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  • 1
    Publication Date: 2017-04-17
    Description: This work is motivated by previous studies of transatlantic transport of Saharan dust and the observed quasi-static nature of coarse mode aerosol with a volume median diameter (VMD) of approximately 3.5 μm. The authors examine coarse mode contributions from transpacific transport of dust to North American aerosol properties using a dataset collected at the high-elevation Storm Peak Laboratory (SPL) and the nearby Atmospheric Radiation Measurement (ARM) Mobile Facility. Collected ground-based data are complemented by quasi-global model simulations and satellite and ground-based observations. The authors identify a major dust event associated mostly with a transpacific plume (about 65% of near-surface aerosol mass) in which the coarse mode with moderate (~3 μm) VMD is distinct and contributes substantially to total aerosol volume (up to 70%) and scattering (up to 40%). The results demonstrate that the identified plume at the SPL site has a considerable fraction of supermicron particles (VMD ~3 μm) and, thus, suggest that these particles have a fairly invariant behavior despite transpacific transport. If confirmed in additional studies, this invariant behavior may simplify considerably parameterizations for size-dependent processes associated with dust transport and removal.
    Print ISSN: 0022-4928
    Electronic ISSN: 1520-0469
    Topics: Geography , Geosciences , Physics
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  • 2
  • 3
    Publication Date: 2008-05-30
    Description: Data taken from the MCMA-2003 and the 2006 MILAGRO field campaigns are used to examine the absorption of solar radiation by the organic component of aerosols. Using irradiance data from a Multi-Filter Rotating Shadowband Radiometer (MFRSR) and an actinic flux spectroradiometer (SR), we derive aerosol single scattering albedo, π0,λ, as a function of wavelength, λ. We find that in the near-UV spectral range (250 to 400 nm) π0,λ is much lower compared to π0,λ at 500 nm indicating enhanced absorption in the near-UV range. Absorption by elemental carbon, dust, or gas cannot account for this enhanced absorption leaving the organic part of the aerosol as the only possible absorber. We use data from a surface deployed Aerodyne Aerosol Mass Spectrometer (AMS) along with the inferred π0,λ to estimate the Mass Absorption Cross section (MAC) for the organic carbon. We find that the MAC is about 10.5 m2/g at 300 nm and falls close to zero at about 500 nm; values that are roughly consistent with other estimates of organic carbon MAC. These MAC values can be considered as "radiatively correct" because when used in radiative transfer calculations the calculated irradiances/actinic fluxes match those measured at the wavelengths considered here. For an illustrative case study described here, we estimate that the light absorption by the "brown" (organic) carbonaceous aerosol can add about 40% to the light absorption of black carbon in Mexico City. This contribution will vary depending on the relative abundance of organic carbon relative to black carbon. Furthermore, our analysis indicates that organic aerosol would slow down photochemistry by selectively scavenging the light reaching the ground at those wavelengths that drive photochemical reactions. Finally, satellite retrievals of trace gases that are used to infer emissions currently assume that the MAC of organic carbon is zero. For trace gases that are retrieved using wavelengths shorter then 420 nm (i.e. SO2, HCHO, halogenoxides, NO2), the assumption of non-zero MAC values will induce an upward correction to the inferred emissions. This will be particularly relevant in polluted urban atmospheres and areas of biomass burning where organic aerosols are particularly abundant.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 4
    Publication Date: 2007-03-27
    Description: During the Mexico City Metropolitan Area (MCMA) field campaign of 2003, measurements of the shortwave radiation field allowed the inference of the black carbon (BC) specific absorption, αλ, defined as the monochromatic absorption cross section per unit mass (with units of m2/g). The averaged values of αλ derived from the method here are either 8.9 m2/g or 8.2 m2/g at 500 nm, depending upon the physical and optical parameters assumed for BC. These results are reasonably consistent with those of Schuster et al. (2005), 9.5 m2/g, and Baumgartner et al. (2002), 7.0 m2/g, both measured at 550 nm. The αλ values reported in this paper should only be considered effective, "radiatively correct" values because when used in radiative transfer calculations the calculated irradiances match the measured irradiances at 500 nm. The specific absorption so defined can assume a wide range of values, depending upon: (1) the assumptions made prior to the retrieval (e.g., shell/core aerosol configuration), and (2) values chosen for BC density and refractive index. The range of possible values is large, corresponding to a "worst case" uncertainty of about ±70%, assuming that all errors are additive and of the same sign so that no error cancellation occurs.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 5
    Publication Date: 2011-06-09
    Description: Much of the large uncertainty in estimates of anthropogenic aerosol effects on climate arises from the multi-scale nature of the interactions between aerosols, clouds and dynamics, which are difficult to represent in conventional general circulation models (GCMs). In this study, we use a multi-scale aerosol-climate model that treats aerosols and clouds across multiple scales to study aerosol indirect effects. This multi-scale aerosol-climate model is an extension of a multi-scale modeling framework (MMF) model that embeds a cloud-resolving model (CRM) within each vertical column of a GCM grid. The extension allows a more physically-based treatment of aerosol-cloud interactions in both stratiform and convective clouds on the global scale in a computationally feasible way. Simulated model fields, including liquid water path (LWP), ice water path, cloud fraction, shortwave and longwave cloud forcing, precipitation, water vapor, and cloud droplet number concentration are in reasonable agreement with observations. The new model performs quantitatively similar to the previous version of the MMF model in terms of simulated cloud fraction and precipitation. The simulated change in shortwave cloud forcing from anthropogenic aerosols is −0.77 W m−2, which is less than half of that (−1.79 W m−2) calculated by the host GCM (NCAR CAM5) with traditional cloud parameterizations and is also at the low end of the estimates of other conventional global aerosol-climate models. The smaller forcing in the MMF model is attributed to a smaller (3.9 %) increase in LWP from preindustrial conditions (PI) to present day (PD) compared with 15.6 % increase in LWP in stratiform clouds in CAM5. The difference is caused by a much smaller response in LWP to a given perturbation in cloud condensation nuclei (CCN) concentrations from PI to PD in the MMF (about one-third of that in CAM5), and, to a lesser extent, by a smaller relative increase in CCN concentrations from PI to PD in the MMF (about 26 % smaller than that in CAM5). The smaller relative increase in CCN concentrations in the MMF is caused in part by a smaller increase in aerosol lifetime from PI to PD in the MMF, a positive feedback in aerosol indirect effects induced by cloud lifetime effects from aerosols. The smaller response in LWP to anthropogenic aerosols in the MMF model is consistent with observations and with high resolution model studies, which may indicate that aerosol indirect effects simulated in conventional global climate models are overestimated and point to the need to use global high resolution models, such as MMF models or global CRMs, to study aerosol indirect effects. The simulated total anthropogenic aerosol effect in the MMF is −1.05 W m−2, which is close to the Murphy et al. (2009) inverse estimate of −1.1±0.4 W m−2 (1σ) based on the examination of the Earth's energy balance. Further improvements in the representation of ice nucleation and low clouds in MMF are needed to refine the aerosol indirect effect estimate.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 6
    Publication Date: 2008-11-19
    Description: Data taken from the MCMA-2003 and the 2006 MILAGRO field campaigns are used to examine the absorption of solar radiation by the organic component of aerosols. Using irradiance data from a Multi-Filter Rotating Shadowband Radiometer (MFRSR) and an actinic flux spectroradiometer (SR), we derive aerosol single scattering albedo, ϖ0, λ, as a function of wavelength, λ. We find that in the near-UV spectral range (250 to 400 nm) ϖ0, λ is much lower compared to ϖ0, λ at 500 nm indicating enhanced absorption in the near-UV range. Absorption by elemental carbon, dust, or gas cannot account for this enhanced absorption leaving the organic carbon component of the aerosol (OA) as the most likely absorber. We use data from a surface deployed Aerodyne Aerosol Mass Spectrometer (AMS) along with the inferred ϖ0, λ to estimate the Mass Absorption Cross section (MAC) for the organic aerosol. We find that the MAC is about 10.5 m2/g at 300 nm and falls close to zero at about 500 nm; values that are roughly consistent with other estimates of organic aerosol MAC. These MAC values can be considered as "radiatively correct", because when used in radiative transfer calculations, the calculated irradiances/actinic fluxes match those measured at the wavelengths considered here. For an illustrative case study described here, we estimate that the light absorption by the "brown" (organic) carbonaceous aerosol can add about 40% to the light absorption of black carbon in Mexico City. This contribution will vary depending on the relative abundance of organic aerosol relative to black carbon. Furthermore, our analysis indicates that organic aerosol would slow down photochemistry by selectively scavenging the light reaching the ground at those wavelengths that drive photochemical reactions. Finally, satellite retrievals of trace gases that are used to infer emissions currently assume that the MAC of organic carbon is zero. For trace gases that are retrieved using wavelengths shorter then 420 nm (i.e. SO2, HCHO, halogenoxides, NO2), the assumption of non-zero MAC values will induce an upward correction to the inferred emissions. This assumption will be particularly relevant in polluted urban atmospheres and areas of biomass burning where organic aerosols are particularly abundant.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 7
    Publication Date: 2007-06-27
    Description: Multi-filter Rotating Shadowband Radiometers (MFRSRs) provide routine measurements of the aerosol optical depth (τ) at six wavelengths (0.415, 0.5, 0.615, 0.673, 0.870 and 0.94 μm). The single-scattering albedo (π0) is typically estimated from the MFRSR measurements by assuming the asymmetry parameter (g). In most instances, however, it is not easy to set an appropriate value of g due to its strong temporal and spatial variability. Here, we introduce and validate an updated version of our retrieval technique that allows one to estimate simultaneously π0 and g for different types of aerosol. We use the aerosol and radiative properties obtained during the Atmospheric Radiation Measurement (ARM) Program's Aerosol Intensive Operational Period (IOP) to validate our retrieval in two ways. First, the MFRSR-retrieved optical properties are compared with those obtained from independent surface, Aerosol Robotic Network (AERONET), and aircraft measurements. The MFRSR-retrieved optical properties are in reasonable agreement with these independent measurements. Second, we perform radiative closure experiments using the MFRSR-retrieved optical properties. The calculated broadband values of the direct and diffuse fluxes are comparable (~5 W/m2) to those obtained from measurements.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 8
    Publication Date: 2007-03-23
    Description: As part of a major atmospheric chemistry and aerosol field program carried out in March 2006, a study was conducted in the area to the north and northeast of Mexico City to investigate the evolution of aerosols and their associated optical properties in the first few hours after their emission. The focus of the T1-T2 aerosol study was to investigate changes in the specific absorption αABS (absorption per unit mass, with unit of m2 g−1) of black carbon as it aged and became coated with compounds such as sulfate and organic carbon, evolving from an external to an internal mixture. Such evolution has been reported in previous studies. The T1 site was located just to the north of the Mexico City metropolitan area; the T2 site was situated approximately 35 km farther to the northeast. Nephelometers, particle soot absorption photometers, photoacoustic absorption spectrometers, and organic and elemental carbon analyzers were used to measure the optical properties of the aerosols and the carbon concentrations at each of the sites. Radar wind profilers and radiosonde systems helped to characterize the meteorology and to identify periods when transport from Mexico City over T1 and T2 occurred. Organic and elemental carbon concentrations at T1 showed diurnal cycles reflecting the nocturnal and early morning buildup from nearby sources, while concentrations at T2 appeared to be more affected by transport from Mexico City. Specific absorption during transport periods was lower than during other times, consistent with the likelihood of fresher emissions being found when the winds blew from Mexico City over T1 and T2. The specific absorption at T2 was larger than at T1, which is also consistent with the expectation of more aged particles with encapsulated black carbon being found at the more distant location. In situ measurements of single scattering albedo with an aircraft and a ground station showed general agreement with column-averaged values derived from rotating shadowband radiometer data, although some differences were found that may be related to boundary-layer evolution.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 9
    Publication Date: 2012-08-22
    Description: Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program's Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites – one within the Sacramento urban area and another about 40 km to the northeast in the foothills area – were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climate-related properties in freshly polluted and "aged" urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: (a) the scientific background and motivation for the study, (b) the operational and logistical information pertinent to the execution of the study, (c) an overview of key observations and initial findings from the aircraft and ground-based sampling platforms, and (d) a roadmap of planned data analyses and focused modeling efforts that will facilitate the integration of new knowledge into improved representations of key aerosol processes and properties in climate models.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 10
    Publication Date: 2011-01-31
    Description: Much of the large uncertainty in estimates of anthropogenic aerosol effects on climate arises from the multi-scale nature of the interactions between aerosols, clouds and large-scale dynamics, which are difficult to represent in conventional global climate models (GCMs). In this study, we use a multi-scale aerosol-climate model that treats aerosols and clouds across multiple scales to study aerosol indirect effects. This multi-scale aerosol-climate model is an extension of a multi-scale modeling framework (MMF) model that embeds a cloud-resolving model (CRM) within each grid cell of a GCM. The extension allows the explicit simulation of aerosol/cloud interactions in both stratiform and convective clouds on the global scale in a computationally feasible way. Simulated model fields, including liquid water path (LWP), ice water path, cloud fraction, shortwave and longwave cloud forcing, precipitation, water vapor, and cloud droplet number concentration are in agreement with observations. The new model performs quantitatively similar to the previous version of the MMF model in terms of simulated cloud fraction and precipitation. The simulated change in shortwave cloud forcing from anthropogenic aerosols is −0.77 W m−2, which is less than half of that in the host GCM (NCAR CAM5) (−1.79 W m−2) and is also at the low end of the estimates of most other conventional global aerosol-climate models. The smaller forcing in the MMF model is attributed to its smaller increase in LWP from preindustrial conditions (PI) to present day (PD): 3.9% in the MMF, compared with 15.6% increase in LWP in large-scale clouds in CAM5. The much smaller increase in LWP in the MMF is caused by a much smaller response in LWP to a given perturbation in cloud condensation nuclei (CCN) concentrations from PI to PD in the MMF (about one-third of that in CAM5), and, to a lesser extent, by a smaller relative increase in CCN concentrations from PI to PD in the MMF (about 26% smaller than that in CAM5). The smaller relative increase in CCN concentrations in the MMF is caused in part by a smaller increase in aerosol lifetime from PI to PD in the MMF, a positive feedback in aerosol indirect effects induced by cloud lifetime effects. The smaller response in LWP to anthropogenic aerosols in the MMF model is consistent with observations and with high resolution model studies, which may indicate that aerosol indirect effects simulated in conventional global climate models are overestimated and point to the need to use global high resolution models, such as MMF models or global CRMs, to study aerosol indirect effects. The simulated total anthropogenic aerosol effect in the MMF is −1.05 W m−2, which is close to the Murphy et al. (2009) inverse estimate of −1.1 ± 0.4 W m−2 (1σ) based on the examination of the Earth's energy balance. Further improvements in the representation of ice nucleation and low clouds are needed.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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