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- ItemHighly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol(Washington, DC : ACS Publ., 2019) Bianchi, Federico; Kurtén, Theo; Riva, Matthieu; Mohr, Claudia; Rissanen, Matti P.; Roldin, Pontus; Berndt, Torsten; Crounse, John D.; Wennberg, Paul O.; Mentel, Thomas F.; Wildt, Jürgen; Junninen, Heikki; Jokinen, Tuija; Kulmala, Markku; Worsnop, Douglas R.; Thornton, Joel A.; Donahue, Neil; Kjaergaard, Henrik G.; Ehn, MikaelHighly oxygenated organic molecules (HOM) are formed in the atmosphere via autoxidation involving peroxy radicals arising from volatile organic compounds (VOC). HOM condense on pre-existing particles and can be involved in new particle formation. HOM thus contribute to the formation of secondary organic aerosol (SOA), a significant and ubiquitous component of atmospheric aerosol known to affect the Earth's radiation balance. HOM were discovered only very recently, but the interest in these compounds has grown rapidly. In this Review, we define HOM and describe the currently available techniques for their identification/quantification, followed by a summary of the current knowledge on their formation mechanisms and physicochemical properties. A main aim is to provide a common frame for the currently quite fragmented literature on HOM studies. Finally, we highlight the existing gaps in our understanding and suggest directions for future HOM research. © 2019 American Chemical Society.
- ItemFrom biota to chemistry and climate: Towards a comprehensive description of trace gas exchange between the biosphere and atmosphere(München : European Geopyhsical Union, 2010) Arneth, A.; Sitch, S.; Bondeau, A.; Butterbach-Bahl, K.; Foster, P.; Gedney, N.; de Noblet-Ducoudré, N.; Prentice, I.C.; Sanderson, M.; Thonicke, K.; Wania, R.; Zaehle, S.Exchange of non-CO2 trace gases between the land surface and the atmosphere plays an important role in atmospheric chemistry and climate. Recent studies have highlighted its importance for interpretation of glacial-interglacial ice-core records, the simulation of the pre-industrial and present atmosphere, and the potential for large climate-chemistry and climate-aerosol feedbacks in the coming century. However, spatial and temporal variations in trace gas emissions and the magnitude of future feedbacks are a major source of uncertainty in atmospheric chemistry, air quality and climate science. To reduce such uncertainties Dynamic Global Vegetation Models (DGVMs) are currently being expanded to mechanistically represent processes relevant to non-CO2 trace gas exchange between land biota and the atmosphere. In this paper we present a review of important non-CO2 trace gas emissions, the state-of-the-art in DGVM modelling of processes regulating these emissions, identify key uncertainties for global scale model applications, and discuss a methodology for model integration and evaluation.
- ItemCauses and importance of new particle formation in the present-day and preindustrial atmospheres(Hoboken, NJ : Wiley, 2017) Gordon, Hamish; Kirkby, Jasper; Baltensperger, Urs; Bianchi, Federico; Breitenlechner, Martin; Curtius, Joachim; Dias, Antonio; Dommen, Josef; Donahue, Neil M.; Dunne, Eimear M.; Duplissy, Jonathan; Ehrhart, Sebastian; Flagan, Richard C.; Frege, Carla; Fuchs, Claudia; Hansel, Armin; Hoyle, Christopher R.; Kulmala, Markku; Kürten, Andreas; Lehtipalo, Katrianne; Makhmutov, Vladimir; Molteni, Ugo; Rissanen, Matti P.; Stozkhov, Yuri; Tröstl, Jasmin; Tsagkogeorgas, Georgios; Wagner, Robert; Williamson, Christina; Wimmer, Daniela; Winkler, Paul M.; Yan, Chao; Carslaw, Ken S.New particle formation has been estimated to produce around half of cloud-forming particles in the present-day atmosphere, via gas-to-particle conversion. Here we assess the importance of new particle formation (NPF) for both the present-day and the preindustrial atmospheres. We use a global aerosol model with parametrizations of NPF from previously published CLOUD chamber experiments involving sulfuric acid, ammonia, organic molecules, and ions. We find that NPF produces around 67% of cloud condensation nuclei at 0.2% supersaturation (CCN0.2%) at the level of low clouds in the preindustrial atmosphere (estimated uncertainty range 45–84%) and 54% in the present day (estimated uncertainty range 38–66%). Concerning causes, we find that the importance of biogenic volatile organic compounds (BVOCs) in NPF and CCN formation is greater than previously thought. Removing BVOCs and hence all secondary organic aerosol from our model reduces low-cloud-level CCN concentrations at 0.2% supersaturation by 26% in the present-day atmosphere and 41% in the preindustrial. Around three quarters of this reduction is due to the tiny fraction of the oxidation products of BVOCs that have sufficiently low volatility to be involved in NPF and early growth. Furthermore, we estimate that 40% of preindustrial CCN0.2% are formed via ion-induced NPF, compared with 27% in the present day, although we caution that the ion-induced fraction of NPF involving BVOCs is poorly measured at present. Our model suggests that the effect of changes in cosmic ray intensity on CCN is small and unlikely to be comparable to the effect of large variations in natural primary aerosol emissions.
- ItemInterfacial photochemistry at the ocean surface is a global source of organic vapors and aerosols([London] : Nature Publishing Group UK, 2018) Brüggemann, Martin; Hayeck, Nathalie; George, ChristianThe surface of the oceans acts as a global sink and source for trace gases and aerosol particles. Recent studies suggest that photochemical reactions at this air/water interface produce organic vapors, enhancing particle formation in the atmosphere. However, current model calculations neglect this abiotic source of reactive compounds and account only for biological emissions. Here we show that interfacial photochemistry serves as a major abiotic source of volatile organic compounds (VOCs) on a global scale, capable to compete with emissions from marine biology. Our results indicate global emissions of 46.4-184 Tg C yr-1 of organic vapors from the oceans into the marine atmosphere and a potential contribution to organic aerosol mass of more than 60% over the remote ocean. Moreover, we provide global distributions of VOC formation potentials, which can be used as simple tools for field studies to estimate photochemical VOC emissions depending on location and season.
- ItemArctic haze over Central Europe(Milton Park : Taylor & Francis, 2017) Heintzenberg, Jost; Tuch, Thomas; Wehner, Birgit; Wiedensohler, Alfred; Wex, Heike; Ansmann, Albert; Mattis, Ina; Müller, Detlef; Wendisch, Manfred; Eckhardt, Sabine; Stohl, AndreasAn extraordinary aerosol situation over Leipzig, Germany in April 2002 was investigated with a comprehensive set of ground-based volumetric and columnar aerosol data, combined with aerosol profiles from lidar, meteorological data from radiosondes and air mass trajectory calculations. Air masses were identified to stem from the Arctic, partly influenced by the greater Moscow region. An evaluation of ground-based measurements of aerosol size distributions during these periods showed that the number concentrations below about 70 nm in diameter were below respective long-term average data, while number, surface and volume concentrations of the particles larger than about 70 nm in diameter were higher than the long-term averages. The lidar aerosol profiles showed that the imported aerosol particles were present up to about 3 km altitude. The particle optical depth was up to 0.45 at 550 nm wavelength. With a one-dimensional spectral radiative transfer model top of the atmosphere (TOA) radiative forcing of the aerosol layer was estimated for a period with detailed vertical information. Solar aerosol radiative forcing values between −23 and −38 W m−2 were calculated, which are comparable to values that have been reported in heavily polluted continental plumes outside the respective source regions. The present report adds weight to previous findings of aerosol import to Europe, pointing to the need for attributing the three-dimensional aerosol burden to natural and anthropogenic sources as well as to aerosol imports from adjacent or distant source regions. In the present case, the transport situation is further complicated by forward trajectories, indicating that some of the observed Arctic haze may have originated in Central Europe. This aerosolwas transported to the European Arctic before being re-imported in the modified and augmented form to its initial source region.