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NASA NTRS1995

Pole-to-Pole Distribution of Stratospheric Black Carbon (Soot) Aerosol from Aircraft

The distribution of black carbon (soot) aerosol (BCA) in the atmosphere is of interest for several reasons: (1) Because BCA has the highest absorption cross section of any compound known, it can absorb solar radiation to cause atmospheric warming. (2) Because it is a strong adsorber of gases, it can catalyze heterogeneous reactions to change the chemical composition of the atmosphere.(3) If aircraft are a major source of BCA, it is an important tracer of aircraft emissions. Analysis for BCA of impactor samples from Arctic and Antarctic deployments, utilizing particle morphology of scanning electron microscopy images, permits the following conclusions: (1) The BCA concentration in the northern stratosphere varies between 0 and 2.6 ng m-3 averaging 0.6 ng/cu m. (2) This BCA loading is commensurate with estimated fuel consumptions in the stratosphere by the current commercial fleet and an emission index E=0.03 g BCA per kg fuel burnt which was measured in jet exhaust at al titude.Thus, most stratospheric BCA in the northern stratosphere results from aircraft emissions. The background BCA concentration in the southern stratosphere varies between 0 and 0.6 ng cu m averaging 0.1 ng/cu m. This strong meridional gradient implies that stratospheric BCA residence time- is shorter than are mixing times between hemispheres. Projected annual fuel consumption of a future supersonic commercial fleet is 7E13 g. This fleet would increase stratospheric BCA loadings by a factor of 2-3, because almost all fuel would be burnt above the tropopause. An improved EI(BCA) by a factor of ten would result in an increase of stratospheric BCA loadings by approximately 50 %.

Pueschel, R. F.↗

NASA NTRS2009

The Seasonal Response of Titan's Troposphere and Stratosphere

The radiative response of Titan's atmosphere varies by several orders of magnitude with altitude. This presents an interesting situation in which most of the stratosphere----at least that part above 100km is characterized by radiative relaxation times that are short compared to the length of a Titan season, and the troposphere and tropopause region by times that are larger than seasonal timescales. Consistent with this, Cassini CIRS spectra indicate stratospheric temperatures at 100-170 kin that are 20-30 K cooler at high northern latitudes in winter than those at equatorial and southern latitudes. Given the expectation that the situation will largely reverse in southern winter, the observed large meridional contrast is likely indicative of the expected seasonal variation at polar latitudes in both hemispheres. CIRS spectra do not as easily yield temperatures below 100 km in the lower stratosphere and tropopause region, because of the contribution of heterogeneously distributed aerosols and condensates to the infrared opacity. However, Cassini radio occultations probe both the stratosphere and troposphere, and below 80 km they show the thermal contrast with latitude to be muted, e.g,, approx.5 K near the tropopause at 40-50 km and approx.3 K just above the surface. This is consistent with the large radiative relaxation times at these altitudes and with efficient meridional heat transport. What is curious is the manner in which temperatures in the north winter polar atmosphere make the transition between the troposphere and lower stratosphere, where seasonal variations are relatively small, and higher altitudes, where they are large. Temperatures at all latitudes sounded by the radio occultations exhibit similar behavior in the lower stratosphere, increasing with altitude. Between 80 and 100 kin, however, the temperatures at high northern latitudes exhibit a sudden drop with increasing altitude, producing the meridional contrast in the upper stratosphere described above. While the radiative relaxation time associated with infrared gaseous coolants decreases with altitude in the stratosphere, it is not likely to account for the abrupt transition observed. Possible mechanisms for this transition are discussed, including the presence of an optically thick. cloud at thermal-infrared wavelengths.

Flasar, F. M.↗

NASA NTRS2011

Response of the Antarctic Stratosphere to Warm Pool EI Nino Events in the GEOS CCM

A new type of EI Nino event has been identified in the last decade. During "warm pool" EI Nino (WPEN) events, sea surface temperatures (SSTs) in the central equatorial Pacific are warmer than average. The EI Nino signal propagates poleward and upward as large-scale atmospheric waves, causing unusual weather patterns and warming the polar stratosphere. In austral summer, observations show that the Antarctic lower stratosphere is several degrees (K) warmer during WPEN events than during the neutral phase of EI Nino/Southern Oscillation (ENSO). Furthermore, the stratospheric response to WPEN events depends of the direction of tropical stratospheric winds: the Antarctic warming is largest when WPEN events are coincident with westward winds in the tropical lower and middle stratosphere i.e., the westward phase of the quasi-biennial oscillation (QBO). Westward winds are associated with enhanced convection in the subtropics, and with increased poleward wave activity. In this paper, a new formulation of the Goddard Earth Observing System Chemistry-Climate Model, Version 2 (GEOS V2 CCM) is used to substantiate the observed stratospheric response to WPEN events. One simulation is driven by SSTs typical of a WPEN event, while another simulation is driven by ENSO neutral SSTs; both represent a present-day climate. Differences between the two simulations can be directly attributed to the anomalous WPEN SSTs. During WPEN events, relative to ENSO neutral, the model simulates the observed increase in poleward planetary wave activity in the South Pacific during austral spring, as well as the relative warming of the Antarctic lower stratosphere in austral summer. However, the modeled response to WPEN does not depend on the phase of the QBO. The modeled tropical wind oscillation does not extend far enough into the lower stratosphere and upper troposphere, likely explaining the model's insensitivity to the phase of the QBO during WPEN events.

Hurwitz, Margaret M.↗

NASA NTRS2011

Seasonal Variations of Stratospheric Age Spectra in GEOSCCM

There are many pathways for an air parcel to travel from the troposphere to the stratosphere, each of which takes different time. The distribution of all the possible transient times, i.e. the stratospheric age spectrum, contains important information on transport characteristics. However, it is computationally very expensive to compute seasonally varying age spectra, and previous studies have focused mainly on the annual mean properties of the age spectra. To date our knowledge of the seasonality of the stratospheric age spectra is very limited. In this study we investigate the seasonal variations of the stratospheric age spectra in the Goddard Earth Observing System Chemistry Climate Model (GEOSCCM). We introduce a method to significantly reduce the computational cost for calculating seasonally dependent age spectra. Our simulations show that stratospheric age spectra in GEOSCCM have strong seasonal cycles and the seasonal cycles change with latitude and height. In the lower stratosphere extratropics, the average transit times and the most probable transit times in the winter/early spring spectra are more than twice as old as those in the summer/early fall spectra. But the seasonal cycle in the subtropical lower stratosphere is nearly out of phase with that in the extratropics. In the middle and upper stratosphere, significant seasonal variations occur in the sUbtropics. The spectral shapes also show dramatic seasonal change, especially at high latitudes. These seasonal variations reflect the seasonal evolution of the slow Brewer-Dobson circulation (with timescale of years) and the fast isentropic mixing (with timescale of days to months).

Li, Feng↗

NASA NTRS2019

CALIPSO Level 3 Stratospheric Aerosol Product: Version 1.00 Algorithm Description and Initial Assessment

In August 2018,the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) project released a new level 3 stratospheric aerosol profile data product derived from nearly 12 years of measurements acquired by the space-borne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP).This monthly averaged, gridded level 3 product is based on version 4.2 of the CALIOP level 1 and level 2 data products, which feature significantly improved calibration that now makes it possible to reliably retrieve profiles of stratospheric aerosol extinction and backscatter coefficients. This paper describes the science algorithm and data handling techniques that were developed to generate the CALIPSO version 1.00 level 3 stratospheric aerosol profile product. Further, we show that the retrieved extinction profiles capture the major stratospheric perturbations over the last decade resulting from volcanic eruptions, extreme smoke events, and signatures of stratospheric dynamics. Initial assessment of the product by inter-comparison with the stratospheric aerosol retrievals from the Stratospheric Aerosol and Gas Experiment III (SAGE III) on the International Space Station (ISS) indicates good agreement in the tropical stratospheric aerosol layer (30oN-30oS),where the average difference between zonal mean extinction profiles is typically less than 25% between 20km and 30km. However, differences can exceed 100% in the very low aerosol loading regimes found above 25 km at higher latitudes.

Jayanta Kar↗

NASA NTRSDate not supplied

GEOS Constituent Data Assimilation Beyond Aura MLS: Assimilating NASA SAGE III/ISS Profiles of Stratospheric Water Vapor and Ozone

Ozone and water vapor in the lower stratosphere are important trace gases for atmospheric chemistry and radiative budget. The Stratospheric Aerosol and Gas Experiment (SAGE) missions have been crucial in monitoring the stratospheric ozone loss and the subsequent recovery as well as the trends in water vapor linked to surface temperature trends. The SAGE III instrument aboard the International Space Station (ISS) continues the SAGE mission record, with high vertical resolution profiles of ozone and water vapor available since mid 2017. The NASA GEOS Earth system model has the new capability to assimilate multi-constituents from ground and space-based instruments using the GEOS Constituent Data Assimilation System (CoDAS). The recently released MERRA-2 Stratospheric Composition Reanalysis with Aura MLS (M2-SCREAM) assimilates version 4.2 MLS ozone, water vapor and other chemically-reactive species with the NASA GEOS model coupled to a stratospheric-only chemistry mechanism and transport constrained to the MERRA-2 reanalysis. While the number of solar occultation observations a day from SAGE III/ISS is about 1% of the total number of profiles observed globally by MLS, the chemical timescales of ozone and water vapor in the lower stratosphere are long enough that the SAGE III/ISS data may provide a useful constraint on the assimilated product. Using the same GEOS CoDAS configuration as M2-SCREAM, we will present a series of experiments to investigate if ozone and water vapor trends are consistent with the assimilation of SAGE observations with and without Aura retrievals, and to determine if the assimilation of SAGE observations produces a steady product for trend analysis, especially as the end of the Aura mission nears. In our experiments, assimilating only SAGE III/ISS water vapor profiles results in water vapor fields more consistent with experiments that assimilate MLS v5; however, in the polar regions SAGE III/ISS observations are not available and the values are unconstrained. We are encouraged by the positive benefit assimilating the less frequent SAGE III/ISS observations has on stratospheric composition. Sensitivity experiments such as these will allow us to assess the added value of SAGE data for continued monitoring of the stratospheric composition for climate and ozone recovery assessments.

SAGE↗

NASA NTRSDate not supplied

GEOS Constituent Data Assimilation Beyond Aura MLS: Assimilating NASA SAGE III/ISS Profiles of Stratospheric Water Vapor

Ozone and water vapor in the lower stratosphere are important trace gases for atmospheric chemistry and radiative budget. The Stratospheric Aerosol and Gas Experiment (SAGE) missions have been crucial in monitoring the stratospheric ozone loss and the subsequent recovery as well as the trends in water vapor linked to surface temperature trends. The SAGE III instrument aboard the International Space Station (ISS) continues the SAGE mission record, with high vertical resolution profiles of ozone and water vapor available since mid 2017. The NASA GEOS Earth system model has the new capability to assimilate multi-constituents from ground and space-based instruments using the GEOS Constituent Data Assimilation System (CoDAS). The recently released MERRA-2 Stratospheric Composition Reanalysis with Aura MLS (M2-SCREAM) assimilates version 4.2 MLS ozone, water vapor and other chemically-reactive species with the NASA GEOS model coupled to a stratospheric-only chemistry mechanism and transport constrained to the MERRA-2 reanalysis. While the number of solar occultation observations a day from SAGE III/ISS is about 1% of the total number of profiles observed globally by MLS, the chemical timescales of ozone and water vapor in the lower stratosphere are long enough that the SAGE III/ISS data may provide a useful constraint on the assimilated product. Using the same GEOS CoDAS configuration as M2-SCREAM, we will present a series of experiments to investigate if water vapor trends are consistent with the assimilation of SAGE observations with and without Aura retrievals, and to determine if the assimilation of SAGE observations produces a steady product for trend analysis, especially as the end of the Aura mission nears. In our experiments, assimilating only SAGE III/ISS water vapor profiles results in water vapor fields more consistent with experiments that assimilate MLS v5; however, in the polar regions SAGE III/ISS observations are not available and the modelled values are unconstrained. We are encouraged by the positive benefit assimilating the less frequent SAGE III/ISS observations has on stratospheric composition. Sensitivity experiments such as these will allow us to assess the added value of SAGE data for continued monitoring of the stratospheric composition for climate and ozone recovery assessments.

K Emma Knowland↗

NASA NTRSDate not supplied

Hunga Tonga-Hunga Ha’apai Water Vapour and Composition of the Stratospheric Polar Vortices

We investigate the impacts of water vapor from the Hunga Tonga-Hunga Ha'apai (HTHH) eruption on the Antarctic stratospheric vortices in 2022 and 2023 and the Arctic stratospheric vortex in 2022/2023. Trace gas abundances from the Aura Microwave Limb Sounder (MLS) and the Modern Era Retrospective-analysis for Research and Applications (MERRA-2) Stratospheric Composition REanalysis with Aura MLS (M2-SCREAM), along with meteorological fields from the longer MERRA-2 record, are used to detail the evolution of the stratospheric polar vortex and its composition during these winter/spring seasons. Through austral winter and spring 2022, HTHH water vapor was effectively excluded from the Antarctic vortex until it broke up. The 2022 Antarctic vortex itself was large, strong, and long-lived, but not exceptionally so. By austral fall 2023, HTHH stratospheric water vapor had spread globally, and Antarctic vortex values in the lower through middle stratosphere were over 2 ppmv higher than usual when the vortex formed; these record-shattering water vapor concentrations led to earlier polar stratospheric cloud formation and chlorine activation, especially at levels that are typically the highest altitudes for polar processing. In the 2022/2023 Arctic winter/spring, HTHH water vapor reached the Arctic vortex region after the vortex had formed and was largely excluded until a major sudden stratospheric warming in mid-February 2023 eroded the vortex and mixed midlatitude and vortex air throughout the hemisphere.

Gloria L Manney↗

NASA NTRSDate not supplied

Hunga Tonga-Hunga Ha’apai Water Vapour and Composition of the Stratospheric Polar Vortices

Gloria L Manney↗

NASA NTRS2021

The 2019 Southern Hemisphere Stratospheric Polar Vortex Weakening and Its Impacts

This study offers an overview of the low-frequency (i.e., monthly to seasonal) evolution, dynamics, predictability, and surface impacts of a rare Southern Hemisphere (SH) stratospheric warming that occurred in austral spring 2019. Between late August to mid- September 2019, the stratospheric circumpolar westerly jet weakened rapidly, and Antarctic stratospheric temperatures rose dramatically. The deceleration of the vortex at 10 hPa was as drastic as that of the first ever observed major sudden stratospheric warming in the SH during 2002, while the mean Antarctic warming over the course of spring 2019 broke the previous record of 2002 by ~50% in the mid-stratosphere. This event was preceded by a poleward shift of the SH polar night jet in the uppermost stratosphere in early winter, which was then followed by record-strong planetary wave-one activity propagating upward from the troposphere in August that acted to dramatically weaken the polar vortex throughout the depth of the stratosphere. The weakened vortex winds and elevated temperatures moved downward to the surface from mid-October to December, promoting a record strong swing of the Southern Annular Mode (SAM) to its negative phase. This record-negative SAM appeared to be a primary driver of the extreme hot and dry conditions over subtropical eastern Australia that accompanied the severe wildfires that occurred in late spring 2019. State-of-the-art dynamical seasonal forecast systems skillfully predicted the significant vortex weakening of spring 2019 and subsequent development of negative SAM from as early as late July.

Antarctic Oscillation↗

NASA NTRS2013

Net Influence of an Internally Generated Guasi-biennial Oscillation on Modelled Stratospheric Climate and Chemistry

A Goddard Earth Observing System Chemistry- Climate Model (GEOSCCM) simulation with strong tropical non-orographic gravity wave drag (GWD) is compared to an otherwise identical simulation with near-zero tropical non-orographic GWD. The GEOSCCM generates a quasibiennial oscillation (QBO) zonal wind signal in response to a tropical peak in GWD that resembles the zonal and climatological mean precipitation field. The modelled QBO has a frequency and amplitude that closely resembles observations. As expected, the modelled QBO improves the simulation of tropical zonal winds and enhances tropical and subtropical stratospheric variability. Also, inclusion of the QBO slows the meridional overturning circulation, resulting in a generally older stratospheric mean age of air. Slowing of the overturning circulation, changes in stratospheric temperature and enhanced subtropical mixing all affect the annual mean distributions of ozone, methane and nitrous oxide. Furthermore, the modelled QBO enhances polar stratospheric variability in winter. Because tropical zonal winds are easterly in the simulation without a QBO, there is a relative increase in tropical zonal winds in the simulation with a QBO. Extratropical differences between the simulations with and without a QBO thus reflect the westerly shift in tropical zonal winds: a relative strengthening of the polar stratospheric jet, polar stratospheric cooling and a weak reduction in Arctic lower stratospheric ozone.

stratosphere↗

NASA NTRS2015

Disentangling the Roles of Various Forcing Mechanisms on Stratospheric Temperature Changes Since 1979 with the NASA GEOSCCM

Observations show that the cooling of global stratospheric temperatures from 1979 to 2015 took place in two major steps coincident with the 1982 El Chichon and 1991 Mount Pinatubo eruptions. In order to attribute the features of the global stratospheric temperature time series to the main forcing agents, we performed a set of simulations with the NASA Goddard Earth Observing System Chemistry Climate Model. Our results show that the characteristic step-like behavior is to be attributed to the effects of the solar cycle, except for the post-1995 flattening of the lower stratospheric temperatures, where the decrease in ozone depleting substances due to the Montreal Protocol slowed ozone depletion and therefore also the cooling of the stratosphere. Volcanic eruptions also caused a significant warming of the stratosphere after 1995. The observed general cooling is mainly caused by increasing ozone depleting substances in the lower stratosphere, and greenhouse gases in the middle and upper stratosphere.

ozone↗

NASA NTRS2014

Understanding Differences in Chemistry Climate Model Projections of Stratospheric Ozone

Chemistry climate models (CCMs) are used to project future evolution of stratospheric ozone as concentrations of ozone-depleting substances (ODSs) decrease and greenhouse gases increase, cooling the stratosphere. CCM projections exhibit not only many common features but also a broad range of values for quantities such as year of ozone return to 1980 and global ozone level at the end of the 21st century. Multiple linear regression is applied to each of 14 CCMs to separate ozone response to ODS concentration change from that due to climate change. We show that the sensitivity of lower stratospheric ozone to chlorine change Delta Ozone/Delta inorganic chlorine is a near-linear function of partitioning of total inorganic chlorine into its reservoirs; both inorganic chlorine and its partitioning are largely controlled by lower stratospheric transport. CCMs with best performance on transport diagnostics agree with observations for chlorine reservoirs and produce similar ozone responses to chlorine change. After 2035, differences in Delta Ozone/Delta inorganic chlorine contribute little to the spread in CCM projections as the anthropogenic contribution to inorganic chlorine becomes unimportant. Differences among upper stratospheric ozone increases due to temperature decreases are explained by differences in ozone sensitivity to temperature change Delta Ozone/Delta T due to different contributions from various ozone loss processes, each with its own temperature dependence. Ozone decrease in the tropical lower stratosphere caused by a projected speedup in the Brewer-Dobson circulation may or may not be balanced by ozone increases in the middle- and high-latitude lower stratosphere and upper troposphere. This balance, or lack thereof, contributes most to the spread in late 21st century projections.

Stratospheric Transport↗

NASA NTRS2023

Convective Impact on the Global Lower Stratospheric Water Vapor Budget

Water vapor in the stratosphere is primarily controlled by temperatures in the tropical upper troposphere and lower stratosphere. However, the direct impact of deep convection on the global lower stratospheric water vapor budget is still an actively debated issue. Two complementary modeling approaches are used to investigate the convective impact in boreal winter and summer. Convective influence is diagnosed by tracing trajectories through convective cloud top altitude fields derived from global rainfall and brightness temperature data. Backward trajectory model simulations coupled with a detailed treatment of cloud microphysical processes indicate that convection moistens the global lower stratosphere by approximately 0.3 ppmv in boreal winter and summer 2010. The diurnal peak in convection is responsible for about half of the total convective moistening during winter and nearly all of the convective moistening during summer. Deep convective clouds overshooting the tropopause have relatively minor effect on global lower stratospheric water vapor. A forward trajectory model coupled with a simplified cloud module is used to estimate the relative magnitude of the interannual variability of the convective impact. Combining the results from the two models, we find that the convective impact on the global lower stratospheric water vapor during 2006-2016 is approximately 0.3 ppmv with year-to-year variations of up to 0.1 ppmv. An important mechanism of convective hydration of the lower stratosphere is via the detrainment of saturated air and ice into the tropical uppermost troposphere and the subsequent upward transport of some of these moist air parcels across relatively warm and subsaturated tropopause.

CONVECTION↗

NASA NTRS2023

Stratospheric Water Vapor Affecting Atmospheric Circulation

Water vapor plays an important role in many aspects of the climate system, by affecting radiation, cloud formation, atmospheric chemistry and dynamics. Even the low stratospheric water vapor content provides an important climate feedback, but current climate models show a substantial moist bias in the lowermost stratosphere. Here we report crucial sensitivity of the atmospheric circulation in the stratosphere and troposphere to the abundance of water vapor in the lowermost stratosphere. We show from a mechanistic climate model experiment and inter-model variability that lowermost stratospheric water vapor decreases local temperatures, and thereby causes an upward and poleward shift of subtropical jets, a strengthening of the stratospheric circulation, a poleward shift of the tropospheric eddy-driven jet and regional climate impacts. The mechanistic model experiment in combination with atmospheric observations further shows that the prevailing moist bias in current models is likely caused by the transport scheme, and can be alleviated by employing a less diffusive Lagrangian scheme. The related effects on atmospheric circulation are of similar magnitude as climate change effects. Hence, lowermost stratospheric water vapor exerts a first order effect on atmospheric circulation and improving its representation in models offers promising prospects for future research.

stratosphere↗

DOE OSTI2021

Is turning down the sun a good proxy for stratospheric sulfate geoengineering?

Deliberately blocking out a small portion of the incoming solar radiation would cool the climate. One such approach would be injecting SO2 into the stratosphere, which would produce sulfate aerosols that would remain in the atmosphere for 1–3 years, reflecting part of the incoming shortwave radiation. The cooling produced by the aerosols can offset the warming produced by increased greenhouse gas (GHG) concentrations, but it would also affect the climate differently, leading to residual differences compared to a climate not affected by either. Many climate model simulations of geoengineering have used a uniform reduction of the incoming solar radiation as a proxy for stratospheric aerosols, both because many models are not designed to adequately capture relevant stratospheric aerosol processes, and because a solar reduction has often been assumed to capture the most important differences between how stratospheric aerosols and GHG would affect the climate. Here we show that dimming the sun does not produce the same surface climate effects as simulating aerosols in the stratosphere. By more closely matching the spatial pattern of solar reduction to that of the aerosols, some improvements in this idealized representation are possible, with further improvements if the stratospheric heating produced by the aerosols is included. This is relevant both for our understanding of the physical mechanisms driving the changes observed in stratospheric-sulfate geoengineering simulations, and in terms of the relevance of impact assessments that use a uniform solar dimming.

Visioni, Daniele↗

DOE OSTI2022

Contrasting Stratospheric Smoke Mass and Lifetime From 2017 Canadian and 2019/2020 Australian Megafires: Global Simulations and Satellite Observations

Stratospheric injections of carbonaceous aerosols and combustion gases by extreme wildfires have become increasingly common. Recent “megafires,” particularly large and intense fires, delivered particulate burdens to the lower stratosphere comparable to those of moderate volcanic eruptions. The 2017 Canadian megafire generated four large Pyrocumulonimbi (pyroCbs), injecting up to ≈0.3 Tg of smoke in the lower stratosphere. Even more extreme, the 2019/2020 Australian event produced a pyroCb activity resulting in stratospheric smoke intrusions of ≈1 Tg. To understand their contrasting behavior, we present global climate simulations of the atmospheric response to these events, applying smoke burdens informed by remote observations. Model outcomes, compared to satellite data of smoke transport, reproduce reasonably well the initial plume rise, at 0.2–0.3 km/day, attaining heights of ≈20 km in Canada and above 30 km in Australia. Global dispersal of the plume occurs within about 3 weeks in both cases, consistent with observations. Smoke removal timescales, ≈5 months for the Canadian megafire, agree with remote measurements. During the Australian megafire, observations indicate stratospheric injections three times as large, and models predict comparatively longer smoke lifetimes, ≈16 months. After the latter event, atmospheric optical depths and radiative cooling achieved values close to those measured following the Pinatubo eruption. Sensitivity tests of model assumptions indicate, in accord with prior studies, that smoke burden, injection heights, and black carbon content can determine plume evolution and possible climate impacts. An empirical relation between peak heights of stratospheric plumes and lifetimes is derived that can help assess megafire impacts on the stratosphere, climate and the Earth system

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Chemical imaging of individual stratospheric particles sampled over North America

The increasing size, severity, and frequency of wildfires have led to dramatic increases in particulate matter concentrations in the troposphere. Severe wildfires can generate intense convective systems capable of transporting large quantities of biomass burning organic aerosols (BBOA) to the upper troposphere and lower stratosphere (UTLS). Chemically complex organic matter and light-absorbing carbonaceous material is introduced into stratospheric regions that were historically isolated from direct surface emissions. In this study, stratospheric particles were sampled over North America during the Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) campaign, an aircraft-based research project designed to characterize convective perturbation in the UTLS. Particle samples collected from six research flights during summer 2022 were analyzed using Computer-Controlled Scanning Electron Microscopy and Scanning Transmission X-ray Microscopy to investigate particle size distributions, morphology, chemical composition, and mixing state of stratospheric particles along transects across the continental United States and adjacent Pacific Ocean airspace. Analysis revealed that all sampled particles contained detectable levels of carbon, with most exhibiting organic volume fractions of 0.37 ± 0.20. Notably, about 5% of the particles also contained soot inclusions, which indicates the presence of refractory black carbon transported to stratospheric altitudes and provides direct evidence of wildfire-derived black carbon reaching the UTLS. Typical particle morphology exhibits organic shells over soot and inorganic cores and suggests secondary processing and aging of BBOA during transport to and within the UTLS. These findings provide compelling evidence that wildfire emissions play a critical role in affecting the long-term composition and radiative properties of stratospheric particles.

Sharpe, Steven [Purdue Univ., West Lafayette, IN (↗