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DOE OSTI2024

Probing the dynamics and bottleneck of the key atmospheric SO 2 oxidation reaction by the hydroxyl radical

SO 2 (Sulfur dioxide) is the major precursor to the production of sulfuric acid (H 2 SO 4 ), contributing to acid rain and atmospheric aerosols. Sulfuric acid formed from SO 2 generates light-reflecting sulfate aerosol particles in the atmosphere. This property has prompted recent geoengineering proposals to inject sulfuric acid or its precursors into the Earth’s atmosphere to increase the planetary albedo to counteract global warming. SO 2 oxidation in the atmosphere by the hydroxyl radical HO to form HOSO 2 is a key rate-limiting step in the mechanism for forming acid rain. However, the dynamics of the HO + SO 2 → HOSO 2 reaction and its slow rate in the atmosphere are poorly understood to date. Herein, we use photoelectron spectroscopy of cryogenically cooled HOSO 2 – anion to access the neutral HOSO 2 radical near the transition state of the HO + SO 2 reaction. Spectroscopic and dynamic calculations are conducted on the first ab initio-based full-dimensional potential energy surface to interpret the photoelectron spectra of HOSO 2 – and to probe the dynamics of the HO + SO 2 reaction. In addition to the finding of a unique pre-reaction complex (HO⋯SO 2 ) directly connected to the transition state, dynamic calculations reveal that the accessible phase space for the HO + SO 2 → HOSO 2 reaction is extremely narrow, forming a key reaction bottleneck and slowing the reaction rate in the atmosphere, despite the low reaction barrier. This study underlines the importance of understanding the full multidimensional potential energy surface to elucidate the dynamics of complex bimolecular reactions involving polyatomic reactants.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Micropulse Lidar (MPL) Handbook

The micropulse lidar (MPL) is a ground-based optical remote sensing system designed primarily to determine the altitude of clouds overhead. The physical principle is the same as for radar. Pulses of energy are transmitted into the atmosphere; the energy scattered back to the transceiver is collected and measured as a time-resolved signal. From the time delay between each outgoing transmitted pulse and the backscattered signal, the distance to the scatterer is infered. Besides real-time detection of clouds, post-processing of the lidar return can also characterize the extent and properties of aerosol or other particle-laden regions.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1992

Climate forcing by anthropogenic aerosols

Although long considered to be of marginal importance to global climate change, tropospheric aerosol contributes substantially to radiative forcing, and anthropogenic sulfate aerosol, in particular, has imposed a major perturbation to this forcing. Both the direct scattering of short-wavelength solar radiation and the modification of the shortwave reflective properties of clouds by sulfate aerosol particles increase planetary albedo, thereby exerting a cooling influence on the planet. Current climate forcing due to anthropogenic sulfate is estimated to be -1 to -2 watts per square meter, globally averaged. This perturbation is comparable in magnitude to current anthropogenic greenhouse gas forcing but opposite in sign. Thus, the aerosol forcing has likely offset global greenhouse warming to a substantial degree. However, differences in geographical and seasonal distributions of these forcings preclude any simple compensation. Aerosol effects must be taken into account in evaluating anthropogenic influences on past, current, and projected future climate and in formulating policy regarding controls on emission of greenhouse gases and sulfur dioxide. Resolution of such policy issues requires integrated research on the magnitude and geographical distribution of aerosol climate forcing and on the controlling chemical and physical processes.

Charlson, R. J.↗

NASA NTRS1993

Probing Venus's cloud structure with Galileo NIMS

The spectral image cubes obtained by the Near-Infrared Mapping Spectrometer (NIMS) on Galileo as it flew by Venus have been analyzed to constrain the vertical structure of the clouds, the nature of the aerosol particles, and the location and particle properties of the opacity variations responsible for high-contrast features observed in the near-infrared windows at 1.7 and 2.3 micrometers. A radiative transfer program was used to simulate mid-latitude curves of limb darkening at 3.7 micrometers. Best-fit models to these curves demonstrate that the upper clouds are dominated by mode 2 particles (r-bar = 1.0 micrometers), with a contribution of approximately 15% of opacity from mode 1 particles (r-bar = 0.3 micrometers). The low-latitude upper cloud is well represented by a dual scale-height model, with a particle scale height of approximately 1 km from an altitude of 61-63 km, and a scale height of approximately 6 km above this, up to the level where tau = 1 at approximately 71 km. This model also successfully simulates limb-darkening curves at 11.5 micrometers from the Pioneer Venus Orbiter Infrared Radiometer. Successful simulations of correlation plots of 1.7 vs 2.3 micrometers intensities reveal that mode 3 particles (r-bar = 3.65 micrometers) represent the dominant source of opacity in the lower and middle clouds, and that variation in total cloud opacity reflects chiefly the addition and removal of mode 3 particles near the cloud base. We find that the full spectrum of brightnesses at 1.7 and 2.3 micrometers implies that the total cloud optical depth varies from approximately 25 to approximately 40.

Grinspoon, D. H.↗

NASA NTRS1981

Reports from Science Mount St. Helens

The following reports describe extensive measurements of the properties of the gases and aerosols (particles) in the volcanic clouds produced by the eruptions of Mount St. Helens from March through August 1980. Volcanic material was first injected into the atmosphere on 27 March 1980. This material, as well as that introduced by subsequent eruptions during the next 2 months, was confined to the troposphere. On 18 May the first of several major explosions occurred in which some of the volcanic cloud penetrated well into the stratosphere. The nature of the volcanic activity at Mount St. Helens from the end of March through June was described.

Pollack, James B.↗

NASA NTRSDate not supplied

Early Fire Detection System for Partial and Low Gravity Environments

We present preliminary results on the development of a fire detection system for partial and low gravity environments. A significant challenge is the design of a system with a low false alarm rate. The detection system therefore has to discriminate between combustion particles, cabin, and lunar dust. Aerosol properties are measured and cross referenced to the target detectors at the Gases and Aerosols from Smoldering Polymers (GASP) Laboratory located at the NASA Glenn Research Center. A computational fluid dynamics plume model is also employed to determine the smoke transport properties of the targeted habitats.

Early fire detectioin↗

NASA NTRS2022

Space-based Passive Aerosol Remote Sensing from the Multi-angle Imaging SpectroRadiometer (MISR) Aboard NASA’s Terra Satellite

The Multi-angle Imaging SpectroRadiometer (MISR) instrument has been acquiring multi-angle imagery of the Earth aboard NASA’s Terra satellite since February 2000, providing an ongoing record of atmosphere and surface properties more than two decades long. MISR offers a combination of moderately high spatial resolution imagery at nine view angles in each of four visible/near-infrared spectral bands, global coverage about once per week, and carefully maintained onboard radiometric calibration. Unique algorithms retrieve aerosol column-amount and constraints on particle microphysical and optical properties, as well as the heights and motion vectors of aerosol plumes from sources such as wildfires, volcanic eruptions, and dust storms. Applications of MISR aerosol data to climate and air quality are discussed here along with a summary of some key scientific findings enabled by the instrument’s unique measurement approach.

aerosols↗

NASA NTRS1991

Volcanic aerosols: Chemistry, evolution, and effects

Stratospheric aerosols have been the subject of scientific speculation since the 1880s, when the powerful eruption of Krakatoa attracted worldwide attention to the upper atmosphere through spectacular optical displays. The presence of a permanent tenuous dust layer in the lower stratosphere was postulated in the 1920s following studies of the twilight glow. Junge collected the first samples of these 'dust' particles and demonstrated that they were actually composed of sulfates, most likely concentrated sulfuric acid (Junge and Manson, 1961; Junge, 1963). Subsequent research has been spurred by the realization that stratospheric particles can influence the surface climate of earth through their effects on atmospheric radiation. Such aerosols can also influence, through chemical and physical effects, the trace composition of the atmosphere, ozone concentrations, and atmospheric electrical properties. The properties of stratospheric aerosols (both the background particles and those enhanced by volcanic eruptions) were measured in situ by balloon ascents and high altitude aircraft sorties. The aerosols were also observed remotely from the ground and from satellites using both active (lidar) and passive (solar occultation) techniques (remote sensing instruments were carried on aircraft and balloon platforms as well). In connection with the experimental work, models were developed to test theories of particle formation and evolution, to guide measurement strategies, to provide a means of connecting laboratory and field data, and to apply the knowledge gained to answer practical questions about global changes in climate, depletion of the ozone layer, and related environmental problems.

Turco, Richard↗

NASA NTRS2008

Sensitivity of Multiangle Imaging to the Optical and Microphysical Properties of Biomass Burning Aerosols

The treatment of biomass burning (BB) carbonaceous particles in the Multiangle Imaging SpectroRadiometer (MISR) Standard Aerosol Retrieval Algorithm is assessed, and algorithm refinements are suggested, based on a theoretical sensitivity analysis and comparisons with near-coincident AERONET measurements at representative BB sites. Over the natural ranges of BB aerosol microphysical and optical properties observed in past field campaigns, patterns of retrieved Aerosol Optical Depth (AOD), particle size, and single scattering albedo (SSA) are evaluated. On the basis of the theoretical analysis, assuming total column AOD of 0.2, over a dark, uniform surface, MISR can distinguish two to three groups in each of size and SSA, except when the assumed atmospheric particles are significantly absorbing (mid-visible SSA approx.0.84), or of medium sizes (mean radius approx.0.13 pin); sensitivity to absorbing, medium-large size particles increases considerably when the assumed column AOD is raised to 0.5. MISR Research Aerosol Retrievals confirm the theoretical results, based on coincident AERONET inversions under BB-dominated conditions. When BB is externally mixed with dust in the atmosphere, dust optical model and surface reflection uncertainties, along with spatial variability, contribute to differences between the Research Retrievals and AERONET. These results suggest specific refinements to the MISR Standard Aerosol Algorithm complement of component particles and mixtures. They also highlight the importance for satellite aerosol retrievals of surface reflectance characterization, with accuracies that can be difficult to achieve with coupled surface-aerosol algorithms in some higher AOD situations.

Chen, Wei-Ting↗

DOE OSTI2025

Understanding Aitken Mode Aerosol Variability over the Southern Ocean and Antarctica: Insights from Cloud Condensation Nuclei Data

Aitken mode aerosol particles play an important role influencing cloud properties and sustenance, acting as a reservoir of potential cloud condensation nuclei against precipitation scavenging. However, there is limited data on Aitken mode aerosols. In this study, we develop a method to estimate Aitken mode aerosol concentrations and size distribution using cloud condensation nuclei measurements (CCN) and κ-Köhler theory. The performance of this method is evaluated using scanning mobility particle sizer (SMPS) data from recent field campaigns to demonstrate its skills and applicability. The method reasonably estimates Aitken- and accumulation-mode aerosol concentrations, achieving correlations of 0.7–0.9 with only modest biases (mean fractional bias within ±23% for Aitken mode and ±34% for accumulation-mode). This method is further applied to measurements collected over the Southern Ocean and Antarctica in recent years from multiple platforms, including ground sites, aircraft, and ships, to derive Aitken and accumulation-mode aerosol concentrations. Using the derived data, we examine the seasonal cycle, latitudinal variations, and vertical distribution of aerosols. Aitken mode aerosol concentrations are elevated over the Southern Ocean and Antarctica during the austral summer similar to the accumulation mode. In the austral summer, the free troposphere has more Aitken mode aerosols and fewer accumulation mode aerosols than the boundary layer, and thus likely serves as an important source of cloud-forming aerosol while also diluting the accumulation mode.

Kang, Litai [University of Washington] (ORCID:0000↗

DOE OSTI2020

A global model–measurement evaluation of particle light scattering coefficients at elevated relative humidity

The uptake of water by atmospheric aerosols has a pronounced effect on particle light scattering properties, which in turn are strongly dependent on the ambient relative humidity (RH). Earth system models need to account for the aerosol water uptake and its influence on light scattering in order to properly capture the overall radiative effects of aerosols. Here we present a comprehensive model–measurement evaluation of the particle light scattering enhancement factor f(RH), defined as the particle light scattering coefficient at elevated RH (here set to 85 %) divided by its dry value. The comparison uses simulations from 10 Earth system models and a global dataset of surface-based in situ measurements. In general, we find a large diversity in the magnitude of predicted f(RH) amongst the different models, which can not be explained by the site types. Based on our evaluation of sea salt scattering enhancement and simulated organic mass fraction, there is a strong indication that differences in the model parameterizations of hygroscopicity and model chemistry are driving at least some of the observed diversity in simulated f(RH). Additionally, a key point is that defining dry conditions is difficult from an observational point of view and, depending on the aerosol, may influence the measured f(RH). The definition of dry also impacts our model evaluation, because several models exhibit significant water uptake between RH = 0 % and 40 %. The multisite average ratio between model outputs and measurements is 1.64 when RH = 0 % is assumed as the model dry RH and 1.16 when RH = 40 % is the model dry RH value. The overestimation by the models is believed to originate from the hygroscopicity parameterizations at the lower RH range which may not implement all phenomena taking place (i.e., not fully dried particles and hysteresis effects). This will be particularly relevant when a location is dominated by a deliquescent aerosol such as sea salt. Our results emphasize the need to consider the measurement conditions in such comparisons and recognize that measurements referred to as dry may not be dry in model terms. Recommendations for future model–measurement evaluation and model improvements are provided.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1984

Properties of the Upper Tropospheres of Uranus and Neptune Derived from Observations at Visible to Near-Infrared Wavelengths

Photons at wavelengths between 0.3 and 4.5 microns penetrate the atmospheres of Uranus and Neptune to pressures between about 0.01 bar and 10 bars. This pressure range brackets the radiative convective boundary in both atmospheres and is therefore designated upper troposphere. Physical processes which govern the transfer of radiation in Uranus's and Neptune's atmospheres at these wavelengths include Rayleigh/Raman scattering by hydrogen, scattering and broadband absorption by suspended aerosol particles and absorption in discrete bands and lines by methane and hydrogen. Consequently, tropospheric properties constrained by observations at these wavelengths include optical properties and distribution of aerosol particles, methane/hydrogen ratio, and ortho/para hydrogen ratio. Recent observations of Uranus and Neptune in this spectral range, are reviewed and compared with predictions based on models of the atmospheric structures. Significant results for Uranus include the presence of an opaque lower boundary to the visible atmosphere very near the level corresponding to 2 bars pressure, and consequently a methane/hydrogen ratio no less than 3 percent.

Bergstralh, J. T.↗

NASA NTRS2023

Dispersion and Aging of Volcanic Aerosols after the La Soufriere Eruption in April 2021

Volcanic aerosols change the atmospheric composition and thereby affect weather and climate. Aerosol dynamic processes such as nucleation, condensation, and coagulation modify the shape, size, and mass of aerosol particles, which influence their atmospheric lifetime and radiative properties. Nevertheless, most models omit these processes for ash particles. In this work, we explore the ash aerosol aging and sulfate production during the first 4 days following the 2021 La Soufrière (St. Vincent) eruption with the ICON-ART model (ICOsahedral Nonhydrostatic model with Aerosol and Reactive Trace gases). Online coupling of ICON-ART with a one-dimensional volcanic plume model calculates volcanic emission, which makes it possible to resolve the different eruption phases of the noncontinuous La Soufrière eruption. We compared our simulated aerosol distribution and composition with observations from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument, the Multiangle Imaging SpectroRadiometer (MISR) Research Aerosol (RA) Algorithm, and the Barbados Cloud Observatory (BCO). We show that online coupling is essential to adequately model the emissions and plume development close to the volcano. The modeled aerosol aging is in very good agreement with observations from MISR near the emission source and with CALIOP at larger distances. Furthermore, particle aging occurs faster in the troposphere than in the stratosphere due to the availability of water vapor and OH, but a layer of coated ash appears at the plume top due to faster oxidation of SO2 and lofting by aerosol-radiation interaction. This paper gives the first direct comparison of aerosol aging in volcanic eruption plumes between simulations and observations

volcanic aerosols↗

NASA NTRS2011

Biogeochemical Impact of Long-Range Transported Dust over Northern South China Sea

Transpacific transport and impact of Asian dust aerosols have been well documented (e.g., results from ACE-Asia and regional follow-on campaigns), but little is known about dust invasion to the South China Sea (SCS). On 19-21 March 2010, a fierce Asian dust storm affected large areas from the Gobi deserts to the West Pacific, including Taiwan and Hong Kong. As a pilot study of the 7-SEAS (Seven South East Asian Studies) in the northern SCS, detailed characteristics of long-range transported dust aerosols were first observed by a comprehensive set of ground-based instruments deployed at the Dongsha islands (20deg42'52" N, 116deg43'51" E). Aerosol measurements such as particle mass concentrations, size distribution, optical properties, hygroscopicity, and vertical profiles help illustrate the evolution of this dust outbreak. Our results indicate that these dust particles were mixed with anthropogenic and marine aerosols, and transported near the surface. Satellite assessment of biogeochemical impact of dust deposition into open oceans is hindered by our current inability in retrieving areal dust properties and ocean colors over an extensive period of time, particularly under the influence of cloudy conditions. In this paper, we analyze the changes of retrieved Chlorophyll-a (Chl-a) concentration over the northern SCS, considered as oligotophic waters in the spring, from long-term SeaWiFS measurements since 1997. Over the past decade, six long-range transported dust events are identified based on spatiotemporal evolutions of PM10 measurements from regional monitoring stations, with the aid of trajectory analysis. Multi-year composites of Chl-a imagery for dust event and non-dust background during March-April are applied to overcome insufficient retrievals of Chl-a due to cloudy environment. Due to anthropogenic modification within a shallow boundary layer off the densely populated and industrial southeast coast of China, the iron ion activation of deliquescent dust particles enhances the efficiency of fertilization for biological productivity. Compared to the West Pacific, the marine ecosystem in the northern SCS is much more susceptible to the biogeochemical impact of long-range transported Asian dust.

Tsay, Si-Chee↗

NASA NTRS2002

Characterization of Dust Properties during ACE-Asia and PRIDE: A Column Satellite-Surface Perspective

Many recent field experiments are designed to study the compelling variability in spatial and temporal scale of both pollution-derived and naturally occurring aerosols, which often exist in high concentration over particular pathways around the globe. For example, the ACE-Asia (Aerosol Characterization Experiment-Asia) was conducted from March-May 2001 in the vicinity of the Taklimakan and Gobi deserts, East Coast of China, Yellow Sea, Korea, and Japan, along the pathway of Kosa (severe events that blanket East Asia with yellow desert dust, peaked in the Spring season). The PRIDE (Puerto RIco Dust Experiment, July 2000) was designed to measure the properties of Saharan dust transported across the Atlantic Ocean to the Caribbean. Dust particles typically originate in desert areas far from polluted urban regions. During transport, dust layers can interact with anthropogenic sulfate and soot aerosols from heavily polluted urban areas. Added to the complex effects of clouds and natural marine aerosols, dust particles reaching the marine environment can have drastically different properties than those from the source. Thus, understanding the unique temporal and spatial variations of dust aerosols is of special importance in regional-to-global climate issues such as radiative forcing, the hydrological cycle, and primary biological productivity in the ocean. During ACE-Asia and PRIDE we had measured aerosol physical/optical/radiative properties, column precipitable water amount, and surface reflectivity over homogeneous areas from ground-based remote sensing. The inclusion of flux measurements permits the determination of aerosol radiative flux in addition to measurements of loading and optical depth. At the time of the Terra/MODIS, SeaWiFS, TOMS and other satellite overpasses, these ground-based observations can provide valuable data to compare with satellite retrievals over land. We will present the results and discuss their implications in regional climatic effects.

Lau, William K. M.↗

NASA NTRS2000

Global Monitoring of Air Pollution Using Spaceborne Sensors

The MODIS sensor onboard EOS-Terra satellite provides not only daily global coverage but also high spectral (36 channels from 0.41 to 14 microns wavelength) and spatial (250m, 500m and 1km) resolution measurements. A similar MODIS instrument will be also configured into EOS-Aqua satellite to be launched soon. Using the complementary EOS-Terra and EOS-Aqua sun-synchronous orbits (10:30 AM and 1:30 PM equator-crossing time respectively), it enables us also to study the diurnal changes of the Earth system. It is unprecedented for the derivation of aerosol properties with such high spatial resolution and daily global converge. Aerosol optical depth and other aerosol properties, e.g., Angstrom coefficient over land and particle size over ocean, are derived as standard products at a spatial resolution of 10 x 10 sq km. The high resolution results are found surprisingly useful in detecting aerosols in both urban and rural regions as a result of urban/industrial pollution and biomass burning. For long-lived aerosols, the ability to monitoring the evolution of these aerosol events could help us to establish an system of air quality especially for highly populated areas. Aerosol scenarios with city pollution and biomass burning will be presented. Also presented are the method used in the derivation of aerosol optical properties and preliminary results will be presented, and issue as well as obstacles in validating aerosol optical depth with AERONET ground-based observations.

Chu, D. A.↗

NASA NTRS1995

Radiative impact of aerosols generated from biomass burning

Atmospheric aerosol particles play a vital role in the Earth's radiative energy budget. They exert a net cooling influence on climate by directly reflecting the solar radiation to space and by modifying the shortwave reflective properties of clouds. Each year, increasing amounts of aerosol particles are released into the atmosphere due to biomass burning, dust storms, forest fires, and volcanic activity. These particles significantly perturb the radiative balance on local, regional, and global scales. While the detection of aerosols over water is a well established procedure, the detection of aerosols over land is often difficult due to the poor contrast between the aerosols and the underlying terrain. In this study, we use textural measures in order to detect aerosols generated from biomass burning over South America, using AVHRR data. The regional radiative effects are then examined using ERBE data. Preliminary results show that the net radiative forcing of aerosols is about -36 W/sq m.

Christopher, Sundar A.↗

NASA NTRS2002

Modeled Aerosol Optical Properties From Measurement-Based Mixtures of Chemical Species: Assessing the Impacts of Particle Morphology and Absorption

This report serves as the final report for the Colorado State University portion of this grant. The original grant was awarded to CSU under the direction of co-Principal Investigators Kirk Fuller and Sonia Kreidenweis. Upon Dr. Fuller's relocation to the University of Alabama - Huntsville, the major portion of the award was also relocated. The following summarizes only that work completed by Prof. Kreidenweis under her remaining award.

Kreidenweis, Sonia↗