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At least 397 records · Page 22

Managing Traffic on the Three-Way Street: Steps Toward Closing the Aerosol Forcing Uncertainty Gap

Understanding changes in the radiative forcing of climate is critical for any effort to attribute, mitigate, or predict climate change. Although greenhouse gases (GHGs) contribute most of the radiative forcing, uncertainty in the climate forcing by airborne particles (aerosols) dominates the uncertainty in forcing changes overall. Yet, aerosol forcing has remained virtually undiminished for more than 20 years despite considerable advances in most of the key contributing elements. Satellite and suborbital measurements, as well as modeling, each have essential roles to play in reducing the uncertainty in the aerosol forcing of climate. This presentation will begin by briefly covering the reasons why aerosols are important for climate study, and will then summarize what we are learning about aerosols from current satellite remote-sensing work, and allude to the roles of suborbital measurements and models. Emphasis will be placed on nascent efforts to link satellite data with models, the need to continue as planned current programs supporting advanced, global-scale satellite and surface-based aerosol and precursor gas observations, climate modeling, as well as intensive field campaigns aimed at characterizing the underlying physical and chemical processes involved. The talk will conclude by highlighting new efforts needed to obtain systematic in situ measurements of aerosol microphysical and chemical properties, along with a greater research focus on integrating the unique contributions of measurements and modeling toward reducing the aerosol climate forcing uncertainty gap.

aerosol↗

Contemporary sources dominate carbonaceous aerosol on the North Slope of Alaska

As the Arctic continues to change and warm rapidly, it is increasingly important to understand the organic carbon (OC) contribution to Arctic aerosol. Biogenic sources of primary and secondary OC in the Arctic will be impacted by climate change, including warming temperatures and earlier snow and ice melt. Here, this study focuses on identifying potential sources and regional influences on the seasonal concentration of organic aerosol through analysis of chemical and isotopic composition. Aerosol samples were collected at two sites on the North Slope of Alaska ($Utqia\dot{g}vik$, UQK, and Oliktok Point, OLK, which is in an Arctic oilfield) over three summers from 2015 to 2017. The elemental carbon (EC) trends at each site were used to understand local combustion influences. Local sources drove EC concentrations at Oliktok Point, where high EC was attributed to oil and gas extraction activity, including diesel combustion emissions. $Utqia\dot{g}vik$ had very low EC in the summer. OC was more similar in concentration and well correlated between the two sites with high contributions of contemporary carbon by radiocarbon apportionment (UQK = 74%, OLK = 63%), which could include both marine and terrestrial sources of contemporary carbon (e.g. primary and secondary biogenic, biomass burning and/or associated SOA, and bioaerosols). OC concentrations are strongly correlated to maximum ambient temperatures on the NSA during the summer, which may have implications for predicting future OC aerosol concentrations in a warming Arctic. Biomass burning was determined to be an episodic influence at both sites, based on interpretation of combined aerosol composition, air mass trajectories, and remote sensing of smoke plumes. The results from this study overall strongly suggests contribution from regional sources of contemporary organic aerosol on the NSA, but additional analysis is needed to better constrain contributions from both biogenic sources (terrestrial and/or marine) and bioaerosol to better understand temperature-related aerosol processes in the Arctic.

54 ENVIRONMENTAL SCIENCES↗

Atmospheric Effects on Remote Sensing of the Earth's Surface

The main causes and magnitude of the atmospheric effects on remote sensing of the Earth's surface are determined. Theoretical study as well as measurements are included. The knowledge gained from this study will be used to develop atmospheric correction algorithms and to test them with satellite data. In a theoretical investigation of the relative effects of the aerosol optical thickness, absorption, and size distribution on remote sensing, it was found that aerosol absorption has a significant effect on satellite measurements of surface reflectivity. The absorption effect is stronger for high than for low surface reflectances. The aerosol optical thickness is dominant for small surface reflectances. The accuracy of clustering algorithms depends on both parameters. The vegetation index, however, is affected by the optical thickness but only weakly affected by the absorption. A laboratory simulation of the atmospheric effect on the radiance of sunlight scattered from the Earth's surface-atmosphere system was performed. This experiment verified the existence of the adjacency effect (the effect of a bright field on the radiance detected above a dark field) and was used to test 3-D radiative transfer models. In a theoretical study it was found that atmospheric scattering resulting from the adjacency effect reduces the separability between surface classes.

Fraser, R. E.↗

3D Radiative Aspects of the Increased Aerosol Optical Depth Near Clouds

To characterize aerosol-cloud interactions it is important to correctly retrieve aerosol optical depth in the vicinity of clouds. It is well reported in the literature that aerosol optical depth increases with cloud cover. Part of the increase comes from real physics as humidification; another part, however, comes from 3D cloud effects in the remote sensing retrievals. In many cases it is hard to say whether the retrieved increased values of aerosol optical depth are remote sensing artifacts or real. In the presentation, we will discuss how the 3D cloud affects can be mitigated. We will demonstrate a simple model that can assess the enhanced illumination of cloud-free columns in the vicinity of clouds. This model is based on the assumption that the enhancement in the cloud-free column radiance comes from the enhanced Rayleigh scattering due to presence of surrounding clouds. A stochastic cloud model of broken cloudiness is used to simulate the upward flux.

Marshak, Alexander↗

Measurements and Modeling of Aerosol Absorption and Single Scattering Albedo at Ambient Relative Hum

Uncertainties in the aerosol single scattering albedo have been identified to be an important source of errors in current large-scale model estimates of the direct aerosol radiative forcing of climate. A number of investigators have obtained estimates of the single scattering albedo from a variety of remote sensing and in situ measurements during aerosol field experiments. During the Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX, 1996) for example, estimates of the aerosol single scattering albedo were obtained (1) as a best-fit parameter in comparing radiative flux changes measured by airborne pyranometer to those computed from independently measured aerosol properties; (2) from estimates of the aerosol complex index of refraction derived using a combination of airborne sunphotometer, lidar backscatter and in situ size distribution measurements; and (3) from airborne measurements of aerosol scattering and absorption using nephelometers and absorption photometers. In this paper, we briefly compare the results of the latter two methods for two TARFOX case studies, since those techniques provide height-resolved information about the aerosol single scattering albedo. Estimates of the aerosol single scattering albedo from nephelometer and absorption photometer measurements require knowledge of the scattering and absorption humidification (i.e., the increase in these properties in response to an increase in ambient relative humidity), since both measurements are usually carried out at a relative humidity different from the ambient atmosphere. In principle, the scattering humidification factor can be measured, but there is currently no technique widely available to measure the absorption of an aerosol sample as a function of relative humidity. Frequently, for lack of better knowledge, the absorption humidification is assumed to be unity (meaning that there is no change in aerosol absorption due to an increase in ambient relative humidity). This assumption then enters the estimate of the single scattering albedo at ambient relative humidity. To investigate the validity of this assumption we have carried out modeling studies of the absorption humidification factor, assuming that the aerosols contain an insoluble soot core and a coating which determines its hygroscopic growth behavior. The aerosol optical properties are then computed on the basis of the shell/core particle morphology using a Mie-code for concentric shells. From basic physical principles, it is conceivable that aerosol absorption increases when an atmospheric aerosol particle collects a non-absorbing shell, since the soot core is then exposed to an increased (focused) electric field strength. Indeed, our preliminary modeling studies show that the absorption of an atmospheric aerosol particle composed of a soot core and an aqueous sulfuric acid shell may increase by a factor of 50% due to a change in ambient relative humidity from 30 to 95%. We will show how this increased absorption is a function of the initial particle size and soot mass fraction.

Redemann, J.↗

A Sensitivity Study on the Effects of Particle Chemistry, Asphericity and Size on the Mass Extinction Efficiency of Mineral Dust in the Earth's Atmosphere: From the Near to Thermal IR

To determine a plausible range of mass extinction efficiencies (MEE) of terrestrial atmospheric dust from the near to thermal IR, sensitivity analyses are performed over an extended range of dust microphysical and chemistry perturbations. The IR values are subsequently compared to those in the near-IR, to evaluate spectral relationships in their optical properties. Synthesized size distributions consistent with measurements, model particle size, while composition is defined by the refractive indices of minerals routinely observed in dust, including the widely used OPAC/Hess parameterization. Single-scattering properties of representative dust particle shapes are calculated using the T-matrix, Discrete Dipole Approximation and Lorenz-Mie light-scattering codes. For the parameterizations examined, MEE ranges from nearly zero to 1.2 square meters per gram, with the higher values associated with non-spheres composed of quartz and gypsum. At near-IR wavelengths, MEE for non-spheres generally exceeds those for spheres, while in the thermal IR, shape-induced changes in MEE strongly depend on volume median diameter (VMD) and wavelength, particularly for MEE evaluated at the mineral resonant frequencies. MEE spectral distributions appear to follow particle geometry and are evidence for shape dependency in the optical properties. It is also shown that non-spheres best reproduce the positions of prominent absorption peaks found in silicates. Generally, angular particles exhibit wider and more symmetric MEE spectral distribution patterns from 8-10 micrometers than those with smooth surfaces, likely due to their edge-effects. Lastly, MEE ratios allow for inferring dust optical properties across the visible-IR spectrum. We conclude the MEE of dust aerosol are significant for the parameter space investigated, and are a key component for remote sensing applications and the study of direct aerosol radiative effects.

Hansell, R. A., Jr.↗

Optimal Estimation Framework for Ocean Color Atmospheric Correction and Pixel-level Uncertainty Quantification

Ocean color remote sensing requires compensation for atmospheric scattering and absorption (aerosol, Rayleigh, and trace gases), referred to as atmospheric correction (AC). AC allows inference of parameters such as spectrally resolved remote sensing reflectance ( R rs )(λ) ; sr 1 ) at the ocean surface from the top-of-atmosphere reflectance. Often, the uncertainty of this process is not fully explored. Bayesian inference techniques provide a simultaneous AC and uncertainty assessment via a full posterior distribution of the relevant variables, given the prior distribution of those variables and the radiative transfer (RT) likelihood function. Given uncertainties in the algorithm inputs, the Bayesian framework enables better constraints on the AC process by using the complete spectral information compared to traditional approaches that use only a subset of bands for AC. This paper investigates a Bayesian inference research method (Optimal Estimation, OE) for ocean color AC by simultaneously retrieving atmospheric and ocean properties using all visible and near-infrared spectral bands. The OE algorithm analytically approximates the posterior distribution of parameters based on normality assumptions and provides a potentially viable operational algorithm with a reduced computational expense. We developed a Neural Network (NN) RT forward model look-up-table-based emulator to increase algorithm efficiency further and thus speed up the likelihood computations. We then applied the OE algorithm to synthetic data and observations from the MODerate resolution Imaging Spectroradiometer (MODIS) on NASA’s Aqua spacecraft. We compared the R rs )(λ) retrieval and its uncertainty estimates from the OE method with in-situ validation data from the SeaWiFS Bio-optical Archive and Storage System (SeaBASS) and Aerosol Robotic Network Ocean Color (AERONET-OC) datasets. The OE algorithm improved R rs )(λ) estimates relative to the NASA standard operational algorithm by improving all statistical metrics at 443, 555, and 667 nm. Unphysical negative R rs )(λ) , which often appear in complex water conditions, was reduced by a factor of 3. The OE-derived pixel-level R rs )(λ) uncertainty estimates were also assessed relative to in-situ data and were shown to have skill.

Atmospheric correction↗

3D Cloud Aerosol Precipitation Experiment at kennaook Cape Grim (3D-CAPE-k) Field Campaign Report

The objective of this campaign was to complement the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) User Facility’s Cloud And Precipitation Experiment at kennaook (CAPE-k) in northwest Tasmania by deploying scanning, fixed pointing angle, and in situ aerosol, cloud, and precipitation remote-sensing instruments during the last six months of the experiment. These instruments provided a three-dimensional (3D) context to the second ARM Mobile Facility (AMF2) vertically pointing observations collected at the kennaook Cape Grim (KCG) site and captured a portion of the life cycle of the clouds before and after the passage over the AMF2 vertical column. These 3D cloud measurements will be used in the near future to 1) investigate how the vertical profiles of aerosol and cloud properties are representative of the broader area and how these properties evolve during the portion of the cloud life cycle captured by the scanning instruments, 2) quantify how accurate the cloud fraction derived with assumptions from vertically pointing observations are compared with direct 3D cloud fraction measurements, 3) evaluate cloud fraction and liquid water path in the Australian Community Climate and Earth-System Simulator–Convective-scale (ACCESS-C) forecast model, and 4) evaluate aerosol and cloud products from the European Space Agency/Japanese Aerospace Exploration Agency (ESA/JAXA) Earth Cloud Aerosol Radiation Explorer (EarthCARE) mission using the scanning measurements, offering more chances of exact collocation, thereby complementing the statistical approach we are planning to employ with AMF2 observations for that same purpose.

54 ENVIRONMENTAL SCIENCES↗

Arctic Radiation-Cloud-Aerosol-Surface Interaction eXperiment (ARCSIX)

The Arctic climate system is amidst a transition. Over the last 40 years, the Arctic sea ice pack has transformed from a predominantly thick, multi-year sea ice to a predominantly thin, seasonal sea ice, termed the “New Arctic”. The observed rapid changes in the Arctic sea ice pack are an integral part of the Arctic Amplification phenomenon and represent a response to and a feedback on global climate change. As a result, the role of the Arctic within the global climate system is changing. Substantial uncertainty exists in our understanding of the atmosphere-surface interactions within the Arctic system, limiting our knowledge of the Arctic’s role in the future climate. Advancing our understanding of the Arctic climate system requires (1) measurements of the coupling between radiative processes and sea ice surface properties during summer sea ice melt; (2) measurements of the processes controlling the predominant Arctic cloud regimes and their properties (Fig. 1); and (3) improvements in the ability to monitor Arctic cloud, radiation, and sea ice processes from space. A key challenge is that thin, low clouds that are radiatively important to the Arctic surface energy budget can go undetected (Fig. 1). The Arctic Radiation-Cloud-Aerosol-Surface-Interaction eXperiment (ARCSIX) is an airborne campaign based at the Pituffik Space Base in Greenland from May-August 2024 sponsored by the National Aeronautics and Space Administration (NASA) to address these needs. ARCSIX consists of two airborne measurement campaigns taking place in two 3-week intervals during the early and late sea ice melt season: late May through early June and late July through early August, respectively. ARCSIX science is guided by three broad science questions that encapsulate the key influences of radiation-cloud-aerosol-sea ice coupling and a remote sensing and modeling objective: Science Question 1 (Radiation): What is the impact of the predominant summer Arctic cloud types on the radiative surface energy budget? Science Question 2 (Cloud Life Cycle): What processes control the evolution and maintenance of the predominant cloud regimes in the summertime Arctic? Science Question 3 (Sea Ice): How do the two-way interactions between surface properties and atmospheric forcings affect the sea ice evolution? Remote Sensing and Modeling Objective: Enhance our long-term space-based monitoring and predictive capabilities of Arctic sea ice, clouds, and aerosols.

Patrick Taylor↗

MISR Multi-Angle Imaging SpectroRadiometer

This viewgraph presentation reviews the concept of the Multi-Angle Imaging SpectroRadiometer (MISR), a methodology to use the MISR to retrieve aerosols over water and land. The presentation shows some of the results of the use of the MISR in graphs and charts. Multi-angle remote sensing provides unique ways of retrieving aerosol properties over many surface types, including bright deserts which are major source regions.

global maps↗

Inversion of Multiangular Polarimetric Measurements Over Open and Coastal Ocean Waters: A Joint Retrieval Algorithm for Aerosol and Water-Leaving Radiance Properties

Ocean color remote sensing is a challenging task over coastal waters due to the complex optical properties of aerosols and hydrosols. In order to conduct accurate atmospheric correction, we previously implemented a joint retrieval algorithm, hereafter referred to as the Multi-Angular Polarimetric Ocean coLor (MAPOL) algorithm, to obtain the aerosol and water-leaving signal simultaneously. The MAPOL algorithm has been validated with synthetic data generated by a vector radiative transfer model, and good retrieval performance has been demonstrated in terms of both aerosol and ocean water optical properties (Gao et al., 2018). In this work we applied the algorithm to airborne polarimetric measurements from the Research Scanning Polarimeter (RSP) over both open and coastal ocean waters acquired in two field campaigns: the Ship-Aircraft Bio-Optical Research (SABOR) in 2014 and the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) in 2015 and 2016. Two different yet related bio-optical models are designed for ocean water properties. One model aligns with traditional open ocean water bio-optical models that parameterize the ocean optical properties in terms of the concentration of chlorophyll a. The other is a generalized bio-optical model for coastal waters that includes seven free parameters to describe the absorption and scattering by phytoplankton, colored dissolved organic matter, and nonalgal particles. The retrieval errors of both aerosol optical depth and the water-leaving radiance are evaluated. Through the comparisons with ocean color data products from both in situ measurements and the Moderate Resolution Imaging Spectroradiometer (MODIS), and the aerosol product from both the High Spectral Resolution Lidar (HSRL) and the Aerosol Robotic Network (AERONET), the MAPOL algorithm demonstrates both flexibility and accuracy in retrieving aerosol and water-leaving radiance properties under various aerosol and ocean water conditions.

Gao, Meng↗

Spectral Derivatives of Optical Depth for Partitioning Aerosol Type and Loading

Quantifying aerosol compositions (e.g., type, loading) from remotely sensed measurements by spaceborne, suborbital and ground-based platforms is a challenging task. In this study, the first and second-order spectral derivatives of aerosol optical depth (AOD) with respect to wavelength are explored to determine the partitions of the major components of aerosols based on the spectral dependence of their particle optical size and complex refractive index. With theoretical simulations from the Second Simulation of a Satellite Signal in the Solar Spectrum (6S) model, AOD spectral derivatives are characterized for collective models of aerosol types, such as mineral dust (DS) particles, biomass-burning (BB) aerosols and anthropogenic pollutants (AP), as well as stretching out to the mixtures among them. Based on the intrinsic values from normalized spectral derivatives, referenced as the Normalized Derivative Aerosol Index (NDAI), a unique pattern is clearly exhibited for bounding the major aerosol components; in turn, fractions of the total AOD (fAOD) for major aerosol components can be extracted. The subtlety of this NDAI method is examined by using measurements of typical aerosol cases identified carefully by the ground-based Aerosol Robotic Network (AERONET) sun–sky spectroradiometer. The results may be highly practicable for quantifying fAOD among mixed-type aerosols by means of the normalized AOD spectral derivatives.

aerosol partition↗

Accounting for 3D Radiative Effects in MODIS Aerosol Retrievals near Clouds using CALIPSO Observations

Retrievals of aerosol properties near clouds from passive remote sensing is challenging. Sunlight scattered by clouds into nearby clear regions can effectively enhance the clear area reflectance. These cloud 3D radiative effects may lead to large biases in aerosol retrievals if uncorrected, risking an incorrect interpretation of satellite observations for aerosol-cloud interaction in cloudy atmosphere. In earlier studies, we developed a simple two-layer model (2LM) to estimate the cloud-induced clear-sky radiance enhancements in cloud fields. In this study, we take advantage of CALIPSO lidar observations, which should not be affected by the 3D radiative effect, to study passive aerosol retrievals in cloud fields in the Amazon region, specifically those produced by the operational Dark Target algorithm applied to Aqua-MODIS. From two-years’ worth of co-located CALIPSO/MODIS aerosol retrievals, we find a larger increase in operationally retrieved MODIS AOD from clear to cloudy regions (~0.075 or ~40%) than for the CALIPSO AOD (~0.021 or ~20%). The much larger increase in MODIS AOD is mainly due to the 3D radiative effects. After using the 2LM model to account for cloud 3D radiative effects, the clear to cloudy increase in MODIS AOD was reduced to ~0.043 (~23%), much closer to CALIPSO observations. The 3D corrected average MODIS AOD for cloudy scenes is significantly larger than AOD for clear conditions, even for cloud fraction (CF) less than 0.1, suggesting aerosols in cloudy scenes are characteristically different from aerosols in clear conditions. Furthermore, the 3D correction of AOD (i.e., τ_1D-τ_3D) increases linearly with CF for a large range of CF. We have also examined the impact of the 3D effect on aerosol Ångström Exponent (AE) and fine model fraction (FMF) of AOD. We found that the uncorrected average AE and FMF depend strongly on CF, ~25% increase in AE (decrease in particle size) and ~60% increase in FMF as CF increases from 0.05 to 0.45. The 3D correction leads to smaller average AE (bigger particle size) and FMF that are almost independent of CF. Thus, the 3D corrected aerosol properties are expected to provide more accurate information for better understanding aerosol-cloud interactions.

MODIS↗

Overview of ACTIVATE’s First Year of Flights Targeting Aerosol-Cloud-Meteorology Interactions

The Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) included 40 research flights in the winter and summer months of 2020 using a two-aircraft approach to simultaneously obtain in situ and remote sensing data of regions below, inside, and above boundary layer clouds. This presentation will summarize early findings from the first year of ACTIVATE flights with focus on aerosol and cloud droplet number concentration behavior, formation and evolution of clouds, and analysis of remote sensing retrievals of aerosol and cloud properties. There is a clear annual cycle in cloud droplet number concentration suggesting a marked annual cycle in aerosol-cloud interactions. Although aerosol particles are more abundant in spring and summer, the conditions needed to activate those particles into cloud droplets are weaker than in other colder months. Several flights targeted post-frontal clouds associated with cold air outbreaks pointing to enhanced levels of nucleated particles immediately above such clouds, and that ice formation hastens the transition from closed to open cloud structures in the sampled CAO events. Also observed in the marine boundary layer during CAOs is the frequent occurrence of non-spherical sea salt particles, which has significant implications for remote sensing retrievals.

Taylor Shingler↗

Excitation of optically trapped single particles using femtosecond pulses

Excitation from optically trapped particles is examined through laser-induced breakdown spectroscopy following interactions with mJ-level fs pulses. Optical emissions from sub-ng ablation of precisely positioned cupric oxide microparticles are used as a method to spatially resolve laser–particle interactions resulting in excitation. External focusing lenses are often used to change the dynamics of nonlinear self-focusing of fs pulses to form laser filaments or, alternatively, to form very intense air plasmas. Given the significant implications external focusing has on laser propagation and plasma conditions, single-particle emissions are studied with focusing lenses ranging from 50 to 300 mm. It is shown that, while single particles are less excited at longer focal lengths due to limited energy transfer through laser–particle interactions, the cooler plasma results in a lower thermal background to reveal resolved single-shot emission peaks. Furthermore, by developing an understanding in the fundamental interaction that occurs between single particles and fs pulses and filaments, practical improvements can be made for atmospheric remote sensing of low-concentration aerosols.

42 ENGINEERING↗

Validation of lidar and satellite remote sensing

Validation of observations is an important part of any remote sensing program. With respect to aerosols this is exceedingly difficult because each technique typically measures a different aerosol parameter. Correlative sensors, therefore, must be capable of measuring the same parameter over the same size range or include enough measurements to properly characterize the aerosol, possibly with the assistance of models. In any correlative measurement program, simultaneity in space and time is required. This can be less restrictive during periods of atmospheric stability. The discussion is presented which is focused on the validation programs developed for NASA's Stratospheric Aerosol Measurement (SAM II), and the Stratospheric Aerosol and Gas Experiments I and II (SAGE I and II). To date these were limited to the stratosphere. Since satellite sensors are capable of providing near-global and long-term observations, periodic correlative observations over various global locations and seasons are required for assuring that data quality is unchanged, or for understanding any changes observed.

Mccormick, M. P.↗

Infrared spectroscopy of homogeneously nucleated hydrazine aerosols - Disordered and crystalline phases

It is shown that aerosols generated at low temperatures and high condensation rate spontaneously form in a highly crystalline state. The resonant absorption bands in the IR spectra of these highly crystalline particles are much sharper than any reported previously in the bulk, and reveal details in the N-H vibrational bands that have not been previously observed. A disordered phase is also observed at somewhat higher temperatures. These results are consistent with this being a supercooled liquid. The fact that the spectra associated with these two aerosol phases are quite different is important to any future attempts at detecting hydrazine aerosols in planetary atmospheres by remote sensing techniques.

Dunder, T.↗