Droplet activation, separation, and compositional analysis: laboratory studies and atmospheric measurements [Discussion paper]

Droplets produced in a cloud condensation nucleus chamber as a function of supersaturation have been separated from unactivated aerosol particles using counterflow virtual impaction. Residual material after droplets were evaporated was chemically analyzed with an Aerodyne Aerosol Mass Spectrometer and the Particle Analysis by Laser Mass Spectrometry instrument. Experiments were initially conducted to verify activation conditions for monodisperse ammonium sulfate particles and to determine the resulting droplet size distribution as a function of supersaturation. Based on the observed droplet size, the counterflow virtual impactor cut-size was set to differentiate droplets from unactivated interstitial particles. Validation experiments were then performed to verify that only droplets with sufficient size passed through the counterflow virtual impactor for subsequent analysis. A two-component external mixture of monodisperse particles was also exposed to a supersaturation which would activate one of the types (ammonium sulfate) but not the other (polystyrene latex spheres). The mass spectrum observed after separation indicated only the former, validating separation of droplets from unactivated particles. Results from atmospheric measurements using this technique indicate that aerosol particles often activate predominantly as a function of particle size. Chemical composition is not irrelevant, however, and we observed enhancement of sulfate in droplet residuals using single particle analysis

Droplet activation, separation, and compositional analysis: laboratory studies and atmospheric measurements

Droplets produced in a cloud condensation nuclei chamber (CCNC) as a function of supersaturation have been separated from unactivated aerosol particles using counterflow virtual impaction. Residual material after droplets were evaporated was chemically analyzed with an Aerodyne Aerosol Mass Spectrometer (AMS) and the Particle Analysis by Laser Mass Spectrometry (PALMS) instrument. Experiments were initially conducted to verify activation conditions for monodisperse ammonium sulfate particles and to determine the resulting droplet size distribution as a function of supersaturation. Based on the observed droplet size, the counterflow virtual impactor cut-size was set to differentiate droplets from unactivated interstitial particles. Validation experiments were then performed to verify that only droplets with sufficient size passed through the counterflow virtual impactor for subsequent analysis. A two-component external mixture of monodisperse particles was also exposed to a supersaturation which would activate one of the types (hygroscopic salts) but not the other (polystyrene latex spheres or adipic acid). The mass spectrum observed after separation indicated only the former, validating separation of droplets from unactivated particles. Results from ambient measurements using this technique and AMS analysis were inconclusive, showing little chemical differentiation between ambient aerosol and activated droplet residuals, largely due to low signal levels. When employing as single particle mass spectrometer for compositional analysis, however, we observed enhancement of sulfate in droplet residuals

Wake Capture, Particle Breakup, and Other Artifacts Associated with Counterflow Virtual Impaction

Counterflow virtual impaction is used to inertially separate cloud elements from inactivated aerosol. Previous airborne, ground-based, and laboratory studies using this technique exhibit artifacts that are not fully explained by the impaction theory. We have performed laboratory studies that show small particles can be carried across the inertial barrier of the counterflow by collision and/or coalescence or riding the wake of larger particles with sufficient inertia. We have also performed theoretical calculations to show that aerodynamic forces associated with the requisite acceleration and deceleration of particles within a counterflow virtual impactor can lead to breakup. The implication of these processes on studies using this technique is discussed

Description of the Columbia Basin Wind Energy Study (CBWES)

The purpose of this Technical Report is to provide background information about the Columbia Basin Wind Energy Study (CBWES). This study, which was supported by the U.S. Department of Energy’s Wind and Water Power Program, was conducted from 16 November 2010 through 21 March 2012 at a field site in northeastern Oregon. The primary goal of the study was to provide profiles of wind speed and wind direction over the depth of the boundary layer in an operating wind farm located in an area of complex terrain. Measurements from propeller and vane anemometers mounted on a 62 m tall tower, Doppler Sodar, and Radar Wind Profiler were combined into a single data product to provide the best estimate of the winds above the site during the first part of CBWES. An additional goal of the study was to provide measurements of Turbulence Kinetic Energy (TKE) near the surface. To address this specific goal, sonic anemometers were mounted at two heights on the 62 m tower on 23 April 2011. Prior to the deployment of the sonic anemometers on the tall tower, a single sonic anemometer was deployed on a short tower 3.1 m tall that was located just to the south of the radar wind profiler. Data from the radar wind profiler, as well as the wind profile data product are available from the Atmospheric Radiation Measurements (ARM) Data Archive (http://www.arm.gov/data/campaigns). Data from the sonic anemometers are available from the authors

RDCDS Meteorologoical Component Quick Installation Guide

This guide provides step-by-step instructions for the deployment of one of the Rapidly Deployable Chemical Defense System (RDCDS) weather stations and central control system. Instructions for the deployment and operation of the Atmospheric Systems Corporation miniSODAR™ (SOnic Detection and Ranging) can be found in accompanying manuals developed by Atmospheric Systems Corporation. A detailed description of the system and its components can be found in the manual entitled Description of the RDCDS Meteorological Component

Evolution of Multispectral Aerosol Optical Properties in a Biogenically-Influenced Urban Environment During the CARES Campaign

Ground-based aerosol measurements made in June 2010 within Sacramento urban area (site T0) and at a 40-km downwind location (site T1) in the forested Sierra Nevada foothills area are used to investigate the evolution of multispectral optical properties as the urban aerosols aged and interacted with biogenic emissions. Along with black carbon and non-refractory aerosol mass and composition observations, spectral absorption (ᵝabs), scattering (ᵝsca), and extinction (ᵝext) coefficients for wavelengths ranging from 355 to 1064nm were measured at both sites using photoacoustic (PA) instruments with integrating nephelometers and using cavity ring-down (CRD) instruments. The daytime average Ångstrӧm exponent of absorption (AEA) was ~ 1.6 for the wavelength pair 405 and 870nm at T0, while it was ~ 1.8 for the wavelength pair 355 and 870nm at T1, indicating a modest wavelength-dependent enhancement of absorption at both sites throughout the study. The measured and Mie theory calculations of multispectral ᵝsca showed good correlation (R2= 0.85–0.94). The average contribution of supermicron aerosol (mainly composed of sea salt particles advected in from the Pacific Ocean) to the total scattering coefficient ranged from less than 20% at 405nm to greater than 80% at 1064 nm. From 22 to 28 June, secondary organic aerosol mass increased significantly at both sites due to increased biogenic emissions coupled with intense photochemical activity and air mass recirculation in the area. During this period, the short wavelength scattering coefficients at both sites gradually increased due to increase in the size of submicron aerosols. At the same time, BC mass-normalized absorption cross-section (MAC) values for ultraviolet wavelengths at T1 increased by ~ 60% compared to the relatively less aged urban emissions at the T0 site. In contrast, the average MAC values for 870nm wavelength were identical at both sites. These results suggest formation of moderately brown secondary organic aerosols formed in biogenically-influenced urban air

Regional Influence of Aerosol Emissions from Wildfires Driven by Combustion Efficiency: Insights from the BBOP Campaign

Wildfires are important contributors to atmospheric aerosols and a large source of emissions that impact regional air quality and global climate. In this study, the regional and nearfield influences of wildfire emissions on ambient aerosol concentration and chemical properties in the Pacific Northwest region of the United States were studied using real-time measurements from a fixed ground site located in Central Oregon at the Mt. Bachelor Observatory (∼2700 m a.s.l.) as well as near their sources using an aircraft. The regional characteristics of biomass burning aerosols were found to depend strongly on the modified combustion efficiency (MCE), an index of the combustion processes of a fire. Organic aerosol emissions had negative correlations with MCE, whereas the oxidation state of organic aerosol increased with MCE and plume aging. The relationships between the aerosol properties and MCE were consistent between fresh emissions (∼1 h old) and emissions sampled after atmospheric transport (6–45 h), suggesting that biomass burning organic aerosol concentration and chemical properties were strongly influenced by combustion processes at the source and conserved to a significant extent during regional transport. These results suggest that MCE can be a useful metric for describing aerosol properties of wildfire emissions and their impacts on regional air quality and global climate

Comparison of aircraft measurements during GoAmazon2014/5 and ACRIDICON-CHUVA

The indirect effect of atmospheric aerosol particles on the Earth's radiation balance remains one of the most uncertain components affecting climate change throughout the industrial period. The large uncertainty is partly due to the incomplete understanding of aerosol–cloud interactions. One objective of the GoAmazon2014/5 and the ACRIDICON (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems)-CHUVA (Cloud Processes of the Main Precipitation Systems in Brazil) projects was to understand the influence of emissions from the tropical megacity of Manaus (Brazil) on the surrounding atmospheric environment of the rainforest and to investigate its role in the life cycle of convective clouds. During one of the intensive observation periods (IOPs) in the dry season from 1 September to 10 October 2014, comprehensive measurements of trace gases and aerosol properties were carried out at several ground sites. In a coordinated way, the advanced suites of sophisticated in situ instruments were deployed aboard both the US Department of Energy Gulfstream-1 (G1) aircraft and the German High Altitude and Long-Range Research Aircraft (HALO) during three coordinated flights on 9 and 21 September and 1 October. Here, we report on the comparison of measurements collected by the two aircraft during these three flights. Such comparisons are challenging but essential for assessing the data quality from the individual platforms and quantifying their uncertainty sources. Similar instruments mounted on the G1 and HALO collected vertical profile measurements of aerosol particle number concentrations and size distribution, cloud condensation nuclei concentrations, ozone and carbon monoxide mixing ratios, cloud droplet size distributions, and downward solar irradiance. We find that the above measurements from the two aircraft agreed within the measurement uncertainties. The relative fraction of the aerosol chemical composition measured by instruments on HALO agreed with the corresponding G1 data, although the total mass loadings only have a good agreement at high altitudes. Furthermore, possible causes of the discrepancies between measurements on the G1 and HALO are examined in this paper. Based on these results, criteria for meaningful aircraft measurement comparisons are discussed

Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

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

The green ocean amazon experiment (GOAMAZON2014/5) observes pollution affecting gases, aerosols, clouds, and rainfall over the rain forest

The susceptibility of air quality, weather, terrestrial ecosystems, and climate to human activities was investigated in a tropical environment. © 2017 American Meteorological Society