The effects of springtime mid-latitude storms on trace gas composition determined from the MACC reanalysis

The relationship between springtime air pollution transport of ozone (O3) and carbon monoxide (CO) and mid-latitude cyclones is explored for the first time using the Monitoring Atmospheric Composition and Climate (MACC) reanalysis for the period 2003–2012. In this study, the most intense spring storms (95th percentile) are selected for two regions, the North Pacific (NP) and the North Atlantic (NA). These storms (∼60 storms over each region) often track over the major emission sources of East Asia and eastern North America. By compositing the storms, the distributions of O3 and CO within a "typical" intense storm are examined. We compare the storm-centered composite to background composites of "average conditions" created by sampling the reanalysis data of the previous year to the storm locations. Mid-latitude storms are found to redistribute concentrations of O3 and CO horizontally and vertically throughout the storm. This is clearly shown to occur through two main mechanisms: (1) vertical lifting of CO-rich and O3-poor air isentropically, from near the surface to the mid- to upper-troposphere in the region of the warm conveyor belt; and (2) descent of O3-rich and CO-poor air isentropically in the vicinity of the dry intrusion, from the stratosphere toward the mid-troposphere. This can be seen in the composite storm's life cycle as the storm intensifies, with area-averaged O3 (CO) increasing (decreasing) between 200 and 500 hPa. The influence of the storm dynamics compared to the background environment on the composition within an area around the storm center at the time of maximum intensity is as follows. Area-averaged O3 at 300 hPa is enhanced by 50 and 36% and by 11 and 7.6% at 500 hPa for the NP and NA regions, respectively. In contrast, area-averaged CO at 300 hPa decreases by 12% for NP and 5.5% for NA, and area-averaged CO at 500 hPa decreases by 2.4% for NP while there is little change over the NA region. From the mid-troposphere, O3-rich air is clearly seen to be transported toward the surface, but the downward transport of CO-poor air is not discernible due to the high levels of CO in the lower troposphere. Area-averaged O3 is slightly higher at 1000 hPa (3.5 and 1.8% for the NP and NA regions, respectively). There is an increase of CO at 1000 hPa for the NP region (3.3%) relative to the background composite and a~slight decrease in area-averaged CO for the NA region at 1000 hPa (-2.7%).

Modelled and observed changes in aerosols and surface solar radiation over Europe between 1960 and 2009

Substantial changes in anthropogenic aerosols and precursor gas emissions have occurred over recent decades due to the implementation of air pollution control legislation and economic growth. The response of atmospheric aerosols to these changes and the impact on climate are poorly constrained, particularly in studies using detailed aerosol chemistry–climate models. Here we compare the HadGEM3-UKCA (Hadley Centre Global Environment Model-United Kingdom Chemistry and Aerosols) coupled chemistry–climate model for the period 1960–2009 against extensive ground-based observations of sulfate aerosol mass (1978–2009), total suspended particle matter (SPM, 1978–1998), PM10 (1997–2009), aerosol optical depth (AOD, 2000–2009), aerosol size distributions (2008–2009) and surface solar radiation (SSR, 1960–2009) over Europe. The model underestimates observed sulfate aerosol mass (normalised mean bias factor (NMBF) = −0.4), SPM (NMBF = −0.9), PM10 (NMBF = −0.2), aerosol number concentrations (N30 NMBF = −0.85; N50 NMBF = −0.65; and N100 NMBF = −0.96) and AOD (NMBF = −0.01) but slightly overpredicts SSR (NMBF = 0.02). Trends in aerosol over the observational period are well simulated by the model, with observed (simulated) changes in sulfate of −68 % (−78 %), SPM of −42 % (−20 %), PM10 of −9 % (−8 %) and AOD of −11 % (−14 %). Discrepancies in the magnitude of simulated aerosol mass do not affect the ability of the model to reproduce the observed SSR trends. The positive change in observed European SSR (5 %) during 1990–2009 ("brightening") is better reproduced by the model when aerosol radiative effects (ARE) are included (3 %), compared to simulations where ARE are excluded (0.2 %). The simulated top-of-the-atmosphere aerosol radiative forcing over Europe under all-sky conditions increased by > 3.0 W m−2 during the period 1970–2009 in response to changes in anthropogenic emissions and aerosol concentrations.

Nitrogen management is essential to prevent tropical oil palm plantations from causing ozone pollution

More than half the world's rainforest has been lost to agriculture since the Industrial Revolution. Among the most widespread tropical crops is oil palm (Elaeis guineensis): global production now exceeds 35 million tonnes per year. In Malaysia, for example, 13% of land area is now oil palm plantation, compared with 1% in 1974. There are enormous pressures to increase palm oil production for food, domestic products, and, especially, biofuels. Greater use of palm oil for biofuel production is predicated on the assumption that palm oil is an “environmentally friendly” fuel feedstock. Here we show, using measurements and models, that oil palm plantations in Malaysia directly emit more oxides of nitrogen and volatile organic compounds than rainforest. These compounds lead to the production of ground-level ozone (O3), an air pollutant that damages human health, plants, and materials, reduces crop productivity, and has effects on the Earth's climate. Our measurements show that, at present, O3 concentrations do not differ significantly over rainforest and adjacent oil palm plantation landscapes. However, our model calculations predict that if concentrations of oxides of nitrogen in Borneo are allowed to reach those currently seen over rural North America and Europe, ground-level O3 concentrations will reach 100 parts per billion (109) volume (ppbv) and exceed levels known to be harmful to human health. Our study provides an early warning of the urgent need to develop policies that manage nitrogen emissions if the detrimental effects of palm oil production on air quality and climate are to be avoided.

Nitrogen management is essential to prevent tropical oil palm plantations from causing ground-level ozone pollution

More than half the world's rainforest has been lost to agriculture since the Industrial Revolution. Among the most widespread tropical crops is oil palm (Elaeis guineensis): global production now exceeds 35 million tonnes per year. In Malaysia, for example, 13% of land area is now oil palm plantation, compared with 1% in 1974. There are enormous pressures to increase palm oil production for food, domestic products, and, especially, biofuels. Greater use of palm oil for biofuel production is predicated on the assumption that palm oil is an "environmentally friendly'' fuel feedstock. Here we show, using measurements and models, that oil palm plantations in Malaysia directly emit more oxides of nitrogen and volatile organic compounds than rainforest. These compounds lead to the production of ground-level ozone (O-3), an air pollutant that damages human health, plants, and materials, reduces crop productivity, and has effects on the Earth's climate. Our measurements show that, at present, O-3 concentrations do not differ significantly over rainforest and adjacent oil palm plantation landscapes. However, our model calculations predict that if concentrations of oxides of nitrogen in Borneo are allowed to reach those currently seen over rural North America and Europe, ground-level O-3 concentrations will reach 100 parts per billion (10(9)) volume (ppbv) and exceed levels known to be harmful to human health. Our study provides an early warning of the urgent need to develop policies that manage nitrogen emissions if the detrimental effects of palm oil production on air quality and climate are to be avoided.

In situ and remote-sensing measurements of the mean microphysical and optical properties of industrial pollution aerosol during ADRIEX

We present a summary of the principal physical and optical properties of aerosol particles using the FAAM BAE-146 instrumented aircraft during ADRIEX between 27 August and 6 September 2004, augmented by sunphotometer, lidar and satellite retrievals. Observations of anthropogenic aerosol, principally from industrial sources, were concentrated over the northern Adriatic Sea and over the Po Valley close to the aerosol sources. An additional flight was also carried out over the Black Sea to compare east and west European pollution. Measurements show the single-scattering albedo of dry aerosol particles to vary considerably between 0.89 and 0.97 at a wavelength of 0.55 μm, with a campaign mean within the polluted lower free troposphere of 0.92. Although aerosol concentrations varied significantly from day to day and during individual days, the shape of the aerosol size distribution was relatively consistent through the experiment, with no detectable change observed over land and over sea. There is evidence to suggest that the pollution aerosol within the marine boundary layer was younger than that in the elevated layer. Trends in the aerosol volume distribution show consistency with multiple-site AERONET radiometric observations. The aerosol optical depths derived from aircraft measurements show a consistent bias to lower values than both the AERONET and lidar ground-based radiometric observations, differences which can be explained by local variations in the aerosol column loading and by some aircraft instrumental artefacts. Retrievals of the aerosol optical depth and fine-mode (<0.5 μm radius) fraction contribution to the optical depth using MODIS data from the Terra and Aqua satellites show a reasonable level of agreement with the AERONET and aircraft measurements.

Statistical inference of OH concentrations and air mass dilution rates from successive observations of non-methane hydrocarbons in single air masses

Bayesian inference has been used to determine rigorous estimates of hydroxyl radical concentrations () and air mass dilution rates (K) averaged following air masses between linked observations of nonmethane hydrocarbons (NMHCs) spanning the North Atlantic during the Intercontinental Transport and Chemical Transformation (ITCT)-Lagrangian-2K4 experiment. The Bayesian technique obtains a refined (posterior) distribution of a parameter given data related to the parameter through a model and prior beliefs about the parameter distribution. Here, the model describes hydrocarbon loss through OH reaction and mixing with a background concentration at rate K. The Lagrangian experiment provides direct observations of hydrocarbons at two time points, removing assumptions regarding composition or sources upstream of a single observation. The estimates are sharpened by using many hydrocarbons with different reactivities and accounting for their variability and measurement uncertainty. A novel technique is used to construct prior background distributions of many species, described by variation of a single parameter . This exploits the high correlation of species, related by the first principal component of many NMHC samples. The Bayesian method obtains posterior estimates of , K and following each air mass. Median values are typically between 0.5 and 2.0 × 106 molecules cm−3, but are elevated to between 2.5 and 3.5 × 106 molecules cm−3, in low-level pollution. A comparison of estimates from absolute NMHC concentrations and NMHC ratios assuming zero background (the “photochemical clock” method) shows similar distributions but reveals systematic high bias in the estimates from ratios. Estimates of K are ∼0.1 day−1 but show more sensitivity to the prior distribution assumed.

Chemical composition observed over the mid-Atlantic and the detection of pollution signatures far from source regions

The atmospheric composition of the central North Atlantic region has been sampled using the FAAM BAe146 instrumented aircraft during the Intercontinental Transport of Ozone and Precursors (ITOP) campaign, part of the wider International Consortium for Atmospheric Research on Transport and Transformation (ICARTT). This paper presents an overview of the ITOP campaign. Between late July and early August 2004, twelve flights comprising 72 hours of measurement were made in a region from approximately 20 to 40°W and 33 to 47°N centered on Faial Island, Azores, ranging in altitude from 50 to 9000 m. The vertical profiles of O3 and CO are consistent with previous observations made in this region during 1997 and our knowledge of the seasonal cycles within the region. A cluster analysis technique is used to partition the data set into air mass types with distinct chemical signatures. Six clusters provide a suitable balance between cluster generality and specificity. The clusters are labeled as biomass burning, low level outflow, upper level outflow, moist lower troposphere, marine and upper troposphere. During this summer, boreal forest fire emissions from Alaska and northern Canada were found to provide a major perturbation of tropospheric composition in CO, PAN, organic compounds and aerosol. Anthropogenic influenced air from the continental boundary layer of the USA was clearly observed running above the marine boundary layer right across the mid-Atlantic, retaining high pollution levels in VOCs and sulfate aerosol. Upper level outflow events were found to have far lower sulfate aerosol, resulting from washout on ascent, but much higher PAN associated with the colder temperatures. Lagrangian links with flights of other aircraft over the USA and Europe show that such signatures are maintained many days downwind of emission regions. Some other features of the data set are highlighted, including the strong perturbations to many VOCs and OVOCs in this remote region.

Air-earth current density measurements at Lerwick; implications for seasonality in the global electric circuit

Atmospheric electricity measurements were made at Lerwick Observatory in the Shetland Isles (60°09′N, 1°08′W) during most of the 20th century. The Potential Gradient (PG) was measured from 1926 to 84 and the air-earth conduction current (Jc) was measured during the final decade of the PG measurements. Daily Jc values (1978–1984) observed at 15 UT are presented here for the first time, with independently-obtained PG measurements used to select valid data. The 15 UT Jc (1978–1984) spans 0.5–9.5 pA/m2, with median 2.5 pA/m2; the columnar resistance at Lerwick is estimated as 70 PΩm2. Smoke measurements confirm the low pollution properties of the site. Analysis of the monthly variation of Lerwick Jc data shows that winter (DJF) Jc is significantly greater than the summer (JJA) Jc by 20%. The Lerwick atmospheric electricity seasonality differs from the global lightning seasonality, but Jc has a similar seasonal phasing to that observed in Nimbostratus clouds globally, suggesting a role for non-thunderstorm rain clouds in the seasonality of the global circuit.

Two daily smoke maxima in eighteenth century London air

Varied electrostatics experiments followed Benjamin Franklin's pioneering atmospheric investigations. In Knightsbridge, Central London, John Read (1726–1814) installed a sensing rod in the upper part of his house and, using a pith ball electrometer and Franklin chimes, monitored atmospheric electricity from 1789 to 1791. Atmospheric electricity is sensitive to weather and smoke pollution. In calm weather conditions, Read observed two daily electrification maxima in moderate weather, around 9 am and 7 pm. This is likely to represent a double diurnal cycle in urban smoke. Before the motor car and steam railways, one source of the double maximum smoke pattern was the daily routine of fire lighting for domestic heating.

Mitigation of diffuse phosphorus pollution during rewetting of fen peat soils: A trans-European case study

Intensive cultivation of fen peat soils (Eutric Histosols) for agricultural purposes, started in Europe about 250 years ago, resulting in decreased soil fertility, increased oxidation of peat and corresponding CO2-emissions to the atmosphere, nutrient transfer to aquatic ecosystems and losses in the total area of the former native wetlands. To prevent these negative environmental effects set-aside programs and rewetting measures were promoted in recent years. Literature results and practical experiences showed that large scale rewetting of intensively used agricultural Histosols may result in the mobilisation of phosphorus (P), its transport to adjacent surface waters and an accelerated eutrophication risk. The paper summarises results from an international European Community sponsored research project and demonstrates how results obtained at different scales and from different scientific disciplines were compiled to derive a strategy to carry out rewetting measures. A decision support system (DSS) for a hydrologically sensitive area in the Droemling catchment in north-eastern Germany was developed and is presented as a tool to regulate rewetting in order to control P release. It is demonstrated that additional laboratory experiments to identify essential processes of P release during rewetting and the site-specific management of the water table, the involvement of specific knowledge and experience of the stakeholders are necessary to develop an applicable DSS. The presented DSS is practically used to prevent freshwater resources from diffuse P pollution.

Results from the Covered Catchment Experiment at Gårdsjön, Sweden, after ten years of clean precipitation treatment

The Covered Catchment Experiment at Gordsjon is a large scale forest ecosystem manipulation, where acid precipitation was intercepted by a 7000 m(2) plastic roof and replaced by 'clean precipitation' sprinkled below the roof for ten years between 1991 and 2001. The treatment resulted in a strong positive response of runoff quality. The runoff sulphate, inorganic aluminium and base cations decreased, while there was a strong increase in runoff ANC and a moderate increase in pH. The runoff continued to improve over the whole duration of the experiment. The achieved quality was, however, after ten years still considerably worse than estimated pre-industrial runoff at the site. Stable isotopes of sulphur were analysed to study the soil sulphur cycling. At the initial years of the experiment, the desorption of SO4 from the mineral soil appeared to control the runoff SO4 concentration. However, as the experiment proceeded, there was growing evidence that net mineralisation of soil organic sulphur in the humus layer was an additional source of SO4 in runoff. This might provide a challenge to current acidification models. The experiment convincingly demonstrated on a catchment scale, that reduction in acid deposition causes an immediate improvement of surface water quality even at heavily acidified sites. The improvement of the runoff appeared to be largely a result of cation exchange processes in the soil due to decreasing concentrations of the soil solution, while any potential change in soil base saturation seemed to be less important for the runoff chemistry over the short time period of one decade. These findings should be considered when interpreting and extrapolating regional trends in surface water chemistry to the terrestrial parts of ecosystems.

Recent oppositely directed trends in solar climate forcings and the global mean surface air temperature. II. Different reconstructions of the total solar irradiance variation and dependence on response time scale

We have previously placed the solar contribution to recent global warming in context using observations and without recourse to climate models. It was shown that all solar forcings of climate have declined since 1987. The present paper extends that analysis to include the effects of the various time constants with which the Earth’s climate system might react to solar forcing. The solar input waveform over the past 100 years is defined using observed and inferred galactic cosmic ray fluxes, valid for either a direct effect of cosmic rays on climate or an effect via their known correlation with total solar irradiance (TSI), or for a combination of the two. The implications, and the relative merits, of the various TSI composite data series are discussed and independent tests reveal that the PMOD composite used in our previous paper is the most realistic. Use of the ACRIM composite, which shows a rise in TSI over recent decades, is shown to be inconsistent with most published evidence for solar influences on pre-industrial climate. The conclusions of our previous paper, that solar forcing has declined over the past 20 years while surface air temperatures have continued to rise, are shown to apply for the full range of potential time constants for the climate response to the variations in the solar forcings.

A new method for evaluating regional air quality forecasts

A Kriging interpolation method is combined with an object-based evaluation measure to assess the ability of the UK Met Office's dispersion and weather prediction models to predict the evolution of a plume of tracer as it was transported across Europe. The object-based evaluation method, SAL, considers aspects of the Structure, Amplitude and Location of the pollutant field. The SAL method is able to quantify errors in the predicted size and shape of the pollutant plume, through the structure component, the over- or under-prediction of the pollutant concentrations, through the amplitude component, and the position of the pollutant plume, through the location component. The quantitative results of the SAL evaluation are similar for both models and close to a subjective visual inspection of the predictions. A negative structure component for both models, throughout the entire 60 hour plume dispersion simulation, indicates that the modelled plumes are too small and/or too peaked compared to the observed plume at all times. The amplitude component for both models is strongly positive at the start of the simulation, indicating that surface concentrations are over-predicted by both models for the first 24 hours, but modelled concentrations are within a factor of 2 of the observations at later times. Finally, for both models, the location component is small for the first 48 hours after the start of the tracer release, indicating that the modelled plumes are situated close to the observed plume early on in the simulation, but this plume location error grows at later times. The SAL methodology has also been used to identify differences in the transport of pollution in the dispersion and weather prediction models. The convection scheme in the weather prediction model is found to transport more pollution vertically out of the boundary layer into the free troposphere than the dispersion model convection scheme resulting in lower pollutant concentrations near the surface and hence a better forecast for this case study.

Open Air Laboratories (OPAL): a community-driven research programme

OPAL is an English national programme that takes scientists into the community to investigate environmental issues. Biological monitoring plays a pivotal role covering topics of: i) soil and earthworms; ii) air, lichens and tar spot on sycamore; iii) water and aquatic invertebrates; iv) biodiversity and hedgerows; v) climate, clouds and thermal comfort. Each survey has been developed by an interdisciplinary team and tested by voluntary, statutory and community sectors. Data are submitted via the web and instantly mapped. Preliminary results are presented, together with a discussion on data quality and uncertainty. Communities also investigate local pollution issues, ranging from nitrogen deposition on heathlands to traffic emissions on roadside vegetation. Over 200,000 people have participated so far, including over 1000 schools and 1000 voluntary groups. Benefits include a substantial, growing database on biodiversity and habitat condition, much from previously unsampled sites particularly in urban areas, and a more engaged public.