Jagoda Crawford

Separating remote fetch and local mixing influences on vertical radon measurements in the lower atmosphere

Two-point radon gradients provide a direct, unambiguous measure of near-surface atmospheric mixing. A 31-month data set of hourly radon measurements at 2 and 50 m is used to characterize the seasonality and diurnal variability of radon concentrations and gradients at a site near Sydney. Vertical differencing allows separation of remote (fetchrelated) effects on measured radon concentrations from those due to diurnal variations in the strength and extent of vertical mixing. Diurnal composites, grouped according to the maximum nocturnal radon gradient (Cmax), reveal strong connections between radon, wind, temperature and mixing depth on subdiurnal timescales. Comparison of the bulk Richardson Number (RiB) and the turbulence kinetic energy (TKE) with the radon-derived bulk diffusivity (KB) helps to elucidate the relationship between thermal stability, turbulence intensity and the resultant mixing. On nights with large Cmax, KB and TKE levels are low and RiB is well above the ‘critical’ value. Conversely, when Cmax is small, KB and TKE levels are high and RiB is near zero. For intermediate Cmax, however, RiB remains small whereas TKE and KB both indicate significantly reduced mixing. The relationship between stability and turbulence is therefore non-linear, with even mildly stable conditions being sufficient to suppress mixing.

Fine particle characterisation, source apportionment and long-range dust transport into the Sydney Basin: a long term study between 1998 and 2009

Ion beam analysis techniques have been used to characterise fine particle (PM2.5) pollution in the Sydney Basin between 1 July 1998 and 31 December 2009. Nearly 1 200 filters were obtained and analysed for more than 21 different chemical species from hydrogen to lead. Positive matrix factorisation was then applied to this significant database to determine 7 different source fingerprints and their contributions to the total PM2.5 mass. Most of these sources originated in the Sydney Basin, however there were significant windblown soil sources that originated not just from desert regions in central Australia but also from large agricultural regions around 500 km south west of the Basin. This long range transport of fine dust was tracked using hourly back trajectories for every sampling day during the study period and showed that 33% of extreme dust events were probably originating from agricultural regions and not the central desert regions of Australia as first thought.

Constraining annual and seasonal radon-222 flux density from the Southern Ocean using radon-222 concentrations in the boundary layer at Cape Grim

ABSTRACT Radon concentrations measured between 2001 and 2008 in marine air at Cape Grim, a baseline site in north-western Tasmania, are used to constrain the radon flux density from the Southern Ocean. A method is described for selecting hourly radon concentrations that are least perturbed by land emissions and dilution by the free troposphere. The distribution of subsequent radon flux density estimates is representative of a large area of the Southern Ocean, an important fetch region for Southern Hemisphere climate and air pollution studies. The annual mean flux density (0.27 mBq m−2 s−1) compares well with the mean of the limited number of spot measurements previously conducted in the Southern Ocean (0.24 mBq m−2 s−1), and to some spot measurements made in other oceanic regions. However, a number of spot measurements in other oceanic regions, as well as most oceanic radon flux density values assumed for modelling studies and intercomparisons, are considerably lower than the mean reported here. The reported radon flux varies with seasons and, in summer, with latitude. It also shows a quadratic dependence on wind speed and significant wave height, as postulated and measured by others, which seems to support our assumption that the selected least perturbed radon concentrations were in equilibrium with the oceanic radon source. By comparing the least perturbed radon observations in 2002–2003 with corresponding ‘TransCom’ model intercomparison results, the best agreement is found when assuming a normally distributed radon flux density with σ=0.075 mBq m−2 s−1.

Estimating the Asian radon flux density and its latitudinal gradient in winter using ground-based radon observations at Sado Island

Terrestrial radon-222 flux density for the Asian continent, integrated over distances of 4500 km, is estimated in two 20. latitudinal bands centred on 48.8.N and 63.2.N. The evaluation is based on three years of wintertime radon measurements at Sado Island, Japan, together with meteorological and trajectory information. A selection of 18% of observations are suitable for evaluation of an analytical expression for the continental surface flux. Various meteorological assumptions are discussed; it is found that there is a substantial effect of increased complexity of the formulation on the flux estimates obtained. The distribution of spatially integrated radon flux over the Asian landmass is reported for the first time. Expressed as geometric means and 1±-ranges, estimated fluxes are 14.1 mBq m.2 s.1 (1±-range: 18 mBq m-2 s-1) and 8.4 mBq m-2 s-1 (1±-range: 10 mBq m-2 s-1) for the lower and higher latitude bands. These results constitute an annual minimum in flux densities for these regions, and are higher than previously reported. The existence of a latitudinal gradient in the continental radon source function is confirmed; the present estimate for Asia (-0.39 mBq m-2 s-1 per degree of latitude) is in agreement with the northern hemisphere terrestrial radon flux gradient proposed previously.

Precipitation stable isotope variability and sub‐cloud evaporation processes in a semi‐arid region.

Cop Abstract: The stable isotopic (H/H and O/O) composition of precipitation has been used for a variety of hydrological and paleoclimate studies, a starting point for which is the behaviour of stable isotopes in modern precipitation. To this end, daily precipitation samples were collected over a 7-year period (2008–2014) at a semi-arid site located at the Macquarie Marshes, New South Wales (Australia). The samples were analysed for stable isotope composition, and factors affecting the isotopic variability were investigated. The best correlation between δO of precipitation was with local surface relative humidity. The reduced major axis precipitation weighted local meteoric water line was δH= 7.20 δO + 9.1. The lower slope and intercept (when compared with the Global Meteoric Water Line) are typical for a warm dry climate, where subcloud evaporation of raindrops is experienced. A previously published model to estimate the degree of subcloud evaporation and the subsequent isotopic modification of raindrops was enhanced to include the vertical temperature and humidity profile. The modelled results for raindrops of 1.0mm radius showed that on average, the measured D-excess (=δH 8 δO) was 19.8‰ lower than that at the base of the cloud, and 18% of the moisture was evaporated before ground level (smaller effects were modelled for larger raindrops). After estimating the isotopic signature at the base of the cloud, a number of data points still plotted below the global meteoric water line, suggesting that some of the moisture was sourced from previously evaporated water. Back trajectory analysis estimated that 38% of the moisture was sourced over land. Precipitation samples for which a larger proportion of the moisture was sourced over land were O and H-enriched in comparison to samples for which the majority of the moisture was sourced over the ocean. The most common weather systems resulting in precipitation were inland trough systems; however, only East Coast Lows contributed to a significant difference in the isotopic values. Copyright

Radon as a tracer of atmospheric influences on traffic-related air pollution in a small inland city

One year of radon, benzene and carbon monoxide (CO) concentrations were analysed to characterise the combined influences of variations in traffic density and meteorological conditions on urban air quality in Bern, Switzerland. A recently developed radon-based stability categorisation technique was adapted to account for seasonal changes in day length and reduction in the local radon flux due to snow/ice cover and high soil moisture. Diurnal pollutant cycles were shown to result from an interplay between variations in surface emissions (traffic density), the depth of the nocturnal atmospheric mixing layer (dilution) and local horizontal advection of cleaner air from outside the central urban/industrial area of this small compact inland city. Substantial seasonal differences in the timing and duration of peak pollutant concentrations in the diurnal cycle were attributable to changes in day length and the switching to/from daylight-savings time in relation to traffic patterns. In summer, average peak benzene concentrations (0.62 ppb) occurred in the morning and remained above 0.5 ppb for 2 hours, whereas in winter average peak concentrations (0.85 ppb) occurred in the evening and remained above 0.5 ppb for 9 hours. Under stable conditions in winter, average peak benzene concentrations (1.1 ppb) were 120% higher than for well-mixed conditions (0.5 ppb). By comparison, summertime peak benzene concentrations increased by 53% from well-mixed (0.45 ppb) to stable nocturnal conditions (0.7 ppb). An idealised box model incorporating a simple advection term was used to derive a nocturnal mixing length scale based on radon, and then inverted to simulate diurnal benzene and CO emission variations at the city centre. This method effectively removes the influences of local horizontal advection and stability-related vertical dilution from the emissions signal, enabling a direct comparison with hourly traffic density. With the advection term calibrated appropriately, excellent results were obtained, with high regression coefficients in spring and summer for both benzene (r2 ~0.90–0.96) and CO (r2 ~0.88–0.98) in the two highest stability categories. Weaker regressions in winter likely indicate additional contributions from combustion sources unrelated to vehicular emissions. Average vehicular emissions during daylight hours were estimated to be around 0.503 (542) kg km−2 h−1 for benzene (CO) in the Bern city centre.

Estimating the near-surface daily fine aerosol load using hourly Radon-222 observations

We investigate the extent to which hourly radon observations can be used to estimate daily PM2.5 loading near the ground. We formulate, test and apply a model that expresses the mean daily PM2.5 load as a linear combination of observed radon concentrations and differences on a given day. The model was developed using two consecutive years of observations (2007–2008) at four sites near Sydney, Australia, instrumented with aerosol samplers and radon detectors. Model performance was subsequently evaluated against observations in 2009. After successfully reproducing mean daily radon concentrations (r2≥0.98), we used the model to estimate daily PM2.5 mass, as well as that of selected elements (Si, K, Fe, Zn, H, S and Black Carbon). When parameterizing the model for elemental mass estimates the highest r2 values were generally obtained for H, BC, K and Si. Separating results by season, the r2 values for K and BC were higher in winter for all sites, a period of time where higher concentrations of these elements are seen and a rapid estimation tool would be of particular benefit. The best overall results were obtained in winter for H and BC [r2 = 0.50, 0.68, 0.70, 0.63 (H) and 0.57, 0.57, 0.78, 0.44 (BC)], respectively for Warrawong, Lucas Heights, Richmond and Muswellbrook. Evaluation of model PM2.5 estimates was most successful for days with typical aerosol loads; loads were usually underestimated for, the less frequent, high–to–extreme pollution days. The best elemental results were obtained for BC at Richmond in winter (r2 = 0.68). However, for Warrawong and Lucas Heights r2 values increased from 0.26 to 0.60, and from 0.33 to 0.73, respectively, when several particularly high concentration events were excluded from the analysis. The model performed best at Richmond, an inland site with relatively flat terrain. However, model parameters need to be evaluated for each site.

Biotic, temporal and spatial variability of tritium concentrations in transpirate samples collected in the vicinity of a near-surface low-level nuclear waste disposal site and nearby research reactor.

The results of a 21 month sampling program measuring tritium in tree transpirate with respect to local sources are reported. The aim was to assess the potential of tree transpirate to indicate the presence of sub-surface seepage plumes. Transpirate gathered from trees near low-level nuclear waste disposal trenches contained activity concentrations of (3)H that were significantly higher (up to ∼700 Bq L(-1)) than local background levels (0-10 Bq L(-1)). The effects of the waste source declined rapidly with distance to be at background levels within 10s of metres. A research reactor 1.6 km south of the site contributed significant (p < 0.01) local fallout (3)H but its influence did not reach as far as the disposal trenches. The elevated (3)H levels in transpirate were, however, substantially lower than groundwater concentrations measured across the site (ranging from 0 to 91% with a median of 2%). Temporal patterns of tree transpirate (3)H, together with local meteorological observations, indicate that soil water within the active root zones comprised a mixture of seepage and rainfall infiltration. The degree of mixing was variable given that the soil water activity concentrations were heterogeneous at a scale equivalent to the effective rooting volume of the trees. In addition, water taken up by roots was not well mixed within the trees. Based on correlation modelling, net rainfall less evaporation (a surrogate for infiltration) over a period of from 2 to 3 weeks prior to sampling seems to be the optimum predictor of transpirate (3)H variability for any sampled tree at this site. The results demonstrate successful use of (3)H in transpirate from trees to indicate the presence and general extent of sub-surface contamination at a low-level nuclear waste site.

Chemical characterisation and source identification of atmospheric aerosols in the Snowy Mountains, south-eastern Australia

Characterisation of atmospheric aerosols is of major importance for: climate, the hydrological cycle, human health and policymaking, biogeochemical and palaeo-climatological studies. In this study, the chemical composition and source apportionment of PM2.5 (particulate matter with aerodynamic diameters less than 2.5μm) at Yarrangobilly, in the Snowy Mountains, SE Australia are examined and quantified. A new aerosol monitoring network was deployed in June 2013 and aerosol samples collected during the period July 2013 to July 2017 were analysed for 22 trace elements and black carbon by ion beam analysis techniques. Positive matrix factorisation and back trajectory analysis and trajectory clustering methods were employed for source apportionment and to isolate source areas and air mass travel pathways, respectively. This study identified the mean atmospheric PM2.5 mass concentration for the study period was (3.3±2.5)μgm-3. It is shown that automobile (44.9±0.8)%, secondary sulfate (21.4±0.9)%, smoke (12.3±0.6)%, soil (11.3±0.5)% and aged sea salt (10.1±0.4)% were the five PM2.5 source types, each with its own distinctive trends. The automobile and smoke sources were ascribed to a significant local influence from the road network and bushfire and hazard reduction burns, respectively. Long-range transport are the dominant sources for secondary sulfate from coal-fired power stations, windblown soil from the inland saline regions of the Lake Eyre and Murray-Darling Basins, and aged sea salt from the Southern Ocean to the remote alpine study site. The impact of recent climate change was recognised, as elevated smoke and windblown soil events correlated with drought and El Niño periods. Finally, the overall implications including potential aerosol derived proxies for interpreting palaeo-archives are discussed. To our knowledge, this is the first long-term detailed temporal and spatial characterisation of PM2.5 aerosols for the region and provides a crucial dataset for a range of multidisciplinary research.

Statistical analysis of Seoul air quality to assess the efficacy of emission abatement strategies since 1987

The combined influences of recent mitigation measures on urban air quality have been assessed using hourly observations of the criteria air pollutants (NO, NO2, O3, CO, and SO2) made from the Yongsan district of Seoul, Korea, over 26years (1987 to 2013). A number of data selection criteria are proposed in order to minimize variability associated with temporal changes (at diurnal, weekly, and seasonal timescales) in source strengths, their spatial distribution, and the atmospheric volume into which they mix. The temporal constraints required to better characterize relationships between observed air quality and changes in source strengths in Seoul were identified as: (i) a 5-hour diurnal sampling window (1300-1700h), (b) weekday measurements (Monday to Friday only), and (c) summer measurements (when pollutant fetch is mostly Korea-specific, and mean wind speeds are the lowest). Using these selection criteria, we were able to closely relate long-term trends identified in criteria pollutants to a number of published changes to traffic-related source strengths brought about by mitigation measures adopted over the last 10-15years.