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172 result(s) for "Chambers, Scott D."
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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 (r 2 ~0.90-0.96) and CO (r 2 ~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.
Inter-Comparison of Radon Measurements from a Commercial Beta-Attenuation Monitor and ANSTO Dual Flow Loop Monitor
Radon (Rn) is a radioactive, colourless, odourless, noble gas that decays rapidly. It’s most stable isotope, 222Rn, has a half-life of around 3.8 days. Atmospheric radon measurements play an important role in understanding our atmospheric environments. Naturally occurring radon can be used as an atmospheric tracer for airmass tracking, to assist in modelling boundary layer development, and is important for understanding background radiation levels and personal exposure to natural radiation. The daughter products from radon decay also play an important role when measuring fine particle pollution using beta-attenuation monitors (BAM). Beta radiation from the 222Rn decay chain interferes with BAM measurements of fine particles; thus, some BAMs incorporate radon measurements into their sampling systems. BAMs are ubiquitous in air quality monitoring networks globally and present a hitherto unexplored source of dense, continuous radon measurements. In this paper, we compare in situ real world 222Rn measurements from a high quality ANSTO dual flow loop, dual filter radon detector, and the radon measurements made by a commercial BAM instrument (Thermo 5014i). We find strong correlations between systems for hourly measurements (R2 = 0.91), daily means (R2 = 0.95), hour of day (R2 = 0.72–0.94), and by month (R2 = 0.83–0.94). The BAM underestimates radon by 22–39%; however, the linear response of the BAM measurements implies that they could be corrected to reflect the ANSTO standard measurements. Regardless, the radon measurements from BAMs could be used with correction to estimate local mixed layer development. Though only a 12-month study at a single location, our results suggest that radon measurements from BAMs can complement more robust measurements from standard monitors, augment radon measurements across broad regions of the world, and provide useful information for studies using radon as a tracer, particularly for boundary layer development and airmass identification.
Dry season aerosol iron solubility in tropical northern Australia
Marine nitrogen fixation is co-limited by the supply of iron (Fe) and phosphorus in large regions of the global ocean. The deposition of soluble aerosol Fe can initiate nitrogen fixation and trigger toxic algal blooms in nitrate-poor tropical waters. We present dry season soluble Fe data from the Savannah Fires in the Early Dry Season (SAFIRED) campaign in northern Australia that reflects coincident dust and biomass burning sources of soluble aerosol Fe. The mean soluble and total aerosol Fe concentrations were 40 and 500 ng m−3 respectively. Our results show that while biomass burning species may not be a direct source of soluble Fe, biomass burning may substantially enhance the solubility of mineral dust. We observed fractional Fe solubility up to 12 % in mixed aerosols. Thus, Fe in dust may be more soluble in the tropics compared to higher latitudes due to higher concentrations of biomass-burning-derived reactive organic species in the atmosphere. In addition, biomass-burning-derived particles can act as a surface for aerosol Fe to bind during atmospheric transport and subsequently be released to the ocean upon deposition. As the aerosol loading is dominated by biomass burning emissions over the tropical waters in the dry season, additions of biomass-burning-derived soluble Fe could have harmful consequences for initiating nitrogen-fixing toxic algal blooms. Future research is required to quantify biomass-burning-derived particle sources of soluble Fe over tropical waters.
Characterizing urban pollution variability in Central Poland using radon-222
Four years of observations of radon, meteorology and atmospheric pollution was used to demonstrate the efficacy of combined diurnal and synoptic timescale radon-based stability classification schemes in relating atmospheric mixing state to urban air quality in Zgierz, Central Poland. Nocturnal radon measurements were used to identify and remove periods of non-stationary synoptic behaviour (13–18% of each season) and classify the remaining data into five mixing states, including persistent temperature inversion (PTI) conditions, and non-PTI conditions with nocturnal conditions ranging from well mixed to stable. Mixing state classifications were performed completely independently of site meteorological measurements. World Health Organization guideline values for daily PM 2.5 /PM 10 were exceeded only under strong PTI conditions (3–15% of non-summer months) or often under non-PTI stable nocturnal conditions (14–20% of all months), when minimum nocturnal mean wind speeds were also recorded. In non-summer months, diurnal amplitudes of NO (CO) increased by the factors of 2–12 (3–7) from well-mixed nocturnal conditions to PTI conditions, with peak concentrations occurring in the morning/evening commuting periods. Analysis of observations within radon-derived atmospheric mixing ‘class types’ was carried out to substantially clarify relationships between meteorological and air quality parameters (e.g. wind speed vs. PM 2.5 concentration, and atmospheric mixing depth vs. PM 10 concentration).
Radon-based technique for the analysis of atmospheric stability – a case study from Central Poland
An economical and easy-to-implement technique is outlined by which the mean nocturnal atmospheric mixing state (“stability”) can be assessed over a broad (city-scale) heterogeneous region solely based on near-surface (2 m above ground level [a.g.l.]) observations of the passive tracer radon-222. The results presented here are mainly based on summer data of hourly meteorological and radon observations near Łodź, Central Poland, from 4 years (2008–2011). Behaviour of the near-surface wind speed and vertical temperature gradient (the primary controls of the nocturnal atmospheric mixing state), as well as the urban heat island intensity, are investigated within each of the four radon-based nocturnal stability categories derived for this study (least stable, weakly stable, moderately stable, and stable). On average, the most (least) stable nights were characterized by vertical temperature gradient of 1.1 (0.5)°C·m , wind speed of ~0.4 (~1.0) m·s , and urban heat island intensity of 4.5 (0.5)°C. For sites more than 20 km inland from the coast, where soils are not completely saturated or frozen, radon-based nocturnal stability classification can significantly enhance and simplify a range of environmental research applications (e.g. urban climate studies, urban pollution studies, regulatory dispersion modelling, and evaluating the performance of regional climate and pollution models).
Seasonal Variation of Biogenic and Anthropogenic VOCs in a Semi-Urban Area Near Sydney, Australia
Volatile organic compounds (VOCs) play a key role in the formation of ozone and secondary organic aerosol, the two most important air pollutants in Sydney, Australia. Despite their importance, there are few available VOC measurements in the area. In this paper, we discuss continuous GC-MS measurements of 10 selected VOCs between February (summer in the southern hemisphere) and June (winter in the southern hemisphere) of 2019 in a semi-urban area between natural eucalypt forest and the Sydney metropolitan fringe. Combined, isoprene, methacrolein, methyl-vinyl-ketone, α-pinene, p-cymene, eucalyptol, benzene, toluene xylene and tri-methylbenzene provide a reasonable representation of variability in the total biogenic VOC (BVOC) and anthropogenic VOC (AVOC) loading in the area. Seasonal changes in environmental conditions were reflected in observed BVOC concentrations, with a summer peak of 8 ppb, dropping to approximately 0.1 ppb in winter. Isoprene, and its immediate oxidation products methacrolein (MACR) and methyl-vinyl-ketone (MVK), dominated BVOC concentrations during summer and early autumn, while monoterpenes comprised the larger fraction during winter. Temperature and solar radiation drive most of the seasonal variation observed in BVOCs. Observed levels of isoprene, MACR and MVK in the atmosphere are closely related with variations in temperature and photosynthetically active radiation (PAR), but chemistry and meteorology may play a more important role for the monoterpenes. Using a nonlinear model, temperature explains 51% and PAR 38% of the isoprene, MACR and MVK variation. Eucalyptol dominated the observed monoterpene fraction (contributing ~75%), with p-cymene (20%) and α-pinene (5%) also present. AVOCs maintain an average concentration of ~0.4 ppb, with a slight decrease during autumn–winter. The low AVOC concentrations observed indicate a relatively small anthropogenic influence, generally occurring when (rare) northerly winds transport Sydney emissions to the measurement site. The site is influenced by domestic, commercial and vehicle AVOC emissions. Our observed AVOC concentrations can be explained by the seasonal changes in meteorology and the emissions in the area as listed in the NSW emissions inventory and thereby act as an independent validation of this inventory. We conclude that the variations in atmospheric composition observed during the seasons are an important variable to consider when formulating air pollution control policies over Sydney given the influence of biogenic sources during summer, autumn and winter.
Skill-Testing Chemical Transport Models across Contrasting Atmospheric Mixing States Using Radon-222
We propose a new technique to prepare statistically-robust benchmarking data for evaluating chemical transport model meteorology and air quality parameters within the urban boundary layer. The approach employs atmospheric class-typing, using nocturnal radon measurements to assign atmospheric mixing classes, and can be applied temporally (across the diurnal cycle), or spatially (to create angular distributions of pollutants as a top-down constraint on emissions inventories). In this study only a short (<1-month) campaign is used, but grouping of the relative mixing classes based on nocturnal mean radon concentrations can be adjusted according to dataset length (i.e., number of days per category), or desired range of within-class variability. Calculating hourly distributions of observed and simulated values across diurnal composites of each class-type helps to: (i) bridge the gap between scales of simulation and observation, (ii) represent the variability associated with spatial and temporal heterogeneity of sources and meteorology without being confused by it, and (iii) provide an objective way to group results over whole diurnal cycles that separates ‘natural complicating factors’ (synoptic non-stationarity, rainfall, mesoscale motions, extreme stability, etc.) from problems related to parameterizations, or between-model differences. We demonstrate the utility of this technique using output from a suite of seven contemporary regional forecast and chemical transport models. Meteorological model skill varied across the diurnal cycle for all models, with an additional dependence on the atmospheric mixing class that varied between models. From an air quality perspective, model skill regarding the duration and magnitude of morning and evening “rush hour” pollution events varied strongly as a function of mixing class. Model skill was typically the lowest when public exposure would have been the highest, which has important implications for assessing potential health risks in new and rapidly evolving urban regions, and also for prioritizing the areas of model improvement for future applications.
Long-term Variability of Aerosol Optical Properties at Mauna Loa
We investigated the variability of the aerosol scattering (σ sp ; 1974–2015) and absorption (σ ap ; 2000–2015) coefficients at the Mauna Loa Observatory using surface in situ measurements. Although σ sp decreased during the morning (1.85 ± 3.43 Mm 1 at 550 nm, 8–11 local standard time [LST]), it increased during the afternoon (3.72 ± 7.63 Mm 1 at 550 nm, 14–17 LST) due to the development of thermally induced boundary layer winds. No distinct diurnal variation was observed in σ ap . The obvious increase in σ sp and σ ap during the spring under free troposphere conditions (8–11 LST) is attributed to long-range-transported aerosols from Asia, especially dust and pollution aerosols from Northeast Asia and biomass burning aerosols from Southeast Asia. Accordingly, σ sp increased from 1974 till 2015 (at 1.89% year −1 ), whereas no significant trend was noted for either σ sp or σ ap from 2000 till 2015. An increasing trend for σ sp prevailed in air masses originating in Northeast Asia (+0.51 Mm −1 decade −1 ).
Identifying persistent temperature inversion events in a subalpine basin using radon-222
One year of meteorological and atmospheric radon observations in a topographically complex subalpine basin are used to identify persistent temperature inversion (PTI) events. PTI events play a key role in public health due to the accumulation of urban pollutants that they cause. Two techniques are compared: a new radon-based method (RBM), based on single-height 222Rn measurements from a single centrally located station, and an existing pseudo-vertical temperature gradient method (TGM) based on observations from eight weather stations around the subalpine basin. The RBM identified six PTI events (four in winter, two in autumn), a subset of the 17 events identified by the TGM. The RBM was more consistent in its identification of PTI events for all seasons and more selective of persistent strongly stable conditions. The comparatively poor performance of the TGM was attributed to seasonal inconsistencies in the validity of the method's key assumptions (influenced by mesoscale processes, such as local drainage flows, nocturnal jets, and intermittent turbulence influence) and a lack of snow cover in the basin for the 2016–2017 winter period. Corresponding meteorological quantities for RBM PTI events (constituting 27 % of the autumn–winter cold season) were well characterized. PTI wind speeds in the basin were consistently low over the whole diurnal cycle (typically 0.2–0.6 m s−1). Suitability of the two techniques for air quality assessment was compared using hourly PM10 observations. Peak PM10 concentrations for winter (autumn) PTI events were underestimated by 13 µg m−3 (11 µg m−3) by the TGM compared with the RBM. Only the RBM indicated that nocturnal hourly mean PM10 values in winter PTI events can exceed 100 µg m−3, the upper threshold of low-level short-term PM10 exposure according to World Health Organization guidelines. The efficacy, simplicity, and cost effectiveness of the RBM for identifying PTI events has the potential to make it a powerful tool for urban air quality management in complex terrain regions, for which it adds an additional dimension to contemporary atmospheric stability classification tools. Furthermore, the long-term consistency of the radon source function will enable the RBM to be used in the same way in future studies, enabling the relative magnitude of PTI events to be gauged, which is expected to assist with the assessment of public health risks.
Marine productivity and synoptic meteorology drive summer-time variability in Southern Ocean aerosols
Cloud–radiation interactions over the Southern Ocean are not well constrained in climate models, in part due to uncertainties in the sources, concentrations, and cloud-forming potential of aerosol in this region. To date, most studies in this region have reported measurements from fixed terrestrial stations or a limited set of instrumentation and often present findings as broad seasonal or latitudinal trends. Here, we present an extensive set of aerosol and meteorological observations obtained during an austral summer cruise across the full width of the Southern Ocean south of Australia. Three episodes of continental-influenced air masses were identified, including an apparent transition between the Ferrel atmospheric cell and the polar cell at approximately 64∘ S, and accompanied by the highest median cloud condensation nuclei (CCN) concentrations, at 252 cm−3. During the other two episodes, synoptic-scale weather patterns diverted air masses across distances greater than 1000 km from the Australian and Antarctic coastlines, respectively, indicating that a large proportion of the Southern Ocean may be periodically influenced by continental air masses. In all three cases, a highly cloud-active accumulation mode dominated the size distribution, with up to 93 % of the total number concentration activating as CCN. Frequent cyclonic weather conditions were observed at high latitudes and the associated strong wind speeds led to predictions of high concentrations of sea spray aerosol. However, these modelled concentrations were not achieved due to increased aerosol scavenging rates from precipitation and convective transport into the free troposphere, which decoupled the air mass from the sea spray flux at the ocean surface. CCN concentrations were more strongly impacted by high concentrations of large-diameter Aitken mode aerosol in air masses which passed over regions of elevated marine biological productivity, potentially contributing up to 56 % of the cloud condensation nuclei concentration. Weather systems were vital for aerosol growth in biologically influenced air masses and in their absence ultrafine aerosol diameters were less than 30 nm. These results demonstrate that air mass meteorological history must be considered when modelling sea spray concentrations and highlight the potential importance of sub-grid-scale variability when modelling atmospheric conditions in the remote Southern Ocean.