Clarifying the Dominant Sources and Mechanisms of Cirrus Cloud Formation
14 Jun 2013-Science (American Association for the Advancement of Science)-Vol. 340, Iss: 6138, pp 1320-1324
TL;DR: Results demonstrate that mineral dust and metallic particles are the dominant source of residual particles, whereas sulfate and organic particles are underrepresented, and elemental carbon and biological materials are essentially absent.
Abstract: Formation of cirrus clouds depends on the availability of ice nuclei to begin condensation of atmospheric water vapor. Although it is known that only a small fraction of atmospheric aerosols are efficient ice nuclei, the critical ingredients that make those aerosols so effective have not been established. We have determined in situ the composition of the residual particles within cirrus crystals after the ice was sublimated. Our results demonstrate that mineral dust and metallic particles are the dominant source of residual particles, whereas sulfate and organic particles are underrepresented, and elemental carbon and biological materials are essentially absent. Further, composition analysis combined with relative humidity measurements suggests that heterogeneous freezing was the dominant formation mechanism of these clouds.
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California Institute of Technology1, University of Washington2, University of Leeds3, University of Manchester4, Colorado State University5, National Academies6, National Oceanic and Atmospheric Administration7, Pacific Northwest National Laboratory8, University of California, Irvine9, Goddard Space Flight Center10, University of California, San Diego11, Foundation for Research & Technology – Hellas12, University of Michigan13, Hebrew University of Jerusalem14
TL;DR: This work suggests strategies for improving estimates of aerosol−cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.
Abstract: The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth’s clouds is the most uncertain component of the overall global radiative forcing from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol−cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol−cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol−cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.
475 citations
University of Leeds1, University of Toronto2, Stony Brook University3, University of Essex4, Pacific Northwest National Laboratory5, University of Denver6, University of British Columbia7, University of Manchester8, Fisheries and Oceans Canada9, Environment Canada10, Leibniz Institute for Baltic Sea Research11
TL;DR: It is shown that organic material in the sea surface microlayer nucleates ice under conditions relevant for mixed-phase cloud and high-altitude ice cloud formation, and suggested that marine organic material may be an important source of ice-nucleating particles in remote marine environments.
Abstract: The amount of ice present in clouds can affect cloud lifetime, precipitation and radiative properties. The formation of ice in clouds is facilitated by the presence of airborne ice-nucleating particles. Sea spray is one of the major global sources of atmospheric particles, but it is unclear to what extent these particles are capable of nucleating ice. Sea-spray aerosol contains large amounts of organic material that is ejected into the atmosphere during bubble bursting at the organically enriched sea-air interface or sea surface microlayer. Here we show that organic material in the sea surface microlayer nucleates ice under conditions relevant for mixed-phase cloud and high-altitude ice cloud formation. The ice-nucleating material is probably biogenic and less than approximately 0.2 micrometres in size. We find that exudates separated from cells of the marine diatom Thalassiosira pseudonana nucleate ice, and propose that organic material associated with phytoplankton cell exudates is a likely candidate for the observed ice-nucleating ability of the microlayer samples. Global model simulations of marine organic aerosol, in combination with our measurements, suggest that marine organic material may be an important source of ice-nucleating particles in remote marine environments such as the Southern Ocean, North Pacific Ocean and North Atlantic Ocean.
472 citations
TL;DR: This work addresses air contaminants and their multiphase chemical interactions at the atmosphere−biosphere interface, including human lungs and skin, plant leaves, cryptogamic covers, soil, and aquatic surfaces, and the chemical interactions of reactive oxygen species and reactive nitrogen species, as well as carbonaceous combustion aerosols.
Abstract: This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited. Review pubs.acs.org/CR Multiphase Chemistry at the Atmosphere−Biosphere Interface Influencing Climate and Public Health in the Anthropocene Ulrich Po schl* and Manabu Shiraiwa* Multiphase Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany air contaminants (SHCC) and their multiphase chemical interactions at the atmosphere−biosphere interface, including human lungs and skin, plant leaves, cryptogamic covers, soil, and aquatic surfaces. After an overview of different groups of SHCC, we address the chemical interactions of reactive oxygen species and reactive nitrogen species (ROS, RNS), primary biological and secondary organic aerosols (PBA, SOA), as well as carbonaceous combustion aerosols (CCA) including soot, black/elemental carbon, polycyclic aromatic hydrocarbons, and related compounds (PAH, PAC). ROS and RNS interact strongly with other SHCC and are central to both atmospheric and physiological processes and their coupling through the atmosphere−biosphere interface, for example, in the formation and aging of biogenic and combustion aerosols as well as in CONTENTS inflammatory and allergic immune responses triggered by air pollution. Deposition of atmospheric ROS/RNS and aerosols 1. Introduction and Motivation can damage biological tissues, modify surface microbiomes, and 2. Health- and Climate-Relevant Air Contaminants induce oxidative stress through Fenton-like reactions and 2.1. Reactive Oxygen and Nitrogen Species immune responses. The chemical mechanisms and kinetics are 2.2. Primary Biological Aerosols not yet fully elucidated, but the available evidence suggests that 2.3. Secondary Organic Aerosols multiphase processes are crucial for the assessment, prediction, 2.4. Carbonaceous Combustion Aerosols and handling of air quality, climate, and public health. Caution 2.5. Other Air Contaminants Linking Atmospher- should be taken to avoid that human activities shaping the ic and Physiological Chemistry Anthropocene create a hazardous or pathogenic atmosphere 3. Multiphase Chemical Reactions at Specific Bio- overloaded with allergenic, corrosive, toxic, or infectious logical Interfaces contaminants. 3.1. Lung Lining Fluid Multiphase chemistry deals with chemical reactions, trans- 3.2. Human Skin port processes, and transformations between gaseous, liquid, 3.3. Plant Surfaces and Cryptogamic Covers and solid matter. These processes are essential for Earth system 3.4. Soil and Aquatic Surfaces science and climate research as well as for life and health 4. Conclusions and Outlook sciences on molecular and global levels, bridging a wide range Author Information of spatial and temporal scales from below nanometers to Corresponding Authors thousands of kilometers and from less than nanoseconds to Notes years and millennia as illustrated in Figure 1. Biographies From a chemical perspective, life and the metabolism of most Acknowledgments living organisms can be regarded as multiphase processes References involving gases like oxygen and carbon dioxide; liquids like water, blood, lymph, and plant sap; and solid or semisolid substances like bone, tissue, skin, wood, and cellular 1. INTRODUCTION AND MOTIVATION membranes. Even primitive forms of life and metabolic activity Multiphase chemistry plays a vital role in the Earth system, under anaerobic conditions generally involve multiple liquid climate, and health. Chemical reactions, mass transport, and and solid or semisolid phases structured by cells, organelles, and phase transitions between gases, liquids, and solids are essential membranes. 2 On global scales, the biogeochemical cycling of for the interaction and coevolution of life and climate. chemical compounds and elements, which can be regarded as Knowledge of the mechanisms and kinetics of these processes the metabolism of planet Earth, also involves chemical is also required to address societally relevant questions of global reactions, mass transport, and phase transitions within and environmental change and public health in the Anthropocene, that is, in the present era of globally pervasive and steeply Special Issue: 2015 Chemistry in Climate increasing human influence on planet Earth. 1 In this work, we review the current scientific understanding and recent advances Received: September 1, 2014 in the investigation of short-lived health- and climate-relevant Published: April 9, 2015 © 2015 American Chemical Society DOI: 10.1021/cr500487s Chem. Rev. 2015, 115, 4440−4475
449 citations
TL;DR: A review of recent theoretical studies and important mechanisms on aerosol-cloud interactions is presented in this article, which discusses the significances of aerosol impacts on radiative forcing and precipitation extremes associated with different cloud systems.
Abstract: Over the past decade, the number of studies that investigate aerosol–cloud interactions has increased considerably. Although tremendous progress has been made to improve the understanding of basic physical mechanisms of aerosol–cloud interactions and reduce their uncertainties in climate forcing, there is still poor understanding of 1) some of the mechanisms that interact with each other over multiple spatial and temporal scales, 2) the feedbacks between microphysical and dynamical processes and between local-scale processes and large-scale circulations, and 3) the significance of cloud–aerosol interactions on weather systems as well as regional and global climate. This review focuses on recent theoretical studies and important mechanisms on aerosol–cloud interactions and discusses the significances of aerosol impacts on radiative forcing and precipitation extremes associated with different cloud systems. The authors summarize the main obstacles preventing the science from making a leap—for exampl...
437 citations
TL;DR: In this paper, new developments in identifying the heterogeneous freezing mechanisms, atmospheric relevance, uncertainties, and unknowns about ice nucleating particles (INPs) have been described, and the change in conventional wisdom regarding the requirements of INPs as new studies discover physical and chemical properties of these particles is explained.
Abstract: Ice particle formation in tropospheric clouds significantly changes cloud radiative and microphysical properties. Ice nucleation in the troposphere via homogeneous freezing occurs at temperatures lower than −38°C and relative humidity with respect to ice above 140%. In the absence of these conditions, ice formation can proceed via heterogeneous nucleation aided by aerosol particles known as ice nucleating particles (INPs). In this chapter, new developments in identifying the heterogeneous freezing mechanisms, atmospheric relevance, uncertainties, and unknowns about INPs are described. The change in conventional wisdom regarding the requirements of INPs as new studies discover physical and chemical properties of these particles is explained. INP sources and known reasons for their ice nucleating properties are presented. The need for more studies to systematically identify particle properties that facilitate ice nucleation is highlighted. The atmospheric relevance of long-range transport, aerosol a...
437 citations
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TL;DR: In this article, the authors focus on one major aspect of cloud microphysics, which involves the processes that lead to the formation of individual cloud and precipitation particles, and provide an account of the major characteristics of atmospheric aerosol particles.
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Abstract: Cause, conseguenze e strategie di mitigazione Proponiamo il primo di una serie di articoli in cui affronteremo l’attuale problema dei mutamenti climatici. Presentiamo il documento redatto, votato e pubblicato dall’Ipcc - Comitato intergovernativo sui cambiamenti climatici - che illustra la sintesi delle ricerche svolte su questo tema rilevante.
4,187 citations
"Clarifying the Dominant Sources and..." refers background in this paper
...The effect of clouds on the climate system is more uncertain than the influence of heat-trapping greenhouse gases (1)....
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...fluence on the rate and direction of evolutionary change (1, 2)....
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