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Solar radiation and geological processes over the first few million years of Earth’s history, followed soon thereafter by the origin of life, steered our planet towards an evolutionary trajectory of long-lived habitability that ultimately enabled the emergence of complex life. We review the most important conditions and feedbacks over the first 2 billion years of this trajectory, which perhaps represent the best analogue for other habitable worlds in the galaxy. Crucial aspects included: (1) the redox state and volatile content of Earth’s building blocks, which determined the longevity of the magma ocean and its ability to degas H 2 O and other greenhouse gases, in particular CO 2 , allowing the condensation of a water ocean; (2) the chemical properties of the resulting degassed mantle, including oxygen fugacity, which would have not only affected its physical properties and thus its ability to recycle volatiles and nutrients via plate tectonics, but also contributed to the timescale of atmospheric oxygenation; (3) the emergence of life, in particular the origin of autotrophy, biological N 2 fixation, and oxygenic photosynthesis, which accelerated sluggish abiotic processes of transferring some volatiles back into the lithosphere; (4) strong stellar UV radiation on the early Earth, which may have eroded significant amounts of atmospheric volatiles, depending on atmospheric CO 2 /N 2 ratios and thus impacted the redox state of the mantle as well as the timing of life’s origin; and (5) evidence of strong photochemical effects on Earth’s sulfur cycle, preserved in the form of mass-independent sulfur isotope fractionation, and potentially linked to fractionation in organic carbon isotopes. The early Earth presents itself as an exoplanet analogue that can be explored through the existing rock record, allowing us to identify atmospheric signatures diagnostic of biological metabolisms that may be detectable on other inhabited planets with next-generation telescopes. We conclude that investigating the development of habitable conditions on terrestrial planets, an inherently complex problem, requires multi-disciplinary collaboration and creative solutions.

The formation and aging of organic aerosols (OA) proceed through multiple steps of chemical reaction and mass transport in the gas and particle phases, which is challenging for the interpretation of field measurements and laboratory experiments as well as accurate representation of OA evolution in atmospheric aerosol models. Based on data from over 30 000 compounds, we show that organic compounds with a wide variety of functional groups fall into molecular corridors, characterized by a tight inverse correlation between molar mass and volatility. We developed parameterizations to predict the saturation mass concentration of organic compounds containing oxygen, nitrogen, and sulfur from the elemental composition that can be measured by soft-ionization high-resolution mass spectrometry. Field measurement data from new particle formation events, biomass burning, cloud/fog processing, and indoor environments were mapped into molecular corridors to characterize the chemical nature of the observed OA components. We found that less-oxidized indoor OA are constrained to a corridor of low molar mass and high volatility, whereas highly oxygenated compounds in atmospheric water extend to high molar mass and low volatility. Among the nitrogen- and sulfur-containing compounds identified in atmospheric aerosols, amines tend to exhibit low molar mass and high volatility, whereas organonitrates and organosulfates follow high O : C corridors extending to high molar mass and low volatility. We suggest that the consideration of molar mass and molecular corridors can help to constrain volatility and particle-phase state in the modeling of OA particularly for nitrogen- and sulfur-containing compounds.

Reconciling the geology of Mars with models of atmospheric evolution remains a major challenge. Martian geology is characterized by past evidence for episodic surface liquid water, and geochemistry indicating a slow and intermittent transition from wetter to drier and more oxidizing surface conditions. Here we present a model that incorporates randomized injection of reducing greenhouse gases and oxidation due to hydrogen escape to investigate the conditions responsible for these diverse observations. We find that Mars could have transitioned repeatedly from reducing (hydrogen-rich) to oxidizing (oxygen-rich) atmospheric conditions in its early history. Our model predicts a generally cold early Mars, with mean annual temperatures below 240 K. If peak reducing-gas release rates and background carbon dioxide levels are high enough, it nonetheless exhibits episodic warm intervals sufficient to degrade crater walls, form valley networks and create other fluvial/lacustrine features. Our model also predicts transient build-up of atmospheric oxygen, which can help explain the occurrence of oxidized mineral species such as manganese oxides at Gale Crater. We suggest that the apparent Noachian–Hesperian transition from phyllosilicate deposition to sulfate deposition around 3.5 billion years ago can be explained as a combined outcome of increasing planetary oxidation, decreasing groundwater availability and a waning bolide impactor flux, which dramatically slowed the remobilization and thermochemical destruction of surface sulfates. Ultimately, rapid and repeated variations in Mars’s early climate and surface chemistry would have presented both challenges and opportunities for any emergent microbial life. Mars’s early climate and surface chemistry varied between a generally cold, oxidizing environment and warmer, more reducing conditions, according to a model of atmospheric evolution driven by stochastic, random injection of greenhouse gases.

The next step on the path toward another Earth is to find atmospheres similar to those of Earth and Venus—high–molecular-weight (secondary) atmospheres—on rocky exoplanets. Many rocky exoplanets are born with thick (>10 kbar) H₂-dominated atmospheres but subsequently lose their H₂; this process has no known Solar System analog. We study the consequences of early loss of a thick H₂ atmosphere for subsequent occurrence of a high–molecular-weight atmosphere using a simple model of atmosphere evolution (including atmosphere loss to space, magma ocean crystallization, and volcanic outgassing). We also calculate atmosphere survival for rocky worlds that start with no H₂. Our results imply that most rocky exoplanets orbiting closer to their star than the habitable zone that were formed with thick H₂-dominated atmospheres lack high–molecularweight atmospheres today. During early magma ocean crystallization, high–molecular-weight species usually do not form long-lived high–molecular-weight atmospheres; instead, they are lost to space alongside H₂. This early volatile depletion also makes it more difficult for later volcanic outgassing to revive the atmosphere. However, atmospheres should persist on worlds that start with abundant volatiles (for example, water worlds). Our results imply that in order to find high–molecular-weight atmospheres on warm exoplanets orbiting M-stars, we should target worlds that formed H₂-poor, that have anomalously large radii, or that orbit less active stars.

Earth's penultimate icehouse period, the late Paleozoic ice age (LPIA), was a time of dynamic glaciation and repeated ecosystem perturbation, which was under conditions of substantial variability in atmospheric pCO2 and O2. Improved constraints on the evolution of atmosphericpCO2 and O2/CO2 ratios during the LPIA and its subsequent demise to permanent greenhouse conditions are crucial for better understanding the nature of linkages between atmospheric composition, climate, and ecosystem perturbation during this time. We present a new and age-recalibrated pCO2 reconstruction for a 40 Myr interval (∼313 to 273 Ma) of the late Paleozoic that (1) confirms a previously hypothesized strongCO2–glaciation linkage, (2) documents synchroneity between major pCO2 and O2/CO2 changes and compositional turnovers in terrestrial and marine ecosystems, (3) lends support for a modeled progressive decrease in the CO2 threshold for initiation of continental ice sheets during the LPIA, and (4) indicates a likely role of CO2 and O2/CO2 thresholds in floral ecologic turnovers. Modeling of the relative role of CO2 sinks and sources active during the LPIA and its demise on steady-state pCO2 using an intermediate-complexity climate–carbon cycle model (GEOCLIM) and comparison to the new multi-proxy CO2 record provides new insight into the relative influences of the uplift of the Central Pangean Mountains, intensifying aridification, and increasing mafic rock to granite rock ratio of outcropping rocks on the global efficiency of CO2 consumption and secular change in steady-state pCO2 through the late Paleozoic.

Biomass burning is a major source of atmospheric brown carbon (BrC), and through its absorption of UV/VIS radiation, it can play an important role in the planetary radiative balance and atmospheric photochemistry. The considerable uncertainty of BrC impacts is associated with its poorly constrained sources, transformations, and atmospheric lifetime. Here we report laboratory experiments that examined changes in the optical properties of the water-soluble (WS) BrC fraction of laboratory-generated biomass burning particles from hardwood pyrolysis. Effects of direct UVB photolysis and OH oxidation in the aqueous phase on molecular-weight-separated BrC were studied. Results indicated that the majority of low-molecular-weight (MW) BrC (<400 Da) was rapidly photobleached by both direct photolysis and OH oxidation on an atmospheric timescale of approximately 1 h. High MW BrC (≥400 Da) underwent initial photoenhancement up to ∼15 h, followed by slow photobleaching over ∼10 h. The laboratory experiments were supported by observations from ambient BrC samples that were collected during the fire seasons in Greece. These samples, containing freshly emitted to aged biomass burning aerosol, were analyzed for both water- and methanol-soluble BrC. Consistent with the laboratory experiments, high-MW BrC dominated the total light absorption at 365 nm for both methanol and water-soluble fractions of ambient samples with atmospheric transport times of 1 to 68 h. These ambient observations indicate that overall, biomass burning BrC across all molecular weights has an atmospheric lifetime of 15 to 28 h, consistent with estimates from previous field studies – although the BrC associated with the high-MW fraction remains relatively stable and is responsible for light absorption properties of BrC throughout most of its atmospheric lifetime. For ambient samples of aged (>10 h) biomass burning emissions, poor linear correlations were found between light absorptivity and levoglucosan, consistent with other studies suggesting a short atmospheric lifetime for levoglucosan. However, a much stronger correlation between light absorptivity and total hydrous sugars was observed, suggesting that they may serve as more robust tracers for aged biomass burning emissions. Overall, the results from this study suggest that robust model estimates of BrC radiative impacts require consideration of the atmospheric aging of BrC and the stability of high-MW BrC.

Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework describing the atmospheric evolution of OA that is constrained by high-time-resolution measurements of its composition, volatility, and oxidation state. OA and OA precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. Our model framework captures the dynamic aging behavior observed in both the atmosphere and laboratory: It can serve as a basis for improving parameterizations in regional and global models.

Wind blowing over sand on Earth produces decimeter-wavelength ripples and hundred-meter— to kilometer-wavelength dunes: bedforms of two distinct size modes. Observations from the Mars Science Laboratory Curiosity rover and the Mars Reconnaissance Orbiter reveal that Mars hosts a third stable wind-driven bedform, with meter-scale wavelengths. These bedforms are spatially uniform in size and typically have asymmetric profiles with angle-of-repose lee slopes and sinuous crest lines, making them unlike terrestrial wind ripples. Rather, these structures resemble fluid-drag ripples, which on Earth include water-worked current ripples, but on Mars instead form by wind because of the higher kinematic viscosity of the low-density atmosphere. A reevaluation of the wind-deposited strata in the Burns formation (about 3.7 billion years old or younger) identifies potential wind-drag ripple stratification formed under a thin atmosphere.

Early Mars climate research has well-defined goals (MEPAG 2018 ). Achieving these goals requires geologists and climate modelers to coordinate. Coordination is easier if results are expressed in terms of well-defined parameters. Key parameters include the following quantitative geologic constraints. (1) Cumulative post-3.4 Ga precipitation-sourced water runoff in some places exceeded 1 km column. (2) There is no single Early Mars climate problem: the traces of ≥2 river-forming periods are seen. Relative to rivers that formed earlier in Mars history, rivers that formed later in Mars history are found preferentially at lower elevations, and show a stronger dependence on latitude. (3) The duration of the longest individual river-forming climate was > ( 10 2 – 10 3 ) yr , based on paleolake hydrology. (4) Peak runoff production was > 0.1 mm / hr . However, (5) peak runoff production was intermittent, sustained (in a given catchment) for only <10% of the duration of river-forming climates. (6) The cumulative number of wet years during the valley-network-forming period was > 10 5 yr . (7) Post-Noachian light-toned, layered sedimentary rocks took > 10 7 yr to accumulate. However, (8) an “average” place on Mars saw water for < 10 7 yr after the Noachian, suggesting that the river-forming climates were interspersed with long globally-dry intervals. (9) Geologic proxies for Early Mars atmospheric pressure indicate pressure was not less than 0.012 bar but not much more than 1 bar. A truth table of these geologic constraints versus currently published climate models shows that the late persistence of river-forming climates, combined with the long duration of individual lake-forming climates, is a challenge for most models.

With the Arctic rapidly changing, the needs to observe, understand, and model the changes are essential. To support these needs, an annual cycle of observations of atmospheric properties, processes, and interactions were made while drifting with the sea ice across the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition from October 2019 to September 2020. An international team designed and implemented the comprehensive program to document and characterize all aspects of the Arctic atmospheric system in unprecedented detail, using a variety of approaches, and across multiple scales. These measurements were coordinated with other observational teams to explore cross-cutting and coupled interactions with the Arctic Ocean, sea ice, and ecosystem through a variety of physical and biogeochemical processes. This overview outlines the breadth and complexity of the atmospheric research program, which was organized into 4 subgroups: atmospheric state, clouds and precipitation, gases and aerosols, and energy budgets. Atmospheric variability over the annual cycle revealed important influences from a persistent large-scale winter circulation pattern, leading to some storms with pressure and winds that were outside the interquartile range of past conditions suggested by long-term reanalysis. Similarly, the MOSAiC location was warmer and wetter in summer than the reanalysis climatology, in part due to its close proximity to the sea ice edge. The comprehensiveness of the observational program for characterizing and analyzing atmospheric phenomena is demonstrated via a winter case study examining air mass transitions and a summer case study examining vertical atmospheric evolution. Overall, the MOSAiC atmospheric program successfully met its objectives and was the most comprehensive atmospheric measurement program to date conducted over the Arctic sea ice. The obtained data will support a broad range of coupled-system scientific research and provide an important foundation for advancing multiscale modeling capabilities in the Arctic.