The 2019 Raikoke Eruption: Can Smoke and Sulfuric acid Aerosol be Separated?
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SAGE aerosol remost sensing↗
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The 2019 Raikoke eruption: Can smoke and Sulfuric acid aerosol be separated?
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Travis N. Knepp↗
Pre‐Industrial, Present and Future Atmospheric Soluble Iron Deposition and the Role of Aerosol Acidity and Oxalate Under CMIP6 Emissions
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Elisa Bergas‐Massó↗
Soluble species in the Arctic summer troposphere - Acidic gases, aerosols, and precipitation
The large-scale spatial distribution from 0.15-to 6 km altitude in the North American Arctic troposphere of several soluble acidic gases and major aerosol species during the summertime is reported. The distribution is found to be compositionally consistent on a large spatial scale. The summertime troposphere is an acidic environment, with HCOOH and CH3COOH the principal acidic gases while acidic sulfate aerosols dominate the particulate phase. There appears to be a surface source of NH3 over the pack ice which may originate from decay of dead marine organisms on the ice surface, evolution from surface ocean waters in open ice leads, or release from rotting sea ice. At low altitude over the pack ice this NH34 appears to partially neutralize aerosol acidity. Over sub-Arctic tundra in southeastern Alaska, inputs of marine biogenic sulfur from the Bering Sea appear to be an important source of boundary layer aerosol SO4(2-). The rainwater acidity over the tundra is typical of remote regions.
Talbot, R. W.↗
Latitudinal distribution of black carbon soot in the upper troposphere and lower stratosphere
Black carbon soot from the upper troposphere and lower stratosphere has been systematically collected at latitudes from 90 deg N to 45 deg S. The measured latitudinal distribution of this soot at 10 to 11 km altitude is found to covary with commercial air traffic fuel use, suggesting that aircraft fuel combustion at altitude is the principal source. In addition, at latitudes where the commercial air traffic is high, measured black carbon soot values are high even at 20 km altitude, suggesting that aircraft-generated soot injected just above the tropopause may be transported to higher altitudes. During the volcanically influenced period in which these samples were collected, the number abundances, total mass, and calculated total surface area of black carbon soot are 2-3 orders of magnitude lower than similar measures of sulfuric acid aerosol. During volcanically quiescent periods, the calculated total surface area of black carbon soot aerosol is of the same order of magnitude as that of the background sulfuric acid aerosol. It appears from this comparison that black carbon soot is only capable of influencing lower stratosphere or upper troposphere chemistry during periods when the aerosol budget is not dominated by volcanic activity. It remains to determine the extent to which black carbon soot particles act as nuclei for sulfuric acid aerosol formation. However, mass balance calculations suggest that aircraft soot injected at altitude does not represent a significant source of condensation nuclei for sulfuric acid aerosols.
Blake, David F.↗
Lessons from Earth Bioaerosol Sampling for Venus Habitability & Biosignature Science
Venus’s clouds are often discussed as a potential habitat. Several high-priority science goals – cloud aerosol composition, internal radiative flux, and aerosol residence time and circulation models – will improve our understanding of Venus in an astrobiology context. Lessons from Earth’s aerobiosphere can inform these requirements and interpretation of results. A stable Venus aerobiosphere would need microorganisms to reproduce faster than they settle out due to gravity. This is a joint constraint of the potential nutrients and energy influx, bioenergetic costs such as desiccation and radiation damage, and aerosol dynamics. Though life cycles involving S- and Fe-based redox metabolism have been proposed, at an optimistic estimate of 75% H2SO4, Venus aerosol water activity (aw) is still ~0.02, far below the observed microbial growth limit of ~0.6. Long-term desiccation with brief spurts of repair, growth and reproduction in response to transient water influx (perhaps volcanism) is the most likely model for Earth-like life on Venus – a ‘desert bloom’ scenario. In Earth’s troposphere, clouds can carry 103 – 105 cells/mL, some metabolically active. A better analogue may be Earth’s stratospheric sulfate aerosol layer: supercooled sulfuric acid aerosols (acid weight fraction 0.6 – 0.85, 0.1 – 1 µm diameter, 0.1 – 1 cm-3) with little water activity, long residence times, high UV radiation, and only sporadic influx from surface particle sources. Viable cells isolated from this region are rare (~102 cells/m3), though ‘hot spots’ at tropospheric mixing occur. Cells are primarily in inactive forms such as spores, and it is unclear if any are associated with sulfate aerosols or simply co-located. Given the heterogeneities in Venus clouds and the model of a sparse, largely dormant ecosystem, a single transect on descent would most likely pass through a low-water, inactive region, missing potential signs of habitability or biosignatures. Even a passive aerial platform (balloon) may end up following a single air mass over its lifetime. A better strategy for Venus would target an aerial region with some upwelling from surface sources, and take multiple transects separated in time and space. Earth’s stratospheric bioaerosol population could provide a starting point for estimating the required lower volume and detection limits.
Earth↗
Fourier transform-infrared studies of thin H2SO4/H2O films: Formation, water uptake, and solid-liquid phase changes
Fourier transform-infrared (FTIR) spectroscopy was used to examine films representative of stratospheric sulfuric acid aerosols. Thin films of sulfuric acid were formed in situ by the condensed phase reaction of SO3 with H2O. FTIR spectra show that the sulfuric acid films absorb water while cooling in the presence of water vapor. Using stratospheric water pressures, the most dilute solutions observed were greater than 40 wt % before simultaneous ice formation and sulfuric acid freezing occurred. FTIR spectra also revealed that the sulfuric acid films crystallized mainly as sulfuric acid tetrahydrate (SAT). Crystallization occurred either when the composition was about 60 wt% H2SO4 or after ice formed on the films at temperatures 1-4 K below the ice frost point. Finally, we determined that the melting point for SAT depended on the background water pressure and was 216-219 K in the presence of 4 x 10(exp -4) Torr H2O. Our results suggest that once frozen, sulfuric acid aerosols in the stratosphere are likely to melt at these temperatures, 30 K colder than previously thought.
Middlebrook, Ann M.↗
Light Absorption of Stratospheric Aerosols: Long-Term Trend and Contribution by Aircraft
Measurements of aerosol light-absorption coefficients are useful for studies of radiative transfer and heating rates. Ogren appears to have published the first light- absorption coefficients in the stratosphere in 1981, followed by Clarke in 1983 and Pueschel in 1992. Because most stratospheric soot appears to be due to aircraft operations, application of an aircraft soot aerosol emission index to projected fuel consumption suggests a threefold increase of soot loading and light absorption by 2025. Together, those four data sets indicate an increase in mid-visible light extinction at a rate of 6 % per year. This trend is similar to the increase per year of sulfuric acid aerosol and of commercial fleet size. The proportionality between stepped-up aircraft operations above the tropopause and increases in stratospheric soot and sulfuric acid aerosol implicate aircraft as a source of stratospheric pollution. Because the strongly light-absorbing soot and the predominantly light-scattering sulfuric acid aerosol increase at similar rates, however, the mid-visible stratospheric aerosol single scatter albedo is expected to remain constant and not approach a critical value of 0.98 at which stratospheric cooling could change to warming.
Pueschel , R. F.↗
A 16-yr Comparison of Fine Particle and Aerosol Strong Acidity at the Interface Zone (1,540 m) and Within (452 m) the Planetary Boundary Layer of the Great Gulf and Presidential-Dry River Class I Wildernesses on the Presidential Range, New Hampshire
Mount Washington, NH in the White Mountain National Forest, is flanked to the north-northeast and south by two Class I Wilderness areas, the Great Gulf and Presidential Range-Dry River Wildernesses, respectively. The Clean Air Act protects Class I area natural resource values from air pollution. Aerosol sulfate, a fine particulate component that is often transported long distances, is a known contributor to visibility degradation and acidic deposition. We examined summertime fine particulate aerosol mass and sulfate, strong acidity and ammonium concentrations from 1988 to 2004 on Mount Washington at two elevations, 452 and 1,540 meters (msl). The former site is within, and the latter at the interface of, the planetary boundary layer. Comparisons of sampling interval durations (10 and 24 hours), site vs. site, and different sampling methods are made. We also examine the extent to which aerosol sulfate is neutralized. Ten hour (daytime) compared to 24 hour samples have higher mass and aerosol sulfate concentrations, however paired samples are well correlated. Fine mass concentrations compared between the 452 m and 1,540 m sites (standard temperature and pressure corrected) show a weak positive linear relationship with the later being approximately 34% lower. We attribute the lack of a strong correlation to the facts that the 1,540 m site is commonly at the interface of and even above the regional planetary boundary layer in summer and that it can intercept different air masses relative to the 452 m site. Sulfate is approximately 19% lower at the higher elevation site, but comprises a greater percentage of total fine mass; 42% compared to 35% for the high and low elevation site, respectively. Aerosol strong acidity was found to increase with increasing sulfate concentrations at both sites. At the high elevation site, elevated mass and sulfate concentrations are associated with westerly and southwesterly regional flows.
Murray, Georgia L.↗
Sulfuric Acid and Soot Particle Formation in Aircraft Exhaust
A combination of CN counts, Ames wire impactor size analyses and optical particle counter data in aircraft exhaust results in a continuous particle size distribution between 0.01 micrometer and 1 micrometer particle radius sampled in the exhaust of a Boeing 757 research aircraft. The two orders of magnitude size range covered by the measurements correspond to 6-7 orders of magnitude particle concentration. CN counts and small particle wire impactor data determine a nucleation mode, composed of aircraft-emitted sulfuric acid aerosol, that contributes between 62% and 85% to the total aerosol surface area and between 31% and 34% to its volume. Soot aerosol comprises 0.5% of the surface area of the sulfuric acid aerosol. Emission indices are: EIH2SO4 = 0.05 g/kgFUEL and (0.2-0.5) g/kgFUEL (for 75 ppmm and 675 ppmm fuel-S, respectively), 2.5E4<EISOOT<1.3E-3 g/kgFUEL, and EICN 8E14 and 1.3E16 particles/kgFUEL (for 75 and 675 ppmm fuel-S). The sulfur (gas) to H2SO4 (particle) conversion efficiency is between 10% and 25%.
Pueschel, Rudolf F.↗
Venus clouds - Structure and composition
The clouds of Venus consist of a fine sulfuric acid aerosol similar to that found in the earth's stratosphere. The acid aerosol on Venus appears to be uniformly mixed with the gas, at least in the visible layers, and possibly down to the cloud base.
Young, A. T.↗
Studies of the exhaust products from solid propellant rocket motors
This study was undertaken to determine the feasibility of conducting environmental chamber tests on the physical processes which occur when a solid rocket motor exhaust mixes with the ambient atmosphere. Of particular interest was the interaction between hydrogen chloride, aluminum oxide, and water vapor. The program consisted of three phases: (1) building a small rocket motor and using it to provide the exhaust species in a controlled environment; (2) evaluating instruments used to detect and measure HCl concentrations and if possible determining whether the HCl existed in the gaseous state or as an acid aerosol; (3) monitoring a series of 6.4-percent scale space shuttle motor tests and comparing the results to the environmental chamber studies. Eighteen firings were conducted in an environmental chamber with the initial ambient relative humidity set at values from 29 to 100 percent. Two additional firings were made in a large shed, and four were made on an open concrete apron. Six test firings at MSFC were monitored, and the ground level concentrations are reported. Evidence is presented which shows that the larger Al2O3 (5 to 50 micrometers) particles from the rocket motor can act as condensation nuclei. Under appropriate ambient conditions where there is sufficient water vapor this results in the formation of an acid aerosol. Droplets of this acid were detected both in the environmental chamber and in the scaled shuttle engine tests.
Dawbarn, R.↗
Balloon-Borne Measurements of Total Reactive Nitrogen, Nitric Acid, and Aerosol in the Cold Arctic Stratosphere
Total reactive nitrogen (NO(Y)) between 15 and 29 km was measured for the first time on board a balloon within the Arctic cold vortex. Observations of HNO3, aerosol, and ozone were made by instruments on the same balloon gondola which was launched from Esrange, Sweden (68 deg N, 20 deg E) on January 23, 1989. The NO(y) mixing ratio was observed to increase very rapidly from 6 ppbv at 18 km altitude to a maximum of 21 ppbv at 21 km, forming a sharp layer with a thickness of about 2 km. A minimum in the NO(y) mixing ratio of 5 ppbv was found at 27 km. The measured HNO3 profile shows broad similarities to that of NO(y). This observation, together with the observed very low column amount of NO2, shows that NO(x) had been almost totally converted to HNO3, and that NO(y) was composed mainly of HNO3. The enhanced aerosol concentration between 19 and 22 km suggests that the maximum abundance of HNO3 trapped in the form of nitric acid trihydrate (NAT) was about 6 ppbv at 21 km. The sampled air parcels were highly supersaturated with respect to NAT. Although extensive denitrification throughout the stratosphere did not prevail, an indication of denitrification was found at altitudes of 27 and 22 km, and between 18 and 15 km.
Kondo, Y.↗
Balloon for Long-Duration, High-Altitude Flight at Venus
A document describes a 5.5-m-diameter, helium-filled balloon designed for carrying a scientific payload having a mass of 44 kg for at least six days at an altitude of about 55 km in the atmosphere of Venus. The requirement for floating at nearly constant altitude dictates the choice of a mass-efficient spherical super-pressure balloon that tracks a constant atmospheric density. Therefore, the balloon is of a conventional spherical super-pressure type, except that it is made of materials chosen to minimize solar radiant heating and withstand the corrosive sulfuric acid aerosol of the Venusian atmosphere. The shell consists of 16 gores of a multilayer composite material. The outer layer, made of polytetrafluoroethylene, protects against sulfuric acid aerosol. Next is an aluminum layer that reflects sunlight to minimize heating, followed by an aluminized polyethylene terephthalate layer that resists permeation by helium, followed by an aromatic polyester fabric that imparts strength to withstand deployment forces and steady super-pressure. A polyurethane coat on the inner surface of the fabric facilitates sealing at gore-to-gore seams. End fittings and seals, and a tether connecting the end fittings to a gondola, are all made of sulfuric-acid-resistant materials.
Hall, Jeffrey↗
Nitric acid in polar stratospheric clouds - Similar temperature of nitric acid condensation and cloud formation
As shown independently by two different techniques, nitric acid aerosols and polar stratospheric clouds (PSCs) both form below similar threshold temperatures. This supports the idea that the PSC particles involved in chlorine activation and ozone depletion in the winter polar stratosphere are composed of nitric acid. One technique used to show this is the inertial impaction of nitric acid aerosols using an Er-2 aircraft; the other method is remote sensing of PSCs by the Stratospheric Aerosol Measurement (SAM II) satellite borne optical sensor. Both procedures were in operation during the Arctic Airborne Stratospheric Expedition in 1989, and the Airborne Antarctic Ozone Experiment in 1987. Analysis of Arctic particles gathered in situ indicates the presence of nitric acid below a 'first appearance' temperature Tfa = 202 K. This is the same highest temperature at which PSCs are seen by the SAM II satellite. In comparison, a 'first appearance' temperature Tfa = 198 K as found for the Antarctic samples.
Pueschel, Rudolf F.↗
Measurements of Nitric Acid and Aerosol Species Aboard the NASA DC-8 Aircraft During the SASS Ozone and Nitrogen Oxide Experiment (SONEX)
The SASS Ozone and Nitrogen Oxides Experiment (SONEX) over the North Atlantic during October/November 1997 offered an excellent opportunity to examine the budget of total reactive nitrogen (NO(sub y)) in the upper troposphere (8 - 12 km altitude). The median measured NO(sub y) mixing ratio was 425 parts per trillion by volume (pptv). Two different methods were used to measure HNO3: (1) the mist chamber technique and, (2) chemical ionization mass spectrometry. Two merged data sets using these HNO3 measurements were used to calculate NO(sub y) by summing the reactive nitrogen species (a combination of measured plus modeled results) and comparing the resultant values to measured NO(sub y) (gold catalytic reduction method). Both comparisons showed good agreement in the two quantities (slope > 0.9 and r(exp 2) > 0.9). Thus, the total reactive nitrogen budget in the upper troposphere over the North Atlantic can be explained in a general manner as a simple mixture of NO(sub x). (NO + NO2), HNO3, and PAN. Median values of NO(sub x)/NO(sub y) were approximately equal to 0.25, HNO3/NO(sub y) were approximately equal to 0.35 and Peroxyacetyl Nitrate (PAN)/NO(sub y) were approximately equal to 0. 17. Particulate NO3 and alkyl nitrates together composed <10 % of NO(sub y), while model estimated HNO4 averaged 12%.
Talbot, Robert W.↗
Measurements of Nitric Acid and Aerosol Species Aboard the NASA DC-8 Aircraft During the SASS OZone and Nitrogen Oxide Experiment (SONEX)
The SASS Ozone and Nitrogen Oxides Experiment (SONEX) over the north Atlantic during October/November 1997 offered an excellent opportunity to examine the budget of total reactive nitrogen (NO(y)) in the upper troposphere (8 - 12 km altitude). The median measured NO(y) mixing ratio was 425 parts per trillion by volume (pptv). Two different methods were used to measure HNO3: (1) the mist chamber technique and, (2) chemical ionization mass spectrometry. Two merged data sets using these HNO3 measurements were used to calculate NO(y) by summing the reactive nitrogen species (a combination of measured plus modeled results) and comparing the resultant values to measured NO(y) (gold catalytic reduction method). Both comparisons showed good agreement in the two quantities (slope greater than 0.9 and r(sup 2) greater than 0.9). Thus, the total reactive nitrogen budget in the upper troposphere over the North Atlantic can be explained in a general manner as a simple mixture of NO(x). (NO + NO2), HNO3, and PAN. Median values of NO(x)/NO(y) were approx. = 0.25, HNO3/NO(y) approx. = 0.35 and PAN/NO(y) approx. = 0.17. Particulate NO3 and alkyl nitrates together composed less than 10% of NO(y), while model estimated HNO4 averaged 12%.
Talbot, Robert W.↗
A New Parameterization of H2SO4/H2O Aerosol Composition: Atmospheric Implications
Recent results from a thermodynamic model of aqueous sulfuric acid are used to derive a new parameterization for the variation of sulfuric acid aerosol composition with temperature and relative humidity. This formulation is valid for relative humidities above 1 % in the temperature range of 185 to 260 K. An expression for calculating the vapor pressure of supercooled liquid water, consistent with the sulfuric acid model, is also presented. We show that the Steele and Hamill [1981] formulation underestimates the water partial pressure over aqueous H2SOI solutions by up to 12% at low temperatures. This difference results in a corresponding underestimate of the H2SO4 concentration in the aerosol by about 6 % of the weight percent at approximately 190 K. In addition, the relation commonly used for estimating the vapor pressure of H2O over supercooled liquid water differs by up to 10 % from our derived expression. The combined error can result in a 20 % underestimation of water activity over a H2SO4 solution droplet in the stratosphere, which has implications for the parameterization of heterogeneous reaction rates in stratospheric sulfuric acid aerosols. The influence of aerosol composition on the rate of homogeneous ice nucleation from a H2SO4 solution droplet is also discussed. This parameterization can also be used for homogeneous gas phase nucleation calculations of H2SO4 solution droplets under various environmental conditions such as in aircraft exhaust or in volcanic plumes.
Tabazadeh, Azadeh↗