Coherent acoustic vibrations of Au nanoblocks and their modulation by Al2O3 layer deposition.

Coherent acoustic phonons induced in metallic nanostructures have attracted tremendous attention owing to their unique optomechanical characteristics. The frequency of the acoustic phonon vibration is highly sensitive to the material adsorption on metallic nanostructures and, therefore, the acoustic phonon offers a promising platform for ultrasensitive mass sensors. However, the physical origin of acoustic frequency modulation by material adsorption has been partially unexplored so far. In this study, we prepared Al2O3-deposited Au nanoblocks and measured their acoustic phonon frequencies using time-resolved pump-probe measurements. By precisely controlling the thickness of the Al2O3 layer, we systematically investigated the relation between the acoustic phonon frequency and the deposited Al2O3 amounts. The time-resolved measurements revealed that the acoustic breathing modes were predominantly excited in the Au nanoblocks, and their frequencies increased with the increment of the Al2O3 thickness. From the relationship between the acoustic phonon frequency and the Al2O3 thickness, we revealed that the acoustic phonon frequency modulation is attributed to the density change of the whole sample. Our results would provide fruitful information for developing quantitative mass sensing devices based on metallic nanostructures.

Rapid Discrimination of Extracellular Vesicles by Shape Distribution Analysis.

A rapid and simple cancer detection method independent of cancer type is an important technology for cancer diagnosis. Although the expression profiles of biological molecules contained in cancer cell-derived extracellular vesicles (EVs) are considered candidates for discrimination indexes to identify any cancerous cells in the body, it takes a certain amount of time to examine these expression profiles. Here, we report the shape distributions of EVs suspended in a solution and the potential of these distributions as a discrimination index to discriminate cancer cells. Distribution analysis is achieved by low-aspect-ratio nanopore devices that enable us to rapidly analyze EV shapes individually in solution, and the present results reveal a dependence of EV shape distribution on the type of cells (cultured liver, breast, and colorectal cancer cells and cultured normal breast cells) secreting EVs. The findings in this study provide realizability and experimental basis for a simple method to discriminate several types of cancerous cells based on rapid analyses of EV shape distributions.

Pore Structures for High-Throughput Nanopore Devices.

Nanopore devices are expected to advance the next-generation of nanobiodevices because of their strong sensing and analyzing capabilities for single molecules and bioparticles. However, the device throughputs are not sufficiently high. Although analytes pass through a nanopore by electrophoresis, the electric field gradient is localized inside and around a nanopore structure. Thus, analytes located far from a nanopore cannot be driven by electrophoresis. Here, we report nanopore structures for high-throughput sensing, namely, inverted pyramid (IP)-shaped nanopore structures. Silicon-based IP-shaped nanopore structures create a homogeneous electric field gradient within a nanopore device, indicating that most of the analytes can pass through a nanopore by electrophoresis, even though the analytes are suspended far from the nanopore entrance. In addition, the nanostructures can be fabricated only by photolithography. The present study suggests a high potential for inverted pyramid shapes to serve as nanopore devices for high-throughput sensing.

Large patternable metal nanoparticle sheets by photo/e-beam lithography.

Techniques for micro/nano-scale patterning of large metal nanoparticle sheets can potentially be used to realize high-performance photoelectronic devices because the sheets provide greatly enhanced electrical fields around the nanoparticles due to localized surface plasmon resonances. However, no single metal nanoparticle sheet currently exists with sufficient durability for conventional lithographical processes. Here, we report large photo and/or e-beam lithographic patternable metal nanoparticle sheets with improved durability by incorporating molecular cross-linked structures between nanoparticles. The cross-linked structures were easily formed by a one-step chemical reaction; immersing a single nanoparticle sheet consisting of core metals, to which capping molecules ionically bond, in a dithiol ethanol solution. The ligand exchange reaction processes were discussed in detail, and we demonstrated 20 µm wide line and space patterns, and a 170 nm wide line of the silver nanoparticle sheets.

High-resolution imaging of a cell-attached nanointerface using a gold-nanoparticle two-dimensional sheet.

This paper proposes a simple, effective, non-scanning method for the visualization of a cell-attached nanointerface. The method uses localized surface plasmon resonance (LSPR) excited homogeneously on a two-dimensional (2D) self-assembled gold-nanoparticle sheet. The LSPR of the gold-nanoparticle sheet provides high-contrast interfacial images due to the confined light within a region a few tens of nanometers from the particles and the enhancement of fluorescence. Test experiments on rat basophilic leukemia (RBL-2H3) cells with fluorescence-labeled actin filaments revealed high axial and lateral resolution even under a regular epifluorescence microscope, which produced higher quality images than those captured under a total internal reflection fluorescence (TIRF) microscope. This non-scanning-type, high-resolution imaging method will be an effective tool for monitoring interfacial phenomena that exhibit relatively rapid reaction kinetics in various cellular and molecular dynamics.

Rapid structural analysis of nanomaterials in aqueous solutions.

Rapid structural analysis of nanoscale matter in a liquid environment represents innovative technologies that reveal the identities and functions of biologically important molecules. However, there is currently no method with high spatio-temporal resolution that can scan individual particles in solutions to gain structural information. Here we report the development of a nanopore platform realizing quantitative structural analysis for suspended nanomaterials in solutions with a high z-axis and xy-plane spatial resolution of 35.8 ± 1.1 and 12 nm, respectively. We used a low thickness-to-diameter aspect ratio pore architecture for achieving cross sectional areas of analyte (i.e. tomograms). Combining this with multiphysics simulation methods to translate ionic current data into tomograms, we demonstrated rapid structural analysis of single polystyrene (Pst) beads and single dumbbell-like Pst beads in aqueous solutions.

Electromagnetically induced transparency of a plasmonic metamaterial light absorber based on multilayered metallic nanoparticle sheets.

In this study, we observed the peak splitting of absorption spectra for two-dimensional sheets of silver nanoparticles due to the electromagnetically induced transparency (EIT) effect. This unique optical phenomenon was observed for the multilayered nanosheets up to 20 layers on a metal substrate, while this phenomenon was not observed on a transparent substrate. The wavelength and intensities of the split peaks depend on the number of layers, and the experimental results were well reproduced by the calculation of the Transfer-Matrix method by employing the effective medium approximation. The Ag nanosheets used in this study can act as a plasmonic metamaterial light absorber, which has a such large oscillator strength. This phenomenon is a fundamental optical property of a thin film on a metal substrate but has never been observed because native materials do not have a large oscillator strength. This new type of EIT effect using a plasmonic metamaterial light absorber presents the potential for the development of future optic and photonic technologies.

Basic aspects for improving the energy conversion efficiency of hetero-junction organic photovoltaic cells.

Hetero-junction organic photovoltaic (OPV) cells consisting of donor (D) and acceptor (A) layers have been regarded as next-generation PV cells, because of their fascinating advantages, such as lightweight, low fabrication cost, resource free, and flexibility, when compared to those of conventional PV cells based on silicon and semiconductor compounds. However, the power conversion efficiency (η) of the OPV cells has been still around 8%, though more than 10% efficiency has been required for their practical use. To fully optimize these OPV cells, it is necessary that the low mobility of carriers/excitons in the OPV cells and the open circuit voltage (V OC), of which origin has not been understood well, should be improved. In this review, we address an improvement of the mobility of carriers/excitons by controlling the crystal structure of a donor layer and address how to increase the V OC for zinc octaethylporphyrin [Zn(OEP)]/C60 hetero-junction OPV cells [ITO/Zn(OEP)/C60/Al]. It was found that crystallization of Zn(OEP) films increases the number of inter-molecular charge transfer (IMCT) excitons and enlarges the mobility of carriers and IMCT excitons, thus significantly improving the external quantum efficiency (EQE) under illumination of the photoabsorption band due to the IMCT excitons. Conversely, charge accumulation of photo-generated carriers in the vicinity of the donor/acceptor (D/A) interface was found to play a key role in determining the V OC for the OPV cells.