Single Gold Nanoparticles Research Articles

Investigations on the damping of acoustic vibrations of single gold nanoparticles in water by continuum and atomistic simulations

Investigations on the damping of acoustic vibrations of single gold nanoparticles in water by continuum and atomistic simulations

Thousand-Fold Enhancement of Photothermal Signals in Near-Critical CO2.

Photothermal (PT) microscopy has shown strong promise in imaging single absorbing nano-objects in soft matter and biological systems. PT imaging at ambient conditions usually requires a high laser power for a sensitive detection, which prevents application to light-sensitive nanoparticles. In a previous study of single gold nanoparticles, we showed that the photothermal signal can be enhanced more than 1000-fold in near-critical xenon compared to that in glycerol, a typical medium for PT detection. In this report, we show that carbon dioxide (CO2), a much cheaper gas than xenon, can enhance PT signals in a similar way. We confine near-critical CO2 in a thin capillary which easily withstands the high near-critical pressure (around 74 bar) and facilitates sample preparation. We also demonstrate enhancement of the magnetic circular dichroism signal of single magnetite nanoparticle clusters in supercritical CO2. We have performed COMSOL simulations to support and explain our experimental findings.

Towards Electrochemiluminescence Microscopy Exploration of Plasmonic-Mediated Phenomena at the Single-Nanoparticle Level.

The rational design of functional plasmonic metasurfaces and metamaterials requires the development of high-throughput characterization techniques compatible with operando conditions and capable of addressing single-nanostructures. In their work, Wei et al. demonstrate the use of electrochemiluminescence microscopy to investigate the mechanism behind plasmon-enhanced luminescence induced by gold nanostructures. The use of gold plasmonic arrays was exploited to achieve the rapid spectroscopic evaluation of all the individual nanostructures, and the correlation of the results with high- resolution electron microscopy analysis, guaranteeing a strict one-to-one correspondence. The authors were able to identify two different mechanisms for the enhancement of [Ru(bpy)3 ]2+ -tri-n-propylamine electrochemiluminescence mediated by single gold nanoparticles and by small plasmonic clusters. In the future, the proposed characterization could be used for the rapid and in situ spectroscopic analysis of more complex plasmonic nanostructures and metasurfaces.

Towards Electrochemiluminescence Microscopy Exploration of Plasmonic‐Mediated Phenomena at the Single‐Nanoparticle Level

AbstractThe rational design of functional plasmonic metasurfaces and metamaterials requires the development of high‐throughput characterization techniques compatible with operando conditions and capable of addressing single‐nanostructures. In their work, Wei et al. demonstrate the use of electrochemiluminescence microscopy to investigate the mechanism behind plasmon‐enhanced luminescence induced by gold nanostructures. The use of gold plasmonic arrays was exploited to achieve the rapid spectroscopic evaluation of all the individual nanostructures, and the correlation of the results with high‐ resolution electron microscopy analysis, guaranteeing a strict one‐to‐one correspondence. The authors were able to identify two different mechanisms for the enhancement of [Ru(bpy)3]2+‐tri‐n‐propylamine electrochemiluminescence mediated by single gold nanoparticles and by small plasmonic clusters. In the future, the proposed characterization could be used for the rapid and in situ spectroscopic analysis of more complex plasmonic nanostructures and metasurfaces.

Multispectral Localized Surface Plasmon Resonance (msLSPR) Reveals and Overcomes Spectral and Sensing Heterogeneities of Single Gold Nanoparticles.

Metal nanoparticles can be sensitive molecular sensors due to enhanced absorption and scattering of light near a localized surface plasmon resonance (LSPR). Variations in both intrinsic properties such as the geometry and extrinsic properties such as the environment can cause heterogeneity in nanoparticle LSPR and impact the overall sensing responses. To date, however, few studies have examined LSPR and sensing heterogeneities, due to technical challenges in obtaining the full LSPR spectra of individual nanoparticles in dynamic assays. Here, we report multispectral LSPR (msLSPR), a wide-field imaging technique for real-time spectral monitoring of light scattering from individual nanoparticles across the whole field of view (FOV) at ∼0.5 nm spectral and ∼100 ms temporal resolutions. Using msLSPR, we studied the spectral and sensing properties of gold nanoparticles commonly used in LSPR assays, including spheres, rods, and bipyramids. Complemented with electron microscopy imaging, msLSPR analysis revealed that all classes of gold nanoparticles exhibited variations in LSPR peak wavelengths that largely paralleled variations in morphology. Compared with the rods and spheres, gold nanobipyramids exhibited both more uniform and stronger sensing responses as long as the bipyramids are structurally intact. Simulations incorporating the experimental LSPR properties demonstrate the negative impact of spectral heterogeneity on the overall performance of conventional, intensity-based LSPR assays and the ability of msLSPR in overcoming both particle heterogeneity and measurement noise. These results highlight the importance of spectral heterogeneity in LSPR-based sensors and the potential advantage of performing LSPR assays in the spectral domain.

Plasmonic hot carrier injection from single gold nanoparticles into topological insulator Bi2Se3 nanoribbons.

Plasmonic gold nanoparticles injecting hot carriers into the topological insulator (TI) interface of Bi2Se3 nanoribbons are studied by resonant Raman spectroscopy. We resolve the impact of individual gold particles with sizes ranging from 140 nm down to less than 40 nm on the topological surface states of the nanoribbons. In resonance at 1.96 eV (633 nm), we find distinct phonon renormalization in the Eg2- and A1g2-modes that can be associated with plasmonic hot carrier injection. The phonon modes are strongly enhanced by a factor of 350 when tuning the excitation wavelengths into interband transition and in resonance with the surface plasmon of gold nanoparticles. At 633 nm wavelength, a plasmonic enhancement factor of 18 is observed indicating a contribution of hot carriers injected from the gold nanoparticles into the TI interface. Raman studies as a function of gold nanoparticle size reveal the strongest hot carrier injection for particles with size of 108 nm in agreement with the resonance energy of its surface plasmon. Hot carrier injection opens the opportunity to locally control the electronic properties of the TI by metal nanoparticles attached to the surface of nanoribbons.

In situ reversible tuning of chemical interface damping in mesoporous silica-coated gold nanorods via direct adsorption and removal of thiol.

Chemical interface damping (CID) is a recently proposed plasmon decay channel in gold nanoparticles. However, thus far, a very limited number of studies have focused on controlling CID in single gold nanoparticles. Herein, we describe a new simple method for reversible tuning of CID in single gold nanorods coated with a mesoporous silica shell (AuNRs@mSiO2). We used 1-alkanethiols with two different carbon chain lengths (1-butanethiol and 1-decanethiol) as adsorbates to induce CID. In addition, NaBH4 solution was used to remove the attached thiol from the AuNR surface. We confirmed the adsorption and removal of 1-alkanethiols on single AuNRs@mSiO2 and the corresponding changes in localized surface plasmon resonance (LSPR) peak wavelengths and linewidths. Furthermore, we investigated the effect of immersion time in NaBH4 solution on thiol removal from AuNRs@mSiO2. Therefore, the LSPR properties and CID can be controlled, thereby paving the way for in situ reversible tuning of CID by repeated adsorption and desorption of thiol molecules on single AuNRs@mSiO2.

In Vivo Voltammetric Imaging of Metal Nanoparticle-Catalyzed Single-Cell Electron Transfer by Fermi Level-Responsive Graphene.

Metal nanomaterials can facilitate microbial extracellular electron transfer (EET) in the electrochemically active biofilm. However, the role of nanomaterials/bacteria interaction in this process is still unclear. Here, we reported the single-cell voltammetric imaging of Shewanella oneidensis MR-1 at the single-cell level to elucidate the metal-enhanced EET mechanism in vivo by the Fermi level-responsive graphene electrode. Quantified oxidation currents of ~20 fA were observed from single native cells and gold nanoparticle (AuNP)-coated cells in linear sweep voltammetry analysis. On the contrary, the oxidation potential was reduced by up to 100 mV after AuNP modification. It revealed the mechanism of AuNP-catalyzed direct EET decreasing the oxidation barrier between the outer membrane cytochromes and the electrode. Our method offered a promising strategy to understand the nanomaterials/bacteria interaction and guide the rational construction of EET-related microbial fuel cells.

Molecular Dynamics Simulations of Polydopamine Nanosphere's Structure Based on Experimental Evidence.

In this work, we show how to obtain internal monodispersed gold nanoparticles inside polydopamine (PDA) nanospheres that are also externally decorated with gold. The number of internal nanoparticles is affected by the size of the PDA nanosphere used, and the lower limit in the number of gold nanoparticles in the center of decorated nanospheres, one single gold nanoparticle, has been reached. In addition, extensive molecular dynamics simulations of PDA nanospheres based on four different chemical motifs, in the presence of water and with different sizes, have been performed to gain insight into the arrangements capable of accommodating cavities. In particular, PDA nanospheres based on pyranoacridinotrione (PYR) units provide good agreement with the experimental attainment of internal metal nanoparticles. In these, the stacking of PYR units leads to a particular morphology, with large portions of space occupied by the solvent, that would explain the observed formation of gold nanoparticles inside the PDA nanosphere.

Early warning of Diaporthe infection in kiwifruit soft rot by plasmonic dimer-enhanced Raman spectroscopy.

Diaporthe genus is the dominant pathogens of kiwifruit soft rot with long incubation period and rapid onset and very hard to detect in advance. It is of great significance to develop point-of-care tests for disease prevention and field management. Here we screen a pair of genus-level primers for constructing plasmonic dimer Rayleigh/Raman spectroscopy, which enables rapid, specific, and sensitive detection of Diaporthe genus in real kiwifruits. Dark-filed Rayleigh scattering clearly visualizes the target-induced dimer assembly of nanoprobes. Plasmonic dimer-enhanced Raman spectroscopy has high specificity for 12 common isolates of Diaporthe genus in one batch samples with highly accurate results and much higher sensitivity than polymerase chain reaction (PCR). It realizes the recognition of Diaporthe infection at an early stage of 24h when the kiwifruits do not have any noticeable symptoms. It demonstrates a bright prospect of point-of-care tests for early warning of kiwifruit soft rot infection and quality control.

Fabrication of CuO nanorod loaded with a single gold nanoparticle for low-temperature NO2 detection

• Au nanoparticles loaded CuO nanorods were prepared by an easy two-step method. • The CuO nanorod could be loaded with a single gold nanoparticle. • The 2 mol% Au@CNRs exhibited room-temperature NO 2 sensing properties. • Enhancement mechanism of Au loading was discussed by activation energy theory. The problem of high operating temperature and high power consumption in practical detection has been existing in semiconducting CuO based gas sensors. With sensitization of noble metals, Au nanoparticles loaded CuO nanorods with different concentrations were prepared with an easy two-step method. The crystal structure, morphology, nanosize, and chemical composition of the samples were examined by XRD, FESEM, TEM, and XPS respectively. The CuO nanorod was loaded with a single gold nanoparticle with the Au-loading concentration of 2 mol%. This 2 mol% Au loaded CuO nanorod sample exhibited enhanced NO 2 sensing performance, which can obtain the same peak response 4.3 to 5 ppm NO 2 at a lower temperature of 100 °C as compared with that of the pure CuO nanorods at 150 °C. Meanwhile, the response/recovery speed and selectivity were also promoted. More importantly, Au loaded CuO nanorods can realize NO 2 detection in room temperature (25 °C). The low-temperature sensitization mechanism with Au-loading was also investigated.

Photothermal Circular Dichroism Measurements of Single Chiral Gold Nanoparticles Correlated with Electron Tomography.

Chemically synthesized metal nanoparticles with morphological chiral features are known to exhibit strong circular dichroism. However, we still lack understanding of the correlation between morphological and chiroptical features of plasmonic nanoparticles. To shed light on that question, single nanoparticle experiments are required. We performed photothermal circular dichroism measurements of single chiral and achiral gold nanoparticles and correlated the chiroptical response to the 3D morphology of the same nanoparticles retrieved by electron tomography. In contrast to an ensemble measurement, we show that individual particles within the ensemble display a broad distribution of strength and handedness of circular dichroism signals. Whereas obvious structural chiral features, such as helical wrinkles, translate into chiroptical ones, nanoparticles with less obvious chiral morphological features can also display strong circular dichroism signals. Interestingly, we find that even seemingly achiral nanoparticles can display large g-factors. The origin of this circular dichroism signal is discussed in terms of plasmonics and other potentially relevant factors.

Hybrid Carbon Nanotubes/Gold Nanoparticles Composites for Trace Nitric Oxide Detection over a Wide Range of Humidity

Composites of functionalized single walled carbon nanotubes (SWCNTs) and gold nanoparticles (Au NPs) of ≈15 nm diameter were drop-cast on a printed circuit board (PCB) substrate equipped with interdigitated electrodes to make a hybrid thin film. Addition of Au NPs decorated the surface of SWCNTs networked films and acted as catalysts which resulted into an enhanced sensitivity and low ppb concentration detection limit. The compositions of the film were characterized by scanning electron microscope (SEM). SWCNTs clusters were loaded with various amount of Au NPs ranging from 1–10% (by weight) and their effect on Nitric oxide (NO) sensitivity was studied and optimized. Further, the optimized composite films were tested in both air and nitrogen environments and as well as over a wide relative humidity range (0–97%). Sensors were also tested for the selectivity by exposing to various gases such as nitrous oxide, ammonia, carbon monoxide, sulfur dioxide and acetone. Sensitivity to NO was found much higher than the other tested gases. The advantage of this sensor is that it is sensitive to NO at low ppb level (10 ppb) with estimated response time within 10 s and recovery time around 1 min, and has excellent reproducibility from sensor to sensor and works within the wide range of relative humidity (0–97%).

Gap Plasmonics of Single Gold Nanoparticle Above a Gold Substrate Covered with Thin Gain Film

Gap Plasmonics of Single Gold Nanoparticle Above a Gold Substrate Covered with Thin Gain Film

Detection of Single Nanoparticles inside a Single Terahertz Resonator

With the rapid advancement of 5G/6G communications using millimeter wavelengths, the concomitant usage of these long wavelength radiation for remote sensing and monitoring of biological and chemical agents is anticipated. However, the ability to detect and identify these agents with sizes ranging from nanometers to microns is hampered by its millimeter wavelength, which drastically reduces the interaction cross‐section. Herein, it is reported that single gold nanoparticles (NPs) drop‐casted on the nanoresonator can be observed by monitoring the far‐field transmitting spectra of individual terahertz (THz) nanoresonators, which enhance the electric field hundreds of times on the nanoscale. Despite the enormous mismatch in length scales, full‐wave 3D numerical modeling of the single THz nanoresonator is also performed to interpret the experimental results, indicating the possibility to turn off the resonance using only one NP embedded in the hotspot of the nanoresonator. Such NP detection becomes the most sensitive when the particle, whose size is comparable to the gap width, is tightly fitted into the nanoresonator. This work unveils the potential associated with refractive index sensing and hyperspectral absorption spectroscopy for detecting and fingerprinting ultra‐low density of bio/chemical molecules such as viruses, lipid vesicles, and explosives.

A novel binding-induced DNAzyme motor triggered by survivin mRNA.

The accurate and sensitive detection of survivin mRNA is of great significance for cancer diagnosis and treatment. However, limited by the low-abundance mRNA in live cells, most strategies of survivin mRNA detection that were one-to-one signal-triggered model (one target triggered one signal) were inapplicable in practice. Here, we reported a binding-induced DNAzyme motor triggered by the survivin mRNA, which was a one-to-more signal-triggered model (one target triggered more signals), amplifying the detection signal and enhancing the sensitivity. The nanomotor is constructed by assembling several DNAzyme motor strands silenced by the blocker strands, and dozens of FAM-labeled substrate strands on a single gold nanoparticle (AuNP), forming three-dimensional DNA tracks. Through building the survivin mRNA bridge between the blocker and the DNAzyme motor strand, the binding-induced DNA nanomotor could be triggered by survivin mRNA. The operation of the DNAzyme motor was self-powered. And each walking step of the DNAzyme motor was fueled by DNAzyme-catalyzed substrate cleavage, along with the cleavage of the fluorescent molecule, resulting in autonomous and progressive walking along the AuNP-based tracks, and the fluorescence increase. The DNAzyme motor exhibited excellent sensitivity and remarkable specificity for survivin mRNA, providing the potential for cell image.

Text-mined dataset of gold nanoparticle synthesis procedures, morphologies, and size entities

Gold nanoparticles are highly desired for a range of technological applications due to their tunable properties, which are dictated by the size and shape of the constituent particles. Many heuristic methods for controlling the morphological characteristics of gold nanoparticles are well known. However, the underlying mechanisms controlling their size and shape remain poorly understood, partly due to the immense range of possible combinations of synthesis parameters. Data-driven methods can offer insight to help guide understanding of these underlying mechanisms, so long as sufficient synthesis data are available. To facilitate data mining in this direction, we have constructed and made publicly available a dataset of codified gold nanoparticle synthesis protocols and outcomes extracted directly from the nanoparticle materials science literature using natural language processing and text-mining techniques. This dataset contains 5,154 data records, each representing a single gold nanoparticle synthesis article, filtered from a database of 4,973,165 publications. Each record contains codified synthesis protocols and extracted morphological information from a total of 7,608 experimental and 12,519 characterization paragraphs.

Genetically Modified Soybean Detection Using a Biosensor Electrode with a Self-Assembled Monolayer of Gold Nanoparticles.

In this study, we proposed a genosensor that can qualitatively and quantitatively detect genetically modified soybeans using a simple electrode with evenly distributed single layer gold nanoparticles. The DNA sensing electrode is made by sputtering a gold film on the substrate, and then sequentially depositing 1,6-hexanedithiol and gold nanoparticles with sulfur groups on the substrate. Then, the complementary to the CaMV 35S promoter (P35S) was used as the capture probe. The target DNA directly extracted from the genetically modified soybeans rather than the synthesized DNA segments was used to construct the detection standard curve. The experimental results showed that our genosensor could directly detect genetically modified genes extracted from soybeans. We obtained two percentage calibration curves. The calibration curve corresponding to the lower percentage range (1–6%) exhibits a sensitivity of 2.36 Ω/% with R2 = 0.9983, while the calibration curve corresponding to the higher percentage range (6–40%) possesses a sensitivity of 0.1 Ω/% with R2 = 0.9928. The limit of detection would be 1%. The recovery rates for the 4% and 5.7% GMS DNA were measured to be 104.1% and 102.49% with RSD at 6.24% and 2.54%. The gold nanoparticle sensing electrode developed in this research is suitable for qualitative and quantitative detection of genetically modified soybeans and can be further applied to the detection of other genetically modified crops in the future.

Optical manipulation of optical vortex beam on gold nanoparticle

ABSTRACT The optomechanical manipulation of an optical vortex beam (Bessel beam) upon a single gold nanoparticle (GNP) was studied theoretically. This structured light carries spin angular momentum (SAM) and orbital angular momentum (OAM) simultaneously via the spin-orbit interaction (SOI) of light. Due to the plasmon-enhanced light absorption and scattering of GNP, the SAM and OAM of photons are transferred to GNP, exhibited by the spin and orbital motions of GNP. The optical force and torque upon GNP are analyzed through the surface integrals of Maxwell's stress tensor. We found that there are specific stable circular orbits of GNP through the simulation of GNP's equation of motion; the revolution direction depends on the sign of the order of Bessel beam. If the order of Bessel beam is a positive integer, the GNP performs an orbital motion with a counterclockwise revolution. On the contrary, for a Bessel beam of a negative order, a clockwise revolution of GNP is induced. Additionally, the spin direction of GNP depends on the handedness of light: right-hand or left-hand circular polarization.

Plasmon color-preserved gold nanoparticle clusters for high sensitivity detection of SARS-CoV-2 based on lateral flow immunoassay

Lateral flow immunoassays (LFI) have shown great promise for point-of-care (POC) sensing applications, however, its clinical translation is often hindered by insufficient sensitivity for early detection of diseases, including severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). This is mainly due to weak absorption signals of single gold nanoparticles (AuNPs). Here, we developed AuNP clusters that maintain the red color of isolated individual AuNPs, but increase the colorimetric readout to improve the detection sensitivity. The plasmon color-preserved (PLASCOP) AuNP clusters is simply made by mixing streptavidin-coated AuNP core with satellite AuNPs coated with biotinylated antibodies. The biotinylated antibody-streptavidin linker forms a gap size over 15 nm to avoid plasmon coupling between AuNPs, thus maintaining the plasmonic color while increasing the overall light absorption. LFI sensing using PLASCOP AuNP clusters composed of 40 nm AuNPs showed a high detection sensitivity for SARS-CoV-2 nucleocapsid proteins with a limit of detection (LOD) of 0.038 ng mL−1, which was 23.8- and 5.9-times lower value than that of single 15 nm and 40 nm AuNP conjugates, respectively. The PLASCOP AuNP clusters-based LFI sensing also shows good specificity for SARS-CoV-2 nucleocapsid proteins from other influenza and coronaviruses. In a clinical feasibility test, we demonstrated that SARS-CoV-2 particles spiked in human saliva could be detected with an LOD of 54 TCID50 mL−1. The developed PLASCOP AuNP clusters are promising colorimetric sensing reporters that present improved sensitivity in LFI sensing for broad POC sensing applications beyond SARS-CoV-2 detection.