Using Measurements of CCN Activity to Characterize the Mixing State, Chemical Composition, and Droplet Growth Kinetics of Atmospheric Aerosols to Constrain the Aerosol Indirect Effect

Using Measurements of CCN Activity to Characterize the Mixing State, Chemical Composition, and Droplet Growth Kinetics of Atmospheric Aerosols to Constrain the Aerosol Indirect Effect PDF Author: Richard Herbert Moore
Publisher:
ISBN:
Category : Atmospheric aerosols
Languages : en
Pages :

Book Description
Atmospheric aerosols are known to exert a significant influence on the Earth's climate system; however, the magnitude of this influence is highly uncertain because of the complex interaction between aerosols and water vapor to form clouds. Toward reducing this uncertainty, this dissertation outlines a series of laboratory and in-situ field measurements, instrument technique development, and model simulations designed to characterize the ability of aerosols to act as cloud condensation nuclei (CCN) and form cloud droplets. Specifically, we empirically quantify the mixing state and thermodynamic properties of organic aerosols (e.g., hygroscopicity and droplet condensational uptake coefficient) measured in polluted and non-polluted environments including Alaska, California, and Georgia. It is shown that organic aerosols comprise a substantial portion of the aerosol mass and are often water soluble. CCN measurements are compared to predictions from theory in order to determine the error associated with simplified composition and mixing state assumptions employed by current large-scale models, and these errors are used to constrain the uncertainty of global and regional cloud droplet number and albedo using a recently-developed cloud droplet parameterization adjoint coupled with the GMI chemical transport model. These sensitivities are important because they describe the main determinants of climate forcing. We also present two novel techniques for fast measurements of CCN concentrations with high size, supersaturation, and temporal resolution that substantially improve the state of the art by several orders of magnitude. Ultimately, this work represents a step toward better understanding how atmospheric aerosols influence cloud properties and Earth's climate.

The Importance of Aerosol Composition and Mixing State on Predicted CCN Concentration and the Variation of the Importance with Atmospheric Processing of Aerosol

The Importance of Aerosol Composition and Mixing State on Predicted CCN Concentration and the Variation of the Importance with Atmospheric Processing of Aerosol PDF Author:
Publisher:
ISBN:
Category :
Languages : en
Pages :

Book Description
The influences of atmospheric aerosols on cloud properties (i.e., aerosol indirect effects) strongly depend on the aerosol CCN concentrations, which can be effectively predicted from detailed aerosol size distribution, mixing state, and chemical composition using Köhler theory. However, atmospheric aerosols are complex and heterogeneous mixtures of a large number of species that cannot be individually simulated in global or regional models due to computational constraints. Furthermore, the thermodynamic properties or even the molecular identities of many organic species present in ambient aerosols are often not known to predict their cloud-activation behavior using Köhler theory. As a result, simplified presentations of aerosol composition and mixing state are necessary for large-scale models. In this study, aerosol microphysics, CCN concentrations, and chemical composition measured at the T0 urban super-site in Mexico City during MILAGRO are analyzed. During the campaign in March 2006, aerosol size distribution and composition often showed strong diurnal variation as a result of both primary emissions and aging of aerosols through coagulation and local photochemical production of secondary aerosol species. The submicron aerosol composition was ~1/2 organic species. Closure analysis is first carried out by comparing CCN concentrations calculated from the measured aerosol size distribution, mixing state, and chemical composition using extended Köhler theory to concurrent CCN measurements at five supersaturations ranging from 0.11% to 0.35%. The closure agreement and its diurnal variation are studied. CCN concentrations are also derived using various simplifications of the measured aerosol mixing state and chemical composition. The biases associated with these simplifications are compared for different supersaturations, and the variation of the biases is examined as a function of aerosol age. The results show that the simplification of internally mixed, size-independent particle composition leads to substantial overestimation of CCN concentration for freshly emitted aerosols in early morning, but can reasonably predict the CCN concentration after the aerosols underwent atmospheric processing for several hours. This analysis employing various simplifications provides insights into the essential information of particle chemical composition that needs to be represented in models to adequately predict CCN concentration and cloud microphysics.

Quantifying Compositional Impacts of Ambient Aerosol on Cloud Formation

Quantifying Compositional Impacts of Ambient Aerosol on Cloud Formation PDF Author: Sara Lance
Publisher:
ISBN:
Category : Aerosols
Languages : en
Pages :

Book Description
It has been historically assumed that most of the uncertainty associated with the aerosol indirect effect on climate can be attributed to the unpredictability of updrafts. We assess the sensitivity of cloud droplet number density to realistic variations in aerosol chemical properties and to variable updraft velocities using a 1-dimensional cloud parcel model. The results suggest that aerosol chemical variability may be as important to the aerosol indirect effect as the effect of unresolved cloud dynamics, especially in polluted environments. We next used a continuous flow streamwise thermal gradient Cloud Condesnation Nuclei counter (CCNc) to study the water-uptake properties of the ambient aerosol, by exposing an aerosol sample to a controlled water vapor supersaturation and counting the resulting number of droplets. The heat transfer properties and droplet growth within the CCNc were first modeled and experimentally characterized. We describe results from the MIRAGE field campaign at a ground-based site during March, 2006. Size-resolved CCN activation spectra and hygroscopic growth factor distributions of the ambient aerosol in Mexico City were obtained, and an analytical technique was developed to quantify a probability distribution of solute volume fractions for the CCN, as well as the aerosol mixing-state. The CCN were shown to be much less CCN active than ammonium sulfate, with water uptake properties more consistent with low molecular weight organic compounds. We also describe results from the GoMACCS field study, an airborne field campaign in Houston, Texas during August-September, 2006. GoMACCS tested our ability to predict CCN for highly polluted conditions with limited chemical information. Assuming the particles were composed purely of ammonium sulfate, CCN closure was obtained with a 10% overprediction bias on average for CCN concentrations ranging from less than 100 cm-3 to over 10,000 cm-3, but with on average 50% variability. Assuming measured concentrations of organics to be internally mixed and insoluble tended to reduce the overprediction bias for less polluted conditions, but led to underprediction bias in the most polluted conditions. Comparing the two campaigns, it is clear that the chemistry of the particles plays an important role in our ability to predict CCN concentrations.

Microphysics of Clouds and Precipitation

Microphysics of Clouds and Precipitation PDF Author: H.R. Pruppacher
Publisher: Springer Science & Business Media
ISBN: 0306481006
Category : Science
Languages : en
Pages : 975

Book Description
Cloud physics has achieved such a voluminous literature over the past few decades that a significant quantitative study of the entire field would prove unwieldy. This book concentrates on one major aspect: cloud microphysics, which involves the processes that lead to the formation of individual cloud and precipitation particles. Common practice has shown that one may distinguish among the following addi tional major aspects: cloud dynamics, which is concerned with the physics respon sible for the macroscopic features of clouds; cloud electricity, which deals with the electrical structure of clouds and the electrification processes of cloud and precipi tation particles; and cloud optics and radar meteorology, which describe the effects of electromagnetic waves interacting with clouds and precipitation. Another field intimately related to cloud physics is atmospheric chemistry, which involves the chemical composition ofthe atmosphere and the life cycle and characteristics of its gaseous and particulate constituents. In view of the natural interdependence of the various aspects of cloud physics, the subject of microphysics cannot be discussed very meaningfully out of context. Therefore, we have found it necessary to touch briefly upon a few simple and basic concepts of cloud dynamics and thermodynamics, and to provide an account of the major characteristics of atmospheric aerosol particles. We have also included a separate chapter on some of the effects of electric fields and charges on the precipitation-forming processes.

Nucleation and Atmospheric Aerosols

Nucleation and Atmospheric Aerosols PDF Author: Colin D. O'Dowd
Publisher: Springer Science & Business Media
ISBN: 1402064748
Category : Science
Languages : en
Pages : 1275

Book Description
Atmospheric particles are ubiquitous in the atmosphere: they form the seeds for cloud droplets and they form haze layers, blocking out incoming radiation and contributing to a partial cooling of our climate. They also contribute to poor air quality and health impacts. A large fraction of aerosols are formed from nucleation processes – that is a phase transition from vapour to liquid or solid particles. Examples are the formation of stable clusters about 1 nm in size from molecular collisions and these in turn can grow into larger (100 nm or more) haze particles via condensation to the formation of ice crystals in mixed phase or cold clouds. This book brings together the leading experts from the nucleation and atmospheric aerosols research communities to present the current state-of-the-art knowledge in these related fields. Topics covered are: Nucleation Experiment & Theory, Binary, Homogeneous and Heterogeneous Nucleation, Ion & Cluster Properties During Nucleation, Aerosol Characterisation & Properties, Aerosol Formation, Dynamics and Growth, Marine Aerosol Production, Aerosol-Cloud Interactions, Chemical Composition & Cloud Drop Activation, Remote Sensing of aerosol & clouds and Air Quality-Climate Interactions

Atmospheric Aerosols

Atmospheric Aerosols PDF Author: Rekha Kale
Publisher: Scitus Academics LLC
ISBN: 9781681171326
Category : Aerosols
Languages : en
Pages : 0

Book Description
Atmospheric Aerosols is a vital problem in current environmental research due to its importance in atmospheric optics, energetics, radiative transfer studies, chemistry, climate, biology and public health. Aerosols can influence the energy balance of the terrestrial atmosphere, the hydrological cycle, atmospheric dynamics and monsoon circulations. Because of the heterogeneous aerosol field with large spatial and temporal variability and reduction in uncertainties in aerosol quantification is a challenging task in atmospheric sciences. Keeping this in view the present study aims to assess the impact of aerosols on coastal Indian station Visakhapatnam and the adjoining Bay of Bengal. An aerosol is a colloid of fine solid particles or liquid droplets, in air or another gas. Aerosols can be natural or not. Examples of natural aerosols are fog, forest exudates and geyser steam.

Aerosol Pollution Impact on Precipitation

Aerosol Pollution Impact on Precipitation PDF Author: Zev Levin
Publisher: Springer Science & Business Media
ISBN: 1402086903
Category : Science
Languages : en
Pages : 399

Book Description
Life on Earth is critically dependent upon the continuous cycling of water between oceans, continents and the atmosphere. Precipitation (including rain, snow, and hail) is the primary mechanism for transporting water from the atmosphere back to the Earth’s surface. It is also the key physical process that links aspects of climate, weather, and the global hydrological cycle. Changes in precipitation regimes and the frequency of extreme weather events, such as floods, droughts, severe ice/snow storms, monsoon fluctuations and hurricanes are of great potential importance to life on the planet. One of the factors that could contribute to precipitation modification is aerosol pollution from various sources such as urban air pollution and biomass burning. Natural and anthropogenic changes in atmospheric aerosols might have important implications for precipitation by influencing the hydrological cycle, which in turn could feed back to climate changes. From an Earth Science perspective, a key question is how changes expected in climate will translate into changes in the hydrological cycle, and what trends may be expected in the future. We require a much better understanding and hence predictive capability of the moisture and energy storages and exchanges among the Earth’s atmosphere, oceans, continents and biological systems. This book is a review of our knowledge of the relationship between aerosols and precipitation reaching the Earth's surface and it includes a list of recommendations that could help to advance our knowledge in this area.

Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles PDF Author:
Publisher:
ISBN:
Category :
Languages : en
Pages : 13

Book Description
Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign and much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol particles: (a) two well-characterized source of soot particles and (b) a flow reactor for controlled OH and/or O3 oxidation of relevant gas phase species to produce well-characterized SOA particles. After formation, the aerosol particles are subjected to physical and chemical processes that simulate aerosol growth and aging. A suite of instruments in our laboratory is used to characterize the physical and chemical properties of aerosol particles before and after processing. The Time of Flight Aerosol Mass Spectrometer (ToF-AMS) together with a Scanning Mobility Particle Sizer (SMPS) measures particle mass, volume, density, composition (including black carbon content), dynamic shape factor, and fractal dimension. The-ToF-AMS was developed at ARI with Boston College participation. About 120 AMS instruments are now in service (including 5 built for DOE laboratories) performing field and laboratory studies world-wide. Other major instruments include a thermal denuder, two Differential Mobility Analyzers (DMA), a Cloud Condensation Nuclei Counter (CCN), a Thermal desorption Aerosol GC/MS (TAG) and the new Soot Particle Aerosol Mass Spectrometer (SP-AMS). Optical instrumentation required for the studies have been brought to our laboratory as part of ongoing and planned collaborative projects with colleagues from DOE, NOAA and university laboratories. Optical instruments that will be utilized include a Photoacoustic Spectrometer (PAS), a Cavity Ring Down Aerosol Extinction Spectrometer (CRD-AES), a Photo Thermal Interferometer (PTI), a new 7-wavelength Aethalometer and a Cavity Attenuated Phase Shift Extinction Monitor (CAPS). These instruments are providing aerosol absorption, extinction and scattering coefficients at a range of atmospherically relevant wavelengths. During the past two years our work has continued along the lines of our original proposal. We report on 12 completed and/or continuing projects conducted during the period 08/14 to 0814/2015. These projects are described in ...

Atmospheric Aerosols

Atmospheric Aerosols PDF Author: Olivier Boucher
Publisher: Springer
ISBN: 9401796491
Category : Science
Languages : en
Pages : 322

Book Description
This textbook aims to be a one stop shop for those interested in aerosols and their impact on the climate system. It starts with some fundamentals on atmospheric aerosols, atmospheric radiation and cloud physics, then goes into techniques used for in-situ and remote sensing measurements of aerosols, data assimilation, and discusses aerosol-radiation interactions, aerosol-cloud interactions and the multiple impacts of aerosols on the climate system. The book aims to engage those interested in aerosols and their impacts on the climate system: graduate and PhD students, but also post-doctorate fellows who are new to the field or would like to broaden their knowledge. The book includes exercises at the end of most chapters. Atmospheric aerosols are small (microscopic) particles in suspension in the atmosphere, which play multiple roles in the climate system. They interact with the energy budget through scattering and absorption of solar and terrestrial radiation. They also serve as cloud condensation and ice nuclei with impacts on the formation, evolution and properties of clouds. Finally aerosols also interact with some biogeochemical cycles. Anthropogenic emissions of aerosols are responsible for a cooling effect that has masked part of the warming due to the increased greenhouse effect since pre-industrial time. Natural aerosols also respond to climate changes as shown by observations of past climates and modelling of the future climate.

Cloud Dynamics

Cloud Dynamics PDF Author: PRUPPACHER
Publisher: Birkhäuser
ISBN:
Category : Juvenile Nonfiction
Languages : en
Pages : 386

Book Description