Experimental optimization of physicochemical factors for spontaneous deposition of 210Po using newly designed deposition kit.

A simple spontaneous deposition kit for 210Po determination using alpha spectrometry was newly designed, and polonium deposition characteristics under various physicochemical conditions were evaluated using it. The high-purity silver disc (99.99%) showed high deposition efficiencies of over 85.1% in the HCl concentration range of 0.01-6 M. Optimal physicochemical factors were determined to be a temperature of 90 °C, deposition time of 90 min, and the use of ascorbic acid as a reducing agent in an amount similar to that of the interfering element (Fe).

Rapid sequential determination of 222Rn and 226Ra in drinking water by liquid scintillation counting.

Since daily drinking water is one of the major source for the ingestion of radiotoxic 222Rn and 226Ra, the demand for a simple method to determine these two radionuclides has significantly increased. In the present study, a rapid, simple sequential analysis method for determining 222Rn and 226Ra in drinking water using a liquid scintillation counter was developed. The method employs solvent extraction and correction equations for the effect of native 222Rn for 226Ra analysis. Validation and examination of applicability for drinking water analysis were conducted using 222Rn-injected water and 226Ra standard source. Minimum required counting times for examining drinking water on Quantulus 1220 and Hidex 300SL were estimated via minimum detectable activity depending on the counting time. In addition, the correction method, including an equation for reducing analysis time by more than 10 days, was suggested based on the analytical results for different elapsed times between sampling and measurement.

Preparation and evaluation of new reference materials for naturally occurring radioactive materials (NORM): Zirconium silicate, bauxite, and phosphogypsum.

New reference materials (RMs), zirconium silicate, bauxite and phosphogypsum, were produced and characterized according to an ISO guide. The homogeneity of the three RMs was evaluated using X-ray fluorescence (XRF), and characterizations of the three candidate materials were performed through a collaborative study with nine expert radioanalytical laboratories. The assigned radionuclides are 230Th, 232Th, 234U, 235U, and 238U for zirconium silicate; 230Th, 232Th, 234U, and 238U for bauxite; and 226Ra, 230Th, 234U, and 238U for phosphogypsum.

Atomic-scale intermolecular interaction of hydrogen with a single VOPc molecule on the Au(111) surface.

Molecular dynamics of hydrogen molecules (H2) on surfaces and their interactions with other molecules have been studied with the goal of improvement of hydrogen storage devices for energy applications. Recently, the dynamic behavior of a H2 at low temperature has been utilized in scanning tunnelling microscopy (STM) for sub-atomic resolution imaging within a single molecule. In this work, we have investigated the intermolecular interaction between H2 and individual vanadyl phthalocyanine (VOPc) molecules on Au(111) substrates by using STM and non-contact atomic force microscopy (NC-AFM). We measured tunnelling spectra and random telegraphic noise (RTN) on VOPc molecules to reveal the origin of the dynamic behavior of the H2. The tunnelling spectra show switching between two states with different tunnelling conductance as a function of sample bias voltage and RTN is measured near transition voltage between the two states. The spatial variation of the RTN indicates that the two-state fluctuation is dependent on the atomic-scale interaction of H2 with the VOPc molecule. Density functional theory calculations show that a H2 molecule can be trapped by a combination of a tip-induced electrostatic potential well and the potential formed by a VOPc underneath. We suggest the origin of the two-state noise as transition of H2 between minima in these potentials with barrier height of 20-30 meV. In addition, the bias dependent AFM images verify that H2 can be trapped and released at the tip-sample junction.

Large seasonal variations in fine aerosol precipitation rates revealed using cosmogenic 7Be as a tracer.

To determine the seasonal variations in the removal efficiency of fine aerosols (PM2.5) in the Northeast Asia, we analyzed 7Be data collected for the surface air and precipitation over 20 years in Korea. The 7Be activity concentrations in the surface air were relatively higher in spring owing to tropopause folding but lower in summer owing to efficient removal by precipitation. The monthly 7Be concentrations decreased as the precipitation amounts increased showing a negative correlation (r2 = 0.34) against the precipitation amount. These results indicate that the concentrations of 7Be and fine aerosols are mainly controlled by the same washout effect, although the sources are different. The mean depositional velocities of fine aerosols, based on the 7Be mass balance model, showed a large seasonal variation, with its maximum value (1.9 cm s-1) in July and minimum value (0.22 cm s-1) in March. The 7Be depositional velocity reflects the net deposition of fine aerosols excluding moisture effects. Thus, the concentrations of fine aerosols can occur as high as five-fold in the dry season, if the input terms of fine aerosols remain the same. Our results imply that precipitation plays a critical role in the seasonal changes in the concentrations of fine aerosols, providing much clean air in the summer monsoon season in the Northeast Asia.

Dispersion and removal characteristics of tritium originated from nuclear power plants in the atmosphere.

The activities of tritium in water-vapor (n = 649) and precipitation (n = 2404) samples were measured from 1998 to 2015 around the Wolsong nuclear power plant (NPP) site where four pressurized heavy water reactors and two pressurized water reactors operated. The activity concentrations of tritium in the water-vapor and precipitation samples were in the ranges of 2.2-2200 Bq/L and 0.3-1090 Bq/L, respectively. The concentrations of tritium in the water-vapor in spring were approximately 7 times higher than those in fall and winter, mainly owing to the wind directions at the power plant location. The annual geometric mean activities of tritium in the water-vapor and precipitation samples varied within 56% and 83% from the average, respectively, depending primarily on the annual discharge amount of tritium to the atmosphere. The activities of tritium in the water-vapor and precipitation samples rapidly decreased away from the power plant. Approximately 0.5-30% of tritium discharged from the NPP site was removed by precipitation to the ground within an area with a radius of 30 km from the NPP site, which linearly depended on the precipitation amount. Our results suggest that the wind direction and precipitation, in addition to the amount of discharge, are important factors that control the tritium concentrations in air near the NPP site.

Characteristics of artificial radionuclides in sedimentary soil cores from a volcanic crater lake.

The distributions of 137Cs, 237Np, and 239+240Pu activity concentrations in sedimentary soil cores of the volcanic crater-lake have been studied. The 240Pu/239Pu atom ratios measured by MC-ICP-MS and mutual activity ratios were examined. These results were used to evaluate the sedimentation characteristics of the crater-lake (Baengnokdam of Mt. Halla, Korea). The 137Cs, 237Np, and 239+240Pu activity concentrations showed similar distribution patterns and one maximum peak was observed in each sediment core, except at St.10. For all sediment cores, the activity concentrations were in the range 1.03 × 100-1.92 × 102 Bq·kg-1 dw for 137Cs, 7.56 × 10-3 - 7.15 × 100 mBq·kg-1 dw for 237Np, and 5.20 × 10-3 - 5.13 × 100 Bq·kg-1 dw for 239+240Pu, respectively. The averaged 240Pu/239Pu atomic ratio (0.159) was slightly less than the global fallout ratio (0.176). The averaged inventories were estimated to be 9.21 × 103±5.34 × 103 Bq·m-2 for 137Cs, 2.27 × 102±1.58 × 102 Bq·m-2 for 239+240Pu, and 3.22 × 10-1±1.78 × 10-1 Bq·m-2 for 237Np. The averaged 239+240Pu/137Cs and 237Np/239+240Pu activity ratios were 2.21 × 10-2 and 2.21 × 10-3, respectively. The mean sedimentation rates calculated using 239+240Pu activity concentrations at the central area (St.30 - St.45) and at all stations (St.5 - St.75) were estimated to be 0.844 cm yr-1, and 0.767 cm yr-1, respectively. In addition, the sedimentation rates calculated using 210Pb and 226Ra were 0.856 cm yr-1 at depths of 0-35 cm and 0.204 cm yr-1 at depths of 35-55 cm. These results imply that the sedimentation in Baengnokdam was relatively slow (0.204 cm yr-1) until about 44 years ago and then became faster (0.856 cm yr-1) to the present. The excess 210Pb dating is consistent with the sedimentation rate calculated from the vertical 239+240Pu profile.

Nanophotonic Atomic Force Microscope Transducers Enable Chemical Composition and Thermal Conductivity Measurements at the Nanoscale.

The atomic force microscope (AFM) offers a rich observation window on the nanoscale, yet many dynamic phenomena are too fast and too weak for direct AFM detection. Integrated cavity-optomechanics is revolutionizing micromechanical sensing; however, it has not yet impacted AFM. Here, we make a groundbreaking advance by fabricating picogram-scale probes integrated with photonic resonators to realize functional AFM detection that achieve high temporal resolution (<10 ns) and picometer vertical displacement uncertainty simultaneously. The ability to capture fast events with high precision is leveraged to measure the thermal conductivity (η), for the first time, concurrently with chemical composition at the nanoscale in photothermal induced resonance experiments. The intrinsic η of metal-organic-framework individual microcrystals, not measurable by macroscale techniques, is obtained with a small measurement uncertainty (8%). The improved sensitivity (50×) increases the measurement throughput 2500-fold and enables chemical composition measurement of molecular monolayer-thin samples. Our paradigm-shifting photonic readout for small probes breaks the common trade-off between AFM measurement precision and ability to capture transient events, thus transforming the ability to observe nanoscale dynamics in materials.

CH3NH3PbI3 perovskites: Ferroelasticity revealed.

Ferroelectricity has been proposed as a plausible mechanism to explain the high photovoltaic conversion efficiency in organic-inorganic perovskites; however, convincing experimental evidence in support of this hypothesis is still missing. Identifying and distinguishing ferroelectricity from other properties, such as piezoelectricity, ferroelasticity, etc., is typically nontrivial because these phenomena can coexist in many materials. In this work, a combination of microscopic and nanoscale techniques provides solid evidence for the existence of ferroelastic domains in both CH3NH3PbI3 polycrystalline films and single crystals in the pristine state and under applied stress. Experiments show that the configuration of CH3NH3PbI3 ferroelastic domains in single crystals and polycrystalline films can be controlled with applied stress, suggesting that strain engineering may be used to tune the properties of this material. No evidence of concomitant ferroelectricity was observed. Because grain boundaries have an impact on the long-term stability of organic-inorganic perovskite devices, and because the ferroelastic domain boundaries may differ from regular grain boundaries, the discovery of ferroelasticity provides a new variable to consider in the quest for improving their stability and enabling their widespread adoption.

Nanoscale imaging and spectroscopy of band gap and defects in polycrystalline photovoltaic devices.

Improving the power conversion efficiency of photovoltaic (PV) devices is challenging because the generation, separation and collection of electron-hole pairs are strongly dependent on details of the nanoscale chemical composition and defects which are often poorly known. In this work, two novel scanning probe nano-spectroscopy techniques, direct-transmission near-field scanning optical microscopy (dt-NSOM) and photothermal induced resonance (PTIR), are implemented to probe the distribution of defects and the bandgap variation in thin lamellae extracted from polycrystalline CdTe PV devices. dt-NSOM provides high-contrast spatially-resolved maps of light transmitted through the sample at selected wavelengths. PTIR provides absorption maps and spectra over a broad spectral range, from visible to mid-infrared. Results show variation of the bandgap through the CdTe thickness and from grain to grain that is spatially uncorrelated with the distributions of shallow and deep defects.

Engineering Near-Field SEIRA Enhancements in Plasmonic Resonators.

Engineering of the optical resonances in plasmonic resonators arrays is achieved by virtue of the intrinsic properties to the constituent structures such as composition, size and shape and by controlling the inter-resonator interactions by of virtue the array geometrical arrangement. The nanoscale confinement of the plasmonic field enhances light-matter interactions enabling, for instance, the surface enhanced infrared absorption (SEIRA) effect. However, the subwavelength confinement also poses an experimental challenge for discriminating the response stemming from the individual resonators and from the collective response in densely packed arrays. In this work, the photothermal induced resonance (PTIR) technique is leveraged to obtain nanoscale images and spectra of near-field SEIRA hot spots observed in isolated plasmonic resonators of different shapes and in selected resonators within closely packed plasmonic arrays informing on whether the interactions with neighboring resonators are beneficial or otherwise. Results are correlated with far-field spectra and theoretical calculations.

Chloride Incorporation Process in CH3NH3PbI(3-x)Cl(x) Perovskites via Nanoscale Bandgap Maps.

CH3NH3PbI(3-x)Cl(x) perovskites enable fabrication of highly efficient solar cells. Chloride ions benefit the morphology, carrier diffusion length, and stability of perovskite films; however, whether those benefits stem from the presence of Cl(-) in the precursor solution or from their incorporation in annealed films is debated. In this work, the photothermal-induced resonance, an in situ technique with nanoscale resolution, is leveraged to measure the bandgap of CH3NH3PbI(3-x)Cl(x) films obtained by a multicycle coating process that produces high efficiency (∼16%) solar cells. Because chloride ions modify the perovskite lattice, thereby widening the bandgap, measuring the bandgap locally yields the local chloride content. After a mild annealing (60 min, 60 °C) the films consist of Cl-rich (x < 0.3) and Cl-poor phases that upon further annealing (110 °C) evolve into a homogeneous Cl-poorer (x < 0.06) phase, suggesting that methylammonium-chrloride is progressively expelled from the film. Despite the small chloride content, CH3NH3PbI(3-x)Cl(x) films show better thermal stability up to 140 °C with respect CH3NH3PbI3 films fabricated with the same methodology.

Metal-dielectric-metal resonators with deep subwavelength dielectric layers increase the near-field SEIRA enhancement.

Plasmonic nanostructures presenting either structural asymmetry or metal-dielectric-metal (M-D-M) architecture are commonly used structures to increase the quality factor and the near-field confinement in plasmonic materials. This characteristic can be leveraged for example to increase the sensitivity of IR spectroscopy, via the surface enhanced IR absorption (SEIRA) effect. In this work, we combine structural asymmetry with the M-D-M architecture to realize Ag-Ag(2)O-Ag asymmetric ring resonators where two Ag layers sandwich a native silver oxide (Ag(2)O) layer. Their IR response is compared with the one of fully metallic (Ag) resonators of the same size and shape. The photothermal induced resonance technique (PTIR) is used to obtain near-field SEIRA absorption maps and spectra with nanoscale resolution. Although the native Ag(2)O layer is only 1 nm to 2 nm thick, it increases the quality factor of the resonators' dark-mode by ≈27% and the SEIRA enhancement by ≈44% with respect to entirely Ag structures.

Renormalization of the graphene dispersion velocity determined from scanning tunneling spectroscopy.

In graphene, as in most metals, electron-electron interactions renormalize the properties of electrons but leave them behaving like noninteracting quasiparticles. Many measurements probe the renormalized properties of electrons right at the Fermi energy. Uniquely for graphene, the accessibility of the electrons at the surface offers the opportunity to use scanned probe techniques to examine the effect of interactions at energies away from the Fermi energy, over a broad range of densities, and on a local scale. Using scanning tunneling spectroscopy, we show that electron interactions leave the graphene energy dispersion linear as a function of excitation energy for energies within ±200 meV of the Fermi energy. However, the measured dispersion velocity depends on density and increases strongly as the density approaches zero near the charge neutrality point, revealing a squeezing of the Dirac cone due to interactions.

Enhanced carrier transport along edges of graphene devices.

The relation between macroscopic charge transport properties and microscopic carrier distribution is one of the central issues in the physics and future applications of graphene devices (GDs). We find strong conductance enhancement at the edges of GDs using scanning gate microscopy. This result is explained by our theoretical model of the opening of an additional conduction channel localized at the edges by depleting accumulated charge by the tip.

Distribution of tritium in water vapour and precipitation around Wolsung nuclear power plant.

The distribution of tritium in water vapour and precipitation with discharge of tritiated water vapour and meteorological factors was studied around the Wolsung nuclear power plant (NPP) site during the period 2004-2008. The tritium concentrations in atmospheric water vapour and precipitation had a temporal variation with relatively high values in the early summer. Spatial distribution of tritium concentrations was affected by various factors such as distance from the NPP site, wind direction, tritium discharge into the atmosphere and atmospheric dispersion factor. The annual mean concentrations of atmospheric HTO and precipitation were correlated with the amount of gaseous tritium released from the Wolsung NPP. The tritium concentrations in precipitation decrease exponentially with an increase of the distance from the Wolsung NPP site.

7Be in ground level air in Daejeon, Korea.

(7)Be concentrations in the ground level air in Daejeon, Korea were determined during the period of January 1998 to December 2009 by gamma-ray spectrometric analysis of particulate samples collected on filter paper with a high-volume air sampler. The monthly concentrations of (7)Be in the ground level air were in the range of 1.3-7.7 mBq m(-3) with strong seasonal trends of low values in the summer and high values in the spring and autumn. The annual mean values of (7)Be concentrations showed weak reverse correlation with the annual average sunspot number.