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At least 19 records

Measurement of mass distribution of chemical species in aerosol particles

Aerosols may be generated through the nebulizing of solutions and the evaporation of their solvent, leaving the dry solute particles. Attention is presently given to a method for the direct determination of the masses of chemical species in individual aerosol particles on a continuous, real-time basis, using mass spectrometry. After the aerosol particles are introduced into the ion source of a quadrupole mass spectrometer, the particles impinge on a hot rhenium filament in the mass spectrometer's ion source. The resulting vapor plume is ionized by electron bombardment, and a pulse of ions is generated by each particle. The intensities of different masses in the ion pulses can then be measured by the mass spectrometer.

Sinha, M. P.↗

Individual Aerosol Particles from Biomass Burning in Southern Africa Compositions and Aging of Inorganic Particles: Compositions and Aging of Inorganic Particles - 2

Individual aerosol particles collected over southern Africa during the SAFARI 2000 field study were studied using transmission electron microscopy and field-emission scanning electron microscopy. The sizes, shapes, compositions, mixing states, surface coatings, and relative abundances of aerosol particles from biomass burning, in boundary layer hazes, and in the free troposphere were compared, with emphasis on aging and reactions of inorganic smoke particles. Potassium salts and organic particles were the predominant species in the smoke, and most were internally mixed. More KCl particles occur in young smoke, whereas more K2SO4 and KNO3 particles were present in aged smoke. This change indicates that with the aging of the smoke, KCl particles from the fires were converted to K2SO4 and KNO3 through reactions with sulfur- and nitrogen- bearing species from biomass burning as well as other sources. More soot was present in smoke from flaming grass fires than bush and wood fires, probably due to the predominance of flaming combustion in grass fires. The high abundance of organic particles and soluble salts can affect the hygroscopic properties of biomass-burning aerosols and therefore influence their role as cloud condensation nuclei. Particles from biomass burning were important constituents of the regional hazes.

Li, Jia↗

Characterization and Analysis of Aerosol Particle Retention and Re-aerosolization from Hook-and-Loop Fasteners on the International Space Station

The extensive use of hook and loop fasteners aboard the International Space Station warrants careful examination of its contribution to indoor air pollution, as its fine fibers catch aerosol particles then re-aerosolize them upon being pulled apart, often within the breathing zone of astronauts. This problem is expanded by the lack of gravity because airborne particles larger than 1 micrometer do not settle. Instead these aerosols remain in the air until removed by filtration. Aerosol inhalation can have negative health effects, ranging from acute symptoms to long-term consequences, depending on particle sizes, mass and material composition. This study characterizes the size distribution, number concentration, and mass concentration of re-aerosolized debris generated by hook and loop fasteners taken from the stray light cover of the Microgravity Science Glovebox in the U.S. Laboratory of the ISS to understand the extent of its impact on air quality. Transmission electron microscopy (TEM) and scanning transmission electron microscopy (STEM), in conjunction with energy dispersive spectroscopy (EDS) were also used to characterize the morphology and composition of the particles.

Boyajian, Barbara↗

Laser-Assisted Analysis of Aerosol Particles

Proposed instrument makes rapid mass-spectrometric analyses of individual particles in aerosols. Each particle vaporized and ionized by intense laser pulse, which creates ions of minimum complexity. Ability to analyze single aerosol particles continuously makes technique suitable for detection of toxic aerosol particles on real-time basis and for identification of their sources.

Sinha, M. P.↗

Individual Aerosol Particles from Biomass Burning in Southern Africa: Compositions and Size Distributions of Carbonaceous Particles - 1

Individual aerosol particles in smoke plumes from biomass fires and in regional hazes in southern Africa were studied using analytical transmission electron microscopy (TEM), which allowed detailed characterization of carbonaceous particle types in smoke and determination of changes in particle properties and concentrations during smoke aging. Based on composition, morphology, and microstructure, three distinct types of carbonaceous particles were present in the smoke: organic particles with inorganic (K-salt) inclusions, tar ball particles, and soot. The relative number concentrations of organic particles were largest in young smoke, whereas tar balls were dominant in a slightly aged (1 hour) smoke from a smoldering fire. Flaming fires emitted relatively more soot particles than smoldering fires, but soot was a minor constituent of all studied plumes. Further aging caused the accumulation of sulfate on organic and soot particles, as indicated by the large number of internally mixed organic/sulfate and soot/sulfate particles in the regional haze. Externally mixed ammonium sulfate particles dominated in the boundary layer hazes, whereas organic/sulfate particles were the most abundant type in the upper hazes. Apparently, elevated haze layers were more strongly affected by biomass smoke than those within the boundary layer. Based on size distributions and the observed patterns of internal mixing, we hypothesize that organic and soot particles are the cloud-nucleating constituents of biomass smoke aerosols. Sea-salt particles dominated in the samples taken in stratus clouds over the Atlantic Ocean, off the coast of Namibia, whereas a distinct haze layer above the clouds consisted of aged biomass smoke particles.

Posfai, Mihaly↗

Airborne measurements of cloud-forming nuclei and aerosol particles in stabilized ground clouds produced by solid rocket booster firings

Airborne measurements of cloud volumes, ice nuclei and cloud condensation nuclei, liquid particles, and aerosol particles were obtained from stabilized ground clouds (SGCs) produced by Titan 3 launches at Kennedy Space Center, 20 August and 5 September 1977. The SGCs were bright, white, cumulus clouds early in their life and contained up to 3.5 g/m3 of liquid in micron to millimeter size droplets. The measured cloud volumes were 40 to 60 cu km five hours after launch. The SGCs contained high concentrations of cloud condensation nuclei active at 0.2%, 0.5%, and 1.0% supersaturation for periods of three to five hours. The SGCs also contained high concentrations of submicron particles. Three modes existed in the particle population: a 0.05 to 0.1 micron mode composed of aluminum-containing particles, a 0.2 to 0.8 micron mode, and a 2.0 to 10 micron mode composed of particles that contained primarily aluminum.

Hindman, E. E., II↗

A numerical determination of the evolution of cloud drop spectra due to condensation on natural aerosol particles

The time variation in size of aerosol particles growing by condensation is studied numerically by means of an air parcel model which allows entrainment of air and aerosol particles. Particles of four types of aerosols typically occurring in atmospheric air masses were considered. The present model circumvents any assumption about the size distribution and chemical composition of the aerosol particles by basing the aerosol particle growth on actually observed size distributions and on observed amounts of water taken up under equilibrium by a deposit of the aerosol particles. Characteristic differences in the drop size distribution, liquid water content and supersaturation were found for the clouds which evolved from the four aerosol types considered.

Lee, I. Y.↗

Microphysical processes affecting stratospheric aerosol particles

Physical processes which affect stratospheric aerosol particles include nucleation, condensation, evaporation, coagulation and sedimentation. Quantitative studies of these mechanisms to determine if they can account for some of the observed properties of the aerosol are carried out. It is shown that the altitude range in which nucleation of sulfuric acid-water solution droplets can take place corresponds to that region of the stratosphere where the aerosol is generally found. Since heterogeneous nucleation is the dominant nucleation mechanism, the stratospheric solution droplets are mainly formed on particles which have been mixed up from the troposphere or injected into the stratosphere by volcanoes or meteorites. Particle growth by heteromolecular condensation can account for the observed increase in mixing ratio of large particles in the stratosphere. Coagulation is important in reducing the number of particles smaller than 0.05 micron radius. Growth by condensation, applied to the mixed nature of the particles, shows that available information is consistent with ammonium sulfate being formed by liquid phase chemical reactions in the aerosol particles. The upper altitude limit of the aerosol layer is probably due to the evaporation of sulfuric acid aerosol particles, while the lower limit is due to mixing across the tropopause.

Hamill, P.↗

Criteria for significance of simultaneous presence of both condensible vapors and aerosol particles on mass transfer (deposition) rates

The simultaneous presence of aerosol particles and condensible vapors in a saturated boundary layer which may affect deposition rates to subcooled surfaces because of vapor-particle interactions is discussed. Scavenging of condensible vapors by aerosol particles may lead to increased particle size and decreased vapor mass fraction, which alters both vapor and particle deposition rates. Particles, if sufficiently concentrated, may also coagulate. Criteria are provided to assess the significance of such phenomena when particles are already present in the mainstream and are not created inside the boundary layer via homogeneous nucleation. It is determined that there is direct proportionality with: (1) the mass concentration of both condensible vapors and aerosol particles; and (2) the square of the boundary layer thickness to particle diameter ratio (delta d sub p) square. Inverse proportionality was found for mainstream to surface temperature difference if thermophoresis dominates particle transport. It is concluded that the square of the boundary layer thickness to particle diameter ratio is the most critical factor to consider in deciding when to neglect vapor-particle interactions.

Gokoglu, S. A.↗

Criteria for significance of simultaneous presence of both condensible vapors and aerosol particles on mass transfer (deposition) rates

The simultaneous presence of aerosol particles and condensible vapors in a saturated boundary layer which may affect deposition rates to subcooled surfaces because of vapor-particle interactions is discussed. Scavenging of condensible vapors by aerosol particles may lead to increased particle size and decreased vapor mass fraction, which alters both vapor and particle deposition rates. Particles, if sufficiently concentrated, may also coagulate. Criteria are provided to assess the significance of such phenomena when particles are already present in the mainstream and are not created inside the boundary layer via homogeneous nucleation. It is determined that there is direct proportionality with: (1) the mass concentration of both condensible vapors and aerosol particles; and (2) the square of the boundary layer thickness to particle diameter ratio (delta d sub p) square. Inverse proportionality was found for mainstream to surface temperature difference if thermophoresis dominates particle transport. It is concluded that the square of the boundary layer thickness to particle diameter ratio is the most critical factor to consider in deciding when to neglect vapor-particle interactions.

Gokoglu, S. A.↗

Evaluation of Global Simulations of Aerosol Particle and Cloud Condensation Nuclei Number, with Implications for Cloud Droplet Formation

A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011-2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of -24% and -35% for particles with dry diameters > 50 and > 120nm, as well as -36% and -34% for CCN at supersaturations of 0.2% and 1.0%, respectively. However, they seem to behave differently for particles activating at very low supersaturations (< 0.1%) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N3 (number concentration of particles with dry diameters larger than 3 nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2% (CCN(0.2)) compared to that for N3, maximizing over regions where new particle formation is important. An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter. Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated on average by the models by 40% during winter and 20% in summer.

cloud droplets↗

Characterizing the Vertical Profile of Aerosol Particle Extinction and Linear Depolarization over Southeast Asia and the Maritime Continent: The 2007-2009 View from CALIOP

Vertical profiles of 0.532 μm aerosol particle extinction coefficient and linear volume depolarization ratio are described for Southeast Asia and the Maritime Continent. Quality-screened and cloud-cleared Version 3.01 Level 2 NASA Cloud Aerosol Lidar with Orthogonal Polarization (CALIOP) 5-km Aerosol Profile datasets are analyzed from 2007 to 2009. Numerical simulations from the U.S. Naval Aerosol Analysis and Predictive System (NAAPS), featuring two-dimensional variational assimilation of NASA Moderate Resolution Imaging Spectroradiometer and Multi-angle Imaging Spectro- Radiometer quality-assured datasets, combined with regional ground-based lidar measurements, are considered for assessing CALIOP retrieval performance, identifying bias, and evaluating regional representativeness. CALIOP retrievals of aerosol particle extinction coefficient and aerosol optical depth (AOD) are high over land and low over open waters relative to NAAPS (0.412/0.312 over land for all data points inclusive, 0.310/0.235 when the per bin average is used and each is treated as single data points; 0.102/0.151 and 0.086/0.124, respectively, over ocean). Regional means, however, are very similar (0.180/0.193 for all data points and 0.155/0.159 when averaged per normalized bin), as the two factors offset one another. The land/ocean offset is investigated, and discrepancies attributed to interpretation of particle composition and a-priori assignment of the extinction-to-backscatter ratio ("lidar ratio") necessary for retrieving the extinction coefficient from CALIOP signals. Over land, NAAPS indicates more dust present than CALIOP algorithms are identifying, indicating a likely assignment of a higher lidar ratio representative of more absorptive particles. NAAPS resolvesmore smoke overwater than identified with CALIOP, indicating likely usage of a lidar ratio characteristic of less absorptive particles to be applied that biases low AOD there. Over open waters except within the Bay of Bengal, aerosol particle scattering is largely capped below 1.5 km MSL, though ground-based lidar measurements at Singapore differ slightly from this finding. Significant aerosol particle presence over land is similarly capped near 3.0 km MSL over most regions. Particle presence at low levels regionally, except over India, is dominated by relatively non-depolarizing particles. Industrial haze, sea salt droplets and fresh smoke are thus most likely present.

linear volume depolarization ratio↗

Polarimeter + Lidar Derived Aerosol Particle Number Concentration

In this study, we propose a simple method to derive vertically resolved aerosol particle number concentration (Na) using combined polarimetric and lidar remote sensing observations. This method relies on accurate polarimeter retrievals of the fine-mode column-averaged aerosol particle extinction cross section and accurate lidar measurements of vertically resolved aerosol particle extinction coefficient such as those provided by multiwavelength high spectral resolution lidar. We compare the resulting lidar + polarimeter vertically resolved Na product to in situ Na data collected by airborne instruments during the NASA aerosol cloud meteorology interactions over the western Atlantic experiment (ACTIVATE). Based on all 35 joint ACTIVATE flights in 2020, we find a total of 32 collocated in situ and remote sensing profiles that occur on 11 separate days, which contain a total of 322 cloud-free vertically resolved altitude bins of 150 m resolution. We demonstrate that the lidar + polarimeter Na agrees to within 106% for 90% of the 322 vertically resolved points. We also demonstrate similar agreement to within 121% for the polarimeter-derived column-averaged Na. We find that the range-normalized mean absolute deviation (NMAD) for the polarimeter-derived column-averaged Na is 21%, and the NMAD for the lidar + polarimeter-derived vertically resolved Na is 16%. Taken together, these findings suggest that the error in the polarimeter-only column-averaged Na and the lidar + polarimeter vertically resolved Na are of similar magnitude and represent a significant improvement upon current remote sensing estimates of Na.

Aerosol number concentration↗

Polarimeter + Lidar–Derived Aerosol Particle Number Concentration

In this study, we propose a simple method to derive vertically resolved aerosol particle number concentration (Na) using combined polarimetric and lidar remote sensing observations. This method relies on accurate polarimeter retrievals of the fine-mode column-averaged aerosol particle extinction cross section and accurate lidar measurements of vertically resolved aerosol particle extinction coefficient such as those provided by multiwavelength high spectral resolution lidar. We compare the resulting lidar + polarimeter vertically resolved N(a) product to in situ N(a) data collected by airborne instruments during the NASA aerosol cloud meteorology interactions over the western Atlantic experiment (ACTIVATE). Based on all 35 joint ACTIVATE flights in 2020, we find a total of 32 collocated in situ and remote sensing profiles that occur on 11separate days, which contain a total of 322 cloud-free vertically resolved altitude bins of 150 m resolution. We demonstrate that the lidar + polarimeter N(a) agrees to within 106% for 90% of the 322 vertically resolved points. We also demonstrate similar agreement to within 121% for the polarimeter-derived column-averaged N(a). We find that the range-normalized mean absolute deviation (NMAD) for the polarimeter-derived column-averaged Na is 21%, and the NMAD for the lidar + polarimeter-derived vertically resolved Na is 16%. Taken together, these findings suggest that the error in the polarimeter-only column-averaged N(a) and the lidar + polarimeter vertically resolved N(a) are of similar magnitude and represent a significant improvement upon current remote sensing estimates of N(a).

RSP↗

Spatiotemporal Coherence of Mean and Extreme Aerosol Particle Events over Eastern North America as Observed from Satellite

Quantifying spatiotemporal scales of coherence and variability of aerosol particle properties provides (i) metrics for evaluating observational data sets and model simulations, (ii) inferences regarding dominant causes of variability, and (iii) information that is necessary to determine their climate forcing and air quality impacts. Accordingly, analyses of columnar aerosol optical depth (AOD) and Ångstrom exponent (AE) from the MODerate resolution Imaging Spectroradiometer (MODIS) on the Aqua and Terra satellites, and AErosol RObotic NETwork (AERONET) stations are used to evaluate the spatially averaged (Level-3) MODIS products, and to characterize the spatiotemporal scales of variability (and coherence) of aerosol particles over eastern North America (2000-2013). Results show a high degree of consistency in AOD retrievals from the different data sets but larger discrepancies in AE estimates, highest mean AOD and lowest day-to-day variability during the summer, and largest scales of spatial coherence in summer and fall. Consistent with the scales of spatial coherence from MODIS data, in both data sets power spectra indicate AOD variability is manifest primarily on synoptic and annual time scales. Conversely, AE variability in MODIS data is primarily focused on seasonal, semiannual, and annual time scales, and there is an additional mode of AE variability at approx. 30 days in the AERONET measurements. The frequency of cooccurrence of extreme AOD values (>local 90th percentile) decreases to below 50% at approx. 150 km from a central grid cell, but is above that expected by random chance over almost all of eastern North America, indicating supra-regional scale extreme events.

MODIS↗

Estimating Marine Aerosol Particle Volume and Number from Maritime Aerosol Network Data

As well as spectral aerosol optical depth (AOD), aerosol composition and concentration (number, volume, or mass) are of interest for a variety of applications. However, remote sensing of these quantities is more difficult than for AOD, as it is more sensitive to assumptions relating to aerosol composition. This study uses spectral AOD measured on Maritime Aerosol Network (MAN) cruises, with the additional constraint of a microphysical model for unpolluted maritime aerosol based on analysis of Aerosol Robotic Network (AERONET) inversions, to estimate these quantities over open ocean. When the MAN data are subset to those likely to be comprised of maritime aerosol, number and volume concentrations obtained are physically reasonable. Attempts to estimate surface concentration from columnar abundance, however, are shown to be limited by uncertainties in vertical distribution. Columnar AOD at 550 nm and aerosol number for unpolluted maritime cases are also compared with Moderate Resolution Imaging Spectroradiometer (MODIS) data, for both the present Collection 5.1 and forthcoming Collection 6. MODIS provides a best-fitting retrieval solution, as well as the average for several different solutions, with different aerosol microphysical models. The average solution MODIS dataset agrees more closely with MAN than the best solution dataset. Terra tends to retrieve lower aerosol number than MAN, and Aqua higher, linked with differences in the aerosol models commonly chosen. Collection 6 AOD is likely to agree more closely with MAN over open ocean than Collection 5.1. In situations where spectral AOD is measured accurately, and aerosol microphysical properties are reasonably well-constrained, estimates of aerosol number and volume using MAN or similar data would provide for a greater variety of potential comparisons with aerosol properties derived from satellite or chemistry transport model data.

Sayer, A. M.↗