Effects of Sea Salt Aerosol Emissions for Marine Cloud Brightening on Atmospheric Chemistry: Implications for Radiative Forcing
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Hannah M. Horowitz↗
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Results for “cloud chemistry”
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Aerosols in polluted versus nonpolluted air masses Long-range transport and effects on clouds
To assess the influence of anthropogenic aerosols on the physics and chemistry of clouds in the northeastern United States, aerosol and cloud-drop size distributions, elemental composition of aerosols as a function of size, and ionic content of cloud water were measured on Whiteface Mountain, NY, during the summers of 1981 and 1982. In several case studies, the data were cross-correlated with different air mass types - background continental, polluted continental, and maritime - that were advected to the sampling site. The results are the following: (1) Anthropogenic sources hundreds of kilometers upwind cause the small-particle (accumulation) mode number to increase from hundreds of thousands per cubic centimeter and the mass loading to increase from a few to several tens of micrograms per cubic meter, mostly in the form of sulfur aerosols. (2) A significant fraction of anthropogenic sulfur appears to act as cloud condensation nuclei (CCN) to affect the cloud drop concentration. (3) Clouds in Atlantic maritime air masses have cloud drop spectra that are markedly different from those measured in continental clouds. The drop concentration is significantly lower, and the drop size spectra are heavily skewed toward large drops. (4) Effects of anthropogenic pollutants on cloud water ionic composition are an increase of nitrate by a factor of 50, an increase of sulfate by more than one order of magnitude, and an increase of ammonium ion by a factor of 7. The net effect of the changes in ionic concentrations is an increase in cloud water acidity. An anion deficit even in maritime clouds suggests an unknown, possibly biogenic, source that could be responsible for a pH below neutral, which is frequently observed in nonpolluted clouds.
Pueschel, R. F.↗
Subsonic Aircraft Contrail and Cloud Effects Special Study (SUCCESS)
During recent years interest in the impact of commercial aircraft on the climate has increased. Aircraft might impact climate in a number of ways. Contrails are clearly a direct radiative forcing mechanism. Exhaust emissions, principally soot and sulfate, might indirectly force the climate by modifying the radiative properties of cirrus clouds. The SUCCESS program was carried out to investigate these issues. It also has several other goals including: better understanding the emissions from aircraft, better understanding the formation of cirrus clouds: better understanding the radiative properties of contrails and clouds and their remote sensing; better understanding the heterogeneous chemistry in the upper atmosphere; and developing new instruments of importance to atmospheric chemistry and cloud physics. SUCCESS took place during April and May of 1997. The NASA DC-8, ER-2, T-39, and 757 aircraft were used as in situ sampling, remote sensing, near field sampling, and emission sources respectively. Most of the operations occurred near the DOE's Atmospheric Radiation Measurement Site in Northern Oklahoma. The DOE operated several other aircraft so that on some days as many as six research aircraft flew together. Numerous new instruments functioned during the mission. This talk will present an overview of SUCCESS from the operational point of view, and provide some of the overall scientific highlights.
Toon, O.B.↗
Subsonic Aircraft Contrail and Cloud Effects Special Study (SUCCESS)
During recent years interest in the impact of commercial aircraft on the climate has increased. Aircraft might impact climate in a number of ways. Contrails are clearly a direct radiative forcing mechanism. Exhaust emissions, principally soot and sulfate, might indirectly radiative force the climate by modifying the properties of cirrus clouds. The SUCCESS program was carried out to investigate these issues. It also had several other goals including: better understanding the emissions from aircraft, better understanding the formation of cirrus clouds: better understanding the radiative properties of contrail and clouds and their remote sensing; better understanding the heterogeneous chemistry in the upper atmosphere; and developing new instruments of importance to atmospheric chemistry and cloud physics. SUCCESS took place during April and May of 1996. The NASA DC-8, ER-2, T-39, and 757 aircraft were used as in situ sampling, remote sensing, near field sampling, and emission sources respectively. Most of the operations occurred near the DOE's Atmospheric Radiation Measurement Site in Northern Oklahoma. The DOE operated several other aircraft so that on some days as many as six research aircraft operated together. Numerous new instruments operated during the mission. This talk will present an overview of SUCCESS from the operational point of view, and provide some of the overall scientific highlights.
Toon, O. B.↗
The role of aqueous chemistry in determining the composition and cloud structure of the upper troposphere on Uranus
Aqueous chemistry on Uranus affects the atmospheric abundances of NH3 and H2S below the methane cloud base. Here a complete thermochemical equilibrium model for the H2O-NH3-H2S system is presented. Inclusion of H2S increases the aqueous removal of NH3 to 20-30 percent, but aqueous chemistry alone cannot account for the depletion of NH3 in the 150-200-K region of the atmosphere required to fit microwave observations. Formation of NH4SH clouds can account for the observed depletion provided the H2S/NH3 ratio is enhanced by a factor of 4 relative to solar. Perturbations to the chemical balance between N and S, for example by the general circulation on Uranus, would then produce regions with either NH3 or H2S aloft.
Carlson, Barbara E.↗
Chemistry of chlorine in dense interstellar clouds
Laboratory experiments and theoretical modeling show that the chemistry of chlorine is fairly simple in dense interstellar clouds, with Cl and HCl as the only species whose fractional abundances are significant. The estimated fraction of gas-phase chlorine present as HCl lies between 25-65 percent, in good agreement with the recent observations of the ground state HCl transition by Blake, Keene, and Philips (1985). These results, combined with the observational limits on HCl, indicate that chlorine is not severely depleted in dense interstellar clouds.
Blake, G. A.↗
The chemistry of phosphorus in dense interstellar clouds
Laboratory experiments show that the ion-molecule chemistry of phosphorus is significantly different from that of nitrogen in dense interstellar clouds. The PH3 molecule is not readily formed by gas-phase, ion-molecule reactions in these regions. Laboratory results used in a simple kinetic model indicate that the most abundant molecule containing phosphorus in dense clouds is PO.
Thorne, L. R.↗
A WRF-Chem Analysis of Flash Rates, Lightning-NOx Production and Subsequent Trace Gas Chemistry of the 29-30 May 2012 Convective Event in Oklahoma During DC3
The Deep Convective Clouds and Chemistry (DC3) field campaign in 2012 provided a plethora of aircraft and ground-based observations (e.g., trace gases, lightning and radar) to study deep convective storms, their convective transport of trace gases, and associated lightning occurrence and production of nitrogen oxides (NOx). This is a continuation of previous work, which compared lightning observations (Oklahoma Lightning Mapping Array and National Lightning Detection Network) with flashes generated by various flash rate parameterization schemes (FRPSs) from the literature in a Weather Research and Forecasting Chemistry (WRF-Chem) model simulation of the 29-30 May 2012 Oklahoma thunderstorm. Based on the Oklahoma radar observations and Lightning Mapping Array data, new FRPSs are being generated and incorporated into the model. The focus of this analysis is on estimating the amount of lightning-generated nitrogen oxides (LNOx) produced per flash in this storm through a series of model simulations using different production per flash assumptions and comparisons with DC3 aircraft anvil observations. The result of this analysis will be compared with previously studied mid-latitude storms. Additional model simulations are conducted to investigate the upper troposphere transport, distribution, and chemistry of the LNOx plume during the 24 hours following the convective event to investigate ozone production. These model-simulated mixing ratios are compared against the aircraft observations made on 30 May over the southern Appalachians.
Cummings, Kristin A.↗
Stratospheric ion and aerosol chemistry and possible links with cirrus cloud microphysics - A critical assessment
Aspects of stratospheric ion chemistry and physics are assessed as they relate to aerosol formation and the transport of aerosols to upper tropospheric regions to create conditions favorable for cirrus cloud formation. It is found that ion-induced nucleation and other known phase transitions involving ions and sulfuric acid vapor are probably not efficient processes for stratospheric aerosol formation, and cannot compete with condensation of sulfuric acid on preexisting particles of volcanic or meteoritic origin which are larger than about 0.15 micron in radius. Thus, galactic cosmic rays cannot have a significant impact on stratospheric aerosol population. Changes in the stratospheric aerosol burden due to volcanos are up to two orders of magnitude larger than changes in ion densities. Thus, volcanic activity may modulate the radiative properties of cirrus clouds.
Mohnen, Volker A.↗
A WRF-Chem Flash Rate Parameterization Scheme and LNOx Analysis of the 29-30 May 2012 Convective Event in Oklahoma During DC3
The Deep Convective Clouds and Chemistry (DC3) field campaign in 2012 provided a plethora of aircraft and ground-based observations (e.g., trace gases, lightning and radar) to study deep convective storms, their convective transport of trace gases, and associated lightning occurrence and production of nitrogen oxides (NOx). Based on the measurements taken of the 29-30 May 2012 Oklahoma thunderstorm, an analysis against a Weather Research and Forecasting Chemistry (WRF-Chem) model simulation of the same event at 3-km horizontal resolution was performed. One of the main objectives was to include various flash rate parameterization schemes (FRPSs) in the model and identify which scheme(s) best captured the flash rates observed by the National Lightning Detection Network (NLDN) and Oklahoma Lightning Mapping Array (LMA). The comparison indicates how well the schemes predicted the timing, location, and number of lightning flashes. The FRPSs implemented in the model were based on the simulated thunderstorms physical features, such as maximum vertical velocity, cloud top height, and updraft volume. Adjustment factors were applied to each FRPS to best capture the observed flash trend and a sensitivity study was performed to compare the range in model-simulated lightning-generated nitrogen oxides (LNOx) generated by each FRPS over the storms lifetime. Based on the best FRPS, model-simulated LNOx was compared against aircraft measured NOx. The trace gas analysis, along with the increased detail in the model specification of the vertical distribution of lightning flashes as suggested by the LMA data, provide guidance in determining the scenario of NO production per intracloud and cloud-to-ground flash that best matches the NOx mixing ratios observed by the aircraft.
Atmospheric chemistry↗
Chemistry and Evolution of Interstellar Clouds
In this chapter we describe how elements have been and are still being formed in the galaxy and how they are transformed into the reservoir of materials present at the time of formation of our protosolar nebula. We discuss the global cycle of matter, beginning at its formation site in stars, where it is ejected through winds and explosions into the diffuse interstellar medium. In the next stage of the global cycle occurs in cold, dense molecular clouds, where the complexity of molecules and ices increases relative to the diffuse ISM.. When a protostar forms in a dense core within a molecular cloud, it heats the surrounding infalling matter warms and releases molecules from the solid phase into the gas phase in a warm, dense core, sponsoring a rich gas-phase chemistry. Some material from the cold and warm regions within molecular clouds probably survives as interstellar matter in the protostellar disk. For the diffuse ISM, for cold, dense clouds, and for dense-warm cores, the physio-chemical processes that occur within the gas and solid phases are discussed in detail.
Wooden, D. H.↗
Ice Chemistry in Interstellar Dense Molecular Clouds, Protostellar Disks, and Comets
Despite the low temperatures (T less than 20K), low pressures, and low molecular densities found in much of the cosmos, considerable chemistry is expected to occur in many astronomical environments. Much of this chemistry happens in icy grain mantles on dust grains and is driven by ionizing radiation. This ionizing radiation breaks chemical bonds of molecules in the ices and creates a host of ions and radicals that can react at the ambient temperature or when the parent ice is subsequently warmed. Experiments that similar these conditions have demonstrated a rich chemistry associated with these environments that leads to a wide variety of organic products. Many of these products are of considerable interest to astrobiology. For example, the irradiation of simple ices has been shown to abiotically produce amino acids, nucleobases, quinones, and amphiphiles, all compounds that play key roles in modern biochemistry. This suggests extraterrestrial chemistry could have played a role in the origin of life on Earth and, by extension, do so on planets in other stellar systems.
Ice Irradiation↗
Heterogeneous Chemistry Involving Methanol in Tropospheric Clouds
In this report we analyze airborne measurements to suggest that methanol in biomass burning smoke is lost heterogeneously in clouds. When a smoke plume intersected a cumulus cloud during the SAFARI 2000 field project, the observed methanol gas phase concentration rapidly declined. Current understanding of gas and aqueous phase chemistry cannot explain the loss of methanol documented by these measurements. Two plausible heterogeneous reactions are proposed to explain the observed simultaneous loss and production of methanol and formaldehyde, respectively. If the rapid heterogeneous processing of methanol, seen in a cloud impacted by smoke, occurs in more pristine clouds, it could affect the oxidizing capacity of the troposphere on a global scale.
Tabazadeh, A.↗
Production of NOx by Lightning and its Effects on Atmospheric Chemistry
Production of NO(x) by lightning remains the NO(x) source with the greatest uncertainty. Current estimates of the global source strength range over a factor of four (from 2 to 8 TgN/year). Ongoing efforts to reduce this uncertainty through field programs, cloud-resolved modeling, global modeling, and satellite data analysis will be described in this seminar. Representation of the lightning source in global or regional chemical transport models requires three types of information: the distribution of lightning flashes as a function of time and space, the production of NO(x) per flash, and the effective vertical distribution of the lightning-injected NO(x). Methods of specifying these items in a model will be discussed. For example, the current method of specifying flash rates in NASA's Global Modeling Initiative (GMI) chemical transport model will be discussed, as well as work underway in developing algorithms for use in the regional models CMAQ and WRF-Chem. A number of methods have been employed to estimate either production per lightning flash or the production per unit flash length. Such estimates derived from cloud-resolved chemistry simulations and from satellite NO2 retrievals will be presented as well as the methodologies employed. Cloud-resolved model output has also been used in developing vertical profiles of lightning NO(x) for use in global models. Effects of lightning NO(x) on O3 and HO(x) distributions will be illustrated regionally and globally.
Pickering, Kenneth E.↗
A Wrf-Chem Flash Rate Parameterization Scheme and LNO(x) Analysis of the 29-30 May 2012 Convective Event in Oklahoma During DC3
The Deep Convective Clouds and Chemistry (DC3) field campaign in 2012 provided a plethora of aircraft and ground-based observations (e.g., trace gases, lightning and radar) to study deep convective storms, their convective transport of trace gases, and associated lightning occurrence and production of nitrogen oxides (NOx). Based on the measurements taken of the 29-30 May 2012 Oklahoma thunderstorm, an analysis against a Weather Research and Forecasting Chemistry (WRF-Chem) model simulation of the same event at 3-km horizontal resolution was performed. One of the main objectives was to include various flash rate parameterization schemes (FRPSs) in the model and identify which scheme(s) best captured the flash rates observed by the National Lightning Detection Network (NLDN) and Oklahoma Lightning Mapping Array (LMA). The comparison indicates how well the schemes predicted the timing, location, and number of lightning flashes. The FRPSs implemented in the model were based on the simulated thunderstorms physical features, such as maximum vertical velocity, cloud top height, and updraft volume. Adjustment factors were added to each FRPS to best capture the observed flash trend and a sensitivity study was performed to compare the range in model-simulated lightning-generated nitrogen oxides (LNOx) generated by each FRPS over the storms lifetime. Based on the best FRPS, model-simulated LNOx was compared against aircraft measured NOx. The trace gas analysis, along with the increased detail in the model specification of the vertical distribution of lightning flashes as suggested by the LMA data, provide guidance in determining the scenario of NO production per intracloud and cloud-to-ground flash that best matches the NOx mixing ratios observed by the aircraft.
Cloud physics↗
Water and the photochemistry of the troposphere
A discussion is presented concerning the role of water in its liquid and gaseous states in the chemistry and photochemistry of the earth's troposphere, with attention to the formation of the hydroxyl radical, oxidation chains involving the gases methane, carbon monoxide and ammonia, the atmospheric chemistry of the sulfur, hydrogen, halogen and nitrogen species, and the function of lightning as a source of tropospheric species. The phenomena of 'rainout', 'washout', and the aqueous chemistry of cloud an rain droplets and of water-covered aerosols, are noted. A section is devoted to the past and anticipated impact of anthropogenic activities on the chemistry and composition of the earth's atmosphere.
Levine, J. S.↗
Diffuse interstellar clouds as a chemical laboratory - The chemistry of diatomic carbon species
The chemistry of C2, CH, and CO in diffuse interstellar clouds is analyzed and compared to absorption line measurements toward background stars. Analytical expressions in terms of column densities are derived for the rate equations. The results indicate that in clouds with 4 mag of visual extinction, the abundance of C+ has to decrease by a factor of about 15 from the value traditionally used for clouds with 1 mag of extinction. The rate coefficients for the reactions C+ + CH - C2+ + H and C+ + H2 - CH2+ + h-nu need to be reduced from previous estimates. Chemical arguments are presented for the revised rate coefficients.
Federman, S. R.↗
Kinematic and Microphysical Control of Lightning Flash Rate over Northern Alabama
The Deep Convective Clouds and Chemistry (DC3) experiment seeks to examine the relationship between deep convection and the production of nitrogen oxides (NO (sub x)) via lightning (LNO (sub x)). A critical step in estimating LNO (sub x) production in a cloud-resolving model (CRM) without explicit lightning is to estimate the flash rate from available model parameters that are statistically and physically correlated. As such, the objective of this study is to develop, improve and evaluate lightning flash rate parameterizations in a variety of meteorological environments and storm types using radar and lightning mapping array (LMA) observations taken over Northern Alabama from 2005-2012, including during DC3. UAH's Advanced Radar for Meteorological and Operational Research (ARMOR) and the Weather Surveillance Radar - 1988 Doppler (WSR 88D) located at Hytop (KHTX) comprises the dual-Doppler and polarimetric radar network, which has been in operation since 2004. The northern Alabama LMA (NA LMA) in conjunction with Vaisala's National Lightning Detection Network (NLDN) allow for a detailed depiction of total lightning during this period. This study will integrate ARMOR-KHTX dual Doppler/polarimetric radar and NA LMA lightning observations from past and ongoing studies, including the more recent DC3 results, over northern Alabama to form a large data set of 15-20 case days and over 20 individual storms, including both ordinary multicell and supercell convection. Several flash rate parameterizations will be developed and tested, including those based on 1) graupel/small hail volume; 2) graupel/small hail mass, and 3) convective updraft volume. Sensitivity of the flash rate parameterizations to storm intensity, storm morphology and environmental conditions will be explored.
Carey, Lawrence D.↗