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The Southern Ocean is covered by a large amount of clouds with high cloud albedo. However, as reported by previous climate model intercomparison projects, underestimated cloudiness and overestimated absorption of solar radiation (ASR) over the Southern Ocean lead to substantial biases in climate sensitivity. The present study revisits this long-standing issue and explores the uncertainty sources in the latest CMIP6 models. We employ 10-year satellite observations to evaluate cloud radiative effect (CRE) and cloud physical properties in five CMIP6 models that provide comprehensive output of cloud, radiation, and aerosol. The simulated longwave, shortwave, and net CRE at the top of atmosphere in CMIP6 are comparable with the CERES satellite observations. Total cloud fraction (CF) is also reasonably simulated in CMIP6, but the comparison of liquid cloud fraction (LCF) reveals marked biases in spatial pattern and seasonal variations. The discrepancies between the CMIP6 models and the MODIS satellite observations become even larger in other cloud macro- and micro-physical properties, including liquid water path (LWP), cloud optical depth (COD), and cloud effective radius, as well as aerosol optical depth (AOD). However, the large underestimation of both LWP and cloud effective radius (regional means ∼20% and 11%, respectively) results in relatively smaller bias in COD, and the impacts of the biases in COD and LCF also cancel out with each other, leaving CRE and ASR reasonably predicted in CMIP6. An error estimation framework is employed, and the different signs of the sensitivity errors and biases from CF and LWP corroborate the notions that there are compensating errors in the modeled shortwave CRE. Further correlation analyses of the geospatial patterns reveal that CF is the most relevant factor in determining CRE in observations, while the modeled CRE is too sensitive to LWP and COD. The relationships between cloud effective radius, LWP, and COD are also analyzed to explore the possible uncertainty sources in different models. Our study calls for more rigorous calibration of detailed cloud physical properties for future climate model development and climate projection.

Atmospheric aerosols play a central role in the Earth’s radiative budget. They represent a significant part of the anthropogenic forcing responsible for climate change. However, uncertainties in the origin and composition of aerosol particles, their size distribution, concentration, spatial and temporal variability, make it difficult to model their radiative effects. In order to quantify the influence of aerosols on Earth’s climate and to better validate climate models, information about their global abundance, properties and height distribution are needed.Prior research has shown that spectrally resolved measurements of gaseous absorption contain information about the vertical distribution of aerosols. We use measurements of the O2 A-band from the Orbiting Carbon Observatory-2 (OCO-2), in conjunction with spectral sorting and machine learning approaches, to retrieve aerosol optical depth and layer height. The retrievals compare well with collocated lidar measurements. This approach also has the potential to reduce biases in greenhouse gas retrievals.© 2023 California Institute of Technology. US Government sponsorship acknowledged.

The flyby of the New Horizons spacecraft in 2015 July revealed an unexpected cold atmosphere of Pluto and confirmed the existence of its atmospheric haze. The observed and simulated vertical profiles of chemical species and microphysical processes suggest that the haze particles in Pluto's middle and lower atmosphere may contain organic ice condensation. Such organic ice components can potentially affect Pluto's haze chemistry and optical properties, as well as its energy budget. This study investigates the influence of the ice components on the scattering properties of Pluto's haze by comparing New Horizons observations and simulated particle scattering properties. Comprehensive tests are performed for various haze particle parameters, including their size, chemical component, ice content, and morphology. Scattering properties of these ice-bearing haze particles are calculated by a discrete dipole approximation method and compared to multispectral observations obtained by four New Horizons instruments in spectral regions ranging from the ultraviolet to the near-infrared. The results indicate that the inclusion of the organic ice component leads to higher ratios of backscattering in the visible to extinction in the ultraviolet and provides better agreement with observations compared to monodispersed homogeneous aggregates. But it alone is not sufficient to explain the observed forward scattering values in the visible and near-infrared. Therefore, other scattering sources and/or mechanisms are still required to explain the full set of scattering observations. Further observations, as well as laboratory measurements and numerical tests, are anticipated to improve our understanding of the morphology and ice content of Pluto's haze., The Planetary Science Journal, 4 (1), ISSN:2632-3338

Pluto, Titan, and Triton make up a unique class of solar system bodies, with icy surfaces and chemically reducing atmospheres rich in organic photochemistry and haze formation. Hazes play important roles in these atmospheres, with physical and chemical processes highly dependent on particle sizes, but the haze size distribution in reducing atmospheres is currently poorly understood. Here we report observational evidence that Pluto’s haze particles are bimodally distributed, which successfully reproduces the full phase scattering observations from New Horizons. Combined with previous simulations of Titan’s haze, this result suggests that haze particles in reducing atmospheres undergo rapid shape change near pressure levels ~0.5 Pa and favors a photochemical rather than a dynamical origin for the formation of Titan’s detached haze. It also demonstrates that both oxidizing and reducing atmospheres can produce multi-modal hazes, and encourages reanalysis of observations of hazes on Titan and Triton., Pluto’s haze is revealed to have two types of particles: small spherical organic haze particles and micron-size fluffy aggregates. The persistence of these two populations has important implications for haze formation and properties on icy worlds.

A full diurnal measurement of stratospheric column NO2 has been made over the Jet Propulsion Laboratory's Table Mountain Facility (TMF) located in the mountains above Los Angeles, California, USA (2.286 km above mean sea level, 34.38∘ N, 117.68∘ W). During a representative week in October 2018, a grating spectrometer measured the telluric NO2 absorptions in direct solar and lunar spectra. The stratospheric column NO2 is retrieved using a modified minimum-amount Langley extrapolation, which enables us to accurately treat the non-constant NO2 diurnal cycle abundance and the effects of tropospheric pollution near the measurement site. The measured 24 h cycle of stratospheric column NO2 on clean days agrees with a 1-D photochemical model calculation, including the monotonic changes during daytime and nighttime due to the exchange with the N2O5 reservoir and the abrupt changes at sunrise and sunset due to the activation or deactivation of the NO2 photodissociation. The observed daytime NO2 increasing rate is (1.34±0.24)×1014 cm−2 h−1. The observed NO2 in one of the afternoons during the measurement period was much higher than the model simulation, implying the influence of urban pollution from nearby counties. A 24 h back-trajectory analysis shows that the wind first came from inland in the northeast and reached southern Los Angeles before it turned northeast and finally arrived at TMF, allowing it to pick up pollutants from Riverside County, Orange County, and downtown Los Angeles.

Hosting a ∼1.5 bar N2 atmosphere and reducing atmospheric composition, Titan has the energy sources needed to drive disequilibrium chemistry and hosts an aerosol layer which shields the surface from incident UV radiation. This world draws parallels to an early Earth-like world (although ∼200 K cooler), and the atmospheric chemistry may be capable of forming relevant prebiotic species. Exo-Titan worlds at close-in orbits host photochemistry relevant to habitability with rich hydrocarbon chemistry. We investigate the effect of stellar type of the host star, equilibrium temperature, incident radiation, and vertical transport efficiency on the production of higher-order hydrocarbons. We find a greater incident radiation (a closer orbit) increases the rate of methane photolysis as well as photolysis of hydrocarbons. A larger H2 abundance and warmer temperature increases the rate of the back reaction H2 + CH3 → CH4 + H, and the temperature dependence is so great that CH3 recycles back into CH4 instead of forming C2H6. A larger H2 abundance and warmer temperature also encourages interesting cycling between C2H2, C2H3, and C2H4via reactions with atomic H.

Hyperspectral infrared sounding contains information about clouds, which plays an important role in modulating Earth's climate. However, there is a great deal of uncertainty in modeling the radiative effect of clouds due to its complex dependence on various parameters. Therefore, cloudy scenarios are often neglected in retrievals of infrared spectral measurements and in data assimilation. One-dimensional radiative transfer (RT) models have a limited capability to represent the cloud three-dimensional multilayer structure. This issue is typically resolved by using a multiple independent column approach, which is computationally demanding. Therefore, it is necessary to find a balance between computational speed and accuracy for infrared RT all-sky radiance simulations. In this study, we utilize the Community Radiative Transfer Model with four different cloud overlap schemes and compare against observations made by the Atmospheric Infrared Sounder (AIRS) using a statistical metric called the first Wasserstein distance. Our results show that the average cloud overlap scheme performs the best and successfully predicts the overall probability distribution of brightness temperature over nonfrozen oceans for a wide range of wavelengths. The mean absolute differences are less than 0.7 K for 846 selected AIRS channels between 790 cm⁻¹ and 1231 cm⁻¹.

International audience; Tropospheric anthropogenic aerosols contribute the second-largest forcing to climate change, but with high uncertainty owing to their spatio-temporal variability and complicated optical properties. In this Review, we synthesize understanding of aerosol observations and their radiative and climate effects. Aerosols offset about one-third of the warming effect by anthropogenic greenhouse gases. Yet, in regions and seasons where the absorbing aerosol fraction is high — such as South America and East and South Asia — substantial atmospheric warming can occur. The internal mixing and the vertical distribution of aerosols, which alters both the direct effect and aerosol-cloud interactions, might further enhance this warming. Despite extensive research in aerosol-cloud interactions, there is still at least a 50% spread in total aerosol forcing estimates. This ongoing uncertainty is linked, in part, to the poor measurement of anthropogenic and natural aerosol absorption, as well as the little-understood effects of aerosols on clouds. Next-generation, space-borne, multi-angle polarization and active remote sensing, combined with in situ observations, offer opportunities to better constrain aerosol scattering, absorption and size distribution, thus, improving models to refine estimates of aerosol forcing and climate effects.

Titan's atmosphere is a natural laboratory for exploring the photochemical synthesis of organic molecules. Significant recent advances in the study of the atmosphere of Titan include: (a) detection of C$_3$ molecules: C$_3$H$_6$, CH$_2$CCH$_2$, c-C$_3$H$_2$, and (b) retrieval of C$_6$H$_6$, which is formed primarily via C$_3$ chemistry, from Cassini-UVIS data. The detection of $c$-C$_3$H$_2$ is of particular significance since ring molecules are of great astrobiological importance. Using the Caltech/JPL KINETICS code, along with the best available photochemical rate coefficients and parameterized vertical transport, we are able to account for the recent observations. It is significant that ion chemistry, reminiscent of that in the interstellar medium, plays a major role in the production of c-C$_3$H$_2$ above 1000 km., 18 pages (+ 27 page appendix), 16 figures

The absence of significant detectable signatures of organic molecules in the atmosphere and on the surface of Mars is a major unsolved puzzle. One possible explanation is that perchlorate-rich Martian soils, activated by solar ultraviolet (UV) radiation, create an environment favorable for the rapid oxidation of organics such as alkanes (including methane or CH₄). In this paper, we measured product formation rates from the methane-perchlorate-UV system at room temperature. Our results show that magnesium perchlorate (Mg(ClO₄)₂•6H₂O) surfaces exposed to UV light at wavelengths reaching the Mars' surface accelerate the decomposition of methane (CH₄), resulting in the formation of carbon dioxide (CO₂), carbon monoxide (CO), and volatile chlorine oxides. The production rates for CO₂ and CO on UV-activated perchlorate surfaces are accelerated by a factor of 2.5 and 4.5, respectively, compared to those in the absence of perchlorate. In addition, with UV radiation exposure, perchlorate (ClO₄⁻) decomposes to chlorate (ClO₃⁻) and chlorine oxides. These results are incorporated into a simple box model to estimate the near-surface atmospheric methane lifetime. The model gives a lower bound of the lifetime on the order of hours to days, substantially shorter than ~300 yrs. calculated from methane loss by gas-phase chemistry alone.

Supercooled water clouds (SWCs) have significant impacts on the Earth's radiation balance, aircraft ice accretion and precipitation augmentation. This study introduces an efficient algorithm to detect SWCs from passive radiometers, which combines information from the reflectance difference between 1.61 and 2.25 μm channels, the brightness temperature difference between the 8.5 and 11 μm channels, and the cloud top temperature. Validated by space radar and lidar measurements, our algorithm can correctly detect 91% of SWC pixels, better than current Visible Infrared Imager Radiometer Suite operational product. SWCs are found mostly over the mid- to high-latitude oceans and have a global occurrence frequency of ∼8% in cloudy skies. Since the channels used for the detection are available in most current operational polar and geostationary satellite radiometers, this SWC detection algorithm can be easily implemented for operations such as cloud monitoring, aviation safety, and SWC-related weather modification.

We present a new approach to exoplanet characterization using techniques from complexity science, with potential applications to biosignature detection. This agnostic method makes use of the temporal variability of light reflected or emitted from a planet. We use a technique known as epsilon machine reconstruction to compute the statistical complexity, a measure of the minimal model size for time series data. We demonstrate that statistical complexity is an effective measure of the complexity of planetary features. Increasing levels of qualitative planetary complexity correlate with increases in statistical complexity and Shannon entropy, demonstrating that our approach can identify planets with the richest dynamics. We also compare Earth time series with Jupiter data, and find that for the three wavelengths considered Earth’s average complexity and entropy rate are approximately 50% and 43% higher than Jupiter’s, respectively. The majority of schemes for the detection of extraterrestrial life rely upon biochemical signatures and planetary context. However, it is increasingly recognized that extraterrestrial life could be very different from life on Earth. Under the hypothesis that there is a correlation between the presence of a biosphere and observable planetary complexity, our technique offers an agnostic and quantitative method for the measurement thereof.

Previous studies suggested that the Amazon, the largest rainforest on Earth, changes from a CO2 sink to a CO2 source during the dry/fire season. However, the biospheric contributions to atmospheric CO2 are not well understood during the two main seasons, the dry/fire season and the wet season. In this article, we utilize Orbiting Carbon Observatory 2 (OCO‐2) Solar‐Induced Fluorescence (SIF) to explore photosynthetic activity during the different seasons. The spatiotemporal variability of OCO‐2 SIF, OCO‐2 CO2, precipitation, and burned area are investigated over the Amazon from September 2014 to December 2019. Averaging over the entire Amazon region, we found a positive temporal correlation (0.94) between OCO‐2 SIF and Global Precipitation Climatology Project precipitation and a negative temporal correlation (−0.64) between OCO‐2 SIF and OCO‐2 CO2, consistent with the fact that precipitation enhances photosynthesis, which results in higher values for SIF and rate of removal of CO2 from the atmosphere above the Amazon region. We also observed seasonality in the spatial variability of these variables within the Amazon region. During the dry/fire (August–October) season, low SIF values, low precipitation, high vapor pressure deficit (VPD), large burned areas, and high atmospheric CO2 are mainly found over the southern Amazon region. In contrast, during the wet season (January–March), high SIF values, high precipitation, low VPD, smaller burned areas, and low CO2 are found over both the central and southern Amazon regions. The seasonal difference in SIF suggests that photosynthetic activity is reduced during the dry/fire season relative to the wet season as a result of low precipitation and high VPD, especially over the southern Amazon region, which will contribute to more CO2 in the atmosphere during the dry/fire season.

Winter extreme weather events receive major public attention due to their serious impacts1, but the dominant factors regulating their interdecadal trends have not been clearly established2,3. Here, we show that the radiative forcing due to geospatially redistributed anthropogenic aerosols mainly determined the spatial variations of winter extreme weather in the Northern Hemisphere during 1970–2005, a unique transition period for global aerosol forcing4. Over this period, the local Rossby wave activity and extreme events (top 10% in wave amplitude) exhibited marked declining trends at high latitudes, mainly in northern Eurasia. The combination of long-term observational data and a state-of-the-art climate model revealed the unambiguous signature of anthropogenic aerosols on the wintertime jet stream, planetary wave activity and surface temperature variability on interdecadal timescales. In particular, warming due to aerosol reductions in Europe enhanced the meridional temperature gradient on the jet’s poleward flank and strengthened the zonal wind, resulting in significant suppression in extreme events over northern Eurasia. These results exemplify how aerosol forcing can impact large-scale extratropical atmospheric dynamics, and illustrate the importance of anthropogenic aerosols and their spatiotemporal variability in assessing the drivers of extreme weather in historical and future climate. Anthropogenic aerosol emissions decreased over North America and Europe but increased over Asia since the 1970s. This caused jet stream winds to shift poleward over the Atlantic, decreasing planetary wave activity and partially inhibiting extreme winter weather over northern Eurasia.

The delta values of the isotope composition of atmospheric ozone is ~100‰ (referenced to atmospheric O2). Previous photochemical models, which considered the isotope fractionation processes from both formation and photolysis of ozone, predicted δ49O3 and δ50O3 values, in δ49O3 versus δ50O3 space, that are >10‰ larger than the measurements. We propose that the difference between the model and observations could be explained either by the temperature variation, Chappuis band photolysis, or a combination of the two and examine them. The isotopic fractionation associated with ozone formation increases with temperature. Our model shows that a hypothetical reduction of ~20 K in the nominal temperature profile could reproduce the observations. However, this hypothesis is not consistent with temperatures obtained by in situ measurements and NCEP Reanalysis. Photolysis of O3 in the Chappuis band causes O3 to be isotopically depleted, which is supported by laboratory measurements for 18O18O18O but not by recent new laboratory data made at several wavelengths for 49O3 and 50O3. Cloud reflection can significantly enhance the photolysis rate and affect the spectral distribution of photons, which could influence the isotopic composition of ozone. Sensitivity studies that modify the isotopic composition of ozone by the above two mechanisms are presented. We conclude isotopic fractionation occurring in photolysis in the Chappuis band remains the most plausible solution to the model-observation discrepancy. Implications of our results for using the oxygen isotopic signature for constraining atmospheric chemical processes related to ozone, such as CO2, nitrate, and the hydroxyl radical, are discussed.

Significance The COVID-19 pandemic and associated lockdowns caused significant changes to human activity that temporarily altered our imprint on the atmosphere, providing a brief glimpse of potential future changes in atmospheric composition. This event demonstrated key feedbacks within and between air quality and the carbon cycle: Improvements in air quality increased the lifetime of methane (an important greenhouse gas), while unusually hot weather and intense wildfires in Los Angeles drove poor air quality. This shows that efforts to reduce greenhouse gas emissions and improve air quality cannot be considered separately., The COVID-19 global pandemic and associated government lockdowns dramatically altered human activity, providing a window into how changes in individual behavior, enacted en masse, impact atmospheric composition. The resulting reductions in anthropogenic activity represent an unprecedented event that yields a glimpse into a future where emissions to the atmosphere are reduced. Furthermore, the abrupt reduction in emissions during the lockdown periods led to clearly observable changes in atmospheric composition, which provide direct insight into feedbacks between the Earth system and human activity. While air pollutants and greenhouse gases share many common anthropogenic sources, there is a sharp difference in the response of their atmospheric concentrations to COVID-19 emissions changes, due in large part to their different lifetimes. Here, we discuss several key takeaways from modeling and observational studies. First, despite dramatic declines in mobility and associated vehicular emissions, the atmospheric growth rates of greenhouse gases were not slowed, in part due to decreased ocean uptake of CO2 and a likely increase in CH4 lifetime from reduced NOx emissions. Second, the response of O3 to decreased NOx emissions showed significant spatial and temporal variability, due to differing chemical regimes around the world. Finally, the overall response of atmospheric composition to emissions changes is heavily modulated by factors including carbon-cycle feedbacks to CH4 and CO2, background pollutant levels, the timing and location of emissions changes, and climate feedbacks on air quality, such as wildfires and the ozone climate penalty.

The northern high latitude (NHL, 40°N to 90°N) is where the second peak region of gross primary productivity (GPP) other than the tropics. The summer NHL GPP is about 80% of the tropical peak, but both regions are still highly uncertain (Norton et al. 2019, https://doi.org/10.5194/bg-16-3069-2019). Carbonyl sulfide (OCS) provides an important proxy for photosynthetic carbon uptake. Here we optimize the OCS plant uptake fluxes across the NHL by fitting atmospheric concentration simulation with the GEOS-CHEM global transport model to the aircraft profiles acquired over Alaska during NASA's Carbon in Arctic Reservoirs Vulnerability Experiment (2012-2015). We use the empirical biome-specific linear relationship between OCS plant uptake flux and GPP to derive the six plant uptake OCS fluxes from different GPP data. Such GPP-based fluxes are used to drive the concentration simulations. We evaluate the simulations against the independent observations at two ground sites of Alaska. The optimized OCS fluxes suggest the NHL plant uptake OCS flux of -247 Gg S year

The Mars Science Laboratory (MSL) recently discovered nitrates in Gale Crater (e.g., Stern et al., 2015; Sutter et al., 2017). One possible mechanism for ancient nitrate deposition on Mars is through HNOx formation and rain out in the atmosphere, for which lightning-induced NO is likely the fundamental source. This study investigates nitrogen (N₂) fixation in early Mars' atmosphere, with implications for early Mars' habitability. We consider a 1 bar atmosphere of background CO₂, with abundance of N₂, hydrogen, and methane varied from 1% to 10% to explore a swath of potential early Mars climates. We derive lightning-induced thermochemical equilibrium fluxes of NO and HCN by coupling the lightning-rate parametrization from the study of Romps et al. (2014) with chemical equilibrium with applications, and we use a Geant4 simulation platform to estimate the effect of solar energetic particle events. These fluxes are used as input into KINETICS, the Caltech/JPL coupled photochemistry and transport code, which models the chemistry of 50 species linked by 495 reactions to derive rain-out fluxes of HNOx and HCN. We compute equilibrium concentrations of cyanide and nitrate in a putative northern ocean at early Mars, assuming hydrothermal vent circulation and photoreduction act as the dominant loss mechanisms. We find average oceanic concentrations of ∼0.1–2 nM nitrate and ∼0.01–2 mM cyanide. HCN is critical for protein synthesis at concentrations >0.01 M (e.g., Holm and Neubeck, 2009), and our result is astrobiologically significant if secondary local concentration mechanisms occurred. Nitrates may act as high-potential electron acceptors for early metabolisms, although the minimum concentration required is unknown. Our study derives concentrations that will be useful for future laboratory studies to investigate the habitability at early Mars. The aqueous nitrate concentrations correspond to surface nitrate precipitates of ∼1–8 × 10⁻⁴ wt % that may have formed after the evaporation of surface waters, and these values roughly agree with recent MSL measurements.

During its first seven years of operation, the Sample Analysis at Mars Tunable Laser Spectrometer (TLS) on board the Curiosity rover has detected seven methane spikes above a low background abundance in Gale crater. The methane spikes are likely sourced by surface emission within or around Gale crater. Here, we use inverse Lagrangian modeling techniques to identify upstream emission regions on the Martian surface for these methane spikes at an unprecedented spatial resolution. Inside Gale crater, the northwestern crater floor casts the strongest influence on the detections. Outside Gale crater, the upstream regions common to all the methane spikes extend toward the north. The contrasting results from two consecutive TLS methane measurements performed on the same sol point to an active emission site to the west or the southwest of the Curiosity rover on the northwestern crater floor. The observed spike magnitude and frequency also favor emission sites on the northwestern crater floor, unless there are fast methane removal mechanisms at work, or either the methane spikes of TLS or the non‐detections of ExoMars Trace Gas Orbiter cannot be trusted.

The large fluctuations in traffic during the COVID-19 pandemic provide an unparalleled opportunity to assess vehicle emission control efficacy. Here we develop a random-forest regression model, based on the large volume of real-time observational data during COVID-19, to predict surface-level NO(2), O(3), and fine particle concentration in the Los Angeles megacity. Our model exhibits high fidelity in reproducing pollutant concentrations in the Los Angeles Basin and identifies major factors controlling each species. During the strictest lockdown period, traffic reduction led to decreases in NO(2) and particulate matter with aerodynamic diameters

Burying Mars' ancient water in the crust Mars once had oceans of liquid water on its surface but little of that water remains today in the planet's ice caps and atmosphere. This discrepancy is usually interpreted as loss of water to space, supported by the atmospheric deuterium/hydrogen (D/H) ratio, but this has been difficult to reconcile with other constraints. Scheller et al. propose that water could instead have been incorporated into minerals in the planet's crust, which were later buried (see the Perspective by Kurokawa). They simulated the evolution of the D/H ratio and atmospheric loss rates for a range of plausible conditions, finding that 30 to 99% of Mars' initial water was buried in the crust. Science , this issue p. 56 ; see also p. 27

Legislation in the State of California mandates reductions in emissions of short‐lived climate pollutants of 40% from 2013 levels by 2030 for CH_4. Identification of the sector(s) responsible for these emissions and their temporal and spatial variability is a key step in achieving these goals. Here, we determine the emissions of CH_4 in Los Angeles from 2011–2017 using a mountaintop remote sensing mapping spectrometer. We show that the pattern of CH_4 emissions contains both seasonal and nonseasonal contributions. We find that the seasonal component peaks in the winter and is correlated (R^2 = 0.58) with utility natural gas consumption from the residential and commercial sectors and not from the industrial and gas‐fired power plant sectors. The nonseasonal component is (22.9 ± 1.4) Gg CH_4/month. If the seasonal correlation is causal, about (1.4 ± 0.1)% of the commercial and residential natural gas consumption in Los Angeles is released into the atmosphere.

Cassini/UVIS FUV observations of stellar occultations at Titan are well suited for probing its atmospheric composition and structure. However, due to instrument pointing motion, only five out of tens of observations have been analyzed. We present an innovative retrieval method that corrects for the effect of pointing motion by forward modeling the Cassini/UVIS instrument response function with the pointing motion value obtained from the SPICE C-kernel along the spectral dimension. To illustrate the methodology, an occultation observation made during flyby T52 is analyzed, when the Cassini spacecraft had insufficient attitude control. A high-resolution stellar model and an instrument response simulator that includes the position of the point source on the detector are used for the analysis of the pointing motion. The Markov Chain Monte-Carlo method is used to retrieve the line-of-sight abundance profiles of eleven species (CH4, C2H2, C2H4, C2H6, C4H2, C6H6, HCN, C2N2, HC3N, C6N2 and haze particles) in the spectral vector fitting process. We obtain tight constraints on all of the species aside from C2H6, C2N2 and C6N2, for which we only retrieved upper limits. This is the first time that the T52 occultation was used to derive abundances of major hydrocarbon and nitrile species in Titan's upper and middle atmosphere, as pointing motion prohibited prior analysis. With this new method, nearly all of the occultations obtained over the entire Cassini mission could yield reliable profiles of atmospheric composition, allowing exploration of Titan's upper atmosphere over seasons, latitudes, and longitudes., Comment: Accepted by Earth and Space Science, 8 pages, 6 figures

A new multilayer (ML) cloud detection algorithm based on three shortwave infrared (SWIR) and two longwave infrared (LWIR) channels is developed and applied to the Visible Infrared Imager Radiometer Suite (VIIRS) onboard the Suomi-NPP satellite. The algorithm identifies ML clouds, i.e., ice clouds overlying water clouds, based on satellite multispectral observations in the 1.38, 1.6, 2.25, 8.5, and 11 μm channels. We perform synthetic radiative transfer simulations to understand the sensitivities of the aforementioned channels on ML and single-layer (SL) clouds. Active CALIOP observations are used to evaluate the algorithm. Compared with the collocated CALIOP results, the algorithm can determine SL and ML clouds correctly with success rates of approximately 80% and 60%, respectively, and has similar performance to that of the current MODIS operational ML cloud detection algorithm. The misclassification of ML clouds as SL clouds is primarily caused by thin ice clouds that are practically undetectable using LWIR tests. Furthermore, the algorithm is extended to analyze data from radiometers onboard the geostationary Himawari-8 and FengYun-4A satellites, and results similar to those of VIIRS are obtained.

Advanced satellite technology has been providing unique observations of global carbon dioxide (CO2) concentrations. These observations have revealed important CO2 variability at different timescales and over regional and planetary scales. Satellite CO2 retrievals have revealed that stratospheric sudden warming and the Madden-Julian Oscillation can modulate atmospheric CO2 concentrations in the mid-troposphere. Atmospheric CO2 also demonstrates variability at interannual timescales. In the tropical region, the El Niño–Southern Oscillation and the Tropospheric Biennial Oscillation can change atmospheric CO2 concentrations. At high latitudes, mid-tropospheric CO2 concentrations can be influenced by the Northern Hemispheric annular mode. In addition to modulations by the large-scale circulations, sporadic events such as wildfires, volcanic eruptions, and droughts, which change CO2 surface emissions, can cause atmospheric CO2 concentrations to increase significantly. The natural variability of CO2 summarized in this review can help us better understand its sources and sinks and its redistribution by atmospheric motion. ▪ Global satellite CO2 data offer a unique opportunity to explore CO2 variability in different regions. ▪ Atmospheric CO2 concentration demonstrates variations at intraseasonal, seasonal, and interannual timescales. ▪ Both large-scale circulations and variations of surface emissions can modulate CO2 concentrations in the atmosphere.

A sensitivity study has been performed to estimate detection limits of various atmospheric trace gases achievable by a Mars‐orbiting solar occultation Fourier transform infrared (FTIR) spectrometer. This was accomplished by first computing realistic limb transmittance spectra based on a model (T, P, VMR, and dust profiles) of the Mars atmosphere and adding appropriate noise and systematic errors based on assumed instrument design/configuration/performance. We then performed spectral fits to the resulting synthetic spectra to derive slant column abundances and their uncertainties. A profile retrieval was performed to infer limits of detection. This methodology was applied to a Mars‐orbiting FTIR solar occultation spectrometer covering the 850–4,300 cm−1 spectral region at 0.025‐cm−1 resolution. We conclude that most gases can be retrieved with a single‐occultation sensitivity of 20–100 ppt. But this sensitivity varies considerably with the dust loading, especially for gases whose strongest absorption bands are toward higher wavenumbers where scattering is large. We conclude that for CH4, the ν4 band centered at 1,305 cm−1, despite being more than 2 times weaker than the ν3 band centered at 3,015 cm−1, offers better sensitivity due to its close spectral proximity to the dust extinction minimum. We also conclude that for the purpose of CH4 detection, a high‐resolution (0.025 cm−1) broadband instrument would have a substantial advantage over a medium‐resolution (0.15 cm−1) instrument, despite the latter having a much larger signal‐to‐noise ratio.

Simulations of tropical atmospheric circulation response to surface warming vary substantially across models, causing large uncertainties in projections of regional precipitation change. Understanding the physical processes that drive the model spread in tropical circulation changes is critically needed. Here we employ the basic mass balance and energetic constraints on tropical circulation to identify the dominant factors that determine multidecadal circulation strength and area changes in climate models. We show that the models produce a robust weakening of descent rate under warming regardless of surface warming patterns; however, ascent rate change exhibits inter-model spread twice as large as descent rate because of diverse model responses in the radiative effects of clouds, water vapor, and aerosols. As ascent area change is dictated by the disparate descent and ascent rate changes due to the mass budget and the inter-model spread in descent rate change is small, the model spread in ascent area change is dominated by that of ascent rate change, resulting in a strong anti-correlation of –0.85 between the fractional changes of ascent strength and area across 77 climate model simulations. This anti-correlation leads to a corresponding inverse relationship between the rates of precipitation intensifying and narrowing of the inter-tropical convergence zone (ITCZ), suggesting tropical ascent area change can be potentially used to constrain the ITCZ precipitation change. Longwave cloud radiative effect at the top-of-atmosphere (TOA) in the convective region is identified to be a major source of uncertainties for tropical ascent rate change and thus for regional precipitation change. Tropical precipitation in the future will be influenced by the balance between changes in the area and rate of atmospheric ascent and descent. Hui Su from the Jet Propulsion Laboratory, together with a multidisciplinary team, probe several climate modeling experiments and show that models consistently simulate a lower descent rate in a warming climate. But changes in ascent rate range from strongly positive to strongly negative, a diversity that is dominated by variations in both the simulated longwave energy fluxes at the top of the atmosphere and the absorption of shortwave energy. Because mass must be conserved and the descent rate change is approximately constant, ascent rate change is anticorrelated with the ascending area change. Consequently, models with a major increase in ascent rate also show a narrowing of the ascending area, leading to a “wetter get narrower” environment. Robust observations are critically needed to constrain the simulated ascent rates and controlling processes.

Black carbon (BC) aerosol plays an important role in the atmosphere as an absorber of solar radiation and contributes significantly to global warming. The optical properties of BC are fundamental for both direct radiative effect studies and remote sensing of BC properties. However, due to the complex aggregation structures of BC particles, accurate simulations of their optical properties are limited and computationally expensive, while equivalent spherical models or approximate methods could easily introduce relative errors up to 30%. This study generates a comprehensive database to calculate aggregate optical properties efficiently and accurately. The database covers a wide range of BC properties including aggregation structure, refractive index, and particle size (both monomer size and number of monomers). An accurate numerical model, i.e. the multiple-sphere T-matrix method, is used to calculate the single-scattering properties of BC clusters in the form of fractal aggregates. By interpolation, the database can be used to give the scattering properties of aggregates with monomer number from 1 up to 3000, monomer size parameter from 0.05 to 0.5, real part of refractive index from 1.2 to 2.0, and imaginary part from 0.2 to 1.0. The relative errors caused by the interpolation are much less than 1% for the single scattering properties. The pre-calculated database and the implementation used to calculate the required aggregate optical properties are publicly available for users interested in remote sensing of BC aerosols and performing radiative effect calculations.

Seasonal variation is significant in Titan's atmosphere due to the large change of solar insolation resulting from Titan's 26.7{\deg} axial tilt relative to the plane of Saturn's orbit. Here we present an investigation of hydrocarbon and nitrile species in Titan's upper atmosphere at 400-1200 km, which includes the mesosphere and the lower thermosphere, over more than one fourth of Titan's year (2006-2014, LS=318{\deg}-60{\deg}), using eighteen stellar occultation observations obtained by Cassini/UVIS. Vertical profiles of eight chemical species (CH4, C2H2, C2H4, C2H6, C4H2, C6H6, HCN, HC3N) and haze particles are retrieved from these observations using an instrument forward model, which considers the technical issue of pointing motion. The Markov-chain Monte Carlo (MCMC) algorithm is used to obtain the posterior probability distributions of parameters in the retrieval, which inherently tests the extent to which species profiles can be constrained. The results show that no change of the species profiles is noticeable before the equinox, while the decrease of atmospheric temperature and significant upwelling in the summer hemisphere are found five terrestrial years afterwards. Altitude of the detached haze layer decreases towards the vernal equinox then it disappears, and no reappearance is identified within the time range of our data, which is consistent with observations from Cassini/ISS. This study provides observational constraints on the seasonal change of Titan's upper atmosphere, and suggests further investigations of the atmospheric chemistry and dynamics therein., Comment: 11 pages, 12 figures, accepted by PSJ

The optical properties of black carbon (BC) are fundamental for radiative transfer and remote sensing. BC geometry is successfully represented by an idealized model named “fractal aggregate”, and numerous methods are available and widely used to simulate the corresponding optical properties. This study systematically evaluates the performance of the Discrete Dipole Approximation (DDA) for optical simulations of BC aggregates. The Multiple Sphere T-Matrix (MSTM) results are used as references for accuracy evaluation. The differences between the DDA and MSTM can be controlled to be less than 3% by using dipole size much smaller than the monomer size, and the DDA efficiency is sensitive to aggregate structures, e.g. lacy or compact. We find that shape representation for small-sized monomers during DDA discretization leads significant errors, i.e., up to 10%, and relatively large refractive indices of BC also affects the DDA accuracy. However, the MSTM treats the BC monomers as perfect spheres without overlapping, and the imperfect structure that is implicitly introduced in the DDA simulations due to the spatial discretization may be a better representation of realistic BC particles. Moreover, the efficiency of the DDA can be improved by defining dipoles on the particle boundary to have refractive indices given by the effective medium approximation (EMA). This leads to the adequate shape representation even using larger dipole sizes, and results in the DDA accuracy comparable to that of the reference MSTM solution.

The direct radiative forcing of black carbon aerosol (BC) on the Earth system remains unsettled, largely due to the uncertainty with physical properties of BC throughout their lifecycle. Here we show that ambient chamber measurements of BC properties provide a novel constraint on the crude BC aging representation in climate models. Observational evidence for significant absorption enhancement of BC can be reproduced when the aging processes in the four‐mode version of the Modal Aerosol Module (MAM4) aerosol scheme in the Community Atmosphere Model version 5 are calibrated by the recent in situ chamber measurements. An observation‐based scaling method is developed in the aging timescale calculation to alleviate the influence of biases in the simulated model chemical composition. Model sensitivity simulations suggest that the different monolayer settings in the BC aging parameterization of MAM4 can cause as large as 26% and 24% differences in BC burden and radiative forcing, respectively. We also find that an increase in coating materials (e.g., sulfate and secondary organic aerosols) reduces BC lifetime by increasing the hygroscopicity of the mixture but enhances its absorption, resulting in a net increase in BC direct radiative forcing. Our results suggest that accurate simulations of BC aging processes as well as other aerosol species are equally important in reducing the uncertainty of BC forcing estimation., Key Points Atmospheric black carbon aging processes in CAM5 are constrained by chamber experimentsThe calibrated model shows that coating results in net enhancement in BC forcing in spite of a reduction in BC lifetimeModeled BC direct radiative forcing varies up to 26% due to the uncertainties in BC aging parameterization and coating aerosol mass

Remote sensing of greenhouse gases (GHGs) in cities, where high GHG emissions are typically associated with heavy aerosol loading, is challenging due to retrieval uncertainties caused by the imperfect characterization of scattering by aerosols. We investigate this problem by developing GFIT3, a full physics algorithm to retrieve GHGs (CO2 and CH4) by accounting for aerosol scattering effects in polluted urban atmospheres. In particular, the algorithm includes coarse- (including sea salt and dust) and fine- (including organic carbon, black carbon, and sulfate) mode aerosols in the radiative transfer model. The performance of GFIT3 is assessed using high-spectral-resolution observations over the Los Angeles (LA) megacity made by the California Laboratory for Atmospheric Remote Sensing Fourier transform spectrometer (CLARS-FTS). CLARS-FTS is located on Mt. Wilson, California, at 1.67 km a.s.l. overlooking the LA Basin, and it makes observations of reflected sunlight in the near-infrared spectral range. The first set of evaluations are performed by conducting retrieval experiments using synthetic spectra. We find that errors in the retrievals of column-averaged dry air mole fractions of CO2 (XCO2) and CH4 (XCH4) due to uncertainties in the aerosol optical properties and atmospheric a priori profiles are less than 1 % on average. This indicates that atmospheric scattering does not induce a large bias in the retrievals when the aerosols are properly characterized. The methodology is then further evaluated by comparing GHG retrievals using GFIT3 with those obtained from the CLARS-GFIT algorithm (used for currently operational CLARS retrievals) that does not account for aerosol scattering. We find a significant correlation between retrieval bias and aerosol optical depth (AOD). A comparison of GFIT3 AOD retrievals with collocated ground-based observations from AErosol RObotic NETwork (AERONET) shows that the developed algorithm produces very accurate results, with biases in AOD estimates of about 0.02. Finally, we assess the uncertainty in the widely used tracer–tracer ratio method to obtain CH4 emissions based on CO2 emissions and find that using the CH4/CO2 ratio effectively cancels out biases due to aerosol scattering. Overall, this study of applying GFIT3 to CLARS-FTS observations improves our understanding of the impact of aerosol scattering on the remote sensing of GHGs in polluted urban atmospheric environments. GHG retrievals from CLARS-FTS are potentially complementary to existing ground-based and spaceborne observations to monitor anthropogenic GHG fluxes in megacities.

Aerosol effects on clouds’ microphysics and dynamics are still considered as an important open question that contributes a major uncertainty to climate research and prediction. Using 7 years of observational and reanalysis data, we show a non-monotonic trend in convective cloud properties and rain intensity as a function of aerosol optical depth (AOD). The invigoration effect shifts into weak suppression beyond an optimal AOD ( of ~ 0.3-0.4). Using a cloud model we explain this shift in trend as the result of a competition between two types of microphysical processes: cloud-core-based invigorating processes vs. peripheral suppressive processes. We show that the optimal AOD, for which cloud and rain reach their maximal values, depends on the environmental thermodynamic conditions and it is higher for more unstable or more humid conditions. Our findings improve the understanding of aerosol-cloud interaction and their link to environmental conditions. It can aid in the improvement of parameterizations of clouds in climate models.

Pluto's atmospheric profiles (temperature and pressure) have been studied for decades from stellar occultation lightcurves. In this paper, we look at recent Pluto Global Climate Model (GCM) results (3D temperature, pressure, and density fields) from Bertrand et al. (2020) and use the results to generate model observer's plane intensity fields (OPIF) and lightcurves by using a Fourier optics scheme to model light passing through Pluto's atmosphere ( Young, 2012 ). This approach can accommodate arbitrary atmospheric structures and 3D distributions of haze. We compared the GCM model lightcurves with the lightcurves observed during the 15-AUG-2018 Pluto stellar occultation. We find that the climate scenario which best reproduces the observed data includes a N2 ice mid latitude band in the southern hemisphere. We have also studied different haze and P/T ratio profiles: the haze effectively reduces the central flash strength, and a lower P/T ratio both reduces the central flash strength and incurs anomalies in the shoulders of the central flash.

Atmospheric isotopologues of water vapor (e.g., HDO) are important tracers for understanding Earth’s hydrological cycles. Most remote sensing measurements of these isotopologues, however, are colum...

The COVID-19 global pandemic and associated government lockdowns dramatically altered human activity, providing a window into how changes in individual behavior, enacted en masse, impact atmospheri...

In the field of astrobiology, the precise location, prevalence, and age of potential extraterrestrial intelligence (ETI) have not been explicitly explored. Here, we address these inquiries using an empirical galactic simulation model to analyze the spatial&ndash, temporal variations and the prevalence of potential ETI within the Galaxy. This model estimates the occurrence of ETI, providing guidance on where to look for intelligent life in the Search for ETI (SETI) with a set of criteria, including well-established astrophysical properties of the Milky Way. Further, typically overlooked factors such as the process of abiogenesis, different evolutionary timescales, and potential self-annihilation are incorporated to explore the growth propensity of ETI. We examine three major parameters: (1) the likelihood rate of abiogenesis (&lambda, A), (2) evolutionary timescales (Tevo), and (3) probability of self-annihilation of complex life (Pann). We found Pann to be the most influential parameter determining the quantity and age of galactic intelligent life. Our model simulation also identified a peak location for ETI at an annular region approximately 4 kpc from the galactic center around 8 billion years (Gyrs), with complex life decreasing temporally and spatially from the peak point, asserting a high likelihood of intelligent life in the galactic inner disk. The simulated age distributions also suggest that most of the intelligent life in our galaxy are young, thus making observation or detection difficult.

International audience; More than 85% of the 23 investigations developed by VEXAG are largely accomplished via a NF mission centered on a variable-altitude balloon (aerobot) supported by a science/comm orbiter. Circling Venus >15 times over ~90 days, the aerobot repeatedly visits 52-62 km alts as it semi-continuously samples a host of environmental & surface parameters.