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This study explores plasmon-induced electrochemical reactions on single nanoparticles using electrogenerated chemiluminescence microscopy (ECLM). Under laser irradiation, real-time screening showed lower plasmon-induced reaction efficiency for bimetallic Au@Pt nanoparticles compared to monometallic Au nanoparticles. ECLM offers a high-throughput imaging and precise quantitative approach for analyzing photo-electrochemical conversion at single nanoparticle level, valuable for both theoretical exploration and optimization of plasmonic nanocatalysts. [ABSTRACT FROM AUTHOR]

By assembling nanotweezers with ATP-splitting aptamers on gold nanorods (AuT123L), we constructed a near-infrared-activated ATP sensing device that could time-controllably image ATP levels in living cells. By replacing the aptamers on the nanotweezers, the nanoplatform can be applied to other important biomolecules, opening up more possibilities for the study of time controllable nanodevices. [ABSTRACT FROM AUTHOR]

Based on the nonlinear plasmonic scattering response to the modulated excitation in time, we realized a single-wavelength super-resolution imaging method on a custom-built system which is named as a scattering saturation STED (ssSTED) microscope. A spatial resolution of λ/7 (65 nm) was obtained on 50 nm gold nanoparticles. [ABSTRACT FROM AUTHOR]

We developed an electrochemiluminescence (ECL) microscopy technique to image the structure-dependent electrocatalytic reactivity of bimetallic Pd–Au nanorods (NRs) at the single-particle level. [ABSTRACT FROM AUTHOR]

Based on the structural programmability and spatial addressability of DNA nanodevices, a target-triggered, enzyme-free 3D DNA walker, comprising of hairpin DNA assembled gold nanoparticles with a local catalytic hairpin assembly reaction, was developed for the highly sensitive detection of intracellular tumor-associated microRNAs. [ABSTRACT FROM AUTHOR]

Gold nanoparticle dimers assembled on the surface of CdS QD thin films served as nano-antennas to mediate the distance-dependent plasmon enhanced electrochemiluminescence of QDs. [ABSTRACT FROM AUTHOR]

Single-cell analysis techniques are essential for understanding the microheterogeneity and functions of cells. Low-copy-number proteins play important roles in cell functioning, but their measurement in single cells remains challenging. Herein, we report an approach, called plasmonic immunosandwich assay (PISA), for probing low-copy-number proteins in single cells. This approach combined in vivo immunoaffinity extraction and plasmon-enhanced Raman scattering (PERS). Target proteins were specifically extracted from the cells by microprobes modified with monoclonal antibody or molecularly-imprinted polymer (MIP), followed by labeling with Raman-active nanotags. The PERS detection, with Raman intensity enhanced by 9 orders of magnitude, provided ultrasensitive detection at the single-molecule level. Using this approach, we found that alkaline phosphatase and survivin were expressed in distinct levels in cancer and normal cells, and that extended culture passage resulted in reduced expression of survivin. We further developed acupuncture needle-based PISA for probing low-copy-number proteins in living bodies. [ABSTRACT FROM AUTHOR]

A novel strategy for the preparation of an aptamer based organic–inorganic hybrid affinity monolithic column was developed successfully using gold nanoparticles (GNPs) as an intermediary for a sandwich structure to realize the functional modification of the surface of the monolithic matrix. This monolithic matrix was facilely pre-synthesized via one-step co-condensation. Due to the high surface-to-volume ratio of GNPs and the large specific surface area of the hybrid matrix, the average coverage density of aptamers on the hybrid monolith reached 342 pmol μL−1. With the combination of an aptamer based hybrid affinity monolithic column and enzymatic chromogenic assay, the quantitation and detection limits of thrombin were as low as 5 nM and 2 nM, respectively. These results indicated that the GNPs attached monolith provided a novel technique to immobilize aptamers on an organic–inorganic hybrid monolith and it could be used to achieve highly selective recognition and determination of trace proteins. [ABSTRACT FROM AUTHOR]

A novel three-dimensionally structured DNA probe is reported to realize in situ“off–on” imaging of intracellular telomerase activity. The probe consists of a DNA tetrahedron and a hairpin DNA on one of the vertices of the DNA tetrahedron. It is composed of four modified DNA segments: S1–Au nanoparticle (NP) inserting a telomerase strand primer (TSP) and S2–S4, three Cy5 dye modified DNA segments. Fluorescence of Cy5 at three vertices of the DNA tetrahedron is quenched by the Au NP at the other vertex due to the effective fluorescence resonance energy transfer (FRET) (“off” state). When the probe meets telomerase, the hairpin structure changes to rod-like through complementary hybridization with the telomerase-triggered stem elongation product, resulting in a large distance between the Au NP and Cy5 and the recovery of Cy5 fluorescence (“on” state). The molar ratio of 3 : 1 between the reporter (Cy5) and the target related TSP makes the probe show high sensitivity and recovery efficiency of Cy5 in the presence of telomerase extracted from HeLa cells. Given the functional and compact nanostructure, the mechanically stable and noncytotoxic nature of the DNA tetrahedron, this FRET-based probe provides more opportunities for biosensing, molecular imaging and drug delivery. [ABSTRACT FROM AUTHOR]

Using single stranded DNA (ssDNA) as a distance controller and Au nanoparticles (NPs) functionalized with ssDNA as novel energy-transfer nanoprobes, an ultrasensitive energy-transfer based photoelectrochemical protein biosensor was realized. [ABSTRACT FROM AUTHOR]

Measurement of electron transfer at single-molecule level is normally restricted by the detection limit of faraday current, currently in a picoampere to nanoampere range. Here we demonstrate a unique graphene-based electrochemical microscopy technique to make an advance in the detection limit. The optical signal of electron transfer arises from the Fermi level-tuned Rayleigh scattering of graphene, which is further enhanced by immobilized gold nanostars. Owing to the specific response to surface charged carriers, graphene-based electrochemical microscopy enables an attoampere-scale detection limit of faraday current at multiple individual gold nanoelectrodes simultaneously. Using the graphene-based electrochemical microscopy, we show the capability to quantitatively measure the attocoulomb-scale electron transfer in cytochrome c adsorbed at a single nanoelectrode. We anticipate the graphene-based electrochemical microscopy to be a potential electrochemical tool for in situ study of biological electron transfer process in organelles, for example the mitochondrial electron transfer, in consideration of the anti-interference ability to chemicals and organisms. Measurement of single-molecule level electron transfer is restricted by detection limits in nanoampere to picoampere ranges. Here the authors develop graphene-based electrochemical microscopy to attain an attoampere-level detection limit for faraday current at single nanoparticles. [ABSTRACT FROM AUTHOR]

We report herein the energy transfer (ET) between semiconducting polymer dots (Pdots) and gold nanoparticles (Au NPs) in a photoelectrochemical (PEC) system and its feasibility for cathodic bioanalysis application. Specifically, COOH-capped Pdots were first fabricated and then assembled onto the indium-tin oxide (ITO) surface, followed by the modification of single-strand (ss) DNA probe (pDNA). After the DNA hybridization with the Au NPtethered complementary ssDNA (Au NP-tDNA), the Au NPs were brought into the close proximity of Pdots. Upon light stimulation, photoluminescence (PL) was annihilated, fluorescence was attenuated, and the photocurrent intensity was evidently decreased. This ET-based PEC DNA sensor exhibited a linear range from 1 fM to 10 pM with a detection limit of 0.97 fM at a signal-to-noise ratio of 3. The present work first exploited the ET between Pdots and Au NPs, and we believe this phenomenon will spark new interest in the study of various Pdots-based ET-influenced PEC systems and thus catalyze increasing studies for specific bioanalytical purposes. [ABSTRACT FROM AUTHOR]

A simple yet powerful polymerase chain reaction (PCR)-free strategy for visualized assay of human telomerase activity was reported in this work. Gold nanoparticles (AuNPs) based colorimetric strategy was applied with well-designed enzyme-aided cyclic amplification. Briefly, the detection relies on the elongated primers of telomerase substrate (TS) induced by telomerase, which open the hairpin DNA and hybridize with linker DNA, the trigger of AuNPs aggregation. Nicking endonuclease was added in the sensing system, which cleaved linker DNA after hybridization and released complimentary strand for cyclic hybridization with linker DNA, resulted in high sensitivity for the detection of telomerase. Down to 25 HeLa cells with high expression of telomerase could be recognized. The proposed strategy provides a good platform for the determination of telomerase activity, differentiation of cancer cell lines from normal cell line and screening of telomerase-targeted anticancer drugs. [ABSTRACT FROM AUTHOR]

Quantification of trace serum circulate microRNAs is extremely important in clinical diagnosis but remains a great challenge. Herein we developed an ultrasensitive platform for microRNA 141 (miR- 141) detection based on a silver coated gold nanorods (Au@Ag NRs) etching process accompanied by surface plasmon resonance (SPR) shift. Both SPR absorption and scattering responses were monitored. Combined amplification cascades of catalyzed hairpin assembly (CHA) and hybridization chain reaction (HCR) with the sensitive SPR responses of plasmonic Au@Ag NRs, the proposed bioassay exhibited ultrahigh sensitivity toward miRNA-141 with dynamic range from 5.0 x 10-17 M to 1.0 x 10-11 M. With target concentration higher than 1.0 x 10-13 M, the color of the solution changed obviously that could be observed with naked eyes. Under dark-field microscopy observation of individual particle, a limit of detection down to 50 aM could be achieved. Owing to the superior sensitivity and selectivity, the proposed method was applied to detecting trace microRNA in serum. Similar SPR assays could be developed simply by redesigning the switching aptamer for the detections of other microRNAs or targets such as small molecule, DNA, or protein. Considering the convenient operation, good performance and simple observation modes of this method, it may have great potential in trace bioanalysis for clinical applications. [ABSTRACT FROM AUTHOR]

Here, a mass-sensitive microRNA sensing surface is developed by utilizing a probe DNA/gold nanoparticles (GNP)/dendrimer composite coupling with an enzymatic amplification process. The probe DNA/GNP/dendrimer composite is prepared via the covalent coupling between the NH 2 groups in PAMAM or DNA and the COOH group on GNP. Target microRNA binds to a stem-loop-structured DNA on maganatic NPs, forming a heteroduplex. By enzyme recycling amplification, a large number of linker sequences are produced on MNPs. Via the combination of probe DNA, the linker DNA on MNPs and a capture DNA on gold chip, the DNA/GNP/dendrimer probe could be assembled on the surface of gold chip inducing a sensitive frequency response. It presents an excellent performance in microRNA-203 quantification with a detection linear range of 1.0×10 −11 –1.0×10 −9 M. Both the success in discriminating expressing miroRNA-203 in MCF-7 cell and the well agreement with the commercial qRT-PCR detection method implied its potential application in early cancer diagnosis for future. [ABSTRACT FROM AUTHOR]

A highly sensitive electrogenerated chemiluminescence (ECL) biosensor was developed on the basis of a closed bipolar electrode (BPE) apparatus for the analysis of prostate specific antigen (PSA). Bipolar modifications bring up two different stages of enhancement on the same electrode. Anodic enhancement was conducted by modifying gold nanoparticles (Au NPs) to catalyze the anodic ECL reaction between luminol and hydrogen peroxide. Cathodic introduction of thionine tagged PSA antibody led to a further pertinently enhancement synchronized with the PSA amount variation, because the existence of thionine greatly increased the rate of electron gains on cathode, leading to the corresponding acceleration of anodic ECL reaction. The more thionine modified target molecules were introduced, the faster luminol was oxidized, the higher faraday current approached, and sensitive quantification was realized in correlation with the responsive ECL intensity differences. The quantification resulted in a good determination range between 0.1 pg/mL and 0.1 µg/mL. This strategy mainly took advantage of the special structure of closed BPE to realize a simultaneous amplification on both ends of BPE. Moreover, the platform had a potential of providing a multi-functional strategy for the realization of other bio-detections by simply substituting the PSA sandwich structure with other bio-structures. [ABSTRACT FROM AUTHOR]

Here we have developed a sensitive cancer cell amplified detection method which combined Au NPs enhanced electrochemiluminescence (ECL) of CdS nanocrystals (NCs) film, with isothermal circular amplification reaction of polymerase. In DNA circular amplification detection system, hairpin DNA beacon/Au NPs composite modified CdS NCs film was used as an ECL emitter. Messenger DNA is hybridized with the aptamer modified on magnetic beads (MBs) to form MB–Au bioconjugates. In the presence of HL-60 cell, the aptamer would conjugate with the glycoprotein at cell surface and messenger DNA sequence would be released. The released messenger DNA sequence was then introduced into the cycle amplification system to trigger circular polymerizations. This assay allows us to determine the released messenger DNA equivalent to 10 cells and exhibits a significant specificity for HL-60 cells. [ABSTRACT FROM AUTHOR]

A novel photoelectrochemical (PEC) sensor for mercury ions (Hg 2 + ) was fabricated based on the energy transfer (ET) between CdS quantum dots (QDs) and Au nanoparticles (NPs) with the formation of T–Hg 2 + –T pairs. In the presence of Hg 2 + ions, a T-rich single-strand (ss) DNA labeled with Au NPs could hybridize with another T-rich ssDNA anchored on the CdS QDs modified electrode, through T–Hg 2 + –T interactions, rendering the Au NPs in close proximity with the CdS QDs and hence the photocurrent decrease due to the ET between the CdS QDs and the Au NPs. Under the optimal condition, the photocurrent decrease was proportional to the Hg 2 + concentration, ranging from 3.0 × 10 − 9 to 1.0 × 10 − 7 M, with the detection limit of 6.0 × 10 − 10 M. [ABSTRACT FROM AUTHOR]