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Air pollution is growing fastest in monsoon-impacted South Asia. During the dry winter monsoon, the fumes disperse toward the Indian Ocean, creating a vast pollution haze. The fate of these fumes during the wet summer monsoon has been unclear. Lelieveld et al. performed atmospheric chemistry measurements by aircraft in the Oxidation Mechanism Observations campaign, sampling the summer monsoon outflow in the upper troposphere between the Mediterranean and the Indian Ocean. The measurements, supported by model calculations, show that the monsoon sustains a remarkably efficient cleansing mechanism in which contaminants are rapidly oxidized and deposited on Earth's surface. However, some pollutants are lofted above the monsoon clouds and chemically processed in a reactive reservoir before being redistributed globally, including to the stratosphere. Science , this issue p. 270 The South Asian monsoon removes some air pollution and disperses the rest. Air pollution is growing fastest in monsoon-affected South Asia. During the dry winter monsoon, the fumes disperse toward the Indian Ocean, creating a vast pollution haze, but their fate during the wet summer monsoon has been unclear. We performed atmospheric chemistry measurements by aircraft in the Oxidation Mechanism Observations campaign, sampling the summer monsoon outflow in the upper troposphere between the Mediterranean and the Indian Ocean. The measurements, supported by model calculations, show that the monsoon sustains a remarkably efficient cleansing mechanism by which contaminants are rapidly oxidized and deposited to Earth’s surface. However, some pollutants are lofted above the monsoon clouds and chemically processed in a reactive reservoir before being redistributed globally, including to the stratosphere.

Ambient OH and HO2 concentrations were measured by laser induced fluorescence (LIF) during the PRIDE-PRD2006 (Program of Regional Integrated Experiments of Air Quality over the Pearl River Delta, 2006) campaign at a rural site downwind of the megacity of Guangzhou in Southern China. The observed OH concentrations reached daily peak values of (15-26) × 106 cm-3 which are among the highest values so far reported for urban and suburban areas. The observed OH shows a consistent high correlation with j(O1 D) over a broad range of NOx conditions. The correlation cannot be reproduced by model simulations, indicating that OH stabilizing processes are missing in current models. The observed OH exhibited a weak dependence on NOx in contrast to model predictions. While modelled and measured OH agree well at NO mixing ratios above 1 ppb, a continuously increasing underprediction of the observed OH is found towards lower NO concentrations, reaching a factor of 8 at 0.02 ppb NO. A dependence of the modelled-to-measured OH ratio on isoprene cannot be concluded from the PRD data. However, the magnitude of the ratio fits into the isoprene dependent trend that was reported from other campaigns in forested regions. Hofzumahaus et al. (2009) proposed an unknown OH recycling process without NO, in order to explain the high OH levels at PRD in the presence of high VOC reactivity and low NO. Taking a recently discovered interference in the LIF measurement of HO2 into account, the need for an additional HO2 -> OH recycling process persists, but the required source strength may be up to 20% larger than previously determined. Recently postulated isoprene mechanisms by Lelieveld et al. (2008) and Peeters and Müller (2010) lead to significant enhancements of OH expected for PRD, but an underprediction of the observed OH by a factor of two remains at low NO (0.1-0.2 ppb). If the photolysis of hydroperoxy aldehydes from isoprene is as efficient as proposed by Peeters and Müller (2010), the corresponding OH formation at PRD would be more important than the primary OH production from ozone and HONO. While the new isoprene mechanisms need to be confirmed by laboratory experiments, there is probably need for other, so far unidentified chemical processes to explain entirely the high OH levels observed in Southern China.

Measurements of ambient OH and HO2 radicals were performed by laser induced fluorescence (LIF) during CAREBeijing2006 (Campaigns of Air Quality Research in Beijing and Surrounding Region 2006) at the suburban site Yufa in the south of Beijing in summer 2006. On most days, local air chemistry was influenced by aged air pollution that was advected by a slow, almost stagnant wind from southern regions. Observed daily concentration maxima were in the range of (4-17) × 106 cm-3 for OH and (2-24) × 108 cm-3 for HO2 (including an estimated interference of 25% from RO2 ). During daytime, OH reactivities were generally high (10-30 s-1 ) and mainly contributed by observed VOCs and their calculated oxidation products. The comparison of modelled and measured HOx concentrations reveals a systematic underprediction of OH as a function of NO. A large discrepancy of a factor 2.6 is found at the lowest NO concentration encountered (0.1 ppb), whereas the discrepancy becomes insignificant above 1 ppb NO. This study extends similar observations from the Pearl-River Delta (PRD) in South China to a more urban environment. The OH discrepancy at Yufa can be resolved, if NO-independent additional OH recycling is assumed in the model. The postulated Leuven Isoprene Mechanism (LIM) has the potential to explain the gap between modelled and measured OH at Beijing taking into account conservative error estimates, but lacks experimental confirmation. This and the hereby unresolved discrepancy at PRD suggest that other VOCs besides isoprene might be involved in the required, additional OH recycling. Fast primary production of ROx radicals up to 7 ppb h-1 was determined at Beijing which was dominated by the photolysis of O3 , HONO, HCHO, and dicarbonyls. For a special case, 20 August, when the plume of Beijing city was encountered, a missing primary HOx source (about 3 ppb h-1 ) was determined under high NOx conditions similar to other urban areas like Mexico City. CAREBeijing2006 emphasizes the important role of OVOCs as a radical source and sink, and the need for further investigation of the chemical degradation of VOCs in order to better understand radical chemistry in VOC-rich air.

Land use change in rangeland ecosystems is pervasive throughout the western United States with widespread ecological, social and economic implications. In California, rangeland habitats have high biodiversity value, provide significant habitat connectivity and form the foundation for a number of ecosystem services. To comprehensively assess the conservation status of these habitats, we analyzed the extent and drivers of habitat loss and the degree of protection against future loss across a 13.5 M ha study area in California. We analyzed rangeland conversion between 1984 and 2008 using time series GIS data and classified resulting land uses with aerial imagery. In total, over 195,000 hectares of rangeland habitats were converted during this period. The majority of conversions were to residential and associated commercial development (49% of the area converted), but agricultural intensification was surprisingly extensive and diverse (40% across six categories). Voluntary enrollment in an agricultural tax incentive program provided widespread protection from residential and commercial conversions across 37% of the remaining rangeland habitat extent (7.5 M ha), though this program did not protect rangeland from conversion to more intensive agricultural uses. Additionally, 24% of the remaining rangeland was protected by private conservation organizations or public agencies through land or easement ownership while 38% had no protection status at all. By developing a spatial method to analyze the drivers of loss and patterns of protection, this study demonstrates a novel approach to prioritize conservation strategies and implementation locations to avert habitat conversion. We propose that this approach can be used in other ecosystem types, and can serve as a regional conservation baseline assessment to focus strategies to effect widespread, cost-effective conservation solutions.

We performed measurements of nitrous acid (HONO) during the PRIDE-PRD2006 campaign in the Pearl River Delta region 60 km north of Guangzhou, China, for 4 weeks in June 2006. HONO was measured by a LOPAP in-situ instrument which was setup in one of the campaign supersites along with a variety of instruments measuring hydroxyl radicals, trace gases, aerosols, and meteorological parameters. Maximum diurnal HONO mixing ratios of 1–5 ppb were observed during the nights. We found that the nighttime build-up of HONO can be attributed to the heterogeneous NO2 to HONO conversion on ground surfaces and the OH + NO reaction. In addition to elevated nighttime mixing ratios, measured noontime values of ≈200 ppt indicate the existence of a daytime source higher than the OH + NO→HONO reaction. Using the simultaneously recorded OH, NO, and HONO photolysis frequency, a daytime additional source strength of HONO (PM) was calculated to be 0.77 ppb h−1 on average. This value compares well to previous measurements in other environments. Our analysis of PM provides evidence that the photolysis of HNO3 adsorbed on ground surfaces contributes to the HONO formation.

This study was part of the international field measurement Campaigns of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing‐2006). We investigated a new particle formation event in a highly polluted air mass at a regional site south of the megacity Beijing and its impact on the abundance and properties of cloud condensation nuclei (CCN). During the 1‐month observation, particle nucleation followed by significant particle growth on a regional scale was observed frequently (∼30%), and we chose 23 August 2006 as a representative case study. Secondary aerosol mass was produced continuously, with sulfate, ammonium, and organics as major components. The aerosol mass growth rate was on average 19 μg m−3 h−1 during the late hours of the day. This growth rate was observed several times during the 1‐month intensive measurements. The nucleation mode grew very quickly into the size range of CCN, and the CCN size distribution was dominated by the growing nucleation mode (up to 80% of the total CCN number concentration) and not as usual by the accumulation mode. At water vapor supersaturations of 0.07–0.86%, the CCN number concentrations reached maximum values of 4000–19,000 cm−3 only 6–14 h after the nucleation event. During particle formation and growth, the effective hygroscopicity parameter κ increased from about 0.1–0.3 to 0.35–0.5 for particles with diameters of 40–90 nm, but it remained nearly constant at ∼0.45 for particles with diameters of ∼190 nm. This result is consistent with aerosol chemical composition data, showing a pronounced increase of sulfate.

Total atmospheric OH reactivities (kOH) have been measured as reciprocal OH lifetimes by a newly developed instrument at a rural site in the densely populated Pearl River Delta (PRD) in Southern China in summer 2006. The deployed technique, LP-LIF, uses laser flash photolysis (LP) for artificial OH generation and laser-induced fluorescence (LIF) to measure the time-dependent OH decay in samples of ambient air. The reactivities observed at PRD covered a range from 10 s−1 to 120 s−1, indicating a large load of chemical reactants. On average, kOH exhibited a pronounced diurnal profile with a mean maximum value of 50 s−1 at daybreak and a mean minimum value of 20 s−1 at noon. The comparison of reactivities calculated from measured trace gases with measured kOH reveals a missing reactivity of about a factor of 2 at day and night. The reactivity explained by measured trace gases was dominated by anthropogenic pollutants (e.g., CO, NOx, light alkenes and aromatic hydrocarbons) at night, while it was strongly influenced by local, biogenic emissions of isoprene during the day. Box model calculations initialized by measured parameters reproduce the observed OH reactivity well and suggest that the missing reactivity is contributed by unmeasured, secondary chemistry products (mainly aldehydes and ketones) that were photochemically formed by hydrocarbon oxidation. Overall, kOH was dominated by organic compounds, which had a maximum contribution of 85% in the afternoon. The paper demonstrates the usefulness of direct reactivity measurements, emphasizes the need for direct measurements of oxygenated organic compounds in atmospheric chemistry studies, and discusses uncertainties of the modelling of OVOC reactivities.

Field measurements have revealed much higher concentrations of hydroxyl radicals than expected in regions with high loads of the biogenic volatile organic compound isoprene. Results from isoprene oxidation experiments suggest that the additional recycling of radicals in the presence of isoprene contributes to hydroxyl radical enhancement in these regions. Most pollutants in the Earth’s atmosphere are removed by oxidation with highly reactive hydroxyl radicals. Field measurements have revealed much higher concentrations of hydroxyl radicals than expected in regions with high loads of the biogenic volatile organic compound isoprene 1 , 2 , 3 , 4 , 5 , 6 , 7 , 8 . Different isoprene degradation mechanisms have been proposed to explain the high levels of hydroxyl radicals observed 5 , 9 , 10 , 11 . Whether one or more of these mechanisms actually operates in the natural environment, and the potential impact on climate and air quality, has remained uncertain 12 , 13 , 14 . Here, we present a complete set of measurements of hydroxyl and peroxy radicals collected during isoprene-oxidation experiments carried out in an atmospheric simulation chamber, under controlled atmospheric conditions. We detected significantly higher concentrations of hydroxyl radicals than expected based on model calculations, providing direct evidence for a strong hydroxyl radical enhancement due to the additional recycling of radicals in the presence of isoprene. Specifically, our findings are consistent with the unimolecular reactions of isoprene-derived peroxy radicals postulated by quantum chemical calculations 9 , 10 , 11 . Our experiments suggest that more than half of the hydroxyl radicals consumed in isoprene-rich regions, such as forests, are recycled by these unimolecular reactions with isoprene. Although such recycling is not sufficient to explain the high concentrations of hydroxyl radicals observed in the field, we conclude that it contributes significantly to the oxidizing capacity of the atmosphere in isoprene-rich regions.

HO2 concentration measurements are widely accomplished by chemical conversion of HO2 to OH including reaction with NO and subsequent detection of OH by laser-induced fluorescence. RO2 radicals can be converted to OH via a similar radical reaction sequence including reaction with NO, so that they are potential interferences for HO2 measurements. Here, the conversion efficiency of various RO2 species to HO2 is investigated. Experiments were conducted with a radical source that produces OH and HO2 by water photolysis at 185 nm, which is frequently used for calibration of LIF instruments. The ratio of HO2 and the sum of OH and HO2 concentrations provided by the radical source was investigated and was found to be 0.50 ± 0.02. RO2 radicals are produced by the reaction of various organic compounds with OH in the radical source. Interferences via chemical conversion from RO2 radicals produced by the reaction of OH with methane and ethane (H-atom abstraction) are negligible consistent with measurements in the past. However, RO2 radicals from OH plus alkene- and aromatic-precursors including isoprene (mainly OH-addition) are detected with a relative sensitivity larger than 80 % with respect to that for HO2 for the configuration of the instrument with which it was operated during field campaigns. Also RO2 from OH plus methyl vinyl ketone and methacrolein exhibit a relative detection sensitivity of 60 %. Thus, previous measurements of HO2 radical concentrations with this instrument were biased in the presence of high RO2 radical concentrations from isoprene, alkenes or aromatics, but were not affected by interferences in remote clean environment with no significant emissions of biogenic VOCs, when the OH reactivity was dominated by small alkanes. By reducing the NO concentration and/or the transport time between NO addition and OH detection, interference from these RO2 species are suppressed to values below 20 % relative to the HO2 detection sensitivity. The HO2 conversion efficiency is also smaller by a factor of four, but this is still sufficient for atmospheric HO2 concentration measurements for a wide range of conditions.

An evocative exploration of the impact of the Mediterranean on British culture, ranging from the mid-eighteenth century to today Ever since the age of the Grand Tour in the eighteenth century, the Mediterranean has had a significant pull for Britons-including many painters and poets-who sought from it the inspiration, beauty, and fulfillment that evaded them at home. Referred to as \"Magick Land\" by one traveler, dreams about the Mediterranean, and responses to it, went on to shape the culture of a nation. Written by one of the world's leading historians of the Mediterranean, this book charts how a new sensibility arose from British engagement with the Mediterranean, ancient and modern. Ranging from Byron's poetry to Damien Hirst's installations, Robert Holland shows that while idealized visions and aspirations often met with disillusionment and frustration, the Mediterranean also offered a notably insular society the chance to enrich itself through an imagined world of color, carnival, and sensual self-discovery.