In conjunction with the OP3 campaign in Danum Valley, Malaysian Borneo, flux measurements of methyl chloride (CH3Cl) and methyl bromide (CH3Br) were performed from both tropical plant branches and leaf litter in June and July 2008. Live plants were mainly from the Dipterocarpaceae family whilst leaf litter samples were representative mixtures of different plant species. Environmental parameters, including photosynthetically-active radiation, total solar radiation and air temperature, were also recorded. The dominant factor determining magnitude of methyl halide fluxes from living plants was plant species, with specimens of the genus Shorea showing persistent high emissions of both gases, e.g. Shorea pilosa: 65 ± 17 ng CH3Cl h-1 g-1 (dry weight foliage) and 2.7 ± 0.6 ng CH3Br h-1 g-1 (dry weight foliage). Mean CH3Cl and CH3Br emissions across 18 species of plant were 19 (range

Background: Air pollution–mortality risk estimates are generally larger at longer-term, compared with short-term, exposure time scales.Objective: We compared associations between short-term exposure to black smoke (BS) and mortality with long-term exposure–mortality associations in cohort participants and with short-term exposure–mortality associations in the general population from which the cohorts were selected.Methods: We assessed short-to-medium–term exposure–mortality associations in the Renfrew–Paisley and Collaborative cohorts (using nested case–control data sets), and compared them with long-term exposure–mortality associations (using a multilevel spatiotemporal exposure model and survival analyses) and short-to-medium–term exposure–mortality associations in the general population (using time-series analyses).Results: For the Renfrew–Paisley cohort (15,331 participants), BS exposure–mortality associations were observed in nested case–control analyses that accounted for spatial variations in pollution exposure and individual-level risk factors. These cohort-based associations were consistently greater than associations estimated in time-series analyses using a single monitoring site to represent general population exposure {e.g., 1.8% [95% confidence interval (CI): 0.1, 3.4%] vs. 0.2% (95% CI: 0.0, 0.4%) increases in mortality associated with 10-μg/m3 increases in 3-day lag BS, respectively}. Exposure–mortality associations were of larger magnitude for longer exposure periods [e.g., 3.4% (95% CI: –0.7, 7.7%) and 0.9% (95% CI: 0.3, 1.5%) increases in all-cause mortality associated with 10-μg/m3 increases in 31-day BS in case–control and time-series analyses, respectively; and 10% (95% CI: 4, 17%) increase in all-cause mortality associated with a 10-μg/m3 increase in geometic mean BS for 1970–1979, in survival analysis].Conclusions: After adjusting for individual-level exposure and potential confounders, short-term exposure–mortality associations in cohort participants were of greater magnitude than in comparable general population time-series study analyses. However, short-term exposure–mortality associations were substantially lower than equivalent long-term associations, which is consistent with the possibility of larger, more persistent cumulative effects from long-term exposures.

[1] Methyl bromide (CH 3 Br) is a trace gas involved in stratospheric ozone depletion with both anthropogenic and natural sources. Estimates of natural source strengths are highly uncertain. In this study, >320 highly temporally and spatially resolved measurements of CH 3 Br emissions from a salt marsh in Scotland (56°00 0 N, 2°35 0 W) were made during one year using eight static enclosures. Net emissions showed both strong seasonal and diurnal cycles. Day-today maxima in emissions were associated with sunny days. Emissions dropped to zero when vegetation was removed. Mean measured CH 3 Br emission was 350 ng m À2 h À1 , but a few ''hot spots'' (measured maximum 4000 ng m À2 h À1 ) dominated integrated emissions. A crude scale-up of the annual mean emission yields an estimate for global CH 3 Br emission of $1 (0.5-3) Gg y À1 (range uses annual mean from lowest and highest emitting enclosures), $10% the global salt marsh emission regularly quoted in the literature.

Abstract. Fluxes of CH 3 Br and CH 3 Cl and their relationship with potential drivers such as sunlight, temperature and soil moisture, were monitored at fortnightly to monthly intervals for more than two years at two contrasting temperate salt marsh sites in Scotland. Manipulation experiments were conducted to further investigate possible links between drivers and fluxes. Fluxes followed both seasonal and diurnal trends with highest fluxes during summer days and lowest (negative) fluxes during winter nights. Mean (± 1 sd) annually and diurnally-weighted net emissions from the two sites were found to be 300 ± 44 ng m −2 h −1 for CH 3 Br and 662 ± 266 ng m −2 h −1 for CH 3 Cl. The fluxes from this work are similar to findings from this and other research groups for salt marshes in cooler, higher latitude climates, but lower than values from salt marshes in the Mediterranean climate of southern California. Statistical analysis generally did not demonstrate a strong link between temperature or sunlight levels and methyl halide fluxes, although it is likely that temperatures have a weak direct influence on emissions, and both certainly have indirect influence via the annual and daily cycles of the vegetation. CH 3 Cl flux magnitudes from different measurement locations depended on the plant species enclosed whereas such dependency was not discernible for CH 3 Br fluxes. In 14 out of 18 collars with vegetation CH 3 Br and CH 3 Cl net fluxes were significantly positively correlated. The CH 3 Cl/CH 3 Br net-emission mass ratio was 2.2, a magnitude lower than mass ratios of global methyl halide budgets (∼22) or emissions from tropical rainforests (∼60). This is likely due to preference for CH 3 Br production by the relatively high bromine content in the salt marsh plant material. Extrapolation based solely on data from this study yields Correspondence to: M. R. Heal (m.heal@ed.ac.uk) salt marsh contributions of 0.5-3.2% and 0.05-0.33%, respectively, of currently-estimated total global production of CH 3 Br and CH 3 Cl, but actual global contributions likely lie between these values and those derived from southern California.

Abstract. The UK Acid Gases and Aerosol Monitoring Network (AGANet) was established in 1999 (12 sites, increased to 30 sites from 2006), to provide long-term national monitoring of acid gases (HNO3, SO2, HCl) and aerosol components (NO3−, SO42−, Cl−, Na+, Ca2+, Mg2+). An extension of a low-cost denuder-filter pack system (DELTA) that is used to measure NH3 and NH4+ in the UK National Ammonia Monitoring Network (NAMN) provides additional monthly speciated measurements for the AGANet. A comparison of the monthly DELTA measurement with averaged daily results from an annular denuder system showed close agreement, while the sum of HNO3 and NO3− and the sum of NH3 and NH4+ from the DELTA are also consistent with previous filter pack determination of total inorganic nitrogen and total inorganic ammonium, respectively. With the exception of SO2 and SO42−, the AGANet provides, for the first time, the UK concentration fields and seasonal cycles for each of the other measured species. The largest concentrations of HNO3, SO2, and aerosol NO3− and SO42− are found in southern and eastern England and smallest in western Scotland and Northern Ireland, whereas HCl are highest in south-eastern, south-western, and central England, that may be attributed to dual contribution from anthropogenic (coal combustion) and marine sources (reaction of sea salt with acid gases to form HCl). Na+ and Cl− are spatially correlated, with largest concentrations at coastal sites, reflecting a contribution from sea salt. Temporally, peak concentrations in HNO3 occurred in late winter and early spring attributed to photochemical processes. NO3− and SO42− have a spring maxima that coincides with the peak in concentrations of NH3 and NH4+, and are therefore likely attributable to formation of NH4NO3 and (NH4)2SO4 from reaction with higher concentrations of NH3 in spring. By contrast, peak concentrations of SO2, Na+, and Cl− during winter are consistent with combustion sources for SO2 and marine sources in winter for sea salt aerosol. Key pollutant events were captured by the AGANet. In 2003, a spring episode with elevated concentrations of HNO3 and NO3− was driven by meteorology and transboundary transport of NH4NO3 from Europe. A second, but smaller episode occurred in September 2014, with elevated concentrations of SO2, HNO3, SO42−, NO3−, and NH4+ that was shown to be from the Icelandic Holuhraun volcanic eruptions. Since 1999, AGANet has shown substantial decrease in SO2 concentrations relative to HNO3 and NH3, consistent with estimated decline in UK emissions. At the same time, large reductions and changes in the aerosol components provide evidence of a shift in the particulate phase from (NH4)2SO4 to NH4NO3. The potential for NH4NO3 to release NH3 and HNO3 in warm weather, together with the surfeit of NH3 also means that a larger fraction of the reduced and oxidized N is remaining in the gas phase as NH3 and HNO3 as indicated by the increasing trend in ratios of NH3 : NH4+ and HNO3 : NO3− over the 16-year period. Due to different removal rates of the component species by wet and dry deposition, this change is expected to affect spatial patterns of pollutant deposition with consequences for sensitive habitats with exceedance of critical loads of acidity and eutrophication. The changes are also relevant for human health effects assessment, particularly in urban areas as NH4NO3 constitutes a significant fraction of fine particulate matter ( < 2.5 µm) that are linked to increased mortality from respiratory and cardiopulmonary diseases.