The paper shows how extreme meteorological conditions change due to the urban land-cover forcing and how this translates to the impact on the extreme air pollution over central European cities. It focuses on ozone, nitrogen dioxide, and particulate matter with a diameter of less than 2.5 μm and shows that, while for the extreme daily maximum 8 h ozone, changes are same as for the mean ones, much larger modifications are calculated for extreme NO2 and PM2.5 compared to their mean changes.
China suffers from serious air pollution, which is thought to cause millions of early deaths each year. Measurements on the ground show that overall air quality is improving. Air quality is also affected by weather conditions, which can vary from year to year. We conduct computer simulations to show it is the reduction of the amount of pollution emitted, rather than weather conditions, which caused air quality to improve during 2015–2017. We then estimate that 150 000 fewer people die early.
After the volcanic eruption of Mt Pinatubo in 1991, ozone decreased in the tropics and increased in the midlatitudes and polar regions for 1 year. The change in the ozone column is solely a result of the volcanic heating, followed by an ozone decrease in the higher latitudes. This is caused by the volcanic aerosol, which changes the heterogeneous chemistry and thus the catalytic ozone loss cycles. Vertical transport of water vapour is enhanced by volcanic heating and increases methane.
Our work suggests that a large corona discharge system is an efficient and possibly economically sustainable way to increase the ion density in the open air and control the precipitation of atmospheric aerosols. Once the system is installed on a mountaintop, it will generate lots of charged nuclei, which may trigger water precipitation or fog elimination within a certain region in the downwind directions.
We simulated the thermodynamic and multiphase reactions in aerosol water during a wintertime haze event over the North China Plain. It was found that aerosol pH exhibited a strong spatiotemporal variability, and multiple oxidation pathways were predominant for particulate sulfate formation in different locations. Sensitivity tests further showed that ammonia, crustal particles, and dissolved transition metal ions were important factors for multiphase chemistry during haze episodes.
We rely on sulfuric acid measurements in four contrasting environments, Hyytiälä, Finland; Agia Marina, Cyprus; Budapest, Hungary; and Beijing, China, representing semi-pristine boreal forest, rural environment in the Mediterranean area, urban environment, and heavily polluted megacity, respectively, in order to define the sources and sinks of sulfuric acid in these environments and to derive a new sulfuric acid proxy to be utilized in locations and during periods when it is not measured.
Secondary ice production (SIP) plays a key role in the formation of ice particles in tropospheric clouds. This work presents a critical review of the laboratory studies related to secondary ice production. It aims to identify gaps in our knowledge of SIP as well as to stimulate further laboratory studies focused on obtaining a quantitative description of efficiencies for each SIP mechanism.
In this work, we make the three main contributions. (1) We reveal the remarkable differences in the geographical distributions of cirrus over the Tibetan Plateau regarding the cloud top height. (2) The orography, gravity wave, and deep convection determine the formation of cirrus with a cloud top below 9, at 9–12, and above 12 km, respectively. (3) It is the first time the contributions of the Tibetan Plateau to the presence of cirrus on a regional scale are discussed.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Black carbon (BC) and greenhouse gases (GHGs) enhance precipitation minus evaporation (P–E) of Asian summer monsoon (ASM). Further analysis reveals distinct mechanisms controlling BC- and GHG-induced ASM P–E increases. The change in ASM P–E by BC is dominated by the dynamic effect of enhanced large-scale monsoon circulation, the GHG-induced change by the thermodynamic effect of increasing atmospheric water vapor. This results from different atmospheric temperature feedbacks due to BC and GHGs.
Janne Lampilahti, Hanna Elina Manninen, Katri Leino, Riikka Väänänen, Antti Manninen, Stephany Buenrostro Mazon, Tuomo Nieminen, Matti Leskinen, Joonas Enroth, Marja Bister, Sergej Zilitinkevich, Juha Kangasluoma, Heikki Järvinen, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
In this work, by using co-located airborne and ground-based measurements, we show that counter-rotating horizontal circulations in the planetary boundary layer (roll vortices) frequently enhance regional new particle formation or induce localized bursts of new particle formation. These observations can be explained by the ability of the rolls to efficiently lift low-volatile vapors emitted from the surface to the top of the boundary layer where new particle formation is more favorable.
Emissions of air pollutants must be known for a wide variety of applications. Different methods of estimating emissions often disagree substantially. In this study, we apply standard methods to a well-known source, a power plant. We explore the uncertainty implied by the different answers that come from the different methods, different samples taken over several years, and different pollutants. We find that the overall uncertainty of emissions estimates is about 30 %.
A 22-year (1996 to 2017) consistent Arctic tropospheric BrO dataset derived from four satellite remote sensing instruments is presented. An increase in tropospheric BrO VCDs over this period, and especially during polar springs, can be seen. Comparisons of tropospheric BrO VCDs with first-year sea ice reveal a moderate spatial and temporal correlation between the two, suggesting that the increase in first-year sea ice in the Arctic has an impact on tropospheric BrO abundancies.
The feedback effect between aerosol particles, radiation and meteorology reduces turbulent motion and results in increased surface aerosol concentrations during Beijing haze. Observational analysis and regional modelling studies have examined the feedback effect but these studies are limited. In this work, we set up a high-resolution model for the Beijing environment to examine the sensitivity of the aerosol feedback effect to initial meteorological conditions and aerosol loading.
In this study, we estimate monthly ammonia emission from synthetic nitrogen fertilizer use across the contiguous US from 1900 to 2015. The results indicate the important role that cropland expansion and nitrogen fertilizer enrichment played in enhancing NH3 emissions. It shows such long-term human activities have dramatically changed the spatiotemporal and seasonal patterns of NH3 emission, impacting air pollution and public health in the US.
Occurrences, size distributions, and number fractions of individual aerosol particles from the Amazon basin during the GoAmazon2014/5 campaign were analyzed using transmission electron microscopy. Aerosol particles from natural sources (e.g., mineral dust, primary biological aerosols, and sea salts) during the wet season originated from the Amazon forest and long-range transports (the Saharan desert and the Atlantic Ocean). They commonly mix at an individual particle scale during transport.
Various sources and meteorological conditions affect the short-term variation in NH3 concentrations in the urban atmosphere. An analysis of 2 years of hourly data suggests that mist evaporation and stomata exchange of tree leaves after the effects of bird droppings engenders a rapid increase in NH3 concentrations. Emissions from urban tree canopies are a new mode of passing reactive nitrogen that has never before been described as an important source in the literature.
Projected changes in man-made aerosol range from large reductions to moderate increases in emissions until 2050. Rapid reductions between the present and the 2050s lead to enhanced increases in global and Asian summer monsoon precipitation relative to scenarios with continued increases in aerosol. Relative magnitude and spatial distribution of aerosol changes are particularly important for South Asian summer monsoon precipitation changes, affecting the sign of the trend in the coming decades.
This paper presents a first cross-comparison of meteor ground-based observations and a meteorological analysis (NAVGEM-HA) to compare a seasonal climatology of winds and temperatures at the mesosphere/lower thermosphere. The validation is insofar unique as we not only compare the mean state but also provide a detailed comparison of the short time variability of atmospheric tidal waves. Our analysis questions previous results claiming the importance of lunar tides.
To understand South Korea's CO2 emissions and sinks as well as those of the surrounding region, we used flask-air samples collected for 2 years at Anmyeondo (36.53° N, 126.32° E; 46 m a.s.l.), South Korea, for analysis of observed 14C in atmospheric CO2 as a tracer of fossil fuel CO2 contribution (Cff). Here, we showed our observation result of 14C and Cff. SF6 and CO can be good proxies of Cff in this study, and the ratio of CO to Cff was compared to a bottom-up inventory.
Guillaume Monteil, Grégoire Broquet, Marko Scholze, Matthew Lang, Ute Karstens, Christoph Gerbig, Frank-Thomas Koch, Naomi E. Smith, Rona L. Thompson, Ingrid T. Luijkx, Emily White, Antoon Meesters, Philippe Ciais, Anita L. Ganesan, Alistair Manning, Michael Mischurow, Wouter Peters, Philippe Peylin, Jerôme Tarniewicz, Matt Rigby, Christian Rödenbeck, Alex Vermeulen, and Evie M. Walton
The paper presents the first results from the EUROCOM project, a regional atmospheric inversion intercomparison exercise involving six European research groups. It aims to produce an estimate of the net carbon flux between the European terrestrial ecosystems and the atmosphere for the period 2006–2015, based on constraints provided by observed CO2 concentrations and using inverse modelling techniques. The use of six different models enables us to investigate the robustness of the results.
Swaleha Inamdar, Liselotte Tinel, Rosie Chance, Lucy J. Carpenter, Prabhakaran Sabu, Racheal Chacko, Sarat C. Tripathy, Anvita U. Kerkar, Alok K. Sinha, Parli Venkateswaran Bhaskar, Amit Sarkar, Rajdeep Roy, Tomás Sherwen, Carlos Cuevas, Alfonso Saiz-Lopez, Kirpa Ram, and Anoop S. Mahajan
Iodine chemistry is generating a lot of interest because of its impacts on the oxidising capacity of the marine boundary and depletion of ozone. However, one of the challenges has been predicting the right levels of iodine in the models, which depend on parameterisations for emissions from the sea surface. This paper discusses the different parameterisations available and compares them with observations, showing that our current knowledge is still insufficient, especially on a regional scale.
We analyzed the characteristics and sources of HONO in the upper boundary layer and lower free troposphere in the North China Plain, based on the field measurements at Mount Tai. Higher-than-expected levels and broad daytime peaks of HONO were observed. Without presence of ground surfaces, aerosol surface plays a key role in the heterogeneous HONO formation at high altitudes. Models without additional HONO sources largely underestimated the oxidation processes in the elevation atmospheres.
Source apportionment studies require information on the chemical fingerprints of pollution sources to correctly quantify source contributions to ambient composition. These chemical fingerprints vary from region to region, depending on fuel composition and combustion conditions, and are poorly constrained over developing regions such as South Asia. This work characterises the chemical fingerprints of urban and agricultural sources using 49 non-methane hydrocarbons and their environmental impacts.
The stratospheric water vapor mixing ratio over North America (NA) region is up to ~ 1 ppmv higher when deep convection occurs. We find substantial consistency in the interannual variations of NA water vapor anomaly and deep convection and explain both the summer seasonal cycle and interannual variability of the convective moistening efficiency. We show that the NA anticyclone and tropical upper tropospheric temperature determine how much deep convection moistens the lower stratosphere.
The number concentration of droplets in clouds in the summertime in the southeastern United States is influenced by aerosol variations but limited by the strong competition for supersaturated water vapor. Concurrent variations in vertical velocity magnify the response of cloud droplet number to aerosol increases by up to a factor of 5. Omitting the covariance of vertical velocity with aerosol number may therefore bias estimates of the cloud albedo effect from aerosols.
Detection of the planetary boundary layer (PBL) height is crucial to various fields, from air pollution assessment to weather prediction. We examined the diurnal summer PBL height by eight ceilometers in Israel, radiosonde profiles, the global IFS, and regional COSMO models. Our analysis utilized the bulk Richardson number method, the parcel method, and the wavelet covariance transform method. A novel correction tool to improve model results against in-situ ceilometer measurements is introduced.
The paper presents and evaluates a transport analysis method to study the convective injection of air in the upper troposphere–lower stratosphere of the Asian monsoon anticyclone region. The approach is thereby used to analyse the trace gas data collected during the StratoClim aircraft campaign. The results showed that fresh convective air can be injected fast at a high level of the atmosphere (above 17 km), with potential impacts on the stratospheric chemistry of the Northern Hemisphere.
Haze events in early winter in North China exhibited rapid growth after 2010, which was completely different from the slow decline observed before 2010. However, global warming and anthropogenic emissions could not explain this trend reversal well, which was puzzling. Our study found that four climate factors, exhibiting completely opposite trends before and after 2010, effectively drove the trend reversal of the haze pollution in North China.
Cloud water pH affects atmospheric chemistry, and acid rain damages ecosystems. We use model simulations along with observations to present a global view of cloud water and precipitation pH. Sulfuric acid, nitric acid, and ammonia control the pH in the northern midlatitudes, but carboxylic acids and dust cations are important in the tropics and subtropics. The acid inputs to many nitrogen-saturated ecosystems are high enough to cause acidification, with ammonium as the main acidifying species.
We determined decennial statistical time trends and diurnal statistical patterns of atmospheric particle number concentrations in various relevant size fractions in the city centre of Budapest in an interval of 2008–2018. The mean overall decrease rate of particles in different size fractions was approximately −5 % scaled for the 10-year measurement interval. The decline can be interpreted as a consequence of the decreased anthropogenic emissions in the city.
In this study we evaluated the model performances for simulating secondary inorganic aerosol (SIA) and organic aerosol (OA) in PM2.5 in China against comprehensive datasets. The potential biases from factors related to meteorology, emission, chemistry, and atmospheric removal are systematically investigated. This study provides a comprehensive understanding of modeling PM2.5, which is important for studies on the effectiveness of emission control strategies.
In this study, we present spatial distributions of occurrence frequency of enhanced total BrO column and various meteorological parameters affecting it in the Arctic and Antarctic sea ice regions by using 10 years of GOME-2 measurements and meteorological model data. Statistical analysis using the long-term dataset shows clear differences in the meteorological conditions between the mean field and the situation of enhanced total BrO columns in both polar sea ice regions.
Airborne lidar measurements in the vicinity of Barbados are used to investigate radiative effects of long-range-transported Saharan air layers. Derived atmospheric heating rates indicate that observed enhanced water vapor concentrations inside these layers are the main drivers for dust vertical mixing inside the layers. Additionally, they may play a major role for the suppression of subjacent convective cloud development.
Lei Zhu, Gonzalo González Abad, Caroline R. Nowlan, Christopher Chan Miller, Kelly Chance, Eric C. Apel, Joshua P. DiGangi, Alan Fried, Thomas F. Hanisco, Rebecca S. Hornbrook, Lu Hu, Jennifer Kaiser, Frank N. Keutsch, Wade Permar, Jason M. St. Clair, and Glenn M. Wolfe
We develop a validation platform for satellite HCHO retrievals using in situ observations from 12 aircraft campaigns. The platform offers an alternative way to quickly assess systematic biases in HCHO satellite products over large domains and long periods, facilitating optimization of retrieval settings and the minimization of retrieval biases. Application to the NASA operational HCHO product indicates that relative biases range from −44.5 % to +112.1 % depending on locations and seasons.
Aviation-attributed nitrogen oxide (NOx) emissions lead to an increase in ozone and a depletion of methane. We investigate the impact of weather-related transport processes on these induced composition changes. Subsidence in high-pressure systems leads to earlier ozone maxima due to an enhanced chemical activity. Background NOx and hydroperoxyl radicals limit the total ozone change during summer and winter, respectively. High water vapour concentrations lead to a high methane depletion.
The presented study reports on airborne measurements of formaldehyde, glyoxal, methylglyoxal, and CO over the Amazon basin and lays a special focus on the influence of biomass burning emissions on the atmospheric profiles of these carbonyl compounds within the planetary boundary layer as well as in the free and upper troposphere.