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Long-term assessment of airborne radiocesium after the Fukushima nuclear accident: re-suspension from bare soil and forest ecosystems

The long-term effect of 137Cs re-suspension from contaminated soil and forests due to the Fukushima nuclear accident has been quantitatively assessed by numerical simulation, a field experiment on dust emission flux in a contaminated area (town of Namie, Fukushima prefecture), and air concentration measurements inside (Namie) and outside (city of Tsukuba, Ibaraki prefecture) the contaminated area. In order to assess the long-term effect, the full year of 2013 was selected to study just after the start of the field experiments. The 137Cs concentrations at Namie and Tsukuba were approximately 10−1–1 and 10−2–10−1 mBq m−3, respectively. The observed monthly median concentration at Namie was 1 to 2 orders of magnitude larger than that at Tsukuba. This observed difference between the two sites was consistent with the simulated difference, indicating successful modeling of 137Cs re-suspension and atmospheric transport. The estimated re-suspension rate was approximately 10−6 day−1, which was significantly lower than the decreasing rate of the ambient gamma dose rate in Fukushima prefecture (10−4–10−3 day−1) as a result of radioactive decay, migration in the soil and biota, and decontamination. Consequently, re-suspension contributed negligibly in reducing ground radioactivity. The dust emission model could reproduce the air concentration of 137Cs in winter, whereas the summer air concentration was underestimated by 1 to 2 orders of magnitude. Re-suspension from forests at a constant rate of 10−7 h−1, multiplied by the green area fraction, could explain the air concentration of 137Cs at Namie and its seasonal variation. The simulated contribution of dust re-suspension to the air concentration was 0.7–0.9 in the cold season and 0.2–0.4 in the warm season at both sites; the remainder of the contribution was re-suspension from forest. The re-suspension mechanisms, especially through the forest ecosystems, remain unknown. This is the first study that provides a crude estimation of the long-term assessment of radiocesium re-suspension. Additional research activities should investigate the processes/mechanisms governing the re-suspension over the long term. This could be achieved through conducting additional field experiments and numerical simulations.
Simple proxies for estimating the concentrations of monoterpenes and their oxidation products at a boreal forest site

The oxidation products of monoterpenes likely have a crucial role in the formation and growth of aerosol particles in boreal forests. However, the continuous measurements of monoterpene concentrations are usually not available on decadal timescales, and the direct measurements of the concentrations of monoterpene oxidation product have so far been scarce. In this study we developed proxies for the concentrations of monoterpenes and their oxidation products at a boreal forest site in Hyytiälä, southern Finland. For deriving the proxies we used the monoterpene concentration measured with a proton transfer reaction mass spectrometer (PTR-MS) during 2006–2013. Our proxies for the monoterpene concentration take into account the temperature-controlled emissions from the forest ecosystem, the dilution caused by the mixing within the boundary layer and different oxidation processes. All the versions of our proxies captured the seasonal variation of the monoterpene concentration, the typical proxy-to-measurements ratios being between 0.8 and 1.3 in summer and between 0.6 and 2.6 in winter. In addition, the proxies were able to describe the diurnal variation of the monoterpene concentration rather well, especially in summer months. By utilizing one of the proxies, we calculated the concentration of oxidation products of monoterpenes by considering their production in the oxidation and their loss due to condensation on aerosol particles. The concentration of oxidation products was found to have a clear seasonal cycle, with a maximum in summer and a minimum in winter. The concentration of oxidation products was lowest in the morning or around noon and highest in the evening. In the future, our proxies for the monoterpene concentration and their oxidation products can be used, for example, in the analysis of new particle formation and growth in boreal environments.
Analysis of the latitudinal variability of tropospheric ozone in the Arctic using the large number of aircraft and ozonesonde observations in early summer 2008

During the 2008 International Polar Year, the POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements, and Models of Climate Chemistry, Aerosols, and Transport) campaign, conducted in summer over Greenland and Canada, produced a large number of measurements from three aircraft and seven ozonesonde stations. Here we present an observation-integrated analysis based on three different types of O3 measurements: airborne lidar, airborne UV absorption or chemiluminescence measurement, and intensified electrochemical concentration cell (ECC) ozonesonde profiles. Discussion of the latitudinal and vertical variability of tropospheric ozone north of 55° N during this period is performed with the aid of a regional model (WFR-Chem). The model is able to reproduce the O3 latitudinal and vertical variability but with a negative O3 bias of 6–15 ppbv in the free troposphere above 4 km, especially over Canada. For Canada, large average CO concentrations in the free troposphere above 4 km ( >  130 ppbv) and the weak correlation (<  30 %) of O3 and PV suggest that stratosphere–troposphere exchange (STE) is not the major contributor to average tropospheric ozone at latitudes less than 70° N, due to the fact that local biomass burning (BB) emissions were significant during the 2008 summer period. Conversely, significant STE is found over Greenland according to the better O3 vs. PV correlation ( >  40 %) and the higher values of the 75th PV percentile. It is related to the persistence of cyclonic activity during the summer over Baffin Bay. Using differences between average concentration above Northern and Southern Canada, a weak negative latitudinal summer ozone gradient of −6 to −8 ppbv is found in the mid-troposphere between 4 and 8 km. This is attributed to an efficient O3 photochemical production from BB emissions at latitudes less than 65° N, while the STE contribution is more homogeneous in the latitude range 55–70° N. A positive ozone latitudinal gradient of 12 ppbv is observed in the same altitude range over Greenland not because of an increasing latitudinal influence of STE, but because of different long-range transport from multiple mid-latitude sources (North America, Europe, and even Asia for latitudes higher than 77° N). For the Arctic latitudes (>  80° N), free tropospheric O3 concentrations during summer 2008 are related to a mixture of Asian pollution and stratospheric O3 transport across the tropopause.
Properties of aerosols and formation mechanisms over southern China during the monsoon season

Measurements of size-resolved aerosols from 0.25 to 18 µm were conducted at three sites (urban, suburban and background sites) and used in tandem with an atmospheric transport model to study the size distribution and formation of atmospheric aerosols in southern China during the monsoon season (May–June) in 2010. The mass distribution showed the majority of chemical components were found in the smaller size bins (< 2.5 µm). Sulfate was found to be strongly correlated with aerosol water and anticorrelated with atmospheric SO2, hinting at aqueous-phase reactions being the main formation pathway. Nitrate was the only major species that showed a bimodal distribution at the urban site and was dominated by the coarse mode in the other two sites, suggesting that an important component of nitrate formation is chloride depletion of sea salt transported from the South China Sea. In addition to these aqueous-phase reactions and interactions with sea salt aerosols, new particle formation, chemical aging, and long-range transport from upwind urban or biomass burning regions was also found to be important in at least some of the sites on some of the days. This work therefore summarizes the different mechanisms that significantly impact the aerosol chemical composition during the monsoon over southern China.
The climatology of planetary boundary layer height in China derived from radiosonde and reanalysis data

The important roles of the planetary boundary layer (PBL) in climate, weather and air quality have long been recognized, but little is known about the PBL climatology in China. Using the fine-resolution sounding observations made across China and reanalysis data, we conducted a comprehensive investigation of the PBL in China from January 2011 to July 2015. The boundary layer height (BLH) is found to be generally higher in spring and summer than that in fall and winter. The comparison of seasonally averaged BLHs derived from observations and reanalysis, on average, shows good agreement, despite the pronounced inconsistence in some regions. The BLH, derived from soundings conducted three or four times daily in summer, tends to peak in the early afternoon, and the diurnal amplitude of BLH is higher in the northern and western subregions of China than other subregions. The meteorological influence on the annual cycle of BLH is investigated as well, showing that BLH at most sounding sites is negatively associated with the surface pressure and lower tropospheric stability, but positively associated with the near-surface wind speed and temperature. In addition, cloud tends to suppress the development of PBL, particularly in the early afternoon. This indicates that meteorology plays a significant role in the PBL processes. Overall, the key findings obtained from this study lay a solid foundation for us to gain a deep insight into the fundamentals of PBL in China, which helps to understand the roles that the PBL plays in the air pollution, weather and climate of China.
Transformation of logwood combustion emissions in a smog chamber: formation of secondary organic aerosol and changes in the primary organic aerosol upon daytime and nighttime aging

Organic aerosols (OA) derived from small-scale wood combustion emissions are not well represented by current emissions inventories and models, although they contribute substantially to the atmospheric particulate matter (PM) levels. In this work, a 29 m3 smog chamber in the ILMARI facility of the University of Eastern Finland was utilized to investigate the formation of secondary organic aerosol (SOA) from a small-scale modern masonry heater commonly used in northern Europe. Emissions were oxidatively aged in the smog chamber for a variety of dark (i.e., O3 and NO3) and UV (i.e., OH) conditions, with OH concentration levels of (0.5–5)  ×  106 molecules cm−3, achieving equivalent atmospheric aging of up to 18 h. An aerosol mass spectrometer characterized the direct OA emissions and the SOA formed from the combustion of three wood species (birch, beech and spruce) using two ignition processes (fast ignition with a VOC-to-NOx ratio of 3 and slow ignition with a ratio of 5). Dark and UV aging increased the SOA mass fraction with average SOA productions 2.0 times the initial OA mass loadings. SOA enhancement was found to be higher for the slow ignition compared with fast ignition conditions. Positive matrix factorization (PMF) was used to separate SOA, primary organic aerosol (POA) and their subgroups from the total OA mass spectra. PMF analysis identified two POA and three SOA factors that correlated with the three major oxidizers: ozone, the nitrate radical and the OH radical. Organonitrates (ONs) were observed to be emitted directly from the wood combustion and additionally formed during oxidation via NO3 radicals (dark aging), suggesting small-scale wood combustion may be a significant ON source. POA was oxidized after the ozone addition, forming aged POA, and after 7 h of aging more than 75 % of the original POA was transformed. This process may involve evaporation and homogeneous gas-phase oxidation as well as heterogeneous oxidation of particulate organic matter. The results generally prove that logwood burning emissions are the subject of intensive chemical processing in the atmosphere, and the timescale for these transformations is relatively short, i.e., hours.
Overview of mercury dry deposition, litterfall, and throughfall studies

The current knowledge concerning mercury dry deposition is reviewed, including dry-deposition algorithms used in chemical transport models (CTMs) and at monitoring sites and related deposition calculations, measurement methods and studies for quantifying dry deposition of gaseous oxidized mercury (GOM) and particulate bound mercury (PBM), and measurement studies of litterfall and throughfall mercury. Measured median GOM plus PBM dry deposition in Asia (10.7 µg m−2 yr−1) is almost double that in North America (6.1 µg m−2 yr−1) due to the higher anthropogenic emissions in Asia. The measured mean GOM plus PBM dry deposition in Asia (22.7 µg m−2 yr−1), however, is less than that in North America (30.8 µg m−2 yr−1). The variations between the median and mean values reflect the influences that single extreme measurements can have on the mean of a data set. Measured median litterfall and throughfall mercury are, respectively, 34.8 and 49.0 µg m−2 yr−1 in Asia, 12.8 and 16.3 µg m−2 yr−1 in Europe, and 11.9 and 7.0 µg m−2 yr−1 in North America. The corresponding measured mean litterfall and throughfall mercury are, respectively, 42.8 and 43.5 µg m−2 yr−1 in Asia, 14.2 and 19.0 µg m−2 yr−1 in Europe, and 12.9 and 9.3 µg m−2 yr−1 in North America. The much higher litterfall mercury than GOM plus PBM dry deposition suggests the important contribution of gaseous elemental mercy (GEM) to mercury dry deposition to vegetated canopies. Over all the regions, including the Amazon, dry deposition, estimated as the sum of litterfall and throughfall minus open-field wet deposition, is more dominant than wet deposition for Hg deposition. Regardless of the measurement or modelling method used, a factor of 2 or larger uncertainties in GOM plus PBM dry deposition need to be kept in mind when using these numbers for mercury impact studies.
Airborne mercury species at the Råö background monitoring site in Sweden: distribution of mercury as an effect of long-range transport

Within the EU-funded project, Global Mercury Observation System (GMOS) airborne mercury has been monitored at the background Råö measurement site on the western coast of Sweden from mid-May 2012 to the beginning of July 2013 and from the beginning of February 2014 to the end of May 2015. The following mercury species/fractions were measured: gaseous elemental mercury (GEM), particulate bound mercury (PBM) and gaseous oxidised mercury (GOM) using the Tekran measurement system. The mercury concentrations measured at the Råö site were found to be low in comparison to other, comparable, European measurement sites. A back-trajectory analysis to study the origin of air masses reaching the Råö site was performed. Due to the remote location of the Råö measurement station it receives background air about 60 % of the time. However, elevated mercury concentrations arriving with air masses coming from the south-east are noticeable. GEM and PBM concentrations show a clear annual variation with the highest values occurring during winter, whereas the highest concentrations of GOM were obtained in spring and summer. An evaluation of the diurnal pattern of GOM, with peak concentrations at midday or in the early afternoon, which often is observed at remote places, shows that it is likely to be driven by local meteorology in a similar way to ozone. Evidence that a significant part of the GOM measured at the Råö site has been formed in free tropospheric air is presented.
The BErkeley Atmospheric CO2 Observation Network: initial evaluation

With the majority of the world population residing in urban areas, attempts to monitor and mitigate greenhouse gas emissions must necessarily center on cities. However, existing carbon dioxide observation networks are ill-equipped to resolve the specific intra-city emission phenomena targeted by regulation. Here we describe the design and implementation of the BErkeley Atmospheric CO2 Observation Network (BEACO2N), a distributed CO2 monitoring instrument that utilizes low-cost technology to achieve unprecedented spatial density throughout and around the city of Oakland, California. We characterize the network in terms of four performance parameters – cost, reliability, precision, and systematic uncertainty – and find the BEACO2N approach to be sufficiently cost-effective and reliable while nonetheless providing high-quality atmospheric observations. First results from the initial installation successfully capture hourly, daily, and seasonal CO2 signals relevant to urban environments on spatial scales that cannot be accurately represented by atmospheric transport models alone, demonstrating the utility of high-resolution surface networks in urban greenhouse gas monitoring efforts.
Non-stomatal exchange in ammonia dry deposition models: comparison of two state-of-the-art approaches

The accurate representation of bidirectional ammonia (NH3) biosphere–atmosphere exchange is an important part of modern air quality models. However, the cuticular (or external leaf surface) pathway, as well as other non-stomatal ecosystem surfaces, still pose a major challenge to translating our knowledge into models. Dynamic mechanistic models including complex leaf surface chemistry have been able to accurately reproduce measured bidirectional fluxes in the past, but their computational expense and challenging implementation into existing air quality models call for steady-state simplifications. Here we qualitatively compare two semi-empirical state-of-the-art parameterizations of a unidirectional non-stomatal resistance (Rw) model after Massad et al. (2010), and a quasi-bidirectional non-stomatal compensation-point (χw) model after Wichink Kruit et al. (2010), with NH3 flux measurements from five European sites. In addition, we tested the feasibility of using backward-looking moving averages of air NH3 concentrations as a proxy for prior NH3 uptake and as a driver of an alternative parameterization of non-stomatal emission potentials (Γw) for bidirectional non-stomatal exchange models. Results indicate that the Rw-only model has a tendency to underestimate fluxes, while the χw model mainly overestimates fluxes, although systematic underestimations can occur under certain conditions, depending on temperature and ambient NH3 concentrations at the site. The proposed Γw parameterization revealed a clear functional relationship between backward-looking moving averages of air NH3 concentrations and non-stomatal emission potentials, but further reduction of uncertainty is needed for it to be useful across different sites. As an interim solution for improving flux predictions, we recommend reducing the minimum allowed Rw and the temperature response parameter in the unidirectional model and revisiting the temperature-dependent Γw parameterization of the bidirectional model.