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Toon, Owen B.

Publications and source records attributed to Toon, Owen B..

At least 19 records

Stratospheric Climate Anomalies and Ozone Loss Caused by the Hunga Tonga-Hunga Ha'apai Volcanic Eruption

We report the Hunga Tonga-Hunga Ha'apai (HTHH) volcanic eruption in January 2022 injected unprecedented amounts of water vapor (H 2 O) and a moderate amount of the aerosol precursor sulfur dioxide (SO 2 ) into the Southern Hemisphere (SH) tropical stratosphere. The H 2 O and aerosol perturbations have persisted during 2022 and early 2023 and dispersed throughout the atmosphere. Observations show large-scale SH stratospheric cooling, equatorward shift of the Antarctic polar vortex and slowing of the Brewer-Dobson circulation. Satellite observations show substantial ozone reductions over SH winter midlatitudes that coincide with the largest circulation anomalies. Chemistry-climate model simulations forced by realistic HTHH inputs of H 2 O and SO 2 qualitatively reproduce the observed evolution of the H 2 O and aerosol plumes over the first year, and the model exhibits stratospheric cooling, circulation changes and ozone effects similar to observed behavior. The agreement demonstrates that the observed stratospheric changes are caused by the HTHH volcanic influences.

58 GEOSCIENCES↗

Radiative Forcing From the 2014–2022 Volcanic and Wildfire Injections

Abstract Volcanic and wildfire events between 2014 and 2022 injected ∼3.2 Tg of sulfur dioxide and 0.8 Tg of smoke aerosols into the stratosphere. With injections at higher altitudes and lower latitudes, the simulated stratospheric lifetime of the 2014–2022 injections is about 50% longer than the volcanic 2005–2013 injections. The simulated global mean effective radiative forcing (ERF) of 2014–2022 is −0.18 W m −2 , ∼40% of the ERF of the period of 1991–1999 with a large‐magnitude volcanic eruption (Pinatubo). Our climate model suggests that the stratospheric smoke aerosols generate ∼60% more negative ERF than volcanic sulfate per unit aerosol optical depth. Studies that fail to account for the different radiative properties of wildfire smoke relative to volcanic sulfate will likely underestimate the negative stratospheric forcings. Our analysis suggests that stratospheric injections offset 20% of the increase in global mean surface temperature between 2014–2022 and 1999–2002.

54 ENVIRONMENTAL SCIENCES↗

Assessment of Wind Energy Resource Potential for Future Human Missions to Mars

Energy sustainability and redundancy for surface habitats, life support systems and scientific instrumentation represent one of the highest-priority issues for future crewed missions to Mars. However, power sources utilized for the current class of robotic missions to Mars may be potentially dangerous near human surface habitats (for example, nuclear) or lack stability on diurnal or seasonal timescales (for example, solar) that cannot be easily compensated for by power storage. Here, we evaluate the power potential for wind turbines as an alternative energy resource on the Mars surface. Using a state-of-the-art Mars global climate model, we analyse the total planetary Martian wind potential and calculate its spatial and temporal variability. We find that wind speeds at some proposed landing sites are sufficiently fast to provide a stand-alone or complementary energy source to solar or nuclear power. While several regions show promising wind energy resource potential, other regions of scientific interest can be discarded based on the natural solar and wind energy potential alone. We demonstrate that wind energy compensates for diurnal and seasonal reductions in solar power particularly in regions of scientific merit in the midlatitudes and during regional dust storms. Critically, proposed turbines stabilize power production when combined with solar arrays, increasing the percent time that power exceeds estimated mission requirements from ~40% for solar arrays alone to greater than 60-90% across a broad fraction of the Mars surface. We encourage additional study aimed at advancing wind turbine technology to operate efficiently under Mars conditions and to extract more power from Mars winds.

atmospheric dynamics↗

Abundant Nitrate and Nitric Acid Aerosol in the Upper Troposphere and Lower Stratosphere

The tropospheric and stratospheric nitrate aerosol is simulated by a sectional aerosol model coupled to the Community Earth System Model. The simulated nitrate mass fractional contribution to aerosols is significantly higher in the upper troposphere and lower stratosphere (UTLS) than that at the surface. Both in situ measurements and simulations show that nitrate aerosol accounts for about 30%–40% of the aerosol mass at the tropopause of the Asian summer monsoon (ASM) region. Furthermore, simulated condensed nitric acid particles account for ~20% of the annual mean aerosol mass at the tropical tropopause, and over 95% in the UTLS at the South Pole in June-July-August. Here, our study suggests that the extremely cold ambient conditions in the UTLS of the tropics, ASM and polar regions thermodynamically favor the condensation of ammonia and nitric acid. The widely distributed nitrate aerosol in the global UTLS may be overlooked by climate models.

54 ENVIRONMENTAL SCIENCES↗

Upper Troposphere Smoke Injection From Large Areal Fires

Abstract Large areal fires, such as those ignited following a nuclear detonation, can inject smoke into the upper troposphere and lower stratosphere. Detailed fire simulations allow for assessment of how local weather interacts with these fires and affects smoke lofting. In this study, we employ the fire simulation package in the Weather Research and Forecasting (WRF‐Fire) model, Version 4.0.1, to explore how smoke lofting from a fire burning a homogeneous fuel bed changes with varying local winds, relative humidity, and atmospheric boundary‐layer stability for two different‐sized areal fires. The presence of moisture has the greatest influence on the results by raising the altitude of lofting, while faster wind speeds dampen lofting and lower the injection height. Stably stratified conditions inhibit plume propagation compared with neutrally stratified conditions, although the impact of stability is not as strong as that of moisture and winds. These findings highlight the importance of using an appropriate atmospheric profile when simulating large fires, as the local weather can have a meaningful influence on smoke lofting.

54 ENVIRONMENTAL SCIENCES↗

Persisting volcanic ash particles impact stratospheric SO 2 lifetime and aerosol optical properties

Volcanic ash is often neglected in climate simulations because ash particles are assumed to have a short atmospheric lifetime, and to not participate in sulfur chemistry. After the Mt. Kelut eruption in 2014, stratospheric ash-rich aerosols were observed for months. Here we show that the persistence of super-micron ash is consistent with a density near 0.5 g cm -3 , close to pumice. Ash-rich particles dominate the volcanic cloud optical properties for the first 60 days. We also find that the initial SO 2 lifetime is determined by SO 2 uptake on ash, rather than by reaction with OH as commonly assumed. About 43% more volcanic sulfur is removed from the stratosphere in 2 months with the SO 2 heterogeneous chemistry on ash particles than without. This research suggests the need for re-evaluation of factors controlling SO 2 lifetime in climate model simulations, and of the impact of volcanic ash on stratospheric chemistry and radiation.

54 ENVIRONMENTAL SCIENCES↗

A regional nuclear conflict would compromise global food security

A limited nuclear war between India and Pakistan could ignite fires large enough to emit more than 5 Tg of soot into the stratosphere. Climate model simulations have shown severe resulting climate perturbations with declines in global mean temperature by 1.8 °C and precipitation by 8%, for at least 5 y. Here we evaluate impacts for the global food system. Six harmonized state-of-the-art crop models show that global caloric production from maize, wheat, rice, and soybean falls by 13 (±1)%, 11 (±8)%, 3 (±5)%, and 17 (±2)% over 5 y. Total single-year losses of 12 (±4)% quadruple the largest observed historical anomaly and exceed impacts caused by historic droughts and volcanic eruptions. Colder temperatures drive losses more than changes in precipitation and solar radiation, leading to strongest impacts in temperate regions poleward of 30°N, including the United States, Europe, and China for 10 to 15 y. Integrated food trade network analyses show that domestic reserves and global trade can largely buffer the production anomaly in the first year. Persistent multiyear losses, however, would constrain domestic food availability and propagate to the Global South, especially to food-insecure countries. By year 5, maize and wheat availability would decrease by 13% globally and by more than 20% in 71 countries with a cumulative population of 1.3 billion people. In view of increasing instability in South Asia, this study shows that a regional conflict using <1% of the worldwide nuclear arsenal could have adverse consequences for global food security unmatched in modern history.

54 ENVIRONMENTAL SCIENCES↗

A Regional Nuclear Conflict Would Compromise Global Food Security

A limited nuclear war between India and Pakistan could ignite fires large enough to emit more than 5 Tg of soot into the stratosphere. Climate model simulations have shown severe resulting climate perturbations with declines in global mean temperature by 1.8 ◦C and precipitation by 8%, for at least 5 y. Here we evaluate impacts for the global food system. Six harmonized state-of-the-art crop models show that global caloric production from maize, wheat, rice, and soybean falls by 13 (±1)%, 11 (±8)%, 3 (±5)%, and 17 (±2)% over 5 y. Total single-year losses of 12 (±4)% quadruple the largest observed historical anomaly and exceed impacts caused by historic droughts and volcanic eruptions. Colder temperatures drive losses more than changes in precipitation and solar radiation, leading to strongest impacts in temperate regions poleward of 30◦N, including the United States, Europe, and China for 10 to 15 y. Integrated food trade network analyses show that domestic reserves and global trade can largely buffer the production anomaly in the first year. Persistent multiyear losses, however, would constrain domestic food availability and propagate to the Global South, especially to food-insecure countries. By year 5, maize and wheat availability would decrease by 13% globally and by more than 20% in 71 countries with a cumulative population of 1.3 billion people. In view of increasing instability in South Asia, this study shows that a regional conflict using <1% of the worldwide nuclear arsenal could have adverse consequences for global food security unmatched in modern history.

Jaegermeyr, Jonas↗

Rapidly expanding nuclear arsenals in Pakistan and India portend regional and global catastrophe

Pakistan and India may have 400 to 500 nuclear weapons by 2025 with yields from tested 12- to 45-kt values to a few hundred kilotons. If India uses 100 strategic weapons to attack urban centers and Pakistan uses 150, fatalities could reach 50 to 125 million people, and nuclear-ignited fires could release 16 to 36 Tg of black carbon in smoke, depending on yield. The smoke will rise into the upper troposphere, be self-lofted into the stratosphere, and spread globally within weeks. Surface sunlight will decline by 20 to 35%, cooling the global surface by 2° to 5°C and reducing precipitation by 15 to 30%, with larger regional impacts. Recovery takes more than 10 years. Net primary productivity declines 15 to 30% on land and 5 to 15% in oceans threatening mass starvation and additional worldwide collateral fatalities.

54 ENVIRONMENTAL SCIENCES↗

Efficient In‐Cloud Removal of Aerosols by Deep Convection

Abstract Convective systems dominate the vertical transport of aerosols and trace gases. The most recent in situ aerosol measurements presented here show that the concentrations of primary aerosols including sea salt and black carbon drop by factors of 10 to 10,000 from the surface to the upper troposphere. In this study we show that the default convective transport scheme in the National Science Foundation/Department of Energy Community Earth System Model results in a high bias of 10–1,000 times the measured aerosol mass for black carbon and sea salt in the middle and upper troposphere. A modified transport scheme, which considers aerosol activation from entrained air above the cloud base and aerosol‐cloud interaction associated with convection, dramatically improves model agreement with in situ measurements suggesting that deep convection can efficiently remove primary aerosols. We suggest that models that fail to consider secondary activation may overestimate black carbon's radiative forcing by a factor of 2.

54 ENVIRONMENTAL SCIENCES↗

Volcanic Radiative Forcing From 1979 to 2015

Using volcanic sulfur dioxide emissions in an aerosol-climate model, we derive a time series of global-mean volcanic effective radiative forcing (ERF) from 1979 to 2015. For 2005–2015, we calculate a global multiannual mean volcanic ERF of 0.08 W/m 2 relative to the volcanically quiescent 1999–2002 period, due to a high frequency of small-to-moderate-magnitude explosive eruptions after 2004. For eruptions of large magnitude such as 1991 Mt. Pinatubo, our model-simulated volcanic ERF, which accounts for rapid adjustments including aerosol perturbations of clouds, is less negative than that reported in the Intergovernmental Panel on Climate Change (IPCC) Fifth Assessment Report (AR5) that only accounted for stratospheric temperature adjustments. We find that, when rapid adjustments are considered, the relation between volcanic forcing and volcanic stratospheric optical depth (SAOD) is 13–21% weaker than reported in IPCC AR5 for large-magnitude eruptions. Further, our analysis of the recurrence frequency of eruptions reveals that sulfur-rich small-to-moderate-magnitude eruptions with column heights =10 km occur frequently, with periods of volcanic quiescence being statistically rare. Small-to-moderate-magnitude eruptions should therefore be included in climate model simulations, given the >50% chance of one or two eruptions to occur in any given year. Not all of these eruptions affect the stratospheric aerosol budget, but those that do increase the nonvolcanic background SAOD by ~0.004 on average, contributing ~50% to the total SAOD in the absence of large-magnitude eruptions. This equates to a volcanic ERF of about 0.10 W/m 2 , which is about two thirds of the ERF from ozone changes induced by ozone-depleting substances.

54 ENVIRONMENTAL SCIENCES↗

Effects of Scavenging, Entrainment, and Aqueous Chemistry on Peroxides and Formaldehyde in Deep Convective Outflow Over the Central and Southeast United States

Deep convective transport of gaseous precursors to ozone (O3) and aerosols to the upper troposphere is affected by liquid phase and mixed-phase scavenging, entrainment of free tropospheric air and aqueous chemistry. The contributions of these processes are examined using aircraft measurements obtained in storm inflow and outflow during the 2012 Deep Convective Clouds and Chemistry (DC3) experiment combined with high-resolution (dx = 3 km) WRF-Chem simulations of a severe storm, an air mass storm, and a mesoscale convective system (MCS). The simulation results for the MCS suggest that formaldehyde (CH2O) is not retained in ice when cloud water freezes, in agreement with previous studies of the severe storm. By analyzing WRF-Chem trajectories, the effects of scavenging, entrainment, and aqueous chemistry on outflow mixing ratios of CH2O, methyl hydroperoxide (CH3OOH), and hydrogen peroxide (H2O2) are quantified. Liquid phase microphysical scavenging was the dominant process reducing CH2O and H2O2 outflow mixing ratios in all three storms. Aqueous chemistry did not significantly affect outflow mixing ratios of all three species. In the severe storm and MCS, the higher than expected reductions in CH3OOH mixing ratios in the storm cores were primarily due to entrainment of low-background CH3OOH. In the air mass storm, lower CH3OOH and H2O2 scavenging efficiencies (SEs) than in the MCS were partly due to entrainment of higher background CH3OOH and H2O2. Overestimated rain and hail production in WRF-Chem reduces the confidence in ice retention fraction values determined for the peroxides and CH2O.

Bela, Megan↗

An Overview of Mesoscale Aerosol Processes, Comparisons, and Validation Studies from DRAGON Networks

Over the past 24 years, the AErosol RObotic NETwork (AERONET) program has provided highly accurate remote-sensing characterization of aerosol optical and physical properties for an increasingly extensive geographic distribution including all continents and many oceanic island and coastal sites. The measurements and retrievals from the AERONET global network have addressed satellite and model validation needs very well, but there have been challenges in making comparisons to similar parameters from in situ surface and airborne measurements. Additionally, with improved spatial and temporal satellite remote sensing of aerosols, there is a need for higher spatial-resolution ground-based remote-sensing networks. An effort to address these needs resulted in a number of field campaign networks called Distributed Regional Aerosol Gridded Observation Networks (DRAGONs) that were designed to provide a database for in situ and remote-sensing comparison and analysis of local to mesoscale variability in aerosol properties. This paper describes the DRAGON deployments that will continue to contribute to the growing body of research related to meso- and microscale aerosol features and processes. The research presented in this special issue illustrates the diversity of topics that has resulted from the application of data from these networks.

Holben, Brent N.↗

Planning, Implementation, and Scientific Goals of the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) Field Missions

The Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field mission based at Ellington Field, Texas, during August and September 2013 employed the most comprehensive airborne payload to date to investigate atmospheric composition over North America. The NASA ER-2, DC-8, and SPEC Inc. Learjet flew 57 science flights from the surface to 20 km. The ER-2 employed seven remote sensing instruments as a satellite surrogate and eight in situ instruments. The DC-8 employed 23 in situ and five remote sensing instruments for radiation, chemistry, and microphysics. The Learjet used 11 instruments to explore cloud microphysics. SEAC4RS launched numerous balloons, augmented Aerosol RObotic NETwork, and collaborated with many existing ground measurement sites. Flights investigating convection included close coordination of all three aircraft. Coordinated DC-8 and ER-2 flights investigated the optical properties of aerosols, the influence of aerosols on clouds, and the performance of new instruments for satellite measurements of clouds and aerosols. ER-2 sorties sampled stratospheric injections of water vapor and other chemicals by local and distant convection. DC-8 flights studied seasonally evolving chemistry in the Southeastern U.S., atmospheric chemistry with lower emissions of NOx and SO2 than in previous decades, isoprene chemistry under high and low NOx conditions at different locations, organic aerosols, air pollution near Houston and in petroleum fields, smoke from wildfires in western forests and from agricultural fires in the Mississippi Valley, and the ways in which the chemistry in the boundary layer and the upper troposphere were influenced by vertical transport in convective clouds.

Toon, Owen B.↗

Ice Nucleation and Dehydration in the Tropical Tropopause Layer

Optically thin cirrus near the tropical tropopause regulate the humidity of air entering the stratosphere, which in turn has a strong influence on the Earth's radiation budget and climate. Recent highaltitude, unmanned aircraft measurements provide evidence for two distinct classes of cirrus formed in the tropical tropopause region: (i) vertically extensive cirrus with low ice number concentrations, low extinctions, and large supersaturations (up to approx. 70%) with respect to ice; and (ii) vertically thin cirrus layers with much higher ice concentrations that effectively deplete the vapor in excess of saturation. The persistent supersaturation in the former class of cirrus is consistent with the long time-scales (several hours or longer) for quenching of vapor in excess of saturation given the low ice concentrations and cold tropical tropopause temperatures. The low-concentration clouds are likely formed on a background population of insoluble particles with concentrations less than 100 L−1 (often less than 20 L−1), whereas the high ice concentration layers (with concentrations up to 10,000 L−1) can only be produced by homogeneous freezing of an abundant population of aqueous aerosols. These measurements, along with past high-altitude aircraft measurements, indicate that the low-concentration cirrus occur frequently in the tropical tropopause region, whereas the high-concentration cirrus occur infrequently. The predominance of the low-concentration clouds means cirrus near the tropical tropopause may typically allow entry of air into the stratosphere with as much as approx. 1.7 times the ice saturation mixing ratio.

dehydration↗

Nitrogen Incorporation in CH4-N2 Photochemical Aerosol Produced by Far UV Irradiation

Nitrile incorporation into Titan aerosol accompanying hydrocarbon chemistry is thought to be driven by extreme UV wavelengths (lambda < 120 nm) or magnetospheric electrons in the outer reaches of the atmosphere. Far UV radiation (120 - 200 nm), which is transmitted down to the stratosphere of Titan, is expected to affect hydrocarbon chemistry only and not initiate the formation of nitrogenated species. We have examined the chemical properties of photochemical aerosol produced at far UV wavelengths using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS), which allows for elemental analysis of particle-phase products. Our results show that aerosol formed from CH4/N2 photochemistry contains a surprising amount of nitrogen, up to 16% by mass, a result of photolysis in the far UV. The proportion of nitrogenated organics to hydrocarbon species is shown to be correlated with that of N2 in the irradiated gas. The aerosol mass greatly decreases when N2 is removed, indicating that N2 plays a major role in aerosol production. Because direct dissociation of N2 is highly improbable given the immeasurably low cross-section at the wavelengths studied, the chemical activation of N2 must occur via another pathway. Any chemical activation of N2 at wavelengths > 120 nm is presently unaccounted for in atmospheric photochemical models. We suggest that reaction with CH radicals produced from CH4 photolysis may provide a mechanism for incorporating N into the molecular structure of the aerosol. Further work is needed to understand the chemistry involved, as these processes may have significant implications for prebiotic chemistry on the early Earth and similar planets.

Trainer, Melissa G.↗

The Formation of Sulfate and Elemental Sulfur Aerosols Under Varying Laboratory Conditions: Implications for Early Earth

The presence of sulfur mass-independent fractionation (S-MIF) in sediments more than 2.45 x 10(exp 9) years old is thought to be evidence for an early anoxic atmosphere. Photolysis of sulfur dioxide (SO2) by UV light with lambda < 220 nm has been shown in models and some initial laboratory studies to create a S-MIF; however, sulfur must leave the atmosphere in at least two chemically different forms to preserve any S-MIF signature. Two commonly cited examples of chemically different sulfur species that could have exited the atmosphere are elemental sulfur (S8) and sulfuric acid (H2S04) aerosols. Here, we use real-time aerosol mass spectrometry to directly detect the sulfur-containing aerosols formed when SO2 either photolyzes at wavelengths from 115 to 400 nm, to simulate the UV solar spectrum, or interacts with high-energy electrons, to simulate lightning. We found that sulfur-containing aerosols form under all laboratory conditions. Further, the addition of a reducing gas, in our experiments hydrogen (H2) or methane (CH4), increased the formation of S8. With UV photolysis, formation of S8 aerosols is highly dependent on the initial SO2 pressure; and S8 is only formed at a 2% SO2 mixing ratio and greater in the absence of a reductant, and at a 0.2% SO2 mixing ratio and greater in the presence of 1000 ppmv CH4. We also found that organosulfur compounds are formed from the photolysis of CH4 and moderate amounts of SO2, The implications for sulfur aerosols on early Earth are discussed.

DeWitt, H. Langley↗

Role of Deep Convection in Establishing the Isotopic Composition of Water Vapor in the Tropical Transition Layer

The transport of H2O and HDO within deep convection is investigated with 3-D large eddy simulations (LES) using bin microphysics. The lofting and sublimation of HDO-rich ice invalidate the Rayleigh fractionation model of isotopologue distribution within deep convection. Bootstrapping the correlation of the ratio of HDO to H2O (deltaD) to water vapor mixing ratio (q(sub v)) through a sequence of convective events produced non-Rayleigh correlations resembling observations. These results support two mechanisms for stratospheric entry. Deep convection can inject air with water vapor of stratospheric character directly into the tropical transition layer (TTL). Alternatively, moister air detraining from convection may be dehydrated via cirrus formation n the TTL to produce stratospheric water vapor. Significant production of subsaturated air in the TTL via convective dehydration is not observed in these simulations, nor is it necessary to resolve the stratospheric isotope paradox.

Smith, Jamison A.↗