ORCID Profile
0000-0001-5495-6428
Current Organisation
Nanyang Technological University
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Publisher: Wiley
Date: 22-01-2021
Publisher: Wiley
Date: 18-09-2023
Publisher: Walter de Gruyter GmbH
Date: 03-11-2009
Abstract: Fabricating well-defined and stable nanoparticle crystals in a controlled fashion receives growing attention in nanotechnology. The order and packing symmetry within a nanoparticle crystal is of utmost importance for the development of materials with unique optical and electronic properties. To generate stable and ordered 3D nanoparticle structures, nanotechnology is combined with supramolecular chemistry to control the self-assembly of 2D and 3D receptor-functionalized nanoparticles. This review focuses on the use of molecular recognition chemistry to establish stable, ordered, and functional nanoparticle structures. The host–guest complexation of β-cyclodextrin (CD) and its guest molecules (e.g., adamantane and ferrocene) are applied to assist the nanoparticle assembly. Direct adsorption of supramolecular guest- and host-functionalized nanoparticles onto (patterned) CD self-assembled monolayers (SAMs) occurs via multivalent host–guest interactions and layer-by-layer (LbL) assembly. The reversibility and fine-tuning of the nanoparticle-surface binding strength in this supramolecular assembly scheme are the control parameters in the process. Furthermore, the supramolecular nanoparticle assembly has been integrated with top-down nanofabrication schemes to generate stable and ordered 3D nanoparticle structures, with controlled geometries and sizes, on surfaces, other interfaces, and as free-standing structures.
Publisher: American Chemical Society (ACS)
Date: 05-01-2021
Publisher: Springer Science and Business Media LLC
Date: 29-04-2015
DOI: 10.1038/NCOMMS7990
Abstract: A major challenge in nanoparticle self-assembly is programming the large-area organization of a single type of anisotropic nanoparticle into distinct superlattices with tunable packing efficiencies. Here we utilize nanoscale surface chemistry to direct the self-assembly of silver octahedra into three distinct two-dimensional plasmonic superlattices at a liquid/liquid interface. Systematically tuning the surface wettability of silver octahedra leads to a continuous superlattice structural evolution, from close-packed to progressively open structures. Notably, silver octahedra standing on vertices arranged in a square lattice is observed using hydrophobic particles. Simulations reveal that this structural evolution arises from competing interfacial forces between the particles and both liquid phases. Structure-to-function characterizations reveal that the standing octahedra array generates plasmonic ‘hotstrips’, leading to nearly 10-fold more efficient surface-enhanced Raman scattering compared with the other more densely packed configurations. The ability to assemble these superlattices on the wafer scale over various platforms further widens their potential applications.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2SC02981B
Abstract: Overview of the current status on emerging, multi-faceted nanosensor platform designs and data analysis strategies for rapid, point-of-need detection and monitoring of small-molecule metabolites.
Publisher: American Chemical Society (ACS)
Date: 11-2017
Abstract: We demonstrate a one-step precise direct metal writing of well-defined and densely packed gold nanoparticle (AuNP) patterns with tunable physical and optical properties. We achieve this by using two-photon lithography on a Au precursor comprising poly(vinylpyrrolidone) (PVP) and ethylene glycol (EG), where EG promotes higher reduction rates of Au(III) salt via polyol reduction. Hence, clusters of monodisperse AuNP are generated along raster scanning of the laser, forming high-particle-density, well-defined structures. By varying the PVP concentration, we tune the AuNP size from 27.3 to 65.0 nm and the density from 172 to 965 particles/μm
Publisher: American Chemical Society (ACS)
Date: 25-09-2012
DOI: 10.1021/LA302795R
Abstract: The effective number of surface-enhanced Raman spectroscopy (SERS) active hot spots on plasmonic nanostructures is the most crucial factor in ensuring high sensitivity in SERS sensing platform. Here we demonstrate a chemical etching method to increase the surface roughness of one-dimensional Ag nanowires, targeted at creating more SERS active hot spots along Ag nanowire's longitudinal axis for increased SERS detection sensitivity. Silver nanowires were first synthesized by the conventional polyol method and then subjected to chemical etching by NH(4)OH and H(2)O(2) mixture. The surfaces of silver nanowires were anisotropically etched off to create miniature "beads on a string" features with increased surface roughness while their crystallinity was preserved. Mapping of single-nanowire SERS measurements showed that the chemical etching method has overcome the limitation of conventional one-dimensional Ag nanowires with limited SERS active area at the tips to produce etched Ag nanowires with an increase in Raman hot spots and polarization-independent SERS signals across tens of micrometers length scale.
Publisher: American Chemical Society (ACS)
Date: 28-01-2020
Publisher: American Chemical Society (ACS)
Date: 10-06-2019
DOI: 10.1021/ACS.ACCOUNTS.9B00163
Abstract: Surface-enhanced Raman scattering (SERS) is a molecular-specific spectroscopic technique that provides up to 10
Publisher: Royal Society of Chemistry (RSC)
Date: 2009
DOI: 10.1039/B909918B
Abstract: Discrete 3D supramolecular hybrid particle structures with controllable morphology and dimensions were fabricated and their ability to encapsulate guest molecules was demonstrated.
Publisher: Proceedings of the National Academy of Sciences
Date: 08-04-2013
Abstract: Shaped colloids can be used as nanoscale building blocks for the construction of composite, functional materials that are completely assembled from the bottom up. Assemblies of noble metal nanostructures have unique optical properties that depend on key structural features requiring precise control of both position and connectivity spanning nanometer to micrometer length scales. Identifying and optimizing structures that strongly couple to light is important for understanding the behavior of surface plasmons in small nanoparticle clusters, and can result in highly sensitive chemical and biochemical sensors using surface-enhanced Raman spectroscopy (SERS). We use experiment and simulation to examine the local surface plasmon resonances of different arrangements of Ag polyhedral clusters. High-resolution transmission electron microscopy shows that monodisperse, atomically smooth Ag polyhedra can self-assemble into uniform interparticle gaps that result in reproducible SERS enhancement factors from assembly to assembly. We introduce a large-scale, gravity-driven assembly method that can generate arbitrary nanoparticle clusters based on the size and shape of a patterned template. These templates enable the systematic examination of different cluster arrangements and provide a means of constructing scalable and reliable SERS sensors.
Publisher: Wiley
Date: 16-09-2020
Publisher: Wiley
Date: 04-07-2022
Abstract: Gas‐phase surface‐enhanced Raman scattering (SERS) remains challenging due to poor analyte affinity to SERS substrates. The reported use of capturing probes suffers from concurrent inconsistent signals and long response time due to the formation of multiple potential probe–analyte interaction orientations. Here, we demonstrate the use of multiple non‐covalent interactions for ring complexation to boost the affinity of small gas molecules, SO 2 and NO 2 , to our SERS platform, achieving rapid capture and multiplex detection down to 100 ppm. Experimental and in‐silico studies affirm stable ring complex formation, and kinetic investigations reveal a 4‐fold faster response time compared to probes without stable ring complexation capability. By synergizing spectral concatenation and support vector machine regression, we achieve 91.7 % accuracy for multiplex quantification of SO 2 and NO 2 in excess CO 2 , mimicking real‐life exhausts. Our platform shows immense potential for on‐site exhaust and air quality surveillance.
Publisher: Elsevier BV
Date: 09-2005
Publisher: American Chemical Society (ACS)
Date: 07-09-2006
DOI: 10.1021/LA0610497
Abstract: Ferrocenyl-functionalized silica nanoparticles (Fc-SiO(2), 6a-6c) of about 60 nm with supramolecular "guest" properties were prepared. Nanoparticles 6a-6c differed by the addition of different molar ratios of starting compounds during the functionalization step, i.e., 1:0, 1:10, and 1:90 of 2-ferrocenyl amidoethoxyethanol and diethylene glycol for 6a,6b, and 6c, respectively. X-ray photoelectron spectroscopy (XPS) proved the presence of ferrocenyl groups on the surfaces of 6a-6c, whereas the elemental analysis revealed an iron content of particles 6a-6c of 0.10-0.16%. Dynamic light scattering (DLS) results showed that, compared with 6a, 6b dispersed well in aqueous media, possibly due to the presence of diethylene glycol at the surfaces of 6b that significantly increases its overall hydrophilicity. Cyclic voltammetry of 6b indicated a totally irreversible system and a "mixed" diffusion-adsorption behavior, which is attributed to sluggish electron transfer. The shifted |I(p,C)/I(p,A*)| ratio showed that the ferrocenyl groups are robustly attached to the nanoparticle surface within the experimental potential range. The supramolecular recognition of Fc-SiO(2) nanoparticles at interfaces was verified by their adsorption on beta-cyclodextrin (beta-CD) self-assembled monolayers, as monitored by surface plasmon resonance (SPR) spectroscopy. The ability of the Fc-SiO(2) nanoparticles to form host-guest interactions was also demonstrated by the attachment of beta-CD-functionalized Au nanoparticles (2.8 nm) on the Fc-SiO(2) surfaces, when mixed in solution.
Publisher: American Chemical Society (ACS)
Date: 18-01-2022
Publisher: American Chemical Society (ACS)
Date: 24-06-2020
Publisher: American Chemical Society (ACS)
Date: 22-09-2015
Abstract: Two-dimensional (2D) geometrical shape-shifting is prevalent in nature, but remains challenging in man-made "smart" materials, which are typically limited to single-direction responses. Here, we fabricate geometrical shape-shifting bovine serum albumin (BSA) microstructures to achieve circle-to-polygon and polygon-to-circle geometrical transformations. In addition, transformative two-dimensional microstructure arrays are demonstrated by the ensemble of these responsive microstructures to confer structure-to-function properties. The design strategy of our geometrical shape-shifting microstructures focuses on embedding precisely positioned rigid skeletal frames within responsive BSA matrices to direct their anisotropic swelling under pH stimulus. This is achieved using layer-by-layer two photon lithography, which is a direct laser writing technique capable of rendering spatial resolution in the sub-micrometer length scale. By controlling the shape, orientation and number of the embedded skeletal frames, we have demonstrated well-defined arc-to-corner and corner-to-arc transformations, which are essential for dynamic circle-to-polygon and polygon-to-circle shape-shifting, respectively. We further fabricate our shape-shifting microstructures in periodic arrays to experimentally demonstrate the first transformative 2D patterned arrays. Such versatile array configuration transformations give rise to structure-to-physical properties, including array porosity and pore shape, which are crucial for the development of on-demand multifunctional "smart" materials, especially in the field of photonics and microfluidics.
Publisher: Royal Society of Chemistry (RSC)
Date: 2009
DOI: 10.1039/B822156A
Abstract: The formation of stable and ordered free-standing porous supramolecular assemblies of nanoparticles with sizes and geometries controlled at different length scales is demonstrated by a double-templating strategy. Our technique combines the directed assembly of particles, templating using nanoimprint lithography (NIL), and supramolecular layer-by-layer (LbL) assembly. First, 500-nm beta-cyclodextrin (CD)-functionalized polystyrene (PS) particles were assembled by convective assembly onto a sacrificial polymer template patterned with a predefined geometry and size using NIL, forming a 3D crystal architecture of particles. LbL assembly of alternating supramolecular host- and guest-functionalized glues of CD-functionalized Au (Au-CD) nanoparticles and adamantyl (Ad) dendrimers, sized between 3-5 nm, within the preformed PS-particle crystal effectively bound the particles together into a particle composite. These particle composites were released from the substrate together with the polymer template, and transferred onto a target substrate. The particle crystal integrity, order and functionality were preserved. Rinsing the structure with dichloromethane removed the PS core material together with the polymer template, resulting in interconnected porous capsules, the sizes and shapes of which are fully determined by the PS core size and the polymer template definition. Again, integrity and shape were preserved in the rinsing step. These capsules were capable of storing organic fluorescent molecules using specific interactions.
Publisher: American Chemical Society (ACS)
Date: 18-03-2016
Abstract: The physical properties of aqueous-based stimuli-responsive photoresists are crucial in fabricating microstructures with high structural integrity and uniform responsiveness during two-photon lithography. Here, we quantitatively investigate how various components within bovine serum albumin (BSA) photoresists affect our ability to achieve BSA microstructures with consistent stimuli-responsive properties over areas exceeding 10(4) μm(2). We unveil a relationship between BSA concentration and dynamic viscosity, establishing a threshold viscosity to achieve robust BSA microstructures. We also demonstrate the addition of an inert polymer to the photoresist as viscosity enhancer. A set of systematically optimized processing parameters is derived for the construction of dynamic BSA microstructures. The optimized BSA photoresists and processing parameters enable us to extend the two-dimensional (2D) microstructures to three-dimensional (3D) ones, culminating in arrays of micropillars with aspect ratio > 10. Our findings foster the development of liquid stimuli-responsive photoresists to build multifunctional complex 3D geometries for applications such as bioimplantable devices or adaptive photonic systems.
Publisher: Royal Society of Chemistry (RSC)
Date: 2003
DOI: 10.1039/B309342E
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C4CC01949K
Abstract: Ag nanowire-based catalytic liquid marbles are fabricated as miniature reactors, which demonstrate highly efficient, support-free and rate-controllable heterogeneous degradation of methylene blue, with catalytic efficiency close to 100%.
Publisher: American Chemical Society (ACS)
Date: 07-2013
DOI: 10.1021/NN401685P
Abstract: Public attention to the food scandals raises an urgent need to develop effective and reliable methods to detect food contaminants. The current prevailing detections are primarily based upon liquid chromatography, mass spectroscopy, or colorimetric methods, which usually require sophisticated and time-consuming steps or s le preparation. Herein, we develop a facile strategy to assemble the vertically aligned monolayer of Au nanorods with a nominal 0.8 nm gap distance and demonstrate their applications in the rapid detection of plasticizers and melamine contamination at femtomolar level by surface-enhanced Raman scattering spectroscopy (SERS). The SERS signals of plasticizers are sensitive down to 0.9 fM concentrations in orange juices. It is the lowest detection limit reported to date, which is 7 orders of magnitude lower than the standard of United States (6 ppb). The highly organized vertical arrays generate the reproducible "SERS-active sites" and can be achieved on arbitrary substrates, ranging from silicon, gallium nitride, glass to flexible poly(ethylene naphthalate) substrates.
Publisher: American Chemical Society (ACS)
Date: 20-12-2017
DOI: 10.1021/ACS.JPCLETT.6B02743
Abstract: The ability of an artificial microdroplet to mimic the rotational behaviors of living systems is crucial for dynamic mass transportation but remains challenging to date. Herein, we report dynamic microdroplet rotation using a liquid marble (RLM) and achieve precise control over mass transportation and distribution in a three-dimensional (3D) microdroplet. RLM rotates synchronously with an external magnetic field, creating circular hydrodynamic flow and an outward centrifugal force. Such spin-induced phenomena direct a spiral movement of entrapped molecules and accelerate their diffusion and homogenization in the entire liquid. Moreover, we demonstrate the rotation rate-controlled (between 0 and 1300 rpm) modulation of shell-catalyzed reaction kinetics from 0.13 to 0.62 min
Publisher: Wiley
Date: 26-06-2015
Abstract: Colloidosomes are robust microcapsules attractive for molecular sensing because of their characteristic micron size, large specific surface area, and dual-phase stability. However, current colloidosome sensors are limited to qualitative fluorogenic receptor-based detection, which restrict their applicability to a narrow range of molecules. Here, we introduce plasmonic colloidosome constructed from Ag nanocubes as an emulsion-based 3D SERS platform. The colloidosomes exhibit excellent mechanical robustness, flexible size tunability, versatility to merge, and ultrasensitivity in SERS quantitation of food/industrial toxins down to sub-femtomole levels. Using just 0.5 μL of s le volumes, our plasmonic colloidosomes exhibit >3000-fold higher SERS sensitivity over conventional suspension platform. Notably, we demonstrate the first high-throughput multiplex molecular sensing across multiple liquid phases.
Publisher: Wiley
Date: 17-12-2007
Abstract: Beta-Cyclodextrin (beta-CD) monolayers have been immobilized in microchannels. The host-guest interactions on the beta-CD monolayers inside the channels were comparable to the interactions on beta-CD monolayers on planar surfaces, and a alent fluorescent guest attached with a comparable binding strength. Proteins were attached to these monolayers inside microchannels in a selective manner by employing a strategy that uses streptavidin and orthogonal linker molecules. The design of the chip, which involved a large channel that splits into four smaller channels, allowed the channels to be addressed separately and led to the selective immobilization of antibodies. Experiments with labeled antibodies showed the selective immobilization of these antibodies in the separate channels.
Publisher: American Chemical Society (ACS)
Date: 24-04-2014
DOI: 10.1021/JA501786S
Abstract: Single-phase Cu2ZnSnS4 (CZTS) is an essential prerequisite toward a high-efficiency thin-film solar cell device. Herein, the selective phase formation of single-phase CZTS nanoparticles by ligand control is reported. Surface-enhanced Raman scattering (SERS) spectroscopy is demonstrated for the first time as a characterization tool for nanoparticles to differentiate the mixed compositional phase (e.g., CZTS, CTS, and ZnS), which cannot be distinguished by X-ray diffraction. Due to the superior selectivity and sensitivity of SERS, the growth mechanism of CZTS nanoparticle formation by hot injection is revealed to involve three growth steps. First, it starts with nucleation of Cu(2-x)S nanoparticles, followed by diffusion of Sn(4+) into Cu(2-x)S nanoparticles to form the Cu3SnS4 (CTS) phase and diffusion of Zn(2+) into CTS nanoparticles to form the CZTS phase. In addition, it is revealed that single-phase CZTS nanoparticles can be obtained via balancing the rate of CTS phase formation and diffusion of Zn(2+) into the CTS phase. We demonstrate that this balance can be achieved by 1 mL of thiol with Cu(OAc)2, Sn(OAc)4, and Zn(acac)2 metal salts to synthesize the CZTS phase without the presence of a detectable binary/ternary phase with SERS.
Publisher: American Chemical Society (ACS)
Date: 18-08-2007
DOI: 10.1021/LA701671S
Abstract: The formation of particle monolayers by convective assembly was studied in situ with three different kinds of particle-surface interactions: adsorption onto native surfaces, with additional electrostatic interactions, and with supramolecular host-guest interactions. In the first case carboxylate-functionalized polystyrene (PS-COOH) particles were assembled onto native silicon oxide surfaces, in the second PS-COOH onto protonated amino-functionalized (NH3+) self-assembled monolayers (SAMs), and in the third beta-CD-functionalized polystyrene (PS-CD) particles onto beta-CD SAMs with pre-adsorbed ferrocenyl-functionalized dendrimers. The adsorption and desorption behaviors of particles onto and from these surfaces were observed in situ on a horizontal deposition setup, and the packing density and order of the adsorbed particle lattices were compared. The desorption behavior of particles from surfaces was evaluated by reducing the temperature below the dew point, thus initiating water condensation. Particle lattices on native oxide surfaces formed the best hexagonal close packed (hcp) order and could be easily desorbed by reducing the temperature to below the dew point. The electrostatically modified assembly resulted in densely packed, but disordered particle lattices. The specificity and selectivity of the supramolecular assembly process were optimized by the use of ferrocenyl-functionalized dendrimers of low generation and by the introduction of competitive interaction by native beta-CD molecules during the assembly. The fine-tuned supramolecularly formed particle lattices were nearly hcp packed. Both electrostatically and supramolecularly formed lattices of particles were strongly attached to the surfaces and could not be removed by condensation.
Publisher: Proceedings of the National Academy of Sciences
Date: 26-11-2019
Abstract: There is a huge interest in developing superrepellent surfaces for antifouling and heat-transfer applications. To characterize the wetting properties of such surfaces, the most common approach is to place a millimetric-sized droplet and measure its contact angles. The adhesion and friction forces can then be inferred indirectly using Furmidge’s relation. While easy to implement, contact angle measurements are semiquantitative and cannot resolve wetting variations on a surface. Here, we attach a micrometric-sized droplet to an atomic force microscope cantilever to directly measure adhesion and friction forces with nanonewton force resolutions. We spatially map the micrometer-scale wetting properties of superhydrophobic surfaces and observe the time-resolved pinning–depinning dynamics as the droplet detaches from or moves across the surface.
Publisher: American Chemical Society (ACS)
Date: 07-07-2016
Publisher: IOP Publishing
Date: 23-10-2015
Publisher: Elsevier BV
Date: 10-2019
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8CC00564H
Abstract: A plasmonic nose is designed using a ZIF-encapsulated Ag nanocube array to concentrate molecules and electromagnetic field at the 3D nanometer scale.
Publisher: American Chemical Society (ACS)
Date: 03-09-2019
Publisher: American Association for the Advancement of Science (AAAS)
Date: 02-03-2018
Abstract: Originally unfavored nitrogen-to-ammonia electroconversion is now preferred over competing reaction using reticular chemistry.
Publisher: American Chemical Society (ACS)
Date: 13-09-2019
Abstract: Stand-off Raman spectroscopy combines the advantages of both Raman spectroscopy and remote detection to retrieve molecular vibrational fingerprints of chemicals at inaccessible sites. However, it is currently restricted to the detection of pure solids and liquids and not widely applicable for dispersed molecules in air. Herein, we realize real-time stand-off SERS spectroscopy for remote and multiplex detection of atmospheric airborne species by integrating a long-range optic system with a 3D analyte-sorbing metal-organic framework (MOF)-integrated SERS platform. Formed via the self-assembly of Ag@MOF core-shell nanoparticles, our 3D plasmonic architecture exhibits micrometer thick SERS hotspot to allow active sorption and rapid detection of aerosols, gas, and volatile organic compounds down to parts-per-billion levels, notably at a distance up to 10 m apart. The platform is highly sensitive to changes in atmospheric content, as demonstrated in the temporal monitoring of gaseous CO
Publisher: Wiley
Date: 23-09-2009
Publisher: Royal Society of Chemistry (RSC)
Date: 2013
DOI: 10.1039/C3NR00981E
Abstract: Interfacial self-assembly of nanoparticles is capable of creating large-area close-packed structures for a variety of applications. However, monolayers of hydrophilic cetyltrimethylammonium bromide (CTAB)-coated Au nanoparticles are challenging to assemble via interfacial self-assembly. This report presents a facile and scalable process to fabricate large-area monolayer films of ultrathin CTAB-coated Au nanoprisms at the air-water interface using the Langmuir-Schaefer technique. This is first achieved by a one-step functionalization of Au nanoprisms with poly(vinylpyrrolidone) (PVP). PVP functionalization is completed within a short time without loss of nanoprisms due to aggregation. Uniform and near close-packed monolayers of the Au nanoprisms formed over large areas (∼1 cm(2)) at the air-water interface can be transferred to substrates with different wettabilities. The inter-prism gaps are tuned qualitatively through the introduction of dodecanethiol and oleylamine. The morphological integrity of the nanoprisms is maintained throughout the entire assembly process, without truncation of the nanoprism tips. The near close-packed arrangement of the nanoprism monolayers generates large numbers of hot spots in the 2D arrays in the tip-to-tip and edge-to-edge inter-particle regions, giving rise to strong surface-enhanced Raman scattering (SERS) signals. When deposited on an Au mirror film, additional hotspots are created in the 3(rd) dimension in the gaps between the 2D nanoprism monolayers and the Au film. SERS enhancement factors reaching 10(4) for non-resonant probe molecules are achieved.
Publisher: American Chemical Society (ACS)
Date: 10-2014
DOI: 10.1021/AC502955W
Abstract: The ultratrace detection and quantification of toxins in both water and organic liquids remains a challenge due to the random spreading and dilution of liquids on substrate-based sensors, especially for organic liquids with low surface tension. Herein, we fabricate a superhydrophobic-oleophobic (SHP-OP) 3D Ag nanowire mesh-like surface-enhanced Raman scattering (SERS) platform to overcome the random spreading issue, demonstrating ultratrace toxin sensing in both water and organic liquid. Our SHP-OP SERS platform is able to concentrate analyte solutions in water and toluene to 100-fold and 8-fold smaller areas, respectively, as compared to its omniphilic counterparts. The synergy of analyte-concentrating ability and intense SERS-enhancing properties on our SHP-OP SERS platform enables quantitative and ultratrace detection of melamine and Sudan I down to 0.1 fmol in water and toluene, respectively, using just 1 μL of analyte solution. These detection limits are 10(3)-fold lower than the regulatory limits, clearly indicating our SHP-OP SERS platform as an appealing universal ultratrace toxin sensor. The ultratrace detection of spiked melamine in liquid milk down to 100 fmol also highlights the suitability of our SHP-OP SERS platform for the sensing of food toxins in real s les.
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9QI00064J
Abstract: Graphene/graphene nanoribbon (GGNR) aerogels facilitate fast electron and ion transfer while S-doping improves the activity of catalytic sites for efficient hydrogen evolution.
Publisher: Wiley
Date: 16-09-2020
Publisher: American Chemical Society (ACS)
Date: 13-05-2004
DOI: 10.1021/JP049422B
Publisher: American Chemical Society (ACS)
Date: 31-10-2017
Abstract: Miniaturizing the continuous multistep operations of a factory into a microchemical plant offers a safe and cost-effective approach to promote high-throughput screening in drug development and enforcement of industrial/environmental safety. While particle-assembled microdroplets in the form of liquid marble are ideal as microchemical plant, these platforms are mainly restricted to single-step reactions and limited to ex situ reaction monitoring. Herein, we utilize plasmonic liquid marble (PLM), formed by encapsulating liquid droplet with Ag nanocubes, to address these issues and demonstrate it as an ideal microchemical plant to conduct reaction-and-detection sequences on-demand in a nondisruptive manner. Utilizing a two-step azo-dye formation as our model reaction, our microchemical plant allows rapid and efficient diazotization of nitroaniline to form diazonium nitrobenzene, followed by the azo coupling of this intermediate with target aromatic compound to yield azo-dye. These molecular events are tracked in situ via SERS measurement through the plasmonic shell and further verified with in silico investigation. Furthermore, we apply our microchemical plant for ultrasensitive SERS detection and quantification of bisphenol A (BPA) with detection limit down to 10 amol, which is 50 000-fold lower than the BPA safety limit. Together with the protections offered by plasmonic shell against external environments, these collective advantages empower PLM as a multifunctional microchemical plant to facilitate small-volume testing and optimization of processes relevant in industrial and research contexts.
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6TC00682E
Abstract: A progressively complex anti-counterfeiting platform with large information density, high security and low-error decoding is achieved by utilizing plasmonic nanopillar arrays fabricated using two-photon photolithography. Multiplex molecular information hidden under the same physical features are read out in the form of fluorescence, SERS, and their signal intensities.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C4CC08596E
Abstract: We demonstrate a multiplex plasmonic anti-counterfeiting platform by embedding multiple molecules on a single substrate with superior spectral and spatial resolution.
Publisher: Wiley
Date: 03-03-2010
Publisher: American Chemical Society (ACS)
Date: 26-05-2016
DOI: 10.1021/ACS.NANOLETT.6B01388
Abstract: Current plasmonic metasurfaces of nanocubes are limited to planar configurations, restricting the ability to create tailored local electromagnetic fields. Here, we report a new chemical strategy to achieve tunable metasurfaces with nonplanar nanocube orientations, creating novel lattice-dependent field localization patterns. We manipulate the interfacial behaviors of Ag nanocubes by controlling the ratio of hydrophilic/hydrophobic molecules added in a binary thiol mixture during the surface functionalization step. The nanocube orientation at an oil/water interface can consequently be continuously tuned from planar to tilted and standing configurations, leading to the organization of Ag nanocubes into three unique large-area metacrystals, including square close-packed, linear, and hexagonal lattices. In particular, the linear and hexagonal metacrystals are unusual open lattices comprising nonplanar nanocubes, creating unique local electromagnetic field distribution patterns. Large-area "hot hexagons" with significant delocalization of hot spots form in the hexagonal metacrystal. With a lowest packing density of 24%, the hexagonal metacrystal generates nearly 350-fold stronger surface-enhanced Raman scattering as compared to the other denser-packing metacrystals, demonstrating the importance of achieving control over the geometrical and spatial orientation of the nanocubes in the metacrystals.
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8CC02855A
Abstract: A live bacteria SERS platform is developed for the precise and sensitive monitoring of nitric oxide release from a single MRSA.
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C4NR01464B
Abstract: Chemical speciation and quantification at trace levels of toxic mercury and methylmercury ions in water is achieved by SERS spectroscopy.
Publisher: American Chemical Society (ACS)
Date: 08-04-2016
DOI: 10.1021/ACS.JPCLETT.6B00501
Abstract: Current microscale tracking of chemical kinetics is limited to destructive ex situ methods. Here we utilize Ag nanocube-based plasmonic liquid marble (PLM) microreactor for in situ molecular-level identification of reaction dynamics. We exploit the ultrasensitive surface-enhanced Raman scattering (SERS) capability imparted by the plasmonic shell to unravel the mechanism and kinetics of aryl-diazonium surface grafting reaction in situ, using just a 2-μL reaction droplet. This reaction is a robust approach to generate covalently functionalized metallic surfaces, yet its kinetics remain unknown to date. Experiments and simulations jointly uncover a two-step sequential grafting process. An initial Langmuir chemisorption of sulfonicbenzene diazonium (dSB) salt onto Ag surfaces forms an intermediate sulfonicbenzene monolayer (Ag-SB), followed by subsequent autocatalytic multilayer growth of Ag-SB3. Kinetic rate constants reveal 19-fold faster chemisorption than multilayer growth. Our ability to precisely decipher molecular-level reaction dynamics creates opportunities to develop more efficient processes in synthetic chemistry and nanotechnology.
Publisher: American Chemical Society (ACS)
Date: 06-09-2022
Abstract: Disease X is a hypothetical unknown disease that has the potential to cause an epidemic or pandemic outbreak in the future. Nanosensors are attractive portable devices that can swiftly screen disease biomarkers on site, reducing the reliance on laboratory-based analyses. However, conventional data analytics limit the progress of nanosensor research. In this Perspective, we highlight the integral role of machine learning (ML) algorithms in advancing nanosensing strategies toward Disease X detection. We first summarize recent progress in utilizing ML algorithms for the smart design and fabrication of custom nanosensor platforms as well as realizing rapid on-site prediction of infection statuses. Subsequently, we discuss promising prospects in further harnessing the potential of ML algorithms in other aspects of nanosensor development and biomarker detection.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2NH00146B
Abstract: Schematic of our bidirectional, ML-empowered approach incorporating plasmonic featurization for rapid ( s) and accurate determination of the size and size distribution of gold nanosphere (Au NSs) ensembles in real s les.
Publisher: American Chemical Society (ACS)
Date: 07-08-2013
DOI: 10.1021/JP4063077
Publisher: American Chemical Society (ACS)
Date: 23-10-2017
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C8TA10162K
Abstract: A series of hollow polyhedrons are constructed with transition-metal doped spinel-structured nanosheets wrapped nitrogen-doped carbon polyhedrons for enhanced water splitting.
Publisher: American Chemical Society (ACS)
Date: 12-07-2017
Publisher: Wiley
Date: 08-2016
Abstract: On page 6322, J. F. Wang and co-workers report a wet-chemistry method for the preparation of colloidal Au nanocups and their plasmonic properties. The Au nanocups are prepared through single-vertex-initiated Au deposition on PbS nano-octahedrons and subsequent selective dissolution of PbS. Owing to the orientation-dependent coupling strengths, the obtained Au nanocups display orientation-dependent plasmonic properties and Raman enhancements when deposited on substrates.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1NR90053F
Abstract: Ramon A. Alvarez-Puebla, Jian-Feng Li and Xing Yi Ling introduce the Nanoscale themed collection on advances in plasmonics and its applications.
Publisher: Elsevier BV
Date: 07-2020
Publisher: Informa UK Limited
Date: 13-08-2009
Publisher: American Chemical Society (ACS)
Date: 12-06-2015
DOI: 10.1021/JACS.5B04310
Abstract: We show that partial inhibition of the emerging Ag domain can be achieved by controlling the growth dynamics. With the symmetry broken by the "fresh" surface, sequentially growth gives (Au sphere)-(Ag wire)-(Ag plate) triblock nanostructures. This new understanding opens doors to sophisticated synthetic designs, broadening the horizon of our search for functional architectures.
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8NR04053B
Abstract: Nanoscale shaping of NPG's thermo-plasmonic effect is investigated to optimize localized light-to-heat conversion and its application in ultrasensitive heat-mediated actuation.
Publisher: American Chemical Society (ACS)
Date: 24-05-2013
DOI: 10.1021/LA4012108
Abstract: The surface-enhanced Raman scattering (SERS) "hot spots" are highly localized regions of enhanced electromagnetic field within a SERS substrate that dominate the overall SERS intensity. This results in inhomogeneous distribution of SERS intensity in a SERS substrate, thus limiting their application as reproducible and ultrasensitive sensing platforms. Here, we address this challenge by fabricating Ag nanowires into three-dimensional (3D) woodpile-like platforms via layer-by-layer Langmuir-Blodgett assembly. We focus on promoting strong electromagnetic coupling between parallel and vertically stacked Ag nanowire pairs within the woodpile structure to achieve a high density of "hot spots" across the entire 3D SERS substrates. Raman mapping (x-y plane) demonstrates that all of the 3D Ag nanowire arrays exhibit a homogeneous SERS Raman intensity over a large area, whereas their monolayer counterpart experiences >50% of zero and/or an undetectable SERS signal. The SERS enhancement factor increases from 3.1 × 10(3) to 2.6 × 10(4), as the assembled Ag nanowire layer increases from monolayer to three layers, respectively. We attribute the homogeneous SERS signal to the high density of "hot spots" arising from the vertical and lateral gaps within the woodpile layers. The SERS signals plateau off when the number of layers increase from three to five, which can be attributed to limited laser penetration depth. The assembled multilayered silver nanowires demonstrate a larger SERS depth cross section and angle-independent SERS intensity, making such woodpile 3D SERS substrate more reliable and versatile for future sensing applications.
Publisher: American Chemical Society (ACS)
Date: 29-08-2016
Abstract: Liquid marble offers an attractive droplet manipulation approach by isolating microdroplet in a nonstick encapsulating shell formed via the spontaneous coating of hydrophobic particles onto the liquid surface. While liquid marble prepared using magnetic nanoparticles enables precise spatiotemporal actuation of microdroplets, these manipulations are generally limited to simple and linear spatial maneuver of microdroplets. Herein, we demonstrate the unique and three-dimensional spinning of microliter-sized liquid marble (LM) and its subsequent dual applications as (1) the world's smallest centrifuge and (2) a miniature and localized viscometer. Our LM is responsive to an applied rotating magnetic field, with its spinning speed programmable between 0 and 1300 rpm. This spinning generates an unprecedented centrifugal force of >2g in a LM of ∼1 mm radius. Such centrifugal force facilitates an outward and radial hydrodynamic flow in the enclosed microdroplet, enabling LM to serve as a microcentrifuge for the sedimentation of nanoparticles with >85% separation efficiency. Furthermore, we apply spinning LM as an ultrasensitive spin-to-viscosity transducer to quantify the viscosity of the external suspended liquid in the relative viscosity (η/ηwater) range of 1-70 using ≤1 mL liquid s le. Collectively, the ensemble of benefits offered by spinning LM creates enormous opportunities in the development of multifunctional micromagneto-mechanical devices as promising surface-sensitive microsensor, miniature centrifugal pump, and even microreactor with directed heat and mass transfer mechanism.
Publisher: Wiley
Date: 07-07-2016
Abstract: Controlling sub-10 nm ligament sizes and open-shell structure in nanoporous gold (NPG) to achieve strained lattice is critical in enhancing catalytic activity, but it remains a challenge due to poor control of reaction kinetics in conventional dealloying approach. Herein, a ligament size-controlled synthesis of open-shell NPG bowls (NPGB) through hetero-epitaxial growth of NPGB on AgCl is reported. The ligament size in NPGB is controlled from 6 to 46 nm by varying the hydroquinone to HAuCl4 ratio. The Williamson-Hall analysis demonstrates a higher lattice strain in smaller ligament size. In particular, NPGB with 6 nm (NPGB 6) ligament size possess the highest strain of 15.4 × 10(-3) , which is nearly twice of conventional 2D NPG sheets (≈8.8 × 10(-3) ). The presence of high surface energy facets in NPGBs is also envisaged. The best electrocatalytic activity toward methanol oxidation is observed in NPGB 6 (27.8 μA μg(-1) ), which is ≈9-fold and 3-fold higher than 8 nm solid Au nanoparticles, and conventional NPG sheets. The excellent catalytic activity in NPGB 6 is attributed to the open-shell structure, lattice strain, and higher electro-active surface area, allowing efficient exposure of catalytic active sites to facilitate the methanol oxidation. The results offer a potential strategy for designing next generation electrocatalysts.
Publisher: MDPI AG
Date: 04-04-2008
DOI: 10.3390/IJMS9040486
Publisher: American Chemical Society (ACS)
Date: 07-06-2020
DOI: 10.1021/JACS.0C04144
Publisher: Wiley
Date: 10-03-2014
Abstract: Most of the surface-enhanced Raman scattering (SERS) substrates are 2D planar systems, which limits the SERS active area to a single Cartesian plane. Here, we fabricate 3D SERS substrates with the aim to break the traditional 2D SERS active area limitation, and to extend the SERS hotspots into the third dimension along the z-axis. Our 3D SERS substrates are tailored with increased SERS hotspots in the z-direction from tens of nanometers to tens of micrometers, increasing the hotspots in the z-direction by at least an order of magnitude larger than the confocal volume (~1 μm) of most Raman spectrometers. Various hierarchical 3D SERS-active microstructures are fabricated by combining 3D laser photolithography with Langmuir-Blodgett nanoparticle assembly. 3D laser photolithography creates microstructured platforms required to extend the SERS-active area into 3D, and the self-assembly of Ag nanoparticles ensures homogeneous coating of SERS-active Ag nanoparticles over the entire microstructured platforms. Large-area 3D Raman imaging demonstrates that homogeneous signals can be collected throughout the entire 3D SERS substrates. We vary the morphology, height, and inclination angles of the 3D microstructures, where the inclination angle is found to exhibit strong influence on the SERS signals. We also demonstrate a potential application of this hierarchical 3D SERS substrate in information tagging, storage and encryption as SERS micro-barcodes, where multiple micro-barcodes can be created within a single set of microstructures.
Publisher: American Chemical Society (ACS)
Date: 08-04-2009
DOI: 10.1021/AM900071Y
Abstract: Mechanically robust and crystalline supramolecular particle structures have been constructed by decoupling nanoparticle assembly and supramolecular glue infiltration into a sequential process. First, beta-cyclodextrin (CD)-functionalized polystyrene particles (d approximately 500 nm) were assembled on a CD-functionalized surface via convective assembly to form highly ordered, but mechanically unstable, particle crystals. Subsequently, the crystals were infiltrated by a solution of adamantyl-functionalized dendrimers, functioning as a supramolecular glue to bind neighboring particles together and to couple the entire particle crystal to the CD surface, both in a noncovalent manner. The supramolecular particle crystals are highly robust, as witnessed by their ability to withstand agitation by ultrasonication. When assembled on a poly(dimethylsiloxane) (PDMS) st , the dendrimer-infiltrated particle crystals could be transfer-printed onto a CD-functionalized target surface. By variation of the geometry and size of the PDMS st s, single particle lines, interconnected particle rings, and V-shaped particle assemblies were obtained. The particle structures served as 3D receptors for the binding of (multiple) complementary guest molecules, indicating that the supramolecular host functionalities of the particle crystals were retained throughout the fabrication process.
Publisher: Wiley
Date: 27-07-2020
Abstract: The electrochemical nitrogen reduction reaction (NRR) offers a sustainable solution towards ammonia production but suffers poor reaction performance owing to preferential catalyst–H formation and the consequential hydrogen evolution reaction (HER). Now, the Pt/Au electrocatalyst d‐band structure is electronically modified using zeolitic imidazole framework (ZIF) to achieve a Faradaic efficiency (FE) of % with high ammonia yield rate of μg mg cat −1 h −1 under ambient conditions. The strategy lowers electrocatalyst d‐band position to weaken H adsorption and concurrently creates electron‐deficient sites to kinetically drive NRR by promoting catalyst–N 2 interaction. The ZIF coating on the electrocatalyst doubles as a hydrophobic layer to suppress HER, further improving FE by ‐fold compared to without ZIF (ca. 1 %). The Pt/Au‐N ZIF interaction is key to enable strong N 2 adsorption over H atom.
Publisher: Springer Science and Business Media LLC
Date: 17-09-2014
DOI: 10.1038/NCOMMS5947
Abstract: Nanoporous gold with networks of interconnected ligaments and highly porous structure holds stimulating technological implications in fuel cell catalysis. Current syntheses of nanoporous gold mainly revolve around de-alloying approaches that are generally limited by stringent and harsh multistep protocols. Here we develop a one-step solution phase synthesis of zero-dimensional hollow nanoporous gold nanoparticles with tunable particle size (150-1,000 nm) and ligament thickness (21-54 nm). With faster mass diffusivity, excellent specific electroactive surface area and large density of highly active surface sites, our zero-dimensional nanoporous gold nanoparticles exhibit ~1.4 times enhanced catalytic activity and improved tolerance towards carbonaceous species, demonstrating their superiority over conventional nanoporous gold sheets. Detailed mechanistic study also reveals the crucial heteroepitaxial growth of gold on the surface of silver chloride templates, implying that our synthetic protocol is generic and may be extended to the synthesis of other nanoporous metals via different templates.
Publisher: American Chemical Society (ACS)
Date: 24-07-2017
Publisher: Wiley
Date: 30-09-2019
Abstract: Full genome sequencing of organisms with large and complex genomes is intractable and cost ineffective under most research budgets. Cycads (Cycadales) represent one of the oldest lineages of the extant seed plants and, partly due to their age, have incredibly large genomes up to ~60 Gbp. Restriction site-associated DNA sequencing (RADseq) offers an approach to find genome-wide informative markers and has proven to be effective with both model and nonmodel organisms. We tested the application of RADseq using ezRAD across all 10 genera of the Cycadales including an ex le data set of Cycas calcicola representing 72 s les from natural populations. Using previously available plastid and mitochondrial genomes as references, reads were mapped recovering plastid and mitochondrial genome regions and nuclear markers for all of the genera. De novo assembly generated up to 138,407 high-depth clusters and up to 1,705 phylogenetically informative loci for the genera, and 4,421 loci for the ex le assembly of C. calcicola. The number of loci recovered by de novo assembly was lower than previous RADseq studies, yet still sufficient for downstream analysis. However, the number of markers could be increased by relaxing our assembly parameters, especially for the C. calcicola data set. Our results demonstrate the successful application of RADseq across the Cycadales to generate a large number of markers for all genomic compartments, despite the large number of plastids present in a typical plant cell. Our modified protocol was adapted to be applied to cycads and other organisms with large genomes to yield many informative genome-wide markers.
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C7NR07793A
Abstract: A ciphertext-embedded machine-readable micro-QR code is constructed using structurally uniform visible-range SERS-active Al nanostructures with an average SERS enhancement factor of 4 .
Publisher: Wiley
Date: 29-09-2014
Abstract: The ability to shape-shift in response to a stimulus increases an organism's survivability in nature. Similarly, man-made dynamic and responsive "smart" microtechnology is crucial for the advancement of human technology. Here, 10-30 μm shape-changing 3D BSA protein hydrogel microstructures are fabricated with dynamic, quantitative, directional, and angle-resolved bending via two-photon photolithography. The controlled directional responsiveness is achieved by spatially controlling the cross-linking density of BSA at a nanometer lengthscale. Atomic force microscopy measurements of Young's moduli of structures indicate that increasing the laser writing distance at the z-axis from 100-500 nm decreases the modulus of the structure. Hence, through nanoscale modulation of the laser writing z-layer distance at the nanoscale, control over the cross-linking density is possible, allowing for the swelling extent of the microstructures to be quantified and controlled with high precision. This method of segmented moduli is applied within a single microstructure for the design of shape-shifting microstructures that exhibit stimulus-induced chirality, as well as for the fabrication of a free-standing 3D microtrap which is able to open and close in response to a pH change.
Publisher: American Chemical Society (ACS)
Date: 13-11-2018
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C3NR04375D
Abstract: We present the next generation covert plasmonic security labels based on Ag nanowire structures and their polarization dependent surface-enhanced Raman scattering (SERS) imaging. The security labels consist of Ag nanowires fabricated by two-photon lithography and thermal evaporation, where molecular probes of choice are deposited. Simulation and experimental results show that the SERS signals from the embedded molecules depend significantly on the polarization of the incident field. The covert molecular information cannot be revealed directly from the physical features, but can only be read-out selectively by polarization-dependent SERS imaging. Our plasmonic security labels exhibit very narrow spectral fingerprint vibration, which is more specific than broadband colorimetry-based systems. The polarization-dependent SERS intensity, molecular fingerprint of SERS spectra, and versatile geometrical design by two-photon lithography have made our plasmonic Ag nanowire structures an ideal candidate as advanced security solutions for anti-counterfeiting application.
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C7CS00786H
Abstract: This review summarizes recent SERS developments, focusing on analyte manipulation strategies and hybrid SERS platforms that venture beyond hotspot engineering.
Publisher: American Chemical Society (ACS)
Date: 10-02-2020
Publisher: Elsevier BV
Date: 06-2016
Publisher: Wiley
Date: 04-02-2015
Abstract: We demonstrate the fabrication of graphene liquid marbles as photothermal miniature reactors with precise temperature control for reaction kinetics modulation. Graphene liquid marbles show rapid and highly reproducible photothermal behavior while maintaining their excellent mechanical robustness. By tuning the applied laser power, swift regulation of graphene liquid marble's surface temperature between 21-135 °C and its encapsulated water temperature between 21-74 °C are demonstrated. The temperature regulation modulates the reaction kinetics in our graphene liquid marble, achieving a 12-fold superior reaction rate constant for methylene blue degradation than at room temperature.
Publisher: Wiley
Date: 19-04-2018
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7NR02194A
Abstract: The agreement of molecular dynamics simulation results and our theoretical prediction of Ag octahedral nanoparticles at a hexane/water interface.
Publisher: Wiley
Date: 13-01-2009
Publisher: Elsevier BV
Date: 05-2007
Publisher: American Chemical Society (ACS)
Date: 04-10-2017
Publisher: Wiley
Date: 11-05-2016
Abstract: Colloidal gold nanocups are synthesized through single-vertex-initiated gold deposition on PbS nanooctahedrons and subsequent selective dissolution of the PbS component. They possess strong magnetic plasmon resonance and exhibit remarkable orientation-dependent plasmonic properties when deposited on flat substrates. They can also effectively couple s-polarized light into the interfacial region between the nanocup and substrate.
Publisher: The Royal Society
Date: 07-2009
Abstract: Barnacles are a major biofouler of man-made underwater structures. Prior to settlement, cypris larvae explore surfaces by reversible attachment effected by a ‘temporary adhesive’. During this exploratory behaviour, cyprids deposit proteinaceous ‘footprints’ of a putatively adhesive material. In this study, footprints deposited by Balanus hitrite cyprids were probed by atomic force microscopy (AFM) in artificial sea water (ASW) on silane-modified glass surfaces. AFM images obtained in air yielded better resolution than in ASW and revealed the fibrillar nature of the secretion, suggesting that the deposits were composed of single proteinaceous nanofibrils, or bundles of fibrils. The force curves generated in pull-off force experiments in sea water consisted of regions of gradually increasing force, separated by sharp drops in extension force manifesting a characteristic saw-tooth appearance. Following the relaxation of fibrils stretched to high strains, force–distance curves in reverse stretching experiments could be described by the entropic elasticity model of a polymer chain. When subjected to relaxation exceeding 500 ms, extended footprint proteins refolded, and again showed saw-tooth unfolding peaks in subsequent force cycles. Observed rupture and hysteresis behaviour were explained by the ‘sacrificial bond’ model. Longer durations of relaxation ( s) allowed more sacrificial bond reformation and contributed to enhanced energy dissipation (higher toughness). The persistence length for the protein chains ( L P ) was obtained. At high elongation, following repeated stretching up to increasing upper strain limits, footprint proteins detached at total stretched length of 10 µm.
Publisher: American Chemical Society (ACS)
Date: 22-12-2008
DOI: 10.1021/JA807611N
Abstract: Porous st s fabricated by one-step phase separation micromolding were used for microcontact printing of polar inks, in particular aqueous solutions of dendrimers, proteins, and nanoparticles. Permanent hydrophilicity was achieved without any additional treatment by tailored choice of the polymer components. Pores with several hundred nanometers to micrometers were obtained during the phase separation process. These pores can act as ink reservoirs. The porous st s were thoroughly characterized by SEM, NMR, and contact angle measurement. The versatility of the porous st s was shown in three printing schemes. First, positive microcontact printing was achieved by printing a polar thioether-modified dendrimer as the ink, followed by backfilling and wet etching. Second, the porous st s were used for multiple printing of fluorescent proteins without reinking. Third, nanoparticles of about 60 nm in diameter, which cannot be directly transferred by oxidized PDMS st s, were successfully printed onto substrates by using these porous st s.
Publisher: Wiley
Date: 27-11-2018
Abstract: Gas–liquid reactions form the basis of our everyday lives, yet they still suffer poor reaction efficiency and are difficult to monitor in situ, especially at ambient conditions. Now, an inert gas–liquid reaction between aniline and CO 2 is driven at 1 atm and 298 K by selectively concentrating these immiscible reactants at the interface between metal–organic framework and solid nanoparticles (solid@MOF). Real‐time reaction SERS monitoring and simulations affirm the formation of phenylcarbamic acid, which was previously undetectable because they are unstable for post‐reaction treatments. The solid@MOF ensemble gives rise to a more than 28‐fold improvement to reaction efficiency as compared to ZIF‐only and solid‐only platforms, emphasizing that the interfacial nanocavities in solid@MOF are the key to enhance the gas–liquid reaction. Our strategy can be integrated with other functional materials, thus opening up new opportunities for ambient‐operated gas–liquid applications.
Publisher: American Chemical Society (ACS)
Date: 02-10-2013
DOI: 10.1021/LA403067H
Abstract: We demonstrate the creation of Ag-based bimetallic platonic Janus nanostructures by confining galvanic replacement reaction at a nanoscale interface on highly symmetrical nanostructures such as Ag nanocubes and nanooctahedra using reactive microcontact printing (μCP). The extent of galvanic replacement reaction can be controlled kinetically to derive Janus nanostructures with Au nanodots deposited on either one or multiple facets of Ag nanocubes. The selective deposition of Au dots on a single facet of Ag nanocubes breaks the cubic symmetry and brings about unique and anisotropic plasmonic responses. High-resolution cathodoluminescence hyperspectral imaging of single Janus nanocube demonstrates that surface plasmon resonances corresponding to Au and Ag can be excited at different spots on one Janus nanocube. In addition, we demonstrate the fabrication of alternating Janus/non-Janus segments on 2D Ag nanowires by using a line-patterned polydimethylsiloxane (PDMS) st for galvanic replacement. Aside from Au, Pt and Pd can also be selectively deposited onto Ag nanocubes. These Janus nanostructures may find important applications in the field of plasmon-enhanced catalysis.
Publisher: Wiley
Date: 04-07-2022
Abstract: Gas‐phase surface‐enhanced Raman scattering (SERS) remains challenging due to poor analyte affinity to SERS substrates. The reported use of capturing probes suffers from concurrent inconsistent signals and long response time due to the formation of multiple potential probe–analyte interaction orientations. Here, we demonstrate the use of multiple non‐covalent interactions for ring complexation to boost the affinity of small gas molecules, SO 2 and NO 2 , to our SERS platform, achieving rapid capture and multiplex detection down to 100 ppm. Experimental and in‐silico studies affirm stable ring complex formation, and kinetic investigations reveal a 4‐fold faster response time compared to probes without stable ring complexation capability. By synergizing spectral concatenation and support vector machine regression, we achieve 91.7 % accuracy for multiplex quantification of SO 2 and NO 2 in excess CO 2 , mimicking real‐life exhausts. Our platform shows immense potential for on‐site exhaust and air quality surveillance.
Publisher: Wiley
Date: 04-2014
Abstract: Inspired by aphids, liquid marbles have been studied extensively and have found application as isolated microreactors, as micropumps, and in sensing. However, current liquid‐marble‐based sensing methodologies are limited to qualitative colorimetry‐based detection. Herein we describe the fabrication of a plasmonic liquid marble as a substrate‐less analytical platform which, when coupled with ultrasensitive SERS, enables simultaneous multiplex quantification and the identification of ultratrace analytes across separate phases. Our plasmonic liquid marble demonstrates excellent mechanical stability and is suitable for the quantitative examination of ultratrace analytes, with detection limits as low as 0.3 fmol, which corresponds to an analytical enhancement factor of 5×10 8 . The results of our simultaneous detection scheme based on plasmonic liquid marbles and an aqueous–solid–organic interface quantitatively tally with those found for the in idual detection of methylene blue and coumarin.
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6AN01239F
Abstract: Designing substrate-less plasmonic metacrystals for the multiplex ultratrace detection of analytes from both organic and aqueous phases.
Publisher: American Chemical Society (ACS)
Date: 11-2013
DOI: 10.1021/AM403655G
Abstract: An analytical platform suitable for trace detection using a small volume of analyte is pertinent to the field of toxin detection and criminology. Plasmonic nanostructures provide surface-enhanced Raman scattering (SERS) that can potentially achieve trace toxins and/or molecules detection. However, the detection of highly diluted, small volume s les remains a challenge. Here, we fabricate a superhydrophobic SERS platform by assembling Ag nanocubes that support strong surface plasmon and chemical functionalization for trace detection with s le volume of just 1 μL. Our strategy integrates the intense electromagnetic field confinement generated by Ag nanocubes with a superhydrophobic surface capable of analyte concentration to lower the molecular detection limit. Single crystalline Ag nanocubes are assembled using the Langmuir-Blodgett technique to create surface roughness. To create a stable superhydrophobic SERS platform, an additional 25 nm Ag coating is evaporated over the Ag nanocubes to "weld" the Ag nanocubes onto the substrate followed by chemical functionalization with perfluorodecanethiol. The resulting substrate has an advancing contact angle of 169° ± 5°. Our superhydrophobic platform confines analyte molecules within a small area and prevents the random spreading of molecules. An analyte concentrating factor of 14-fold is attained, as compared to a hydrophilic surface. Consequently, the detection limit of our superhydrophobic SERS substrate reaches 10(-16) M (100 aM) for rhodamine 6G using 1 μL analyte solutions. An analytical SERS enhancement factor of 10(11) is achieved. Our protocol is a general method that provides a simple, cost-effective approach to develop a stable and uniform superhydrophobic SERS platform for trace molecular sensing.
Publisher: Wiley
Date: 14-06-2017
Abstract: Liquid marbles are emergent microreactors owing to their isolated environment and the flexibility of materials used. Plasmonic liquid marbles (PLMs) are demonstrated as the smallest spectroelectrochemical microliter-scale reactor for concurrent spectro- and electrochemical analyses. The three-dimensional Ag shell of PLMs are exploited as a bifunctional surface-enhanced Raman scattering (SERS) platform and working electrode for redox process modulation. The combination of SERS and electrochemistry (EC) capabilities enables in situ molecular read-out of transient electrochemical species, and elucidate the potential-dependent and multi-step reaction dynamics. The 3D configuration of our PLM-based EC-SERS system exhibits 2-fold and 10-fold superior electrochemical and SERS performance than conventional 2D platforms. The rich molecular-level electrochemical insights and excellent EC-SERS capabilities offered by our 3D spectroelectrochemical system are pertinent in charge transfer processes.
Publisher: Wiley
Date: 08-06-2009
Abstract: Freestanding particle bridges with controlled composition and macroscopic robustness are demonstrated by the use of supramolecular nanoparticle assembly. Self-assembly of nanoparticles, templating, and supramolecular glue infiltration are combined to form stable and ordered three-dimensional polystyrene particle composites on a polydimethylsiloxane st . Freestanding hybrid polystyrene nanoparticle bridges are obtained by transfer printing of the hybrid structures onto topographically patterned substrates via host-guest interactions. The mechanical robustness and rigidity of the particle bridges can be controlled by manipulating the layer-by-layer cycles of supramolecular glues of gold nanoparticles and dendrimers. Atomic force microscopy-based microbending results, in particular the location and force-dependent deflection behavior, confirm that the particle bridge fulfills the classical supported-beam characteristics. As estimated from classical beam theory, the bending moduli of the particle bridges vary between 0.8 and 1.1 GPa, depending on the degree of filling by the supramolecular glues. Failure analysis on the particle structure indicates linear elastic behavior and a plastic deformation upon failure.
Publisher: Wiley
Date: 11-04-2017
Abstract: 3D plasmonic colloidosomes are superior SERS sensors owing to their high sensitivity and excellent tolerance to laser misalignment. Herein, we incorporate plasmonic colloidosomes in a microfluidic channel for online SERS detection. Our method resolves the poor signal reproducibility and inter-s le contamination in the existing online SERS platforms. Our flow system offers rapid and continuous online detection of 20 s les in less than 5 min with excellent signal reproducibility. The isolated colloidosomes prevent cross-s le and channel contamination, allowing accurate quantification of s les over a concentration range of five orders of magnitude. Our system demonstrates high-resolution multiplex detection with fully preserved signal and Raman features of in idual analytes in a mixture. High-throughput multi-assay analysis is performed, which highlights that our system is capable of rapid identification and quantification of a sequence of s les containing various analytes and concentrations.
Publisher: Wiley
Date: 18-09-2023
Publisher: Wiley
Date: 19-04-2018
Abstract: Molecular-level airborne sensing is critical for early prevention of disasters, diseases, and terrorism. Currently, most 2D surface-enhanced Raman spectroscopy (SERS) substrates used for air sensing have only one functional surface and exhibit poor SERS-active depth. "Aerosolized plasmonic colloidosomes" (APCs) are introduced as airborne plasmonic hotspots for direct in-air SERS measurements. APCs function as a macroscale 3D and omnidirectional plasmonic cloud that receives laser irradiation and emits signals in all directions. Importantly, it brings about an effective plasmonic hotspot in a length scale of approximately 2.3 cm, which affords 100-fold higher tolerance to laser misalignment along the z-axis compared with 2D SERS substrates. APCs exhibit an extraordinary omnidirectional property and demonstrate consistent SERS performance that is independent of the laser and analyte introductory pathway. Furthermore, the first in-air SERS detection is demonstrated in stand-off conditions at a distance of 200 cm, highlighting the applicability of 3D omnidirectional plasmonic clouds for remote airborne sensing in threatening or inaccessible areas.
Publisher: American Chemical Society (ACS)
Date: 12-04-2021
Publisher: Wiley
Date: 30-05-2016
Abstract: Miniaturized liquid-liquid interfacial reactors offer enhanced surface area and rapid confinement of compounds of opposite solubility, yet they are unable to provide in situ reaction monitoring at a molecular level at the interface. A picoreactor operative at the liquid-liquid interface is described, comprising plasmonic colloidosomes containing Ag octahedra strategically assembled at the water-in-decane emulsion interface. The plasmonic colloidosomes isolate ultrasmall amounts of solutions (<200 pL), allowing parallel monitoring of multiple reactions simultaneously. Using the surface-enhanced Raman spectroscopy (SERS) technique, in situ monitoring of the interfacial protonation of dimethyl yellow (p-dimethylaminoazobenzene (DY)) is performed, revealing an apparent rate constant of 0.09 min(-1) for the first-order reaction. The presence of isomeric products with similar physical properties is resolved, which would otherwise be indiscernible by other analytical methods.
Publisher: American Chemical Society (ACS)
Date: 08-05-2008
DOI: 10.1021/CM703597W
Publisher: American Chemical Society (ACS)
Date: 12-03-2021
Publisher: American Chemical Society (ACS)
Date: 16-02-2010
DOI: 10.1021/AM9009007
Abstract: Dithiocarbamate-mediated bond formation combined with soft lithography was used for the selective immobilization of amine-functionalized silica nanoparticles on gold substrates. The available amine groups on the upper surface of the immobilized silica nanoparticles were further utilized for postdeposition of additional materials including particles, dyes, and biomolecules. The robustness of dithiocarbamate-mediated immobilization enables orthogonal assembly on surfaces via selective removal of the masking thiol ligands using iodine vapor etching followed by further functionalization.
Publisher: Springer Science and Business Media LLC
Date: 19-12-2013
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C3NR06316J
Abstract: Ag octahedron nanoparticles are assembled with graphene oxide (GO) sheets to form Ag octahedron@GO hybrids. Owing to the excellent chemical enhancement of GO, single particle SERS demonstrates an enhancement factor of 9 × 10 5 , which is twice as large as that of a pure octahedron.
Publisher: IOP Publishing
Date: 12-12-2006
Publisher: American Chemical Society (ACS)
Date: 10-12-2009
DOI: 10.1021/JA906954F
Abstract: The understanding of the localized surface plasmons (LSPs) that occur at the geometrically bounded surface of metal nanoparticles continues to advance as new and more complex nanostructures are found. It has been shown that the oscillation of electrons at the metal dielectric interface is strongly dependent on the size, symmetry, and proximity of nanoparticles. Here, we present a new method to chemically control the shape of silver nanocrystals by using a highly anisotropic etching process. Tuning of the etchant strength and reaction conditions allows the preparation of new nanoparticle shapes in high yield and purity, which cannot be synthesized with conventional nanocrystal growth methods. The etching process produces intraparticle gaps, which introduce modified plasmonic characteristics and significant scattering intensity in the near-infrared. These new silver particles serve as excellent substrates for wavelength-tunable, single-particle surface enhanced Raman spectroscopy (spSERS).
Publisher: American Chemical Society (ACS)
Date: 03-02-2009
DOI: 10.1021/LA8040715
Abstract: A superhydrophobic surface with a static water contact angle (theta(w)) > 150 degrees was created by a simple "dip-coating" method of 60-nm SiO2 nanoparticles onto an amine-terminated (NH2) self-assembled monolayer (SAM) glass/silicon oxide substrate, followed by chemical vapor deposition of a fluorinated adsorbate. For comparison, a close-packed nanoparticle film, formed by convective assembly, gave theta(w) approximately 120 degrees. The stability of the superhydrophobic coating was enhanced by sintering of the nanoparticles in an O2 environment at high temperature (1100 degress C). A sliding angle of < 5 degrees indicated the self-cleaning properties of the surface. The dip-coating method can be applied to glass substrates to prepare surfaces that are superhydrophobic and transparent.
Publisher: Springer Science and Business Media LLC
Date: 17-07-2018
DOI: 10.1038/S41467-018-05102-X
Abstract: Organizing nanoparticles into supercrystals comprising multiple structures remains challenging. Here, we achieve one assembly with dual structures for Ag polyhedral building blocks, comprising truncated cubes, cuboctahedra, truncated octahedra, and octahedra. We create two micro-environments in a solvent evaporation-driven assembly system: one at the drying front and one at the air/water interface. Dynamic solvent flow concentrates the polyhedra at the drying front, generating hard particle behaviors and leading to morphology-dependent densest-packed bulk supercrystals. In addition, monolayers of nanoparticles adsorb at the air/liquid interface to minimize the air/liquid interfacial energy. Subsequent solvent evaporation gives rise to various structurally erse dual-structure supercrystals. The topmost monolayers feature distinct open crystal structures with significantly lower packing densities than their densest-packed supercrystals. We further highlight a 3.3-fold synergistic enhancement of surface-enhanced Raman scattering efficiency arising from these dual-structure supercrystals as compared to a uniform one.
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C4CP03679D
Abstract: A high-throughput fabrication of a stable and uniform superhydrophobic SERS platform is demonstrated. It is able to detect trace molecules at ultra-low detection limit of 10 −17 M (10 aM) using just 4 μL of analyte solutions.
Publisher: AIP Publishing
Date: 27-12-2019
DOI: 10.1063/1.5130649
Abstract: Hybrid materials of earth abundant transition metal dichalcogenides and noble metal nanoparticles, such as molybdenum sulfide (MoSx) and gold nanoparticles, exhibit synergistic effects that can enhance electrocatalytic reactions. However, most current hybrid MoSx-gold synthesis requires an energy intensive heat source of & °C or chemical plating to achieve deposition of MoSx on the gold surface. Herein, we demonstrate the direct overgrowth of MoSx over colloidal nanoporous gold (NPG), conducted feasibly under ambient conditions, to form hybrid particles with enhanced electrocatalytic performance toward hydrogen evolution reaction. Our strategy exploits the localized surface plasmon resonance-mediated photothermal heating of NPG to achieve & °C surface temperature, which induces the decomposition of the (NH4)2MoS4 precursor and direct overgrowth of MoSx over NPG. By tuning the concentration ratio between the precursor and NPG, the amount of MoSx particles deposited can be systematically controlled from 0.5% to 2% of the Mo/(Au + Mo) ratio. Importantly, we find that the hybrid particles exhibit higher bridging and an apical S to terminal S atomic ratio than pure molybdenum sulfide, which gives rise to their enhanced electrocatalytic performance for hydrogen evolution reaction. We demonstrate that hybrid MoSx-NPG exhibits & mV lower onset potential and a 1.7-fold lower Tafel slope as compared to pure MoSx. Our methodology provides an energy- and cost-efficient synthesis pathway, which can be extended to the synthesis of various functional hybrid structures with unique properties for catalysis and sensing applications.
Publisher: Wiley
Date: 22-07-2014
Abstract: A major challenge in plasmonic hot spot fabrication is to efficiently increase the hot spot volumes on single metal nanoparticles to generate stronger signals in plasmon-enhanced applications. Here, the synthesis of designer nanoparticles, where plasmonic-active Au nanodots are selectively deposited onto the edge/tip hot spot regions of Ag nanoparticles, is demonstrated using a two-step seed-mediated precision synthesis approach. Such a "hot spots over hot spots" strategy leads to an efficient enhancement of the plasmonic hot spot volumes on single Ag nanoparticles. Through cathodoluminescence hyperspectral imaging of these selective edge gold-deposited Ag octahedron (SEGSO), the increase in the areas and emission intensities of hot spots on Ag octahedra are directly visualized after Au deposition. Single-particle surface-enhanced Raman scattering (SERS) measurements demonstrate 10-fold and 3-fold larger SERS enhancement factors of the SEGSO as compared to pure Ag octahedra and non-selective gold-deposited Ag octahedra (NSEGSO), respectively. The experimental results corroborate well with theoretical simulations, where the local electromagnetic field enhancement of our SEGSO particles is 15-fold and 1.3-fold stronger than pure Ag octahedra and facet-deposited particles, respectively. The growth mechanisms of such designer nanoparticles are also discussed together with a demonstration of the versatility of this synthetic protocol.
Publisher: American Chemical Society (ACS)
Date: 14-08-2017
DOI: 10.1021/JACS.7B04936
Abstract: We demonstrate a molecular-level observation of driving CO
Publisher: American Chemical Society (ACS)
Date: 11-06-2014
DOI: 10.1021/PH5001154
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2CC00597B
Abstract: ‘Plasmonic bubbles’ as a versatile, air-stable, centimetre-sized 3D SERS platform with bi-directional gas sensing capabilities.
Publisher: Wiley
Date: 21-05-2009
Publisher: Wiley
Date: 26-11-2015
Abstract: Localized photoluminescence manipulation of 1L-MoS2 is achieved by using single shape-controlled Ag nanoantenna. By varying the antenna morphology, the photoluminescence of 1L-MoS2 is continuously tunable from enhanced (>2-fold) to weakened (>2-fold) states. A heterogeneous optical platform is realized by depositing various antennas on the same 1L-MoS2 , with an unprecedented range of photoluminescence output being observed simultaneously.
Publisher: Wiley
Date: 30-05-2016
Publisher: Wiley
Date: 27-07-2020
Publisher: No publisher found
Date: 2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2010
DOI: 10.1039/C0NR00007H
Abstract: A new approach for fabricating porous structures on silicon substrates and on polymer surfaces, using colloidal particle arrays with a polymer mask of a highly etch-resistant organometallic polymer, is demonstrated. Monolayers of silica particles, with diameters of 60 nm, 150 nm, 300 nm, or 500 nm, were deposited either on a silicon substrate or on a surface coated with polyethersulfone (PES), and the voids of the arrays were filled with poly(ferrocenylmethylphenylsilane) (PFMPS). Argon ion sputtering removed the excess PFMPS on the particles which enabled removal of the particles with HF. Further pattern transfer steps with reactive ion etching for different time intervals provided structures in silicon or in a PES layer. Free-standing PES membranes exhibiting regular arrays of circular holes with high porosity were fabricated by using cellulose acetate as a sacrificial layer. The pores obtained on silicon substrates after etching were used as molds for nanoimprint lithography (NIL). A combination of the techniques of nanosphere lithography (NSL) and NIL has resulted in 3D nanostructures with a hemispherical shape (inherited from the nanoparticles) which was obtained both in silicon and in PMMA.
Publisher: American Chemical Society (ACS)
Date: 12-11-2015
No related grants have been discovered for Xing Yi Ling.