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At least 865 records · Page 48

The Modulation of Gulf Stream Influence on the Troposphere by the Eddy-Driven Jet

This study suggests that the Gulf Stream influence on the wintertime North Atlantic troposphere is most pronounced when the eddy-driven jet (EDJ) is farthest south and better collocated with the Gulf Stream. Using the reanalysis dataset NCEP-CFSR for December–February 1979–2009, the daily EDJ latitude is separated into three regimes (northern, central, and southern). It is found that the average trajectory of atmospheric fronts covaries with EDJ latitude. In the southern EDJ regime (~19% of the time), the frequency of near-surface atmospheric fronts that pass across the Gulf Stream is maximized. Analysis suggests that this leads to significant strengthening in near-surface atmospheric frontal convergence resulting from strong air–sea sensible heat flux gradients (due to strong temperature gradients in the atmosphere and ocean). In recent studies, it was shown that the pronounced band of time-mean near-surface wind convergence across the Gulf Stream is set by atmospheric fronts. Here, it is shown that an even smaller subset of atmospheric fronts—those associated with a southern EDJ—primarily sets the time mean, due to enhanced Gulf Stream air–sea interaction. Furthermore, statistically significant anomalies in vertical velocity extending well above the boundary layer are identified in association with changes in EDJ latitude. These anomalies are particularly strong for a southern EDJ and are spatially consistent with increases in near-surface atmospheric frontal convergence over the Gulf Stream. These results imply that much of the Gulf Stream influence on the time-mean atmosphere is modulated on synoptic time scales, and enhanced when the EDJ is farthest south.

54 ENVIRONMENTAL SCIENCES↗

Robust Anthropogenic Signal Identified in the Seasonal Cycle of Tropospheric Temperature

Previous work identified an anthropogenic fingerprint pattern in T AC (x, t), the amplitude of the seasonal cycle of mid- to upper-tropospheric temperature (TMT), but did not explicitly consider whether fingerprint identification in satellite T AC (x, t) data could have been influenced by real-world multidecadal internal variability (MIV). Here we address this question here using large ensembles (LEs) performed with five climate models. LEs provide many different sequences of internal variability noise superimposed on an underlying forced signal. Despite differences in historical external forcings, climate sensitivity, and MIV properties of the five models, their T AC (x, t) fingerprints are similar and statistically identifiable in 239 of the 240 LE realizations of historical climate change. Comparing simulated and observed variability spectra reveals that consistent fingerprint identification is unlikely to be biased by model underestimates of observed MIV. Even in the presence of large (factor of 3–4) intermodel and inter-realization differences in the amplitude of MIV, the anthropogenic fingerprints of seasonal cycle changes are robustly identifiable in models and satellite data. This is primarily due to the fact that the distinctive, global-scale fingerprint patterns are spatially dissimilar to the smaller-scale patterns of internal T AC (x, t) variability associated with the Atlantic multidecadal oscillation and El Niño–Southern Oscillation. The robustness of the seasonal cycle detection and attribution results shown here, taken together with the evidence from idealized aquaplanet simulations, suggest that basic physical processes are dictating a common pattern of forced T AC (x, t) changes in observations and in the five LEs. The key processes involved include GHG-induced expansion of the tropics, lapse-rate changes, land surface drying, and sea ice decrease.

54 ENVIRONMENTAL SCIENCES↗

Airborne Bacteria in Earth's Lower Stratosphere Resemble Taxa Detected in the Troposphere: Results From a New NASA Aircraft Bioaerosol Collector (ABC)

Airborne microorganisms in the upper troposphere and lower stratosphere remain elusive due to a lack of reliable sample collection systems. To address this problem, we designed, installed, and flight-validated a novel Aircraft Bioaerosol Collector (ABC) for NASA's C-20A that can make collections for microbiological research investigations up to altitudes of 13.7 km. Herein we report results from the first set of science flights—four consecutive missions flown over the United States (US) from 30 October to 2 November, 2017. To ascertain how the concentration of airborne bacteria changed across the tropopause, we collected air during aircraft Ascent/Descent (0.3 to 11 km), as well as sustained Cruise altitudes in the lower stratosphere (~12 km). Bioaerosols were captured on DNA-treated gelatinous filters inside a cascade air sampler, then analyzed with molecular and culture-based characterization. Several viable bacterial isolates were recovered from flight altitudes, including Bacillus sp., Micrococcus sp., Arthrobacter sp., and Staphylococcus sp. from Cruise samples and Brachybacterium sp. from Ascent/Descent samples. Using 16S V4 sequencing methods for a culture-independent analysis of bacteria, the average number of total OTUs was 305 for Cruise samples and 276 for Ascent/Descent samples. Some taxa were more abundant in the flight samples than the ground samples, including OTUs from families Lachnospiraceae , Ruminococcaceae and Erysipelotrichaceae as well as the following genera: Clostridium, Mogibacterium, Corynebacterium, Bacteroides, Prevotella, Pseudomonas, and Parabacteroides . Surprisingly, our results revealed a homogeneous distribution of bacteria in the atmosphere up to 12 km. The observation could be due to atmospheric conditions producing similar background aerosols across the western US, as suggested by modeled back trajectories and satellite measurements. However, the influence of aircraft-associated bacterial contaminants could not be fully eliminated and that background signal was reported throughout our dataset. Furthermore considering the tremendous engineering challenge of collecting biomass at extreme altitudes where contamination from flight hardware remains an ever-present issue, we note the utility of using the stratosphere as a proving ground for planned life detection missions across the solar system.

59 BASIC BIOLOGICAL SCIENCES↗

A Wideband Self-consistent Disk-averaged Spectrum of Jupiter Near 30 GHz and Its Implications for NH{sub 3} Saturation in the Upper Troposphere

We present a new set of measurements obtained with the Combined Array for Research in Millimeter-wave Astronomy (CARMA) of Jupiter’s microwave thermal emission near the 1.3 cm ammonia (NH{sub 3}) absorption band. We use these observations to investigate the ammonia mole fraction in the upper troposphere, near 0.3 < P < 2 bar, based on radiative transfer modeling. We find that the ammonia mole fraction must be ∼2.4 × 10{sup −4} below the NH{sub 3} ice cloud, i.e., at 0.8 < P < 8 bar, in agreement with results by de Pater et al. We find the NH{sub 3} cloud-forming region between 0.3 < P < 0.8 bar to be globally sub-saturated by ∼55% on average, in accordance with the result in Gibson et al. Although our data are not very sensitive to the region above the cloud layer, we are able to set an upper limit of 2.4×10{sup −7} on the mole fraction here, a factor of ∼10 above the saturated vapor curve.

79 ASTRONOMY AND ASTROPHYSICS↗

Measurements of Tropospheric Ice Clouds with a Ground-based CMB Polarization Experiment, POLARBEAR

The polarization of the atmosphere has been a constant concern for ground-based experiments targeting cosmic microwave background (CMB) polarization. Ice crystals in upper tropospheric clouds scatter thermal radiation from the ground and produce a horizontally polarized signal. We report a detailed analysis of the cloud signal using a ground-based CMB experiment, Polarbear, located at the Atacama desert in Chile and observing at 150 GHz. We determine horizontally polarized temporal increases of low-frequency fluctuations ("polarized bursts," hereafter) of ≲0.1 K when clouds appear in a webcam monitoring the telescope and the sky. The hypothesis of no correlation between polarized bursts and clouds is rejected with >24σ statistical significance using three years of data. We report many other possibilities including instrumental and environmental effects, and find no reasons other than clouds that can explain the data better. We additionally discuss the impact of the cloud polarization on future ground-based CMB polarization experiments.

polarization↗

Viscous organic aerosol particles in the upper troposphere: diffusivity-controlled water uptake and ice nucleation?

Here, new measurements of water diffusion in secondary organic aerosol (SOA) material produced by oxidation of α-pinene and in a number of organic/inorganic model mixtures (3-methylbutane-1,2,3-tricarboxylic acid (3-MBTCA), levoglucosan, levoglucosan/NH 4 HSO 4 , raffinose) are presented. These indicate that water diffusion coefficients are determined by several properties of the aerosol substance and cannot be inferred from the glass transition temperature or bouncing properties. Our results suggest that water diffusion in SOA particles is faster than often assumed and imposes no significant kinetic limitation on water uptake and release at temperatures above 220 K. The fast diffusion of water suggests that heterogeneous ice nucleation on a glassy core is very unlikely in these systems. At temperatures below 220 K, model simulations of SOA particles suggest that heterogeneous ice nucleation may occur in the immersion mode on glassy cores which remain embedded in a liquid shell when experiencing fast updraft velocities. The particles absorb significant quantities of water during these updrafts which plasticize their outer layers such that these layers equilibrate readily with the gas phase humidity before the homogeneous ice nucleation threshold is reached. Glass formation is thus unlikely to restrict homogeneous ice nucleation. Only under most extreme conditions near the very high tropical tropopause may the homogeneous ice nucleation rate coefficient be reduced as a consequence of slow condensed-phase water diffusion. Since the differences between the behavior limited or non limited by diffusion are small even at the very high tropical tropopause, condensed-phase water diffusivity is unlikely to have significant consequences on the direct climatic effects of SOA particles under tropospheric conditions.

54 ENVIRONMENTAL SCIENCES↗

Organic photolysis reactions in tropospheric aerosols: effect on secondary organic aerosol formation and lifetime

This paper presents the first modeling estimates of the potential effect of gas- and particle-phase organic photolysis reactions on the formation and lifetime of secondary organic aerosols (SOAs). Typically only photolysis of smaller organic molecules (e.g., formaldehyde) for which explicit data exist is included in chemistry–climate models. Here, we specifically examine the photolysis of larger molecules that actively partition between the gas and particle phases. The chemical mechanism generator GECKO-A is used to explicitly model SOA formation from α-pinene, toluene, and C 12 and C 16 n-alkane reactions with OH at low and high NO x . Simulations are conducted for typical mid-latitude conditions and a solar zenith angle of 45° (permanent daylight). The results show that after 4 days of chemical aging under those conditions (equivalent to 8 days in the summer mid-latitudes), gas-phase photolysis leads to a moderate decrease in SOA yields, i.e., ~15 % (low NO x ) to ~45 % (high NO x ) for α-pinene, ~15 % for toluene, ~25 % for C 12 n-alkane, and ~10 % for C 16 n-alkane. The small effect of gas-phase photolysis on low-volatility n-alkanes such as C 16 n-alkane is due to the rapid partitioning of early-generation products to the particle phase, where they are protected from gas-phase photolysis. Minor changes are found in the volatility distribution of organic products and in oxygen to carbon ratios. The decrease in SOA mass is increasingly more important after a day of chemical processing, suggesting that most laboratory experiments are likely too short to quantify the effect of gas-phase photolysis on SOA yields. Our results also suggest that many molecules containing chromophores are preferentially partitioned into the particle phase before they can be photolyzed in the gas phase. Given the growing experimental evidence that these molecules can undergo in-particle photolysis, we performed sensitivity simulations using an empirically estimated SOA photolysis rate of J SOA = 4 × 10 &minus;4 J NO 2 . Modeling results indicate that this photolytic loss rate would decrease SOA mass by 40–60 % for most species after 10 days of equivalent atmospheric aging at mid-latitudes in the summer. It should be noted that in our simulations we do not consider in-particle or aqueous-phase reactions which could modify the chemical composition of the particle and thus the quantity of photolabile species. The atmospheric implications of our results are significant for both the SOA global distribution and lifetime. GEOS-Chem global model results suggest that particle-phase photolytic reactions could be an important loss process for SOA in the atmosphere, removing aerosols from the troposphere on timescales of less than 7 days that are comparable to wet deposition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Free tropospheric aerosols at the Mt. Bachelor Observatory: more oxidized and higher sulfate content compared to boundary layer aerosols

Abstract. Understanding the properties and life cycle processes of aerosol particles in regional air masses is crucial for constraining the climate impacts of aerosols on a global scale. In this study, characteristics of aerosols in the boundary layer (BL) and free troposphere (FT) of a remote continental region in the western US were studied using a high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) deployed at the Mount Bachelor Observatory (MBO; 2763 m a.s.l.) in central Oregon in summer 2013. In the absence of wildfire influence, the average ( ± 1 σ ) concentration of non-refractory submicrometer particulate matter (NR- PM 1 ) at MBO was 2.8 ( ± 2.8) µ g m -3 and 84 % of the mass was organic. The other NR- PM 1 components were sulfate (11 %), ammonium (2.8 %), and nitrate (0.9 %). The organic aerosol (OA) at MBO from these clean periods showed clear diurnal variations driven by the boundary layer dynamics with significantly higher concentrations occurring during daytime, upslope conditions. NR- PM 1 contained a higher mass fraction of sulfate and was frequently acidic when MBO resided in the FT. In addition, OA in the FT was found to be highly oxidized (average O/C of 1.17) with low volatility while OA in BL-influenced air masses was moderately oxidized (average O/C of 0.67) and semivolatile. There are indications that the BL-influenced OA observed at MBO was more enriched in organonitrates and organosulfur compounds (e.g., MSA) and appeared to be representative of biogenic secondary organic aerosol (SOA) originated in the BL. A summary of the chemical compositions of NR- PM 1 measured at a number of other high-altitude locations in the world is presented and similar contrasts between FT and BL aerosols were observed. The significant compositional and physical differences observed between FT and BL aerosols may have important implications for understanding the climate effects of regional background aerosols.

54 ENVIRONMENTAL SCIENCES↗

Climate response to off-equatorial stratospheric sulfur injections in three Earth system models – Part 2: Stratospheric and free-tropospheric response

The paper constitutes Part 2 of a study performing a first systematic inter-model comparison of the atmospheric responses to stratospheric aerosol injection (SAI) at various single latitudes in the tropics, as simulated by three state-of-the-art Earth system models – CESM2-WACCM6, UKESM1.0, and GISS-E2.1-G. Building on Part 1 (Visioni et al., 2023) we demonstrate the role of biases in the climatological circulation and specific aspects of the model microphysics in driving the inter-model differences in the simulated sulfate distributions. We then characterize the simulated changes in stratospheric and free-tropospheric temperatures, ozone, water vapor, and large-scale circulation, elucidating the role of the above aspects in the surface SAI responses discussed in Part 1. We show that the differences in the aerosol spatial distribution can be explained by the significantly faster shallow branches of the Brewer–Dobson circulation in CESM2, a relatively isolated tropical pipe and older tropical age of air in UKESM, and smaller aerosol sizes and relatively stronger horizontal mixing (thus very young stratospheric age of air) in the two GISS versions used. We also find a large spread in the magnitudes of the tropical lower-stratospheric warming amongst the models, driven by microphysical, chemical, and dynamical differences. These lead to large differences in stratospheric water vapor responses, with significant increases in stratospheric water vapor under SAI in CESM2 and GISS that were largely not reproduced in UKESM. For ozone, good agreement was found in the tropical stratosphere amongst the models with more complex microphysics, with lower stratospheric ozone changes consistent with the SAI-induced modulation of the large-scale circulation and the resulting changes in transport. In contrast, we find a large inter-model spread in the Antarctic ozone responses that can largely be explained by the differences in the simulated latitudinal distributions of aerosols as well as the degree of implementation of heterogeneous halogen chemistry on sulfate in the models. The use of GISS runs with bulk microphysics demonstrates the importance of more detailed treatment of aerosol processes, with contrastingly different stratospheric SAI responses to the models using the two-moment aerosol treatment; however, some problems in halogen chemistry in GISS are also identified that require further attention. Overall, our results contribute to an increased understanding of the underlying physical mechanisms as well as identifying and narrowing the uncertainty in model projections of climate impacts from SAI.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic

Abstract. Atmospheric ice nucleation impacts the hydrological cycle and climate by modifying the radiative properties of clouds. To improve our predictive understanding of ice formation, ambient ice-nucleating particles (INPs) need to be collected and characterized. Measurements of INPs at lower latitudes in a remote marine region are scarce. The Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign, in the region of the Azores islands, provided the opportunity to collect particles in the marine boundary layer (MBL) and free troposphere (FT) by aircraft during the campaign's summer and winter intensive operation period. The particle population in samples collected was examined by scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy. The identified INPs were analyzed by scanning electron microscopy with energy-dispersive X-ray analysis. We observed differences in the particle population characteristics in terms of particle diversity, mixing state, and organic volume fraction between seasons, mostly due to dry intrusion events during winter, as well as between the sampling locations of the MBL and FT. These differences are also reflected in the temperature and humidity conditions under which water uptake, immersion freezing (IMF), and deposition ice nucleation (DIN) proceed. Identified INPs reflect typical particle types within the particle population on the samples and include sea salt, sea salt with sulfates, and mineral dust, all associated with organic matter, as well as carbonaceous particles. IMF and DIN kinetics are analyzed with respect to heterogeneous ice nucleation rate coefficients, Jhet, and ice nucleation active site density, ns, as a function of the water criterion Δaw. DIN is also analyzed in terms of contact angles following classical nucleation theory. Derived MBL IMF kinetics agree with previous ACE-ENA ground-site INP measurements. FT particle samples show greater ice nucleation propensity compared to MBL particle samples. This study emphasizes that the types of INPs can vary seasonally and with altitude depending on sampling location, thereby showing different ice nucleation propensities, which is crucial information when representing mixed-phase cloud and cirrus cloud microphysics in models.

54 ENVIRONMENTAL SCIENCES↗

Tropospheric aerosols over the western North Atlantic Ocean during the winter and summer deployments of ACTIVATE 2020: life cycle, transport, and distribution

The Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) is a NASA mission to characterize aerosol–cloud interactions over the western North Atlantic Ocean (WNAO). Such characterization requires understanding of life cycle, composition, transport pathways, and distribution of aerosols over the WNAO. This study uses the GEOS-Chem model to simulate aerosol distributions and properties that are evaluated against aircraft, ground-based, and satellite observations during the winter and summer field deployments in 2020 of ACTIVATE. Transport in the boundary layer (BL) behind cold fronts was a major mechanism for the North American continental outflow of pollution to the WNAO in winter. Turbulent mixing was the main driver for the upward transport of sea salt within and ventilation out of BL in winter. The BL aerosol composition was dominated by sea salt, which increased in the summer, followed by organics and sulfate. Aircraft in situ aerosol measurements provided useful constraints on wet scavenging in GEOS-Chem. The model generally captured observed features such as continental outflow, land–ocean gradient, and mixing of anthropogenic aerosols with sea salt. Model sensitivity experiments with elevated smoke injection heights to the mid-troposphere (versus within BL) better reproduced observations of smoke aerosols from the western US wildfires over the WNAO in the summer. Model analysis suggests strong hygroscopic growth of sea salt particles and their seeding of marine BL clouds over the WNAO (< 35° N). Future modeling efforts should focus on improving parameterizations for aerosol wet scavenging, implementing realistic smoke injection heights, and applying high-resolution models that better resolve vertical transport.

54 ENVIRONMENTAL SCIENCES↗

Dust semi-direct effects: low-level cloud response to free-tropospheric dust-induced longwave radiation over the North Atlantic Ocean

Aerosol semi-direct effect is the adjustment of the radiative budget due to the cloud response to radiation absorption. Although dust accounts for about a third of aerosols' shortwave absorption, our understanding of its semi-direct effect often relies on traditional shortwave-focused mechanisms previously established for biomass-burning aerosols, and implications of dust longwave absorption on clouds have yet to be explored. Here, we assess the low-level cloud cover (LLCC) response to changes in properties and characteristics of the free-tropospheric dust layer over the North Atlantic Ocean (May–August, 2007–2017). We find that, consistent with previous studies, LLCC typically responds positively (increases in clouds) to an overlying dust layer. However, this response weakens with increasing dust optical depth (DOD), dust geometric thickness (DGT), and dust-layer base height (DBH). Specifically, we find that the LLCC response weakens by 4.3 ± 1.04 % and 1.6 ± 0.65 %, respectively, for a one-standard-deviation increase in DOD and DGT, and a smaller response to DBH (0.19 ± 0.45 %). We also find that the weakened LLCC response is primarily due to enhanced dust-induced longwave-dominated cloud-top warming, which counteracts the mean cloud-top cooling by as much as 19 % (mean of 9 %). Sensitivity analysis further indicates that the variability in dust properties, influenced by dust size distribution and refractive index, dominates the changes in dust-induced cloud-top warming, rather than variabilities in cloud properties or thermodynamic profiles. Our result adds to the traditional understanding of LLCC enhancement through shortwave-driven atmospheric stability, often associated with aerosol semi-direct effects, and highlights the role of dust-induced cloud-top longwave warming in dust semi-direct effects.

Pandey, Satyendra K. [Univ. of California, Merced,↗

Tropospheric Ozone Profiles

The files are from the LASIC field campaign during the period of 17 August through 5 November. The data contains thermodynamic, wind and ozone data in the troposphere.

54 ENVIRONMENTAL SCIENCES↗