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At least 451 records · Page 25
All sourcesNASA NTRSDOE OSTI
NASA NTRS1993

The Atmospheric Impact of the 1991 Mount Pinatubo Eruption

The 1991 eruption of Pinatubo produced about 5 cubic kilometers of dacitic magma and may be the second largest volcanic eruption of the century. Eruption columns reached 40 kilometers in altitude and emplaced a giant umbrella cloud in the middle to lower stratosphere that injected about 17 megatons of SO2, slightly more than twice the largest yielded by the 1982 eruption of El Chichon, Mexico. The SO2 formed sulfate aerosols that produced the largest perturbation to the stratospheric aerosol layer since the eruption of Krakatau in 1883. The aerosol cloud spread rapidly around the Earth in about 3 weeks and attained global coverage by about 1 year after the eruption. Peak local midvisible optical depths of up to 0.4 were measured in late 1992, and globally averaged values were about 0.1 to 0.15 for 2 years. The large aerosol cloud caused dramatic decreases in the amount of net radiation reaching the Earth's surface, producing a climate forcing that was two times stronger than the aerosols of El Chichon. Effects on climate were an observed surface cooling in the northern hemisphere of up to 0.5 to 0.6 C, equivalent to a hemispheric-wide reduction in net radiation of 4 watts per square meter and a cooling of perhaps as large as -0.4 C over large parts of the earth in 1992-93. Climate models seem to have predicted the cooling with a reasonable degree of accuracy. The Pinatubo climate forcing was stronger than the opposite warming of either the El Nino event or anthropogenic greenhouse gases in the period 1991-93. As a result of the presence of the aerosol particles, midlatitude ozone concentrations reached their lowest levels on record during 1992-93, the southern hemisphere 'ozone hole' increased in 1992 to an unprecedented size and ozone depletion rates were observed to be faster than ever before recorded. The atmospheric impact of the Pinatubo eruption has been profound, and it has sparked a lively interest in the role that volcanic aerosols play in climate change. This event has shown that a powerful eruption providing a 15 to 20 megaton release of SO2 into the stratosphere can produce sufficient aerosols to offset the present global warming trends and severely impact the ozone budget.

Self, Stephen↗
NASA NTRS1999

Engine Test and Measurements

Although the importance of aerosols and their precursors are now well recognized, the characterization of current subsonic engines for these emissions is far from complete. Furthermore, since the relationship of engine operating parameters to aerosol emissions is not known, extrapolation to untested and unbuilt engines necessarily remains highly uncertain. 1997 NASA LaRC engine test, as well as the parallel 1997 NASA LaRC flight measurement, attempts to address both issues by expanding measurements of aerosols and aerosol precursors with fuels containing different levels of fuel sulfur content. The specific objective of the 1997 engine test is to obtain a database of sulfur oxides emissions as well as the non-volatile particulate emission properties as a function of fuel sulfur and engine operating conditions. Four diagnostic systems, extractive and non-intrusive (optical), will be assembled for the gaseous and particulate emissions characterization measurements study. NASA is responsible for the extractive gaseous emissions measurement system which contains an array of analyzers dedicated to examining the concentrations of specific gases (NO, NO(x), CO, CO2, O2, THC, SO2) and the smoke number. University of Missouri-Rolla uses the Mobile Aerosol Sampling System to measure aerosol/particulate total concentration, size distribution, volatility and hydration property. Air Force Research Laboratory uses the Chemical Ionization Mass Spectrometer to measure SO2, SO3/H2SO4, and HN03 Aerodyne Research, Inc. uses Infrared Tunable Diode Laser system to measure SO2, SO3, NO, H2O, and CO2.

Wey, Chown Chou↗
NASA NTRS2002

Jupiter Systems Data Analysis Program Galileo Multi-Spectral Analysis of the Galilean Satellites

Progress was made on this project at the University of Colorado, particularly concerning analysis of data of the galilean moons Io and Europa. The goal of the Io portion of this study is to incorporate Near Infrared Mapping Spectrometer (NIMS) measured sulfur dioxide (SO2) frost amounts into models used with Ultraviolet spectrometer (UVS) spectra, in order to better constrain SO2 gas amounts determined by the UVS. The overall goal of this portion of the study is to better understand the thickness and distribution of Io's SO2 atmosphere. The goal of the analysis of the Europa data is to better understand the source of the UV absorption feature centered near 280 rim which has been noted in disk-integrated spectra primarily on the trailing hemisphere. The NIMS data indicate asymmetric water ice bands on Europa, particularly over the trailing hemisphere, and especially concentrated in the visibly dark regions associated with chaotic terrain and lines. The UPS data, the first-ever disk-resolved UV spectra of Europa, shown that the UV absorber is likely concentrated in regions where the NIMS data show asymmetric water ice bands. The material that produces both spectral features is likely the same, and we use data from both wavelength regions to better understand this material, and whether it is endogenically or exogenically produced. This work is still in progress at JPL.

Hendrix, Amanda↗
NASA NTRS2003

Sulfur Oxidation and Contrail Precursor Chemistry

Sulfuric acid (H2SO4), formed in commercial aircraft operations via fuel-S (goes to) SO2 (goes to) SO3 (goes to) H2SO4 plays an important role in the formation of contrails. It is believed that the first step occurs inside the combustor, the second step in the engine exit nozzle, and the third step in the exhaust plume. Thus, measurements of the sulfur oxidation rates are critical to the understanding of contrail formation. Field measurements of contrails formed behind commercial aircraft indicate that significantly greater conversion of fuel-bound sulfur to sulfate aerosol occurs than can be explained by our current knowledge of contrail physics and chemistry. The conversion of sulfur from S(IV) to S(VI) oxidation state, required for sulfate aerosol formation, is thermodynamically favored for the conditions that exist within jet engines but is kinetically disfavored. The principal reaction pathway is O+SO2+M (goes to) SO3+M. The rates of this reaction have never been measured in the temperature and pressure regimes available to aircraft operation. In the first year (FY02) of this project, we performed a series of experiments to elucidate the rate information for the O+SO2+M (goes to) SO3+M reaction. The work performed is described following the proposed work plan. Because we used the H2/O2 system for an O-atom source and rate coefficients were obtained via computer simulation, construction of a reaction mechanism and either recalculation or estimation of thermodynamic properties of H(x)SO(y) species are described first.

DeWitt, Kenneth J.↗
NASA NTRS1997

Energy, volatile production, and climatic effects of the Chicxulub Cretaceous/Tertiary impact

A comprehensive analysis of volatiles in the Chicxulub impact strongly supports the hypothesis that impact-generated sulfate aerosols caused over a decade of global cooling, acid rain, and disruption of ocean circulation, which contributed to the mass extinction at the Cretaceous/Tertiary (K/T) boundary. The crater size, meteoritic content of the K/T boundary clay, and impact models indicate that the Chicxulub crater was formed by a short period comet or an asteroid impact that released 0.7-3.4 x 10(31) ergs of energy. Impact models and experiments combined with estimates of volatiles in the projectile and target rocks predict that over 200 gigatons (Gt) each of SO2 and water vapor, and over 500 Gt of CO2, were globally distributed in the stratosphere by the impact. Additional volatiles may have been produced on a global or regional scale that formed sulfate aerosols rapidly in cooler parts of the vapor plume, causing an early, intense pulse of sulfuric acid rain. Estimates of the conversion rate of stratospheric SO2 and water vapor to sulfate aerosol, based on volcanic production of sulfate aerosols, coupled with calculations of diffusion, coagulation, and sedimentation, demonstrate that the 200 Gt stratospheric SO2 and water vapor reservoir would produce sulfate aerosols for 12 years. These sulfate aerosols caused a second pulse of acid rain that was global. Radiative transfer modeling of the aerosol clouds demonstrates (1) that if the initial rapid pulse of sulfate aerosols was global, photosynthesis may have been shut down for 6 months and (2) that for the second prolonged aerosol cloud, solar transmission dropped 80% by the end of first year and remained 50% below normal for 9 years. As a result, global average surface temperatures probably dropped between 5 degrees and 31 degrees K, suggesting that global near-freezing conditions may have been reached. Impact-generated CO2 caused less than 1 degree K greenhouse warming and therefore was insignificant compare to the sulfate cooling. The magnitude of sulfate cooling depends largely upon the rate of ocean mixing as surface waters cool, sink, and are replaced by upwelling of deep ocean water. This upwelling apparently drastically altered ocean stratification and circulation, which may explain the global collapse of the delta 13C gradient between surface and deep ocean waters at the K/T boundary.

NASA Center JPL↗
NASA NTRS2003

Chemical Composition of Asian Continental Outflow over the Western Pacific: Results from Transport and Chemical Evolution over the Pacific (TRACE-P)

We characterize the chemical composition of Asian continental outflow observed during the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) mission during February-April 2001 in the western Pacific using data collected on the NASA DC-8 aircraft. A significant anthropogenic impact was present in the free troposphere and as far east as 150degE longitude reflecting rapid uplift and transport of continental emissions. Five-day backward trajectories were utilized to identify five principal Asian source regions of outflow: central, coastal, north-northwest(NNW), southeast (SE), and west-southwest (WSW). The maximum mixing ratios for several species, such as CO, C2Cl4, CH3Cl, and hydrocarbons, were more than a factor of 2 larger in the boundary layer of the central and coastal regions due to industrial activity in East Asia. CO was well correlated with C2H2, C2H6, C2Cl4, and CH3Cl at low altitudes in these two regions (r(sup 2) approx. 0.77-0.97). The NNW, WSW, and SE regions were impacted by anthropogenic sources above the boundary layer presumably due to the longer transport distances of air masses to the western Pacific. Frontal and convective lifting of continental emissions was most likely responsible for the high altitude outflow in these three regions. Photochemical processing was influential in each source region resulting in enhanced mixing ratios of O3, PAN, HNO3, H2O2, and CH3OOH. The air masses encountered in all five regions were composed of a complex mixture of photcrchemically aged air with more recent emissions mixed into the outflow as indicated by enhanced hydrocarbon ratios (C2H2/CO greater than or equal to 3 and C3H8/C2H6 greater than or equal to 0.2). Combustion, industrial activities, and the burning of biofuels and biomass all contributed to the chemical composition of air masses from each source region as demonstrated by the H6, SO2, and C2Cl4 were compared for the TRACE-P and PEM-West B missions. In the more northern regions, O3, CO, and SO2 were higher at low altitudes during TRACE-P. In general, mixing ratios were fairly similar between the two missions in the southern regions. A comparison between CO/CO2, CO/CH4, C2H6/C3H8, NO(x)/SO2, and NO(y)/(SO2 + nss-SO4) ratios for the five source regions and for the 2000 Asian emissions summary showed vay close agreement indicating that Asian emissions were well represented by the TRACE-P data and tbe emissions inventory.

Russo, R. S.↗
NASA NTRS2005

Sulfur Oxidation and Contrail Precursor Chemistry

Sulfuric acid (H2SO4), formed in commercial aircraft operations via Fuel-S (right arrow) SO2 + SO3 (right arrow) H2SO4, plays an important role in affecting the global climate change through atmospheric chemical reactions and radiative forcing. Measurement of the sulfur oxidation rates is critical to the understanding of the contrail formation. The principle reaction pathway is SO2 + O + M (right arrow) SO3 + M. Although there are many measurements for the rates of this reaction, it has never been measured in the temperature and pressure regime available to aircraft operation. In this investigation, a series of experiments were performed behind the reflected shock waves in a shock tube. OH radicals were produced in lean, shock heated SO2/H2/O2/Ar mixtures. The reaction progress was followed using OH absorption spectroscopy at 310 nm. The data were analyzed with the aid of computer modeling/simulation. The mean value of the rate coefficients of R21 determined is k(sub 21,0)/[M]= 3.9 x 10(exp 15) cm(sup 6) per square mole per second at T = 960 - 1150 K and rho = 16-30 micromole per cubic centimeter with uncertainty limits of plus or minus 30%. A non-Arrhenius fit to our data together with all existing data gives k(sub 21,0)/[M] = 1.3 x 10(exp 24) T (exp -2.5) exp(-2350 K/T) cm(sup 6) per square mole per second at T = 300 - 2500 K with the same uncertainty limits given above. The calculated conversion of S(IV)(SO2) to S(VI) (SO3 + H2SO4) was about 2% in our experimental conditions.

DeWitt, Kenneth↗
NASA NTRS1998

F100 Engine Emissions Tested in NASA Lewis' Propulsion Systems Laboratory

Recent advances in atmospheric sciences have shown that the chemical composition of the entire atmosphere of the planet (gases and airborne particles) has been changed due to human activity and that these changes have changed the heat balance of the planet. National Research Council findings indicate that anthropogenic aerosols1 reduce the amount of solar radiation reaching the Earth's surface. Atmospheric global models suggest that sulfate aerosols change the energy balance of the Northern Hemisphere as much as anthropogenic greenhouse gases have. In response to these findings, NASA initiated the Atmospheric Effects of Aviation Project (AEAP) to advance the research needed to define present and future aircraft emissions and their effects on the Earth's atmosphere. Although the importance of aerosols and their precursors is now well recognized, the characterization of current subsonic engines for these emissions is far from complete. Furthermore, since the relationship of engine operating parameters to aerosol emissions is not known, extrapolation to untested and unbuilt engines necessarily remains highly uncertain. Tests in 1997-an engine test at the NASA Lewis Research Center and the corresponding flight measurement test at the NASA Langley Research Center-attempted to address both issues by measuring emissions when fuels containing different levels of sulfur were burned. Measurement systems from four research groups were involved in the Lewis engine test: A Lewis gas analyzer suite to measure the concentration of gaseous species 1. including NO, NOx, CO, CO2, O2, THC, and SO2 as well as the smoke number; 2. A University of Missouri-Rolla Mobile Aerosol Sampling System to measure aerosol and particulate properties including the total concentration, size distribution, volatility, and hydration property; 3. An Air Force Research Laboratory Chemical Ionization Mass Spectrometer to measure the concentration of SO2 and SO3/H2SO4; and 4. An Aerodyne Research Inc. Tunable Diode Laser System to measure the concentrations of SO2, SO3, NO, NO2, CO2, and H2O. By September 1997, an F100 engine operating at several power levels at sea level and up to six simulated altitudes had been tested with commercial jet fuels with three levels of sulfur content and one military jet fuel. The data are being vigorously analyzed. A complete report is anticipated for the 1998 Atmospheric Effects of Aviation Project Annual Conference.

Wey, Chowen C.↗
NASA NTRS2011

Thermally-Induced Chemistry and the Jovian Icy Satellites: A Laboratory Study of the Formation of Sulfur Oxyanions

Laboratory experiments have demonstrated that magnetospheric radiation in the Jovian system drives reaction chemistry in ices at temperatures relevant to Europa and other icy satellites. Here we present new results on thermally-induced reactions at 50-100 K in solid H2O-SO2 mixtures, reactions that take place without the need for a high-radiation environment. We find that H2O and SO2 react to produce sulfur Oxyanions, such as bisulfite, that as much as 30% of the SO2 can be consumed through this reaction, and that the products remain in the ice when the temperature is lowered, indicating that these reactions are irreversible. Our results suggest that thermally-induced reactions can alter the chemistry at temperatures relevant to the icy satellites in the Jovian system.

Loeffler, Mark J.↗
NASA NTRS2013

Insights into the Sulfur Mineralogy of Martian Soil at Rocknest, Gale Crater, Enabled by Evolved Gas Analyses

The first solid samples analysed by the Chemistry and Mineralogy (CheMin) instrument and Sample Analysis at Mars (SAM) instrument suite on the Mars Science Laboratory (MSL) consisted of < 150 m fines sieved from aeolian bedform material at a site named Rocknest. All four samples of this material analyzed by SAM s evolved gas analysis mass spectrometry (EGA-MS) released H2O, CO2, O2, and SO2 (Fig. 1), as well as H2S and possibly NO. This is the first time evolved SO2 (and evolved H2S) has been detected from thermal analysis of martian materials. The identity of these evolved gases and temperature (T) of evolution can support mineral detection by CheMin and place constraints on trace volatile-bearing phases present below the CheMin detection limit or difficult to characterize with XRD (e.g., X-ray amorphous phases). Constraints on phases responsible for evolved CO2 and O2 are detailed elsewhere [1,2,3]. Here, we focus on potential constraints on phases that evolved SO2, H2S, and H2O during thermal analysis.

McAdam, A.↗
NASA NTRS2014

Anthropogenic and Volcanic Contributions to the Decadal Variations of Aerosols in the Upper Troposphere and Lower Stratosphere

We investigated the anthropogenic and volcanic contributions to sulfate aerosol in the stratosphere through modeling and analysis of satellite data. We use a global model GOCART to simulate SO2 and sulfate aerosol in the period of 2000 to 2010, during which numerous volcanic eruptions occurred although nothing like the magnitudes of El Chichon or Pinatubo. We compared the model results with the column SO2 data from OMI and stratospheric SO2 data from MLS instrument on Aura satellite and the aerosol vertical profiles from the SCIAMACHY instrument on Envisat and the CALIOP instrument on CALIPSO satellites. Finally, we assessed the relative contributions of volcanic aerosols vs. anthropogenic aerosols to the observed decadal stratospheric aerosol trends.

HTAP2/AeroCom3 model↗
NASA NTRS2015

Descent Without Modification? The Thermal Chemistry of H2O2 on Europa and Other Icy Worlds

The strong oxidant H2O2 is known to exist in solid form on Europa and is suspected to exist on several other Solar System worlds at temperatures below 200 K. However, little is known of the thermal chemistry that H2O2 might induce under these conditions. Here, we report new laboratory results on the reactivity of solid H2O2 with eight different compounds in H2O-rich ices. Using infrared spectroscopy, we monitored compositional changes in ice mixtures during warming. The compounds CH4 (methane), C3H4 (propyne), CH3OH (methanol), and CH3CN (acetonitrile) were unaltered by the presence of H2O2 in ices, showing that exposure to either solid H2O2 or frozen H2O+H2O2 at cryogenic temperatures will not oxidize these organics, much less convert them to CO2. This contrasts strongly with the much greater reactivity of organics with H2O2 at higher temperatures, and particularly in the liquid and gas phases. Of the four inorganic compounds studied, CO, H2S, NH3, and SO2, only the last two reacted in ices containing H2O2, NH3 making NHþ 4 and SO2 making SO2 4 by H+ and e - transfer, respectively. An important astrobiological conclusion is that formation of surface H2O2 on Europa and that molecule's downward movement with H2O-ice do not necessarily mean that all organics encountered in icy subsurface regions will be destroyed by H2O2 oxidation.

Europa↗
NASA NTRS2015

Assessing Eruption Column Height in Ancient Flood Basalt Eruptions

A buoyant plume model is used to explore the ability of flood basalt eruptions to inject climate-relevant gases into the stratosphere. An example from the 1986 Izu-Oshima basaltic fissure eruption validates the model's ability to reproduce the observed maximum plume heights of 12-16 km above sea level, sustained above fire-fountains. The model predicts maximum plume heights of 13-17 km for source widths of between 4-16 m when 32% (by mass) of the erupted magma is fragmented and involved in the buoyant plume (effective volatile content of 6 wt%). Assuming that the Miocene-age Roza eruption (part of the Columbia River Basalt Group) sustained fire-fountains of similar height to Izu-Oshima (1.6 km above the vent), we show that the Roza eruption could have sustained buoyant ash and gas plumes that extended into the stratosphere at approximately 45 deg N. Assuming 5 km long active fissure segments and 9000 Mt of SO2 released during explosive phases over a 10-15 year duration, the approximately 180 km of known Roza fissure length could have supported approximately 36 explosive events/phases, each with a duration of 3-4 days. Each 5 km fissure segment could have emitted 62 Mt of SO2 per day into the stratosphere while actively fountaining, the equivalent of about three 1991 Mount Pinatubo eruptions per day. Each fissure segment could have had one to several vents, which subsequently produced lava without significant fountaining for a longer period within the decades-long eruption. Sensitivity of plume rise height to ancient atmospheric conditions is explored. Although eruptions in the Deccan Traps (approximately 66 Ma) may have generated buoyant plumes that rose to altitudes in excess of 18 km, they may not have reached the stratosphere because the tropopause was substantially higher in the late Cretaceous. Our results indicate that some flood basalt eruptions, such as Roza, were capable of repeatedly injecting large masses of SO2 into the stratosphere. Thus sustained flood basalt eruptions could have influenced climate on time scales of decades to centuries but the location (i.e., latitude) of the province and relevant paleoclimate is important and must be considered.

climate↗
NASA NTRS1973

Laser Radar Study Using Resonance Absorption for Remote Detection Of Air Pollutants

A laser radar using resonance absorption has an advantage of increased detection range and sensitivity compared with that achieved by Raman or resonance back scattering. In this paper, new laser radar system using resonance absorption is proposed and results obtained from this laser radar system are discussed. NO2, SO2 gas has an absorption spectrum at 4500 A and 3000 A respectively as shown in Fig. 1. A laser light including at least a set of an absorption peak (lambda)1 and a valley (lambda)2 is emitted into a pollutant atmosphere. The light reflected with a topographical reflector or an atmospheric Mie scattering as distributed reflectors is received and divided into two wavelength components (lambda)1 and (lambda)2. The laser radar system used in the investigation is shown in Fig', 2 and consists of a dye laser transmitter, an optical receiver with a special monochrometer and a digital processer. Table 1 shows the molecular constants of NO2, and SO2 and the dye laser used in this experiment. In this system, the absolute concentration of the pollutant gas can be measured in comparison with a standard gas cell. The concentration of NO2, SO2 as low as 0.1 ppm have been measured at 100 m depth resolution. For a 1 mJ laser output, the observable range of this system achieved up to 300 m using the distributed Mie reflector. The capability and technical limitation of the system will be discussed in detail.

Igarashi, Takashi↗
NASA NTRS2016

Agricultural Fires in the Southeastern U.S. During SEAC4RS: Emissions of Trace Gases and Particles and Evolution of Ozone, Reactive Nitrogen, and Organic Aerosol

Emissions from 15 agricultural fires in the southeastern U.S. were measured from the NASA DC-8 research aircraft during the summer 2013 Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) campaign. This study reports a detailed set of emission factors (EFs) for 25 trace gases and 6 fine particle species. The chemical evolution of the primary emissions in seven plumes was examined in detail for ~1.2 h. A Lagrangian plume cross-section model was used to simulate the evolution of ozone (O3), reactive nitrogen species, and organic aerosol (OA). Observed EFs are generally consistent with previous measurements of crop residue burning, but the fires studied here emitted high amounts of SO2 and fine particles, especially primary OA and chloride. Filter-based measurements of aerosol light absorption implied that brown carbon (BrC) was ubiquitous in the plumes. In aged plumes, rapid production of O3, peroxyacetyl nitrate (PAN), and nitrate was observed with (Delta)O3/(Delta)CO, (Delta)PAN/(Delta)NOy, and (Delta)nitrate/(Delta)NOy reaching approx. 0.1, approx. 0.3, and approx.0.3. For five selected cases, the model reasonably simulated O3 formation but underestimated PAN formation. No significant evolution of OA mass or BrC absorption was observed. However, a consistent increase in oxygen-to-carbon (O/C) ratios of OA indicated that OA oxidation in the agricultural fire plumes was much faster than in urban and forest fire plumes. Finally, total annual SO2, NOx, and CO emissions from agricultural fires in Arkansas, Louisiana, Mississippi, and Missouri were estimated (within a factor of approx. 2) to be equivalent to approx. 2% SO2 from coal combustion and approx. 1% NOx and approx. 9% CO from mobile sources.

OA mass or BrC absorption↗
NASA NTRS2021

Investigation of several proxies to estimate sulfuric acid concentration in volcanic plume conditions

Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle formation (NPF). However, direct measurements of [H2SO4] remain challenging, thus preventing the determination of this important quantity, and, consequently, a complete understanding of its contribution to the NPF process. Several proxies have been developed to bridge the gaps, but their ability to predict [H2SO4] in very specific conditions such as those encountered in volcanic plumes (including in particular high sulphur dioxide mixing ratios) has not been evaluated so far. In this context, the main objective of the present study was to develop new proxies for daytime [H2SO4] in volcanic plume conditions and compare their performance to that of the proxies available in the literature. In specific, the data collected at Maïdo during the OCTAVE 2018 campaign, in the volcanic eruption plume of the Piton de la Fournaise, were first used to derive seven proxies based on the knowledge of sulphur dioxide (SO2) mixing ratio, global radiation, condensation sink (CS) and relative humidity (RH). In three of the seven proxies (F1–F3), all variables were given equal weight in the prediction of [H2SO4], while adjusted powers were allowed for the different variables in the other four proxies (A1–A4). Proxies A1–A4 were overall found to perform better compared to F1–F3, with, in specific, improved predictive ability for [H2SO4] > 2 × 108 per cu.cm. The CS was observed to play an important role in regulating [H2SO4], while, in contrast, the inclusion of RH did not improve the predictions. A last expression accounting for an additional sink term related to cluster formation, S1, was also tested and showed a very good predictive ability over the whole range of measured [H2SO4]. The newly developed proxies were in a second step further evaluated using airborne measurements performed in the passive degassing plume of Etna during the STRAP 2016 campaign. Increased correlations between observed and predicted [H2SO4] were obtained when the dependence of predicted [H2SO4] over CS was the lowest, and when the dependence over [SO2] was concurrently the highest. The best predictions were finally retrieved by the simple formulation of F2 (in which [SO2] and radiation alone were assumed to explain the variations of [H2SO4] with equal contributions), with a pre factor adapted to the STRAP data. All in all, our results illustrate the fairly good capacity of the proxy available in the literature to describe [H2SO4] in volcanic plume conditions, but highlight at the same time the benefit of the newly developed proxies for the prediction of the highest concentrations ([H2SO4] > 2–3 × 108 per cu.cm). Also, the contrasting behaviours of the new proxies in the two investigated datasets indicate that in volcanic plumes like in other environments, the relevance of a proxy can be affected by changes in environmental conditions, and that location specific coefficients do logically improve the predictions.

new particle formation↗
NASA NTRS2020

VolKilau: Volcano Rapid Response Balloon Campaign During the 2018 Kilauea Eruption

After nearly 35 years of stable activity, the Kilauea volcanic system in Hawaiʽi, went through sudden changes in May 2018 with the emergence of 20 volcanic fissures along the Lower Eastern Rift Zone(LERZ) destroying 700 homes in Leilani Estates and forcing more than 2000 people to evacuate. Volcanic emissions lasted for several months between June and September 2018 leading to low visibility and poor air quality in Hawaiʽi and across the Western Pacific. The NASA-funded VolKilau mission was rapidly mounted and conducted between 11-18 June 2018 to: i) Profile volcanic emissions with SO2and aerosol measurements, ii) Validate satellite observations and iii) Be prepared for the next large volcanic eruption. Through a series of balloon-borne measurements with tethered and free released launches, we measured SO2 concentration, aerosol concentration and optical properties 60 to 80km downwind from the volcanic fissures using gas sensors, optical particle counters, backscatter sondes, and an aerosol impactor. While most of measurements made during the Kilauea eruption were ground-based, the VolKilau mission represented a unique opportunity to characterize plume properties, constrain emission profiles, study early chemistry involving the conversion of SO2 into sulfuric acid and understand the influence of water clouds in the removal of SO2. Our team continues to be better prepared for deploying in the event of a major volcanic eruption

J-P Vernier↗
NASA NTRS2021

Present and future aerosol impacts on Arctic climate change in the GISS-E2.1 Earth system model

The Arctic is warming 2 to 3 times faster than the global average, partly due to changes in short-lived climate forcers (SLCFs) including aerosols. In order to study the effects of atmospheric aerosols in this warming, recent past (1990–2014) and future (2015–2050) simulations have been carried out using the GISS-E2.1 Earth system model to study the aerosol burdens and their radiative and climate impacts over the Arctic (>60°N), using anthropogenic emissions from the Eclipse V6b and the Coupled Model Intercomparison Project Phase 6 (CMIP6) databases, while global annual mean greenhouse gas concentrations were prescribed and kept fixed in all simulations. Results showed that the simulations have underestimated observed surface aerosol levels, in particular black carbon (BC) and sulfate (SO2−4), by more than 50 %, with the smallest biases calculated for the atmosphere-only simulations, where winds are nudged to reanalysis data. CMIP6 simulations performed slightly better in reproducing the observed surface aerosol concentrations and climate parameters, compared to the Eclipse simulations. In addition, simulations where atmosphere and ocean are fully coupled had slightly smaller biases in aerosol levels compared to atmosphere-only simulations without nudging. Arctic BC, organic aerosol (OA), and SO2−4 burdens decrease significantly in all simulations by 10 %–60 % following the reductions of 7 %–78 % in emission projections, with the Eclipse ensemble showing larger reductions in Arctic aerosol burdens compared to the CMIP6 ensemble. For the 2030–2050 period, the Eclipse ensemble simulated a radiative forcing due to aerosol–radiation interactions (RFARI) of −0.39 ± 0.01 W/sq. m, which is −0.08 W/sq. m larger than the 1990–2010 mean forcing (−0.32 W/sq. m), of which −0.24 ± 0.01 W/sq. m was attributed to the anthropogenic aerosols. The CMIP6 ensemble simulated a RFARI of −0.35 to −0.40 W/sq. m for the same period, which is −0.01 to −0.06 W/sq. m larger than the 1990–2010 mean forcing of −0.35 W/sq. m. The scenarios with little to no mitigation (worst-case scenarios) led to very small changes in the RFARI, while scenarios with medium to large emission mitigations led to increases in the negative RFARI, mainly due to the decrease in the positive BC forcing and the decrease in the negative SO2−4 forcing. The anthropogenic aerosols accounted for −0.24 to −0.26 W/sq. m of the net RFARI in 2030–2050 period, in Eclipse and CMIP6 ensembles, respectively. Finally, all simulations showed an increase in the Arctic surface air temperatures throughout the simulation period. By 2050, surface air temperatures are projected to increase by 2.4 to 2.6 °C in the Eclipse ensemble and 1.9 to 2.6 °C in the CMIP6 ensemble, compared to the 1990–2010 mean. Overall, results show that even the scenarios with largest emission reductions leads to similar impact on the future Arctic surface air temperatures and sea-ice extent compared to scenarios with smaller emission reductions, implying reductions of greenhouse emissions are still necessary to mitigate climate change.

Aerosols↗