Author
Chao Yan
Other affiliations: Carnegie Mellon University, Helsinki Institute of Physics, Beijing University of Chemical Technology ...read more
Bio: Chao Yan is an academic researcher from University of Helsinki. The author has contributed to research in topics: Aerosol & Environmental chemistry. The author has an hindex of 31, co-authored 107 publications receiving 3322 citations. Previous affiliations of Chao Yan include Carnegie Mellon University & Helsinki Institute of Physics.
Topics: Aerosol, Environmental chemistry, Haze, Particle, Beijing
Papers
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Paul Scherrer Institute1, Carnegie Mellon University2, CERN3, Goethe University Frankfurt4, University of Helsinki5, Stockholm University6, ETH Zurich7, Earth System Research Laboratory8, Cooperative Institute for Research in Environmental Sciences9, California Institute of Technology10, Helsinki Institute of Physics11, University of Innsbruck12, University of Eastern Finland13, Finnish Meteorological Institute14, National Center for Atmospheric Research15, Karlsruhe Institute of Technology16, University of Leeds17, University of California, Irvine18, University of Vienna19, University of Beira Interior20
TL;DR: It is shown that organic vapours alone can drive nucleation, and a particle growth model is presented that quantitatively reproduces the measurements and implements a parameterization of the first steps of growth in a global aerosol model that can change substantially in response to concentrations of atmospheric cloud concentration nuclei.
Abstract: About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday. Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres. In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles, thereby failing to form new cloud condensation nuclei that are typically 50 to 100 nanometres across. Sulfuric acid vapour is often involved in nucleation but is too scarce to explain most subsequent growth, leaving organic vapours as the most plausible alternative, at least in the planetary boundary layer. Although recent studies predict that low-volatility organic vapours contribute during initial growth, direct evidence has been lacking. The accelerating growth may result from increased photolytic production of condensable organic species in the afternoon, and the presence of a possible Kelvin (curvature) effect, which inhibits organic vapour condensation on the smallest particles (the nano-Kohler theory), has so far remained ambiguous. Here we present experiments performed in a large chamber under atmospheric conditions that investigate the role of organic vapours in the initial growth of nucleated organic particles in the absence of inorganic acids and bases such as sulfuric acid or ammonia and amines, respectively. Using data from the same set of experiments, it has been shown that organic vapours alone can drive nucleation. We focus on the growth of nucleated particles and find that the organic vapours that drive initial growth have extremely low volatilities (saturation concentration less than 10(-4.5) micrograms per cubic metre). As the particles increase in size and the Kelvin barrier falls, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility (saturation concentrations of 10(-4.5) to 10(-0.5) micrograms per cubic metre). We present a particle growth model that quantitatively reproduces our measurements. Furthermore, we implement a parameterization of the first steps of growth in a global aerosol model and find that concentrations of atmospheric cloud concentration nuclei can change substantially in response, that is, by up to 50 per cent in comparison with previously assumed growth rate parameterizations.
507 citations
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Goethe University Frankfurt1, CERN2, University of Helsinki3, Helsinki Institute of Physics4, University of Leeds5, Paul Scherrer Institute6, University of Washington7, University of Innsbruck8, University of Lisbon9, ETH Zurich10, California Institute of Technology11, University of Eastern Finland12, Finnish Meteorological Institute13, Lebedev Physical Institute14, Stockholm University15, University of Vienna16, Leibniz Association17, University of Beira Interior18, Carnegie Mellon University19
TL;DR: Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.
Abstract: Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere, and that ions have a relatively minor role. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.
502 citations
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TL;DR: Investigation of new particle formation in Shanghai found that the observed concentration of sulfuric acid was high enough to explain the particle growth to ~3 nanometers under the very high condensation sink, whereas the subsequent higher growth rate beyond this size is believed to result from the added contribution of condensing organic species.
Abstract: Atmospheric new particle formation (NPF) is an important global phenomenon that is nevertheless sensitive to ambient conditions. According to both observation and theoretical arguments, NPF usually requires a relatively high sulfuric acid (H2SO4) concentration to promote the formation of new particles and a low preexisting aerosol loading to minimize the sink of new particles. We investigated NPF in Shanghai and were able to observe both precursor vapors (H2SO4) and initial clusters at a molecular level in a megacity. High NPF rates were observed to coincide with several familiar markers suggestive of H2SO4-dimethylamine (DMA)-water (H2O) nucleation, including sulfuric acid dimers and H2SO4-DMA clusters. In a cluster kinetics simulation, the observed concentration of sulfuric acid was high enough to explain the particle growth to ~3 nanometers under the very high condensation sink, whereas the subsequent higher growth rate beyond this size is believed to result from the added contribution of condensing organic species. These findings will help in understanding urban NPF and its air quality and climate effects, as well as in formulating policies to mitigate secondary particle formation in China.
387 citations
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TL;DR: The results of the present study provide a scientific basis for the development of PM2.5 control strategies on a regional scale and suggest local emission may be non-negligible at YRDNNR in summer.
190 citations
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University of Leeds1, CERN2, Goethe University Frankfurt3, Paul Scherrer Institute4, University of Helsinki5, Harvard University6, Carnegie Mellon University7, Finnish Meteorological Institute8, Helsinki Institute of Physics9, Max Planck Society10, California Institute of Technology11, University of Innsbruck12, Lebedev Physical Institute13, Leibniz Association14, Cooperative Institute for Research in Environmental Sciences15, University of Vienna16
TL;DR: In this article, the authors assess the importance of new particle formation (NPF) for both the present-day and the pre-industrial atmospheres using a global aerosol model with parametrizations of NPF from previously published CLOUD chamber experiments involving sulfuric acid, ammonia, organic molecules and ions.
Abstract: 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.
186 citations
Cited by
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TL;DR: This work aims to provide a comprehensive overview of electrospun nanofibers, including the principle, methods, materials, and applications, and highlights the most relevant and recent advances related to the applications by focusing on the most representative examples.
Abstract: Electrospinning is a versatile and viable technique for generating ultrathin fibers. Remarkable progress has been made with regard to the development of electrospinning methods and engineering of electrospun nanofibers to suit or enable various applications. We aim to provide a comprehensive overview of electrospinning, including the principle, methods, materials, and applications. We begin with a brief introduction to the early history of electrospinning, followed by discussion of its principle and typical apparatus. We then discuss its renaissance over the past two decades as a powerful technology for the production of nanofibers with diversified compositions, structures, and properties. Afterward, we discuss the applications of electrospun nanofibers, including their use as "smart" mats, filtration membranes, catalytic supports, energy harvesting/conversion/storage components, and photonic and electronic devices, as well as biomedical scaffolds. We highlight the most relevant and recent advances related to the applications of electrospun nanofibers by focusing on the most representative examples. We also offer perspectives on the challenges, opportunities, and new directions for future development. At the end, we discuss approaches to the scale-up production of electrospun nanofibers and briefly discuss various types of commercial products based on electrospun nanofibers that have found widespread use in our everyday life.
2,289 citations
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2,261 citations
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TL;DR: In this paper, an inventory of air pollutant emissions in Asia in the year 2000 is developed to support atmospheric modeling and analysis of observations taken during the TRACE-P experiment funded by the National Aeronautics and Space Administration (NASA) and the ACE-Asia experiment, in which emissions are estimated for all major anthropogenic sources, including biomass burning, in 64 regions of Asia.
Abstract: [i] An inventory of air pollutant emissions in Asia in the year 2000 is developed to support atmospheric modeling and analysis of observations taken during the TRACE-P experiment funded by the National Aeronautics and Space Administration (NASA) and the ACE-Asia experiment funded by the National Science Foundation (NSF) and the National Oceanic and Atmospheric Administration (NOAA). Emissions are estimated for all major anthropogenic sources, including biomass burning, in 64 regions of Asia. We estimate total Asian emissions as follows: 34.3 Tg SO 2 , 26.8 Tg NO x , 9870 Tg CO 2 , 279 Tg CO, 107 Tg CH 4 , 52.2 Tg NMVOC, 2.54 Tg black carbon (BC), 10.4 Tg organic carbon (OC), and 27.5 Tg NH 3 . In addition, NMVOC are speciated into 19 subcategories according to functional groups and reactivity. Thus we are able to identify the major source regions and types for many of the significant gaseous and particle emissions that influence pollutant concentrations in the vicinity of the TRACE-P and ACE-Asia field measurements. Emissions in China dominate the signature of pollutant concentrations in this region, so special emphasis has been placed on the development of emission estimates for China. China's emissions are determined to be as follows: 20.4 Tg SO 2 , 11.4 Tg NO x , 3820 Tg CO 2 , 116 Tg CO, 38.4 Tg CH 4 , 17.4 Tg NMVOC, 1.05 Tg BC, 3.4 Tg OC, and 13.6 Tg NH 3 . Emissions are gridded at a variety of spatial resolutions from 1° × 1° to 30 s x 30 s, using the exact locations of large point sources and surrogate GIS distributions of urban and rural population, road networks, landcover, ship lanes, etc. The gridded emission estimates have been used as inputs to atmospheric simulation models and have proven to be generally robust in comparison with field observations, though there is reason to think that emissions of CO and possibly BC may be underestimated. Monthly emission estimates for China are developed for each species to aid TRACE-P and ACE-Asia data interpretation. During the observation period of March/ April, emissions are roughly at their average values (one twelfth of annual). Uncertainties in the emission estimates, measured as 95% confidence intervals, range from a low of ±16% for SO 2 to a high of ±450% for OC.
1,828 citations
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TL;DR: This review summarizes the main findings from published papers on the characteristics and sources and processes of ozone and ozone precursors in the boundary layer of urban and rural areas of China, including concentration levels, seasonal variation, meteorology conducive to photochemistry and pollution transport, key production and loss processes, ozone dependence on nitrogen oxides and volatile organic compounds, and the effects of ozone on crops and human health.
952 citations