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Abstract Methane, with a global warming potential roughly 86 times greater than carbon dioxide over a 20‐year timeframe, plays a crucial role in global warming. Remote sensing retrieval is a pivotal methodology for identifying methane emission sources, with accuracy influenced largely by surface and atmospheric properties, including aerosols. In this study, we propose an Aerosol‐Calibrated Matched Filter (ACMF) algorithm to improve the traditional Matched Filter (MF) method. Our new approach incorporates an aerosol scattering correction factor to reduce the aerosol‐induced bias on methane retrievals. Validating our algorithm through simulated spectra, we demonstrate that considering the aerosol scattering effect significantly reduces retrieval errors compared to MF methods by an average of approximately 90%. We apply our newly developed algorithm to hyperspectral data obtained from the Airborne Visible/Infrared Imaging Spectrometer—Next Generation in the Los Angeles Basin and focus on 11 plumes identified through case studies. Our results reveal that ACMF estimates of emission rates and inversion uncertainties exhibit an average reduction of approximately 4% compared to corresponding MF results, with deviation increasing with aerosol optical depth (AOD).

Abstract Methane, a powerful greenhouse gas, has a short atmospheric lifetime ( ~ 12 years), so that emissions reductions will have a rapid impact on climate forcing. In megacities such as Los Angeles (LA), natural gas (NG) leakage is the primary atmospheric methane source. The magnitudes and trends of fugitive NG emissions are largely unknown and need to be quantified to verify compliance with emission reduction targets. Here we use atmospheric remote sensing data to show that, in contrast to the observed global increase in methane emissions, LA area emissions decreased during 2011-2020 at a mean rate of (–1.57 ± 0.41) %/yr. However, the NG utility calculations indicate a much larger negative emissions trend of −5.8 %/yr. The large difference between top-down and bottom-up trends reflects the uncertainties in estimating the achieved emissions reductions. Actions taken in LA can be a blueprint for COP28 and future efforts to reduce methane emissions.

Fixed nitrogen species generated by the early Earth’s atmosphere are thought to be critical to the emergence of life and the sustenance of early metabolisms. A previous study estimated nitrogen fixation in the Hadean Earth’s N2/CO2-dominated atmosphere; however, that previous study only considered a limited chemical network that produces NOx species (i.e., no HCN formation) via the thermochemical dissociation of N2 and CO2 in lightning flashes, followed by photochemistry. Here, we present an updated model of nitrogen fixation on Hadean Earth. We use the Chemical Equilibrium with Applications (CEA) thermochemical model to estimate lightning-induced NO and HCN formation and an updated version of KINETICS, the 1-D Caltech/JPL photochemical model, to assess the photochemical production of fixed nitrogen species that rain out into the Earth’s early ocean. Our updated photochemical model contains hydrocarbon and nitrile chemistry, and we use a Geant4 simulation platform to consider nitrogen fixation stimulated by solar energetic particle deposition throughout the atmosphere. We study the impact of a novel reaction pathway for generating HCN via HCN2, inspired by the experimental results which suggest that reactions with CH radicals (from CH4 photolysis) may facilitate the incorporation of N into the molecular structure of aerosols. When the HCN2 reactions are added, we find that the HCN rainout rate rises by a factor of five in our 1-bar case and is about the same in our 2- and 12-bar cases. Finally, we estimate the equilibrium concentration of fixed nitrogen species under a kinetic steady state in the Hadean ocean, considering loss by hydrothermal vent circulation, photoreduction, and hydrolysis. These results inform our understanding of environments that may have been relevant to the formation of life on Earth, as well as processes that could lead to the emergence of life elsewhere in the universe.

Abstract Mid‐tropospheric Carbonyl sulfide (OCS) retrievals from the Tropospheric Emission Spectrometer (TES) are utilized to study OCS distributions during the dry/wet seasons over the Amazon rainforest. TES OCS retrievals reveal positive OCS anomalies (∼16 ppt) over the central and southern parts of the Amazon during August–October (dry season) compared to January–March (wet season). There is less OCS taken up by vegetation and soil and more OCS released from biomass burning during the dry season, which causes an increase in OCS concentrations. Strong sinking air during the dry season also helps to trap OCS and this contributes to positive OCS anomalies. MOZART‐4 model captures positive OCS anomalies over the central and southern regions of the Amazon and negative OCS anomalies over the northern part of the Amazon, which are similar to those from TES mid‐tropospheric OCS retrievals. Our studies can help us better understand OCS variations and photosynthetic activities.

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.

Abstract Plant growth and crop harvest are impacted by both climate change and air pollution. However, their relative importance in crop yields remains elusive, especially in heavily polluted regions. Here we develop crop yield prediction models, based on a large volume of historical crop data, as well as climate and pollution records in China since 1980. A long‐term surface ozone concentration data set is developed from a machine‐learning model and various observations. An assessment of four climate and pollution factors reveals the critical role of particulate and ozone pollution in regulating interannual variations of crop yields in China. During 2010–2018, we find that the particulate pollution mitigation outweighs the negative impacts of concurrent climate change, resulting in 0.5%–1.9% net yield increases nationwide, despite of the ozone increases in the North China Plain. Looking to the future, the impacts of climate change, particularly from surface temperature increase, will dominate over pollution factors and profoundly reduce future maize and rice yields by 0.6 to 2.8% 10 yr−1 by 2050. Our findings call for attention on the threat to future global food security from the absence of pollution mitigation and the persistence of global warming.

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.

Abstract 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.

Photochemistry of sulfur species in the upper Venus atmosphere is not well understood and the identity of ultraviolet (UV) absorber(s) remain unknown. Here, the authors show that sulfur monoxide dimer chemistry is a possible source of polysulfur, which could be responsible for the UV absorption.

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.

Abstract 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.

Abstract The California wildfires of October 2017 were one of the largest wildfires in the state's history. Using surface temperature, surface pressure, cloud liquid and ice water contents, precipitation data, and wind data, we explore possible reasons for the wildfires. It is found that the mean surface temperature in California has increased, while mean cloud water contents and mean precipitation in California has decreased over the past 39 years. Higher temperatures, higher surface pressures, lower cloud water contents, lower precipitation, enhanced surface Santa Ana winds, and enhanced sinking air have set up favorable meteorological conditions for stronger wildfires in California, such as the October 2017 wildfires. Furthermore, the CO2 data from the Orbiting Carbon Observatory 2 satellite have, for the first time, made it possible for us to quantitatively characterize the impact of wildfires on atmospheric CO2 in California, which revealed that atmospheric CO2 increased by 2 ppm after the October 2017 California wildfires. Analyses in this study can help us better understand the causes and impacts of wildfires.

Abstract Cassini/Ultraviolet Imaging Spectrograph (UVIS) Far‐UV observations of stellar occultations at Titan are well suited for probing its atmospheric composition and structure. However, due to instrument pointing motion, only 5 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, HCN, C4H2, C6N2, C6H6, haze, HC3N, and C2N2) 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.

Abstract The interannual variability of tropical carbon monoxide from the Microwave Limb Sounder over 2004–2018 period is dominated by the quasi‐biennial oscillation (QBO). We simulate the carbon monoxide variability over this period using the 2‐D Caltech/JPL chemistry‐transport model. The chemistry‐transport model includes the photochemical sources and sinks and transport driven by a stream function and eddy diffusivity derived from the assimilated winds of National Centers for Environmental Prediction Reanalysis 2. The results show good agreement between model and Microwave Limb Sounder observations. We also investigate the anomalous period 2015–2016, when the QBO winds deviated significantly from their climatological values. The model simulations could capture the QBO features in agreement with observations for the anomalous period.

Abstract Aerosol effects on convective clouds and associated precipitation constitute an important open-ended question in climate research. Previous studies have linked an increase in aerosol concentration to a delay in the onset of rain, invigorated clouds and stronger rain rates. Here, using observational data, we show that the aerosol effect on convective clouds shifts from invigoration to suppression with increasing aerosol optical depth. We explain this shift in trend (using a cloud model) 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 aerosol optical depth value that marks the shift between invigoration and suppression depends on the environmental thermodynamic conditions. These findings can aid in better parameterizing aerosol effects in climate models for the prediction of climate trends.

Abstract 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.

Abstract 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.

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.

The sensitivity of global precipitation to warming is largely governed by changes in atmospheric longwave radiation, a function of cloud cover. Here the authors show that tightening of the tropical circulation with warming drives a decrease in high cloud cover, resulting in higher precipitation changes.

Abstract Analyzing retrieval accuracy and precision is an important element of space‐based CO2 retrievals. However, this error analysis is sometimes challenging to perform rigorously because of the subtlety of Multivariate Statistics. To help address this issue, we revisit some fundamentals of Multivariate Statistics that help reveal the statistical essence of the associated error analysis. We show that the related statistical methodology is useful for revealing the intrinsic discrepancy and relation between the retrieval error for a nonzero‐variate CO2 state and that for a zero‐variate one. Our study suggests that the two scenarios essentially yield the same‐magnitude accuracy, while the latter scenario yields a better precision than the former. We also use this methodology to obtain a rigorous framework systematically and explore a broadly used approximate framework for analyzing CO2 retrieval errors. The approximate framework introduces errors due to an essential, but often forgotten, fact that a priori climatology in reality is never equal to the true state. Due to the nature of the problem considered, realistic numerical simulations that produce synthetic spectra may be more appropriate than remote sensing data for our specific exploration. As highlighted in our retrieval simulations, utilizing the approximate framework may not be universally satisfactory in assessing the accuracy and precision of Xco2 retrievals (with errors up to 0.17–0.28 ppm and 1.4–1.7 ppm, respectively, at SNR = 400). In situ measurements of CO2 are needed to further our understanding of this issue and related implications.

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–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 (λA); (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.

Metal compounds abundant on Early Earth are thought to play an important role in the origins of life. Certain iron-sulfur minerals for example, are proposed to have served as primitive metalloenzyme cofactors due to their ability to catalyze organic synthesis processes and facilitate electron transfer reactions. An inherent difficulty with studying the catalytic potential of many metal compounds is the wide range of data and parameters to consider when searching for individual minerals and ligands of interest. Detecting mineral-ligand pairs that are structurally analogous enables more relevant selections of data to study, since structural affinity is a key indicator of comparable catalytic function. However, current structure-oriented approaches tend to be subjective and localized, and do not quantify observations or compare them with other potential targets. Here, we present a mathematical approach that compares structural similarities between various minerals and ligands using molecular similarity metrics. We use an iterative substructure search in the crystal lattice, paired with benchmark structural similarity methods. This structural comparison may be considered as a first stage in a more advanced analysis tool that will include a range of chemical and physical factors when computing mineral-ligand similarity. This approach will seek relationships between the mineral and enzyme worlds, with applications to the origins of life, ecology, catalysis, and astrobiology.

When retrieving Aerosol Optical Depth (AOD) from passive satellite sensors, the vertical distribution of aerosols usually needs to be assumed, potentially causing uncertainties in the retrievals. In this study, we use the Moderate Resolution Spectroradiometer (MODIS) and Visible Infrared Imaging Radiometer Suite (VIIRS) sensors as examples to investigate the impact of aerosol vertical distribution on AOD retrievals. A series of sensitivity experiments was conducted using radiative transfer models with different aerosol profiles and surface conditions. Assuming a 0.2 AOD, we found that the AOD retrieval error is the most sensitive to the vertical distribution of absorbing aerosols; a −1 km error in aerosol scale height can lead to a ~30% AOD retrieval error. Moreover, for this aerosol type, ignoring the existence of the boundary layer can further result in a ~10% AOD retrieval error. The differences in the vertical distribution of scattering and absorbing aerosols within the same column may also cause −15% (scattering aerosols above absorbing aerosols) to 15% (scattering aerosols below absorbing aerosols) errors. Surface reflectance also plays an important role in affecting the AOD retrieval error, with higher errors over brighter surfaces in general. The physical mechanism associated with the AOD retrieval errors is also discussed. Finally, by replacing the default exponential profile with the observed aerosol vertical profile by a micro-pulse lidar at the Beijing-PKU site in the VIIRS retrieval algorithm, the retrieved AOD shows a much better agreement with surface observations, with the correlation coefficient increased from 0.63 to 0.83 and bias decreased from 0.15 to 0.03. Our study highlights the importance of aerosol vertical profile assumption in satellite AOD retrievals, and indicates that considering more realistic profiles can help reduce the uncertainties.