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At least 19 records

Quantifying structural errors in cloud condensation nuclei activity from reduced representation of aerosol size distributions

Aerosol effects on clouds and radiation are the dominant contribution to uncertainty in radiative forcing relative to the pre-industrial atmosphere. While previous studies have assessed the impact of parametric uncertainty on modeled forcing, structural errors from the numerical representation of particle distributions have not been well quantified. Here we present a framework for quantifying error in aerosol size distributions and cloud condensation nuclei activity, which we apply to the widely used 4-mode version of the Modal Aerosol Module (MAM4). Box model predictions from the MAM4 are evaluated against the Particle Monte Carlo Model for Simulating Aerosol Interactions and Chemistry (PartMC-MOSAIC), a benchmark model that tracks the evolution of individual particles. We show that size distributions simulated by MAM4 diverge from those simulated by PartMC-MOSAIC after only a few hours of aging by condensation and coagulation in polluted conditions, which leads to large errors in modeled cloud condensation nuclei concentrations. We find that differences between MAM4 and PartMC-MOSAIC are largest under polluted conditions, where the size distribution evolves rapidly though aging by condensation of semi-volatile substances and coagulation among particles. These findings suggest that structural error in modeled aerosol properties contributes to the large inter-model variability in aerosol radiative forcing.

Fierce, Laura M.↗

Aerosol size distribution, composition, and CO2 backscatter

The aerosol size distribution, composition, and CO2 backscatter at 10.6 microns (beta-CO2) were measured continuosly at the Mauna Loa Observatory (Hawaii) during January-March and November-December, 1988 periods to compare the characteristics of periods associated with appreciable Asian dust transport to that site (January-March) with those of periods characterized by low-dust condition. The aerosol size distribution in the range 0.15 micron to 7.6 microns was measured at temperatures of 40, 150, and 340 C to differentiate between volatile and nonvolatile aerosols. Large ranges of variability was found in measurements of aerosol size distribution during both periods, but the average distributions were similar for both the high-dust and the low-dust periods. However, values for beta-CO2 were more elevated (by about six times) during periods associated with active Asian dust transport to the observatory site than during the low-dust periods.

Clarke, Antony D.↗

Artifacts in the Aerosol Size Distribution Measured by the Ultra-High-Sensitivity Aerosol Spectrometer (UHSAS)

The ultra-high-sensitivity aerosol spectrometer (UHSAS) (Droplet Measurement Technologies, Longmont, Colorado) is an optical particle size spectrometer that determines aerosol size distributions in the diameter range from 60 to 1000 nm in 100 logarithmically spaced diameter bins1 by measuring the amount of light scattered by individual aerosol particles from a 1054-nm laser. Recently, it was noticed that aerosol size distributions determined by the UHSAS from all U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility sites exhibited modes at diameters greater than ~500 nm (Figure 1, blue arrows). These modes were not present in size distributions determined by another aerosol spectrometer that was co-located with the UHSAS, the Grimm 11D optical particle counter (OPC) (GRIMM Aerosol Technik Ainring GmbH & Co. KG, Germany), which sizes particles into 31 linearly spaced diameters bins from 253 to 35,150 nm using a 683-nm wavelength laser. Additionally, abrupt changes in aerosol particle number concentration with changing particle diameter are seen in UHSAS data at several diameters (Figure 1, red arrows). The purpose of this report is to explain the origin of the modes and the abrupt changes in aerosol size distributions observed by the UHSAS and why they are absent in the data from the Grimm OPC.

54 ENVIRONMENTAL SCIENCES↗

CACTI: Best Estimate Aerosol Size Distribution by airborne measurements

These data were collected during the Cloud, Aerosol, and Complex Terrain Interactions (CACTI; https://www.arm.gov/research/campaigns/amf2018cacti ) field campaign in the Sierras de Córdoba mountain range of north-central Argentina as part of ARM Aerial Facility (AAF) deployment. The ARM Aerial Facility Gulfstream-1 was operated from Las Higueras Airport (IATA: RCU, ICAO: SAOC), Río Cuarto, Córdoba, Argentina, for the Intensive Observation Period (IOP) from Nov. 1 through Dec. 15, 2018. The G-1 aircraft performed 22 research flights over the first ARM Mobile Facility (AMF1) location in the Sierras de Córdoba mountain range to measure atmospheric state and turbulence, cloud water content and droplet size distributions, aerosol precursor gases, aerosol chemical composition and size distributions. The current data set presents Best Estimate Aerosol Size Distribution: a merged aerosol size distribution composed of the data from 5 sensors; three aerosol spectrometers: Scanning Mobility Particle Sizer (SMPS), Ultra-High Sensitivity Aerosol Spectrometer (UHSAS), and Passive Cavity Aerosol Spectrometer (PCASP); and two cloud probes: Cloud Aerosol Spectrometer (CAS) and Fast Cloud Droplet Probe (FCDP). The SMPS data were interpolated to 1 second from “native” time resolution of about 64 second to match all other probes.

54 ENVIRONMENTAL SCIENCES↗

A diagnostic stratospheric aerosol size distribution inferred from SAGE II measurements

An aerosol size distribution model for the stratosphere is inferred based on 5 years of Stratospheric Aerosol and Gas Experiment (SAGE) II measurements of multispectral aerosol and water vapor extinction. The SAGE II aerosol and water vapor extinction data strongly suggest that there is a critical particle radius below which there is a relatively weak dependence of particle number density with size and above which there are few, if any, particles. A segmented power law model, as a simple representation of this dependence, is used in theoretical calculations and intercomparisons with a variety of aerosol measurements including dustsondes, longwave lidar, and wire impactors and shows a consistently good agreement.

Thomason, Larry W.↗

Three optical methods for remotely measuring aerosol size distributions.

Three optical probing methods for remotely measuring atmospheric aerosol size distributions are discussed and contrasted. The particular detection methods which are considered make use of monostatic lidar (laser radar), bistatic lidar, and solar radiometer sensing techniques. The theory of each of these measurement techniques is discussed briefly, and the necessary constraints which must be applied to obtain aerosol size distribution information from such measurements are pointed out. Theoretical and/or experimental results are also presented which demonstrate the utility of the three proposed probing methods.

Reagan, J. A.↗

Retrieval of stratospheric aerosol size distribution from atmospheric extinction of solar radiation at two wavelengths

A parametric study is presented of the effects of the size distribution and composition of stratospheric aerosols on the value R, the ratio of the extinction of solar radiation at wavelength 0.45 micron to the extinction at wavelength 1.0 micron. The aerosol size distributions under study comprise nine analytical expressions, including most of the stratospheric aerosol models used by investigators. The aerosol compositions considered are the supercooled sulfuric-acid droplets, with different weight percentages of H2SO4 in the aerosol. It is found that whereas R is not very sensitive to either the composition or the radii limits of the stratospheric aerosols under consideration, it is quite sensitive to the value of the variable parameter governing the mode radius of the size distribution of aerosol particles. The results of the parametric study underlie the method proposed here of retrieving the size distribution of aerosol particles in the stratosphere from the experimental results of the extinction of solar radiation at two wavelengths.

Yue, G. K.↗

Analytic modeling of aerosol size distributions

Mathematical functions commonly used for representing aerosol size distributions are studied parametrically. Methods for obtaining best fit estimates of the parameters are described. A catalog of graphical plots depicting the parametric behavior of the functions is presented along with procedures for obtaining analytical representations of size distribution data by visual matching of the data with one of the plots. Examples of fitting the same data with equal accuracy by more than one analytic model are also given.

Deepack, A.↗

Retrieval of aerosol size distribution moments from multiwavelength particulate extinction measurements

Two methods for inferring aerosol size distribution moments from multiwavelength particulate extinction measurements are studied. The methods are an eigenvalue technique that approximates an appropriate moment-weighting function by a linear combination of kernel functions and a conversion ratio approach that uses the ratio of the particulate extinction measurements at two wavelengths to choose a model moment-to-extinction conversion ratio. The techniques are applied to infer the third moment, or volume, of the aerosol size distribution from actual particulate extinction measurements taken as part of the Stratospheric Aerosol and Gas Experiment II during a correlative measurement experiment in Brazil in April 1985.

Livingston, John M.↗

Aerosol size distributions obtained by inversion of spectral optical depth measurements

Columnar aerosol size distributions have been inferred by numerically inverting particulate optical depth measurements as a function of wavelength. An inversion formula which explicitly includes the magnitude of the measurement variances is derived and applied to optical depth measurements obtained in Tucson with a solar radiometer. It is found that the individual size distributions of the aerosol particles (assumed spherical), at least for radii greater than or approximately equal to 0.1 micron, fall into one of three distinctly different categories. Approximately 50% of all distributions examined thus far can best be represented as a composite of a Junge distribution plus a distribution of relatively monodispersed larger particles centered at a radius of about 0.5 micron. Scarcely 20% of the distributions yielded Junge size distributions, while 30% yielded relatively monodispersed distributions of the log-normal or gamma distribution types. A representative selection of each of these types will be presented and discussed. The sensitivity of spectral attenuation measurements to the radii limits and refractive index assumed in the numerical inversion will also be addressed.

King, M. D.↗

In Situ Aerosol Size Distributions and Clear Column Radiative Closure During ACE-2

As part of the second Aerosol Characterization Experiment (ACE-2) during June and July of 1997, aerosol size distributions were measured on board the CIRPAS Pelican aircraft through the use of a DMA and two OPCS. During the campaign, the boundary layer aerosol typically possessed characteristics representative of a background marine aerosol or a continentally influenced aerosol, while the free tropospheric aerosol was characterized by the presence or absence of a Saharan dust layer. A range of radiative closure comparisons were made using the data obtained during vertical profiles flown on four missions. Of particular interest here are the comparisons made between the optical properties as determined through the use of measured aerosol size distributions and those measured directly by an airborne 14-wavelength sunphotometer and three nephelometers. Variations in the relative humidity associated with each of the direct measurements required consideration of the hygroscopic properties of the aerosol for size distribution based calculations. Simultaneous comparison with such a wide range of directly measured optical parameters not only offers evidence of the validity of the physicochemical description of the aerosol when closure is achieved, but also provides insight into potential sources of error when some or all of the comparisons result in disagreement. Agreement between the derived and directly measured optical properties varied for different measurements and for different cases. Averaged over the four case studies, the derived extinction coefficient at 525 nm exceeded that measured by the sunphotomoter by 2.5% in the clean boundary later, but underestimated measurements by 13% during pollution events. For measurements within the free troposphere, the mean derived extinction coefficient was 3.3% and 17% less than that measured by the sunphotometer during dusty and nondusty conditions, respectively. Likewise, averaged discrepancies between the derived and measured scattering coefficient were -9.6%, +4.7%, +17%, and -41% for measurements within the clean boundary layer, polluted boundary layer, free troposphere with a dust layer, and free troposphere without a dust layer, respectively. Each of these quantities, as well as the majority of the > 100 individual comparisons from which they were averaged, were within estimated uncertainties.

Collins, D. R.↗

Aerosol size distributions - Remote determination from air-borne measurements of the solar aureole

Aerosol-size distributions were determined remotely using an airborne scanning photometer. This instrument consists of a sunshade, optics, and a large-dynamic-range photodetector-amplifier system that scans about the vertical, recording both the direct attenuated solar beam and the diffuse sky radiance in the almucantar of the sun at an effective wavelength of 0.54 micron. Inversion of the measured radiances determined aerosol radii from approximately 0.2 to 8.0 microns. Data were taken during flights over western Lake Superior and southwestern Wisconsin. Inverted aerosol-size distributions are compared with results obtained by other methods.

Twitty, J. T.↗

In Situ Aerosol-Size Distributions and Clear-Column Radiative Closure During ACE-2

As part of the second Aerosol Characterization Experiment (ACE-2) during June and July of 1997, aerosol-size distributions were measured on board the CIRPAS Pelican aircraft through the use of a Differential Mobility Analyzer (DMA) and 2 Optical Particle Counters (OPCs). During the campaign, the boundary-layer aerosol typically possessed characteristics representative of a background marine aerosol or a continentally influenced aerosol, while the free-tropospheric aerosol was characterized by the presence or absence of a Saharan dust layer. A range of radiative closure comparisons were made using the data obtained during vertical profiles flown on 4 missions. Of particular interest here are the comparisons made between the optical properties as determined through the use of measured aerosol-size distributions and those measured directly by an airborne 14-wavelength sunphotometer and 3 nephelometers. Variations in the relative humidity associated with each of the direct measurements required consideration of the hygroscopic properties of the aerosol for size-distribution-based calculations. Simultaneous comparison with such a wide range of directly-measured optical parameters not only offers evidence of the validity of the physicochemical description of the aerosol when closure is achieved, but also provides insight into potential sources of error when some or all of the comparisons result in disagreement. Agreement between the derived and directly-measured optical properties varied for different measurements and for different cases. Averaged over the 4 case studies, the derived extinction coefficient at 525 nm exceeded that measured by the sunphotometer by 2.5% in the clean boundary layer, but underestimated measurements by 13% during pollution events. For measurements within the free troposphere, the mean derived extinction coefficient was 3.3% and 17% less than that measured by the sunphotometer during dusty and non-dusty conditions, respectively. Likewise, averaged discrepancies between the derived and measured scattering coefficient were -9.6%, +4.7%, +17%, and -41% for measurements within the clean boundary layer, polluted boundary layer, free troposphere with a dust layer, and free troposphere without a dust layer, respectively. Each of these quantities, as well as the majority of the more than 100 individual comparisons from which they were averaged, were within estimated uncertainties.

Collins, R.↗

The Angstrom Exponent and Bimodal Aerosol Size Distributions

Powerlaws have long been used to describe the spectral dependence of aerosol extinction, and the wavelength exponent of the aerosol extinction powerlaw is commonly referred to as the Angstrom exponent. The Angstrom exponent is often used as a qualitative indicator of aerosol particle size, with values greater than two indicating small particles associated with combustion byproducts, and values less than one indicating large particles like sea salt and dust. In this study, we investigate the relationship between the Angstrom exponent and the mode parameters of bimodal aerosol size distributions using Mie theory calculations and Aerosol Robotic Network (AERONET) retrievals. We find that Angstrom exponents based upon seven wavelengths (0.34, 0.38, 0.44, 0.5, 0.67, 0.87, and 1.02 micrometers) are sensitive to the volume fraction of aerosols with radii less then 0.6 micrometers, but not to the fine mode effective radius. The Angstrom exponent is also known to vary with wavelength, which is commonly referred to as curvature; we show how the spectral curvature can provide additional information about aerosol size distributions for intermediate values of the Angstrom exponent. Curvature also has a significant effect on the conclusions that can be drawn about two-wavelength Angstrom exponents; long wavelengths (0.67, 0.87 micrometers) are sensitive to fine mode volume fraction of aerosols but not fine mode effective radius, while short wavelengths (0.38, 0.44 micrometers) are sensitive to the fine mode effective radius but not the fine mode volume fraction.

Schuster, Gregory L.↗

Simulation of the Aerosol Size Distribution Using a Neural Network Surrogate for the Modal Aerosol Module (MAM7)

One objective of atmospheric simulations is to quantify the distribution of aerosols and their properties. Accurate parameterizations of the processes governing aerosol mass, particle number, and particle size distribution are important for predicting the Earth’s net radiative balance and aerosol-cloud interactions. The Modal Aerosol Module (MAM7) is a two-moment aerosol model that simulates mass, number, and size distribution of seven modes comprised of internally mixed aerosol species. The two-moment scheme adds significant computational expense but allows for the prediction of varying particle size distribution relative to the bulk method which predicts only total mass. In this work, we developed a neural network surrogate model for MAM7 (MAMnet) to predict the aerosol number concentration in NASA’s Global Earth Observing System (GEOS) without adding prohibitive computational expense. MAMnet, can be driven by output from a single moment, mass-based, aerosol scheme (Goddard Chemistry Aerosol and Radiation model (GOCART)) or from reanalysis products (Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2)). MAMnet was trained using number concentrations from a 5-year GEOS/MAM7 simulation at 1-degree horizontal resolution and using the total mass calculated across modes as inputs, as well as temperature and air density. The model architecture for MAMnet was based on AlexNet, the 2012 winner of the ImageNet Large Scale Visual Recognition Challenge. While some modifications were necessary to accommodate our problem, important aspects of the network were preserved. MAMnet was able to reproduce zonal dynamics and spatial distributions of the aerosol number concentration however predictability in the upper troposphere was poor.

Katherine H Breen↗

Retrieval of aerosol size distributions from scattering and extinction measurements in the presence of multiple scattering

A fast technique, based on approximation to atmospheric radiative transfer in the solar aureole, is presented for the retrieval of aerosol size distribution from multispectral measurements of both scattered sky radiance and extinction by aerosol media. In this approximation, it is assumed that for a relatively clear day, the sky radiance is due to single scattering by molecules and aerosols, and to multiple scattering by molecules alone. The accuracy of this approximation is discussed in connection with the inversion of scattered radiation data. Results for aerosol size distributions retrieved from multispectral solar extinction measurements by the nonlinear least squares method are discussed, and the retrievals are found to be accurate when checked against ground truth measurements.

Deepak, A.↗

Tethered Balloon Observations of Vertically Resolved Aerosol Size Distributions during the U.S. DOE ARM CoURAGE and BNF Campaigns

This dataset contains vertically resolved aerosol particle number size distributions measured using a miniature Scanning Electrical Mobility Spectrometer (mSEMS) deployed aboard the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) Tethered Balloon System (TBS) during the 2025 Coast-Urban-Rural Atmospheric Gradient Experiment (CoURAGE) and Bankhead National Forest (BNF) field campaigns. The mSEMS measured aerosol size distributions over approximately 10–300 nm during repeated TBS vertical profiles through the atmospheric boundary layer. The dataset provides measurements of particle number size distributions as a function of particle diameter, altitude, and time and supports investigation of aerosol vertical structure, elevated ultrafine and Aitken-mode particle layers, boundary-layer evolution, and residual-layer processes.

ARM↗