(24): 12208-12278, 2019 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-31794202

RESUMO

Plasmonic nanostructures possessing unique and versatile optoelectronic properties have been vastly investigated over the past decade. However, the full potential of plasmonic nanostructure has not yet been fully exploited, particularly with single-component homogeneous structures with monotonic properties, and the addition of new components for making multicomponent nanoparticles may lead to new-yet-unexpected or improved properties. Here we define the term "multi-component nanoparticles" as hybrid structures composed of two or more condensed nanoscale domains with distinctive material compositions, shapes, or sizes. We reviewed and discussed the designing principles and synthetic strategies to efficiently combine multiple components to form hybrid nanoparticles with a new or improved plasmonic functionality. In particular, it has been quite challenging to precisely synthesize widely diverse multicomponent plasmonic structures, limiting realization of the full potential of plasmonic heterostructures. To address this challenge, several synthetic approaches have been reported to form a variety of different multicomponent plasmonic nanoparticles, mainly based on heterogeneous nucleation, atomic replacements, adsorption on supports, and biomolecule-mediated assemblies. In addition, the unique and synergistic features of multicomponent plasmonic nanoparticles, such as combination of pristine material properties, finely tuned plasmon resonance and coupling, enhanced light-matter interactions, geometry-induced polarization, and plasmon-induced energy and charge transfer across the heterointerface, were reported. In this review, we comprehensively summarize the latest advances on state-of-art synthetic strategies, unique properties, and promising applications of multicomponent plasmonic nanoparticles. These plasmonic nanoparticles including heterostructured nanoparticles and composite nanostructures are prepared by direct synthesis and physical force- or biomolecule-mediated assembly, which hold tremendous potential for plasmon-mediated energy transfer, magnetic plasmonics, metamolecules, and nanobiotechnology.

7.
Nanoscale ; 11(43): 20379-20391, 2019 Nov 21.
Artigo em Inglês | MEDLINE | ID: mdl-31642457

RESUMO

Surface-enhanced Raman scattering (SERS)-based sensors utilize the electromagnetic-field enhancement of plasmonic substrates with the chemical specificity of vibrational Raman spectroscopy to identify trace amounts of a wide variety of different target analytes while being minimally affected by photobleaching. However, despite many advantageous features of this method, SERS sensors, particularly for detecting hazardous chemicals, suffer from several limitations such as requirement of gigantic signal enhancement that is often poorly controllable, subtle change and degradation of the SERS substrate, consecutive fluctuation of the signal, the lack of reliable receptors for capturing targets of interest and the absence of general principles for detecting various chemicals in different phases and matrices. To overcome these limitations and for SERS sensors to find practical use, one must (1) acknowledge the characteristics of the matrices of target systems, (2) finely engineer and tune the receptors of the SERS sensor to properly extract the target analyte from the phase, and (3) implement additional mechanistic modifications to enhance the plasmonic signal. This minireview underlines the difficulties associated with different phases and a wide range of target analytes, and introduces the practical measures undertaken to overcome the respective difficulties in SERS-based detection of hazardous chemicals.

8.
Acc Chem Res ; 52(10): 2793-2805, 2019 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-31553568

RESUMO

Plasmonic nanoparticles are widely exploited in diverse bioapplications ranging from therapeutics to biosensing and biocomputing because of their strong and tunable light-matter interactions, facile and versatile chemical/biological ligand modifications, and biocompatibility. With the rapid growth of nanobiotechnology, understanding dynamic interactions between nanoparticles and biological systems at the molecular or single-particle level is becoming increasingly important for interrogating biological systems with functional nanostructures and for developing nanoparticle-based biosensors and therapeutic agents. Therefore, significant efforts have been devoted to precisely design and create nano-bio interfaces by manipulating the nanoparticles' size, shape, and surface ligand interactions with complex biological systems to maximize their performance and avoid unwanted responses, such as their agglomeration and cytotoxicity. However, investigating physicochemical interactions at the nano-bio interfaces in a quantitative and controllable manner remains challenging, as the interfaces involve highly complex networks between nanoparticles, biomolecules, and cells across multiple scales, each with a myriad of different chemical and biological interactions. A lipid bilayer is a membrane made of two layers of lipid molecules that forms a barrier around cells and plays structural and functional roles in diverse biological processes because they incorporate and present functional molecules (such as membrane proteins) with lateral fluidity. Plasmonic nanoparticles conjugated on lipid membranes provide reliable analytical labels and functional moieties that allow for studying and manipulating interactions between nanoparticles and molecules with single-particle resolution; they also serve as efficient tools for applying optical, mechanical, and thermal stimuli to biological systems, which stem from plasmonic properties. Recently, new opportunities have emerged by interfacing nanoparticle-modified lipid bilayers (NLBs) with complex systems such as molecular circuits and living systems. In this Account, we briefly review how plasmonic properties can be beneficially harnessed on lipid bilayer membranes to investigate the structures and functions of cellular membranes and to develop new platforms for biomedical applications. In particular, we discuss the versatility of supported lipid bilayers (SLBs), which are planar lipid bilayers on hydrophilic substrates, as dynamic biomaterials that provide lateral fluidity and cell membrane-like environments. We then summarize our efforts to create a quantitative analytical platform utilizing nanoparticles as active building blocks and SLBs as integrative substrates. Through this bottom-up approach, various functionalized nanoparticles have been introduced onto lipid bilayers to render nanoparticle-nanoparticle, nanoparticle-lipid bilayer, and biomolecule-lipid bilayer interfaces programmable. Our system provides a new class of tools for studying thermodynamics and kinetics in complex networks of nanostructures and for realizing unique applications in biosensing and biocomputing.

9.
Adv Sci (Weinh) ; 6(17): 1900471, 2019 Sep 04.
Artigo em Inglês | MEDLINE | ID: mdl-31508273

RESUMO

Recent advances of plasmonic nanoparticles include fascinating developments in the fields of energy, catalyst chemistry, optics, biotechnology, and medicine. The plasmonic photothermal properties of metallic nanoparticles are of enormous interest in biomedical fields because of their strong and tunable optical response and the capability to manipulate the photothermal effect by an external light source. To date, most biomedical applications using photothermal nanoparticles have focused on photothermal therapy; however, to fully realize the potential of these particles for clinical and other applications, the fundamental properties of photothermal nanoparticles need to be better understood and controlled, and the photothermal effect-based diagnosis, treatment, and theranostics should be thoroughly explored. This Progress Report summarizes recent advances in the understanding and applications of plasmonic photothermal nanoparticles, particularly for sensing, imaging, therapy, and drug delivery, and discusses the future directions of these fields.

10.
Chem Sci ; 10(27): 6594-6603, 2019 Jul 21.
Artigo em Inglês | MEDLINE | ID: mdl-31367310

RESUMO

In this work, we showed the tuning of the catalytic behavior of dendritic plasmonic colloidosomes (DPCs) by plasmonic hotspots. A cycle-by-cycle solution-phase synthetic protocol yielded high-surface-area DPCs by controlled nucleation-growth of gold nanoparticles. These DPCs, which had varying interparticle distances and particle-size distribution, absorb light over the entire visible region as well as in the near-infrared region of the solar spectrum, transforming gold into black gold. They produced intense hotspots of localized electric fields as well as heat, which were quantified and visualized by Raman thermometry and electron energy loss spectroscopy plasmon mapping. These DPCs can be effectively utilized for the oxidation reaction of cinnamyl alcohol using pure oxygen as the oxidant, hydrosilylation of aldehydes, temperature jump assisted protein unfolding and purification of seawater to drinkable water via steam generation. Black gold DPCs also convert CO2 to methane (fuel) at atmospheric pressure and temperature, using solar energy.

11.
Anal Chem ; 91(16): 10467-10476, 2019 Aug 20.
Artigo em Inglês | MEDLINE | ID: mdl-31265240

RESUMO

Surface-enhanced Raman scattering (SERS)-based sensing is promising in that it has potential to allow for highly sensitive, selective, and multiplexed detection and imaging. However, the controlled assembly and gap formation between plasmonic particles for generating strong SERS signals in a quantitative manner is highly challenging, especially on biodetection platforms, and particle-to-particle variation in the signal enhancement can vary by several orders of magnitude in a single batch, largely limiting the reliable use of SERS for practical sensing applications. Here, a hierarchic-nanocube-assembly based SERS (H-Cube-SERS) bioassay to controllably amplify the electromagnetic field between gold nanocubes (AuNCs) is developed. Based on this strategy, H-Cube-SERS assay allows for detecting target DNA with a wide dynamic range from 100 aM to 10 pM concentrations in a stable and reproducible manner. It is also found that the uniformly formed AuNCs with flat surfaces are much more suitable for highly sensitive, reliable, and quantitative biodetection assays due to faster DNA binding kinetics, sharper DNA melting transition, wider hot spot regions, and less dependence on light polarization direction than spherical Au nanoparticles with curved interfaces. This work paves the pathways to the quantitative and sensitive biodetection on a SERS platform and can be extended to other particle assembly systems.

12.
Small ; 15(26): e1900998, 2019 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-31026121

RESUMO

Biocomputation is the algorithmic manipulation of biomolecules. Nanostructures, most notably DNA nanostructures and nanoparticles, become active substrates for biocomputation when modified with stimuli-responsive, programmable biomolecular ligands. This approach-biocomputing with nanostructures ("nano-bio computing")-allows autonomous control of matter and information at the nanoscale; their dynamic assemblies and beneficial properties can be directed without human intervention. Recently, lipid bilayers interfaced with nanostructures have emerged as a new biocomputing platform. This new nano-bio interface, which exploits lipid bilayers as a chemical circuit board for information processing, offers a unique reaction space for realizing nanostructure-based computation at a previously unexplored dimension. In this Concept, recent advances in nano-bio computing are briefly reviewed and the newly emerging concept of biocomputing with nanostructures on lipid bilayers is introduced.

13.
Sci Adv ; 5(2): eaau2124, 2019 02.
Artigo em Inglês | MEDLINE | ID: mdl-30801008

RESUMO

Using nanoparticles as substrates for computation enables algorithmic and autonomous controls of their unique and beneficial properties. However, scalable architecture for nanoparticle-based computing systems is lacking. Here, we report a platform for constructing nanoparticle logic gates and circuits at the single-particle level on a supported lipid bilayer. Our "lipid nanotablet" platform, inspired by cellular membranes that are exploited to compartmentalize and control signaling networks, uses a lipid bilayer as a chemical circuit board and nanoparticles as computational units. On a lipid nanotablet, a single-nanoparticle logic gate senses molecules in solution as inputs and triggers particle assembly or disassembly as an output. We demonstrate a set of Boolean logic operations, fan-in/fan-out of logic gates, and a combinational logic circuit such as a multiplexer. We envisage that our approach to modularly implement nanoparticle circuits on a lipid bilayer will create new paradigms and opportunities in molecular computing, nanoparticle circuits, and systems nanoscience.

14.
ACS Cent Sci ; 4(10): 1303-1314, 2018 Oct 24.
Artigo em Inglês | MEDLINE | ID: mdl-30410968

RESUMO

Plasmonics, the study of the interactions between photons and collective oscillations of electrons, has seen tremendous advances during the past decade. Controllable nanometer- and sub-nanometer-scale engineering in plasmonic resonance and electromagnetic field localization at the subwavelength scale have propelled diverse studies in optics, materials science, chemistry, biotechnology, energy science, and various applications in spectroscopy. However, for translation of these accomplishments from research into practice, major hurdles including low reproducibility and poor controllability in target structures must be overcome, particularly for reliable quantification of plasmonic signals and functionalities. This Outlook introduces and summarizes the recent attempts and findings of many groups toward more quantitative and reliable nanoplasmonics, and discusses the challenges and possible future directions.

16.
Nano Lett ; 18(10): 6475-6482, 2018 10 10.
Artigo em Inglês | MEDLINE | ID: mdl-30153413

RESUMO

Synthesizing plasmonic nanostructures in an ultraprecise manner is of paramount importance because the nanometer-scale structural details can significantly affect their plasmonic properties. Au nanocubes (AuNCs) have been a highly promising, heavily studied nanostructure with high potential in various fields, but an ultraprecise synthesis from 10 to 100 nm in size over a large number of AuNCs has not been well established. Precisely structured AuNC-based studies for a highly reproducible, quantitative plasmonic signal generation [e.g., quantitative surface-enhanced Raman scattering (SERS)] are needed for reliable use and exploration in the beneficial properties of AuNCs. Here, we developed a strategy for AuNC synthesis with the desired size and shape, ranging from 17 to 78 nm particularly with highly controlled corner sharpness, by precisely controlling the growth rate of different facets and AuNC-specific flocculation which enabled ultrahigh yields (∼98-99%). Importantly, the precisely shaped AuNCs can scatter light in a spectrally reproducible manner, and the SERS enhancement factors (EFs) for the AuNC dimers are very narrowly distributed (the EFs of 72 nm sharp-cornered cube dimers have a distribution within 1 order of magnitude). Our results pave the paths to ultrahigh yield synthesis of metal nanocubes with a precise size and shape and offer single-particle-level spectral controllability and reproducibility over a large number of particles.

17.
Adv Mater ; 30(42): e1704528, 2018 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-29572964

RESUMO

The application scope of plasmonic nanostructures is rapidly expanding to keep pace with the ongoing development of various scientific findings and emerging technologies. However, most plasmonic nanostructures heavily depend on rare, expensive, and extensively studied noble metals such as Au and Ag, with the limited choice of elements hindering their broad and practical applications in a wide spectral range. Therefore, abundant and inexpensive nonnoble metals have attracted attention as new plasmonic nanomaterial components, allowing these nonnoble-metal-based materials to be used in areas such as photocatalysis, sensing, nanoantennas, metamaterials, and magnetoplasmonics with new compositions, structures, and properties. Furthermore, the use of nonnoble metal hybrids results in newly emerging or synergistic properties not observed from single-metal component systems. Here, the synthetic strategies and recent advances in nonnoble-metal-based plasmonic nanostructures comprising Cu, Al, Mg, In, Ga, Pb, Ni, Co, Fe, and related hybrids are highlighted, and a discussion and perspectives in their synthesis, properties, applications, and challenges are presented.

18.
ACS Cent Sci ; 4(2): 277-287, 2018 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-29532028

RESUMO

Uniformly controlling a large number of metal nanostructures with a plasmonically enhanced signal to generate quantitative optical signals and the widespread use of these structures for surface-enhanced Raman scattering (SERS)-based biosensing and bioimaging applications are of paramount importance but are extremely challenging. Here, we report a highly controllable, facile selective-interdiffusive dealloying chemistry for synthesizing the dealloyed intra-nanogap particles (DIPs) with a ∼2 nm intragap in a high yield (∼95%) without the need for an interlayer. The SERS signals from DIPs are highly quantitative and polarization-independent with polarized laser sources. Remarkably, all the analyzed particles displayed the SERS enhancement factors (EFs) of ≥1.1 × 108 with a very narrow distribution of EFs. Finally, we show that DIPs can be used as ultrasensitive SERS-based DNA detection probes for detecting 10 aM to 1 pM target concentrations and highly robust, quantitative real-time cell imaging probes for long-term imaging with low laser power and short exposure time.

19.
Small ; 13(43)2017 11.
Artigo em Inglês | MEDLINE | ID: mdl-29136355
20.
Small ; 13(43)2017 11.
Artigo em Inglês | MEDLINE | ID: mdl-28902980

RESUMO

Highly reliable detection, imaging, and monitoring of reactive oxygen species (ROS) are critical for understanding and studying the biological roles and pathogenesis of ROS. This study describes the design and synthesis of myoglobin and polydopamine-engineered surface-enhanced Raman scattering (MP-SERS) nanoprobes with strong, tunable SERS signals that allow for specifically detecting and imaging ROS sensitively and quantitatively. The study shows that a polydopamine nanolayer can facilitate the modification of Raman-active myoglobins and satellite Au nanoparticles (s-AuNPs) to a plasmonic core AuNP (c-AuNP) in a controllable manner and the generation of plasmonically coupled hot spots between a c-AuNP and s-AuNPs that can induce strong SERS signals. The six-coordinated Fe(III)-OH2 of myoglobins in plasmonic hotspots is reacted with ROS (H2 O2 , •OH, and O2- ) to form Fe(IV)O. The characteristic Raman peaks of Fe(IV)O from the Fe-porphyrin is used to analyze and quantify ROS. This chemistry allows for these probes to detect ROS in solution and image ROS in cells in a highly designable, specific, and sensitive manner. This work shows that these MP-SERS probes allow for detecting and imaging ROS to differentiate cancerous cells from noncancerous cells. Importantly, for the first time, SERS-based monitoring of the autophagy process in living cells under starvation conditions is validated.


Assuntos
Indóis/química , Nanopartículas Metálicas/química , Mioglobina/metabolismo , Polímeros/química , Espécies Reativas de Oxigênio/metabolismo , Análise Espectral Raman , Autofagia , Sobrevivência Celular , Ouro/química , Células HeLa , Humanos , Lisossomos/metabolismo , Nanopartículas Metálicas/ultraestrutura
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