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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.↗

Remote Sensing of Aerosol Water Fraction, Dry Size Distribution and Soluble Fraction Using Multi-Angle, Multi-Spectral Polarimetry

A framework to infer volume water fraction, soluble fraction and dry size distributions of fine-mode aerosol from multi-angle, multi-spectral polarimetry retrievals of column-averaged ambient aerosol properties is presented. The method is applied to observations of the Research Scanning Polarimeter (RSP) obtained during two NASA aircraft campaigns, namely the Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) and the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex). All aerosol retrievals are statistically evaluated using in situ data. Volume water fraction is inferred from the retrieved ambient real part of the refractive index, assuming a dry refractive index of 1.54 and by applying a volume mixing rule to obtain the effective ambient refractive index. The uncertainties in inferred volume water fraction resulting from this simplified model are discussed and estimated to be lower than 0.2 and decreasing with increasing volume water fraction. The daily mean retrieved volume water fractions correlate well with the in situ values with a mean absolute difference of 0.09. Polarimeter-retrieved ambient effective radius for daily data is shown to increase as a function of volume water fraction as expected. Furthermore, the effective variance of the size distributions also increases with increasing effective radius, which we show is consistent with an external mixture of soluble and insoluble aerosol. The relative variations of effective radius and variance over an observation period are then used to estimate the soluble fraction of the aerosol. Daily results of soluble fraction correlate well with in situ-observed sulfate mass fraction with a correlation coefficient of 0.79. Subsequently, inferred water and soluble fractions are used to derive dry fine-mode size distributions from their ambient counterparts. While dry effective radii obtained in situ and from RSP show similar ranges, in situ values are generally substantially smaller during the ACTIVATE deployments, which may be due to biases in RSP retrievals or in the in situ observations, or both. Both RSP and in situ observations indicate the dominance of aerosol with low hygroscopicity during the ACTIVATE and CAMP2Ex campaigns. Furthermore, RSP indicates a high degree of external mixing of particles with low and high hygroscopicity. These retrievals of fine-mode water volume fraction and soluble fraction may be used for the evaluation of water uptake in atmospheric models. Furthermore, the framework allows us to estimate the variation in the concentration of fine-mode aerosol larger than a specific dry radius limit, which can be used as a proxy for the variation in cloud condensation nucleus concentrations. This framework may be applied to multi-angle, multi-spectral satellite data expected to be available in the near future.

Amount of water in particulate matter↗

Size distribution of dust grains: A problem of self-similarity

Distribution functions describing the results of natural processes frequently show the shape of power laws, e.g., mass functions of stars and molecular clouds, velocity spectrum of turbulence, size distributions of asteroids, micrometeorites and also interstellar dust grains. It is an open question whether this behavior is a result simply coming about by the chosen mathematical representation of the observational data or reflects a deep-seated principle of nature. The authors suppose the latter being the case. Using a dust model consisting of silicate and graphite grains Mathis et al. (1977) showed that the interstellar extinction curve can be represented by taking a grain radii distribution of power law type n(a) varies as a(exp -p) with 3.3 less than or equal to p less than or equal to 3.6 (example 1) as a basis. A different approach to understanding power laws like that in example 1 becomes possible by the theory of self-similar processes (scale invariance). The beta model of turbulence (Frisch et al., 1978) leads in an elementary way to the concept of the self-similarity dimension D, a special case of Mandelbrot's (1977) fractal dimension. In the frame of this beta model, it is supposed that on each stage of a cascade the system decays to N clumps and that only the portion beta N remains active further on. An important feature of this model is that the active eddies become less and less space-filling. In the following, the authors assume that grain-grain collisions are such a scale-invarient process and that the remaining grains are the inactive (frozen) clumps of the cascade. In this way, a size distribution n(a) da varies as a(exp -(D+1))da (example 2) results. It seems to be highly probable that the power law character of the size distribution of interstellar dust grains is the result of a self-similarity process. We can, however, not exclude that the process leading to the interstellar grain size distribution is not fragmentation at all. It could be, e.g., diffusion-limited growth discussed by Sander (1986), who applied the theory of fractal geometry to the classification of non-equilibrium growth processes. He received D=2.4 for diffusion-limited aggregation in 3d-space.

Henning, TH.↗

Particle size distributions of several commonly used seeding aerosols

During the course of experimentation, no solid particle powder could be found which produced an aerosol with a narrow particle size distribution when fluidization was the only flow process used in producing the aerosol. The complication of adding particle size fractionation processes to the aerosol generation effort appears to be avoidable. In this regard, a simple sonic orifice is found to be effective in reducing the percentage of agglomerates in the several metal oxide powders tested. Marginally beneficial results are obtained for a 0.5/99.5 percent by weight mixture of the flow agent and metal oxide powder. However, agglomeration is observed to be enhanced when the flow agent percentage is increased to 5 percent. Liquid atomization using the Collison nebulizer as well as a version of the Laskin nozzle resulted in polydispersed aerosols with particle size distributions heavily weighted by the small particle end of the size spectrum. The aerosol particle size distributions produced by the vaporization/condensation seeder are closer to the ideal monodispersed aerosol than any of the other aerosols tested. In addition, this seeding approach affords a measure of control over particle size and particle production rate.

Crosswy, F. L.↗

Determination of the cumulus size distribution from LANDSAT pictures

Varying insolation causes undesirable thermic stress to the receiver of a solar power plant. The rapid change of insolation depends on the size distribution of the clouds; in order to measure these changes, it is suitable to determine typical cumulus size distributions. For this purpose, LANDSAT-images are adequate. Several examples of cumulus size distributions will be presented and their effects on the operation of a solar power plant are discussed.

Karg, E.↗

Effect of particle size distribution and chlorophyll content on beam attenuation spectra

The relationships between beam attenuation spectra, chlorophyll and pheophytin pigment concentrations, and particle size distributions are examined for a coastal region believed to have negligible concentrations of terrestrially derived dissolved organic compounds but large quantities of phytoplankton and resuspended sediments. It was found that the slope of the beam attenuation spectra increases when the hyperbolic slope of the size distribution increases. The magnitude of this increase in slope was consistent with calculations based on a range of particle diameters from 0.5 to 30 microns so that it would be possible to predict the slope of the particle size distribution if the slope of the beam attenuation spectra is known. The ratio of chlorophyll and pheophytin pigments to suspended volume concentrations affected the beam attenuation spectra to a lesser degree and in a more complex manner. Because of the strong effect of slope, it was concluded that the chlorophyll and pheophytin pigment content of suspended particles could not be efficiently predicted by means of beam attenuation measurements.

Kitchen, J. C.↗

Remote sensing of environmental particulate pollutants - Optical methods for determinations of size distribution and complex refractive index

A unifying approach, based on a generalization of Pearson's differential equation of statistical theory, is proposed for both the representation of particulate size distribution and the interpretation of radiometric measurements in terms of this parameter. A single-parameter gamma-type distribution is introduced, and it is shown that inversion can only provide the dimensionless parameter, r/ab (where r = particle radius, a = effective radius, b = effective variance), at least when the distribution vanishes at both ends. The basic inversion problem in reconstructing the particle size distribution is analyzed, and the existing methods are reviewed (with emphasis on their capabilities) and classified. A two-step strategy is proposed for simultaneously determining the complex refractive index and reconstructing the size distribution of atmospheric particulates.

Fymat, A. L.↗

Deriving representative size distributions from UW OPC data for SAGE II extinction measurements

For the purposes of studying the impacts of aerosols on the chemistry and climate of the atmosphere, size distribution information has been inferred from extinction measurements for decades. Using the measurements from the University of Wyoming balloon-borne optical particle counter experiment we have derived representative size distributions at SAGE II channel wavelengths. These are bimodal lognormal size distributions grouped into bins of 525 to 1020 nm extinction ratio. Future work will include expanding this analysis to SAGE III’s channels and considering the effect of a absorbing channel in the IR would have.

Aerosol↗

Deriving Representative Size Distributions From UW OPC Data for Sage II Extinction Measurements

For the purposes of studying the impacts of aerosols on the chemistry and climate of the atmosphere, size distribution information has been inferred from extinction measurements for decades. Using the measurements from the University of Wyoming balloon-borne optical particle counter experiment we have derived representative size distributions at SAGE II channel wavelengths. These are bimodal lognormal size distributions grouped into bins of 525 to 1020 nm extinction ratio. However there exists fundamental limitations to the information that can be derived from SAGE measurements. Future work will include expanding this analysis to SAGE III’s channels and considering the effect of a absorbing channel in the IR would have.

Aerosol↗

Deriving Representative Size Distributions From UW OPC Data for Sage II Extinction Measurements

For the purposes of studying the impacts of aerosols on the chemistry and climate of the atmosphere, size distribution information has been inferred from extinction measurements for decades. Using the measurements from the University of Wyoming balloon-borne optical particle counter experiment we have derived representative size distributions at SAGE II channel wavelengths. These are bimodal lognormal size distributions grouped into bins of 525 to 1020 nm extinction ratio. However there exists fundamental limitations to the information that can be derived from SAGE measurements. Future work will include expanding this analysis to SAGE III’s channels and considering the effect of a absorbing channel in the IR would have.

Aerosol↗

Deriving Representative Size Distributions From UW OPC Data for Sage II Extinction Measurements

For the purposes of studying the impacts of aerosols on the chemistry and climate of the atmosphere, size distribution information has been inferred from extinction measurements for decades. Using the measurements from the University of Wyoming balloon-borne optical particle counter experiment we have derived representative size distributions at SAGE II channel wavelengths. These are bimodal lognormal size distributions grouped into bins of 525 to 1020 nm extinction ratio. However there exists fundamental limitations to the information that can be derived from SAGE measurements

Atmospheric composition↗

Retrieval of Stratospheric Aerosol Size Distribution Parameters Using Satellite Solar Occultation Measurements at Three Wavelengths

In this work, a novel approach for the determination of the particle size distribution (PSD) parameters of stratospheric sulfate aerosols is presented. For this, ratios of extinction coefficients obtained from SAGE III/ISS (Stratospheric Aerosol and Gas Experiment III on the International Space Station) solar occultation measurements at 449, 756 and 1544 nm were used to retrieve the mode width and median radius of a size distribution assumed to be monomodal lognormal. The estimated errors at the peak of the stratospheric aerosol layer, on average, lie between 20% and 25% for the median radius and 5% and 7% for the mode width. The results are consistent in magnitude with other retrieval results from the literature, but a robust comparison is difficult, mainly because of differences in temporal and spatial coverage. Other quantities like number density and effective radius were also calculated. A major advantage of the described method over other retrieval techniques is that both the median radius and the mode width can be retrieved simultaneously, without having to assume one of them. This is possible due to the broad wavelength spectrum covered by the SAGE III/ISS measurements. Also, the presented method – being based on the analysis of three wavelengths – allows unique solutions for the retrieval of PSD parameters for almost all of the observed extinction spectra, which is not the case when using only two spectral channels. In addition, the extinction coefficients from SAGE III/ISS solar occultation measurements, on which the retrieval is based, are calculated without a priori assumptions about the PSD. For those reasons, the data produced with the presented retrieval technique may be a valuable contribution for a better understanding of the variability of stratospheric aerosol size distributions, e.g. after volcanic eruptions. While this study focuses on describing the retrieval method, and a future study will discuss the PSD parameter data set produced in depth, some exemplary results for background conditions in June 2017 are shown.

Felix Wrana↗

Sensitivity of C-Band Polarimetric Radar-Based Drop Size Distribution Measurements to Maximum Diameter Assumptions

The estimation of rain drop size distribution (DSD) parameters from polarimetric radar observations is accomplished by first establishing a relationship between differential reflectivity (Z(sub dr)) and the central tendency of the rain DSD such as the median volume diameter (D0). Since Z(sub dr) does not provide a direct measurement of DSD central tendency, the relationship is typically derived empirically from rain drop and radar scattering models (e.g., D0 = F[Z (sub dr)] ). Past studies have explored the general sensitivity of these models to temperature, radar wavelength, the drop shape vs. size relation, and DSD variability. Much progress has been made in recent years in measuring the drop shape and DSD variability using surface-based disdrometers, such as the 2D Video disdrometer (2DVD), and documenting their impact on polarimetric radar techniques. In addition to measuring drop shape, another advantage of the 2DVD over earlier impact type disdrometers is its ability to resolve drop diameters in excess of 5 mm. Despite this improvement, the sampling limitations of a disdrometer, including the 2DVD, make it very difficult to adequately measure the maximum drop diameter (D(sub max)) present in a typical radar resolution volume. As a result, D(sub max) must still be assumed in the drop and radar models from which D0 = F[Z(sub dr)] is derived. Since scattering resonance at C-band wavelengths begins to occur in drop diameters larger than about 5 mm, modeled C-band radar parameters, particularly Z(sub dr), can be sensitive to D(sub max) assumptions. In past C-band radar studies, a variety of D(sub max) assumptions have been made, including the actual disdrometer estimate of D(sub max) during a typical sampling period (e.g., 1-3 minutes), D(sub max) = C (where C is constant at values from 5 to 8 mm), and D(sub max) = M*D0 (where the constant multiple, M, is fixed at values ranging from 2.5 to 3.5). The overall objective of this NASA Global Precipitation Measurement Mission (GPM/PMM Science Team)-funded study is to document the sensitivity of DSD measurements, including estimates of D0, from C-band Z(sub dr) and reflectivity to this range of D(sub max) assumptions. For this study, GPM Ground Validation 2DVD's were operated under the scanning domain of the UAHuntsville ARMOR C-band dual-polarimetric radar. Approximately 7500 minutes of DSD data were collected and processed to create gamma size distribution parameters using a truncated method of moments approach. After creating the gamma parameter datasets the DSD's were then used as input to a T-matrix model for computation of polarimetric radar moments at C-band. All necessary model parameterizations, such as temperature, drop shape, and drop fall mode, were fixed at typically accepted values while the D(sub max) assumption was allowed to vary in sensitivity tests. By hypothesizing a DSD model with D(sub max) (fit) from which the empirical fit to D0 = F[Z(sub dr)] was derived via non-linear least squares regression and a separate reference DSD model with D(sub max) (truth), bias and standard error in D0 retrievals were estimated in the presence of Z(sub dr) measurement error and hypothesized mismatch in D(sub max) assumptions. Although the normalized standard error for D0 = F[Z(sub dr)r] can increase slightly (as much as from 11% to 16% for all 7500 DSDs) when the D(sub max) (fit) does not match D(sub max) (truth), the primary impact of uncertainty in D(sub max) is a potential increase in normalized bias error in D0 (from 0% to as much as 10% over all 7500 DSDs, depending on the extent of the mismatch between D(sub max) (fit) and D(sub max) (truth)). For DSDs characterized by large Z(sub dr) (Z(sub dr) > 1.5 to 2.0 dB), the normalized bias error for D0 estimation at C-band is sometimes unacceptably large (> 10%), again depending on the extent of the hypothesized D(sub max) mismatch. Modeled errors in D0 retrievals from Z(sub dr) at C-band are demonstrated in detail and comparedo similar modeled retrieval errors at S-band and X-band where the sensitivity to D(sub max) is expected to be less. The impact of D(sub max) assumptions to the retrieval of other DSD parameters such as Nw, the liquid water content normalized intercept parameter, are also explored. Likely implications for DSD retrievals using C-band polarimetric radar for GPM are assessed by considering current community knowledge regarding D(sub max) and quantifying the statistical distribution of Z(sub dr) from ARMOR over a large variety of meteorological conditions. Based on these results and the prevalence of C-band polarimetric radars worldwide, a call for more emphasis on constraining our observational estimate of D(sub max) within a typical radar resolution volume is made

Carey, Lawrence D.↗

The measurement of the size distribution of artificial fogs

The size-distribution of the fog droplets at various fog particle concentrations in fog chamber was determined by two methods: (1) the Stokes' velocity photographic method and (2) using the active scattering particle spectrometer. It is shown that the two techniques are accurate in two different ranges of particle size - the former in the radii range (0.1 micrometers to 10.0 micrometers), and the latter for radii greater than 10.0 micrometers. This was particularly true for high particle concentration, low visibility fogs.

Deepak, A.↗

Enhanced resolution particle size distributions by multiple angle photon correlation spectroscopy

Photon correlation spectroscopy (PCS) has become a method of choice for measuring submicrometer particles. It is capable of rapid, accurate measurements of mean particle size. Since the measurements are nonperturbing, it is ideal for monitoring systems undergoing dynamic changes. Despite its widespread acceptance, the information content of PCS measurements for particle size distributions is low and provides limited resolution. A method is presented whereby PCS measurements made at several scattering angles plus the angular distribution of light scattered from the particles are combined in a single simultaneous analysis to effect an enhanced resolution particle size distribution. The efficacy of the method is assessed by recovering size distributions from computer simulated data and by comparisons of conventional PCS measurements of polystyrene spheres with those made by the new method.

Bott, Steven E.↗

Hydrometeor Size Distribution Measurements by Imaging the Attenuation of a Laser Spot

The optical extinction of a laser due to scattering of particles is a well-known phenomenon. In a laboratory environment, this physical principle is known as the Beer-Lambert law, and is often used to measure the concentration of scattering particles in a fluid or gas. This method has been experimentally shown to be a usable means to measure the dust density from a rocket plume interaction with the lunar surface. Using the same principles and experimental arrangement, this technique can be applied to hydrometeor size distributions, and for launch-pad operations, specifically as a passive hail detection and measurement system. Calibration of a hail monitoring system is a difficult process. In the past, it has required comparison to another means of measuring hydrometeor size and density. Using a technique recently developed for estimating the density of surface dust dispersed during a rocket landing, measuring the extinction of a laser passing through hail (or dust in the rocket case) yields an estimate of the second moment of the particle cloud, and hydrometeor size distribution in the terrestrial meteorological case. With the exception of disdrometers, instruments that measure rain and hail fall make indirect measurements of the drop-size distribution. Instruments that scatter microwaves off of hydrometeors, such as the WSR-88D (Weather Surveillance Radar 88 Doppler), vertical wind profilers, and microwave disdrometers, measure the sixth moment of the drop size distribution (DSD). By projecting a laser onto a target, changes in brightness of the laser spot against the target background during rain and hail yield a measurement of the DSD's second moment by way of the Beer-Lambert law. In order to detect the laser attenuation within the 8-bit resolution of most camera image arrays, a minimum path length is required. Depending on the intensity of the hail fall rate for moderate to heavy rainfall, a laser path length of 100 m is sufficient to measure variations in optical extinction using a digital camera. For hail fall only, the laser path may be shorter because of greater scattering due to the properties of hailstones versus raindrops. A photodetector may replace the camera in automated installations. Laser-based rain and hail measurement systems are available, but they are based on measuring the interruption of a thin laser beam, thus counting individual hydrometeors. These systems are true disdrometers since they also measure size and velocity. The method reported here is a simple method, requiring far less processing, but it is not a disdrometer.

Lane, John↗

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↗