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The morphology and metal oxidation states of atmospheric aerosols are pertinent to their formation processes and ensuing interactions with surrounding gases, vapors and other environments upon deposition, such as human respiratory tract, soil and water. Although much progress has been made in recent years through single-particle techniques, considerably less is known with respect to the three-dimensional (3D) internal morphology of single atmospheric aerosol particles due to the limited penetration depth of electron microscopy. In this study, for the first time, a novel synchrotron-based transmission X-ray microscopy (TXM) methodology has been developed to visualize the 3D internal chemical mixing state and structure of single particles. The results show that the TXM is more applicable to the imaging of solid particles containing high-density elements, e.g., iron (Fe), aluminum (Al), silicone (Si), carbon (C) and sulfur (S), and/or solid particles of sizes larger than about 100 nm. In addition, the TXM is capable to reveal the fine 3D topographic features of single particles. The derived 3D internal and external information would be difficult to discern in the 2D images from electron microscopy. The TXM 3D images illustrate that aerosol particles exhibit complex internal mixing state and structure, e.g., homogeneously-, heterogeneously-mixed, multiple inclusions, fibrous, porous, and core-shell configuration. When coupled with the synchrotron-based X-ray fluorescence spectrometry (XRF) and absorption near-edge spectroscopy (XANES) of an X-ray nanoprobe in the energy range of 4-15 keV, the 3D morphology of single particles is further supplemented with the spatial distribution and oxidation sates of selected elements, including Fe, vanadium (V), manganese (Mn), chromium (Cr) and arsenic (As). The presented cross-platform, synchrotron-based methodology shows promise in complementing existing single-particle techniques and providing new insights to the heterogeneity of single-particle micro-physicochemical states relevant to the aerosol chemistry, optical properties, and their environmental and health impacts.

Time-resolved X-ray excited optical luminescence (TR-XEOL) was developed successfully for the 23A X-ray nanoprobe beamline located at the Taiwan Photon Source (TPS). The advantages of the TR-XEOL facility include (i) a nano-focused X-ray beam (

The multifunctional hard X-ray nanoprobe at Taiwan Photon Source (TPS) exhibits the excellent ability to simultaneously characterize the X-ray absorption, X-ray excited optical luminescence (XEOL) as well as the dynamics of XEOL of materials. Combining the scanning electron microscope (SEM) into the TPS 23A end-station, we can easily and quickly measure the optical properties to map out the morphology of a ZnO microrod. A special phenomenon has been observed that the oscillations in the XEOL associated with the confinement of the optical photons in the single ZnO microrod shows dramatical increase while the X-ray excitation energy is set across the Zn K-edge. Besides having the nano-scale spatial resolution, the synchrotron source also gives a good temporal domain measurement to investigate the luminescence dynamic process. The decay lifetimes of different emission wavelengths and can be simultaneously obtained from the streak image. Besides, SEM can provide the cathodoluminescence (CL) to be a complementary method to analyze the emission properties of materials, we anticipate that the X-ray nanoprobe will open new avenues with great characterization ability for developing nano/microsized optoelectronic devices.

Polarization-dependent hard X-ray excited optical luminescence (XEOL) was used to study not only the optical properties but also the crystallographic orientations of a non-polar a-plane ZnO wafer. In addition to a positive-edge jump and extra oscillations in the near-band-edge (NBE) XEOL yield, we observed a blue shift of the NBE emission peak that follows the polarization-dependent X-ray absorption near-edge structure (XANES) as the X-ray energy is tuned across the Zn K-edge. This NBE blue shift is caused by the larger X-ray absorption, generating higher free carriers to reduce the exciton-LO phonon coupling, which causes a decrease in the exciton activation energy. The extra oscillations in XANES and XEOL as the polarization is set parallel to the c-axis is attributed to simultaneous excitations of the Zn 4p - O 2pπ -bond along the c-axis and the bilayer σ-bond, whereas only the σ-bond is excited when the polarization is perpendicular to the c-axis. The polarization-dependent XEOL spectra can be used to determine the crystallographic orientations.

Convenient, rapid, and accurate detection of chemical and biomolecules would be a great benefit to medical, pharmaceutical, and environmental sciences. Many chemical and biosensors based on metal nanoparticles (NPs) have been developed. However, as a result of the inconvenience and complexity of most of the current preparation techniques, surface plasmon-based test papers are not as common as, for example, litmus paper, which finds daily use. In this paper, we propose a convenient and practical technique, based on the photothermal effect, to fabricate the plasmonic test paper. This technique is superior to other reported methods for its rapid fabrication time (a few seconds), large-area throughput, selectivity in the positioning of the NPs, and the capability of preparing NP arrays in high density on various paper substrates. In addition to their low cost, portability, flexibility, and biodegradability, plasmonic test paper can be burned after detecting contagious biomolecules, making them safe and eco-friendly.

This study synthesized a europium (Eu(3+)) complex Eu(DBM)(3)Cl-MIP (DBM = dibenzoyl methane; Cl-MIP = 2-(2-chlorophenyl)-1-methyl-1H-imidazo[4,5-f][1,10]phenanthroline) dispersed in a benzyl methacrylate (BMA) monomer and treated with ultraviolet (UV) light for polymerization. Spectral results showed that the europium complex containing an antenna, Cl-MIP, which had higher triplet energy into the Eu(3+) energy level, was an energetically enhanced europium emission. Typical stacking behaviors of π-π interactions between the ligands and the Eu(3+)-ion were analyzed using single crystal X-ray diffraction. Regarding the luminescence performance of this europium composite, the ligand/defect emission was suppressed by dispersion in a poly-BMA (PBMA) matrix. The underlying mechanism of the effective enhancement of the pure Eu(3+) emission was attributed to the combined effects of structural modifications, defect emissions, and carrier charge transfer. Fluorescence spectra were compared to the composite of optimized Eu3+ emission where they were subsequently chelated to four metal ions via carboxylate groups on the BMA unit. The optical enhanced europium composite clearly demonstrated highly efficient optical responses and is, therefore a promising application as an optical detection material.

[*] Dr. K. H. Chen, M. H. Wu, W. C. Chen Institute of Atomic and Molecular Sciences, Academia Sinica No. 1, Sec. 4, Roosevelt Rd., Taipei 106 (Taiwan) E-mail: chenkh@pub.iams.sinica.edu.tw Dr. L. C. Chen, Dr. C. H. Chen, Dr. K. H. Chen Center for Condensed Matter Sciences, National Taiwan University No. 1, Sec. 4, Roosevelt Rd., Taipei 106 (Taiwan) E-mail: chenlc@ntu.edu.tw C. H. Lin, Prof. J. H. Lee Graduate Institute of Photonics and Optoelectronics and Department of Electrical Engineering, National Taiwan University No. 1, Sec. 4, Roosevelt Rd., Taipei 106 (Taiwan)

The hard X-ray nanoprobe facility at Taiwan Photon Source (TPS) provides versatile X-ray analysis techniques, with tens of nanometer resolution, including XRF, XAS, XEOL, projection microscope, CDI, etc. Resulting from the large numerical aperture obtained by utilizing Montel KB mirrors, the beamline with a moderate length 75 meters can conduct similar performance with those beamlines longer than 100 meters. The two silica-made Montel mirrors are 45 degree cut and placed in a V-shape to eliminate the gap loss and the deformation caused by gravity. The slope error of the KB mirror pair is less than 0.04 µrad accomplished by elastic emission machining (EEM) method. For the beamline, a horizontal DCM and two-stage focusing in horizontal direction is applied. For the endstation, a combination of SEM for quickly positioning the sample, a fly scanning system with laser interferometers, a precise temperature control system, and a load lock transfer system will be implemented. In this presentation, the design and...

The hard X-ray nanoprobe facility at Taiwan Photon Source (TPS) provides multimodal X-ray detections, including XRF, XAS, XEOL, projection microscope, CDI, etc. Resulting from the large numerical aperture obtained by utilizing nested Montel mirrors, the beamline with a moderate length 75 meters can conduct similar performance with those beamlines longer than 100 meters. The mirrors are symmetrically placed with a 45 degrees cut. The beamline optics is thus designed to take the advantage of the symmetry of mirrors such that a round focal spot is accomplished. The size and the divergence of the focus spot are simulated around 40 nm and 6.29 mrad, respectively. The whole facility including the beamline and the stations will be operated under vacuum to preserve the photon coherence as well as to prevent the system from unnecessary environmental interference. A SEM in close cooperation with laser interferometers is equipped to precisely locate the position of the sample. This endstation is scheduled to be commissioned in the fall of 2016.

In this study, we used the autocloning effect on pyramid structures to develop broad-bandwidth, omnidirectional antireflection structures for silicon solar cells. The angular dependence of reflectance on several pyramid structures was systematically investigated. The deposition of three-layer autocloned films reduced the refractive index gap between air and silicon, resulting in an increase in the amount of transmitted light and a decrease in the total light escaping. The average reflectance decreased dramatically to ca. 2–3% at incident angles from 0 to 60° for both sub-wavelength– and micrometer–scale pyramid structures. The measured reflectance of the autocloned structure was less than 4% in the wavelength range from 400 to 1000 nm for incident angles from 0 to 60°. Therefore, the autocloning technique, combined with optical thin films and optical gradient structures, is a practical and compatible method for the fabrication of broad-bandwidth, omnidirectional antireflection structures on silicon solar cells.

In this paper, we report a new optical data storage method: photomodification of hollow gold nanoparticle (HGN) monolayers induced by one-shot deep-ultraviolet (DUV) KrF laser recording. As far as we are aware, this study is the first to apply HGNs in optical data storage and also the first to use a recording light source for the metal nanoparticles (NPs) that is not a surface plasmon resonance (SPR) wavelength. The short wavelength of the recording DUV laser improved the optical resolution dramatically. We prepared HGNs exhibiting two absorbance regions: an SPR peak in the near-infrared (NIR) region and an intrinsic material extinction in the DUV region. A single pulse from a KrF laser heated the HGNs and transformed them from hollow structures to smaller solid spheres. This change in morphology for the HGNs was accompanied by a significant blue shift of the SPR peak. Employing this approach, we demonstrated its patterning ability with a resolving power of a half-micrometer (using a phase mask) and developed a readout method (using a blue-ray laser microscope). Moreover, we prepared large-area, uniform patterns of monolayer HGNs on various substrates (glass slides, silicon wafers, flexible plates). If this spectral recording technique could be applied onto thin flexible tapes, the recorded data density would increase significantly relative to that of current rigid discs (e.g., compact discs).

A new and general approach to achieving efficient electrically driven light emission from a Si-based nano p-n junction array is introduced. A wafer-scale array of p-type silicon nanotips were formed by a single-step self-masked dry etching process, which is compatible with current semiconductor technologies. On top of the silicon nanotip array, a layer of n-type ZnO film was grown by pulsed laser deposition. Both the narrow line width of 10 nm in cathodoluminescence spectra and the appearance of multiphonon Raman spectra up to the fourth order indicate the excellent quality of the ZnO film. The turn-on voltage of our ZnO/Si nanotip array is found to be approximately 2.4 V, which is 2 times smaller than its thin film counterpart. Moreover, electroluminescence (EL) from our ZnO/Si nanotips array light-emitting diode (LED) has been demonstrated. Our results could open up new possibilities to integrate silicon-based optoelectronic devices, such as highly efficient LEDs, with standard Si ultralarge-scale integrated technology.

The use of metal catalyst to prepare nanostructures on semiconductor materials has attracted much attention because of the improved device performance. In this study, we employed the intruded Au nanocluster (INC) technique to prepare highly uniform, “atomic-scale” Au nanoclusters as highly active catalysts within Si wafers. The Au nanoclusters were readily prepared through the thermal coating of a Au film on a Si wafer followed by its removal using adhesive tape. Employing the Au nanoclusters as highly active catalysts allowed us to readily and rapidly prepare, at room temperature, unique Si nanostalactite (SNS) structures of ultrahigh density and very narrow diameter (ca. 10 nm). These SNS structures possessed superior light trapping capability relative to corresponding structures prepared using electroless metal deposition or self-assembled catalytic nanoparticle methods; in addition, the etching duration was much shorter. A field emission study revealed that the SNS structures, with their much narrower diameters, required a much lower turn-on voltage relative to that of corresponding Si nanowires.

In this paper we demonstrate an optical storage medium having advantages of ultrahigh contrast, superior stability, and broadband working wavelengths. Combining a single shot of deep-ultraviolet (UV) laser illumination with a Au particle-assisted etching process, we formed broadband antireflective, one-dimensional silicon nanowire arrays (SiNWs) with selectively at specific positions. Optical measurements and three-dimensional finite-difference time domain (3D-FDTD) simulations revealed ultrahigh reflection contrast between the Au and the SiNWs for both far- and near-field regimes. Relative to typical organic-based storage media, Au films and SiNWs are more stable, both chemically and thermally; therefore, we suspect that this new storage medium would exhibit high stability toward moisture, sunshine, and elevated temperatures.

We demonstrate a low series resistance contact of gold (anode)/zinc-phthalocyznine in a reverse organic photovoltaic device aided by oxygen plasma treatment. The power conversion efficiency appreciated from 0.2% to 2.13%, post O2 plasma treatment, predominantly due to the reduction in the series resistance of the device. A depth profile of zinc from x-ray photoelectron spectroscopy study revealed a gold layer with graded zinc composition, instead of pure gold, to be an efficient hole-collector from the organic interface. The zinc alloying of the gold layer has clearly been promoted by the oxygen plasma treatment.