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NASA NTRS1996

Physical and Optical/Radiative Characteristics of Aerosol and Cloud Particles in Tropical Cirrus: Importance in Radiation Balance

Whether cirrus clouds heat or cool the Earth-atmosphere system depends on the relative importance of the cloud shortwave albedo effect and the cloud thermal greenhouse effect. Both are determined by the distribution of ice condensate with cloud particle size. The microphysics instrument package flown aboard the NASA DC-8 in TOGA/COARE included an ice crystal replicator, a 2D Greyscale Cloud Particle Probe and a Forward Scattering Spectrometer Aerosol Probe. In combination, the electro-optical instruments permitted particle size measurements between 0.5 micrometer and 2.6 millimeter diameter. Ice crystal replicas were used to validate signals from the electrooptical instruments. Both optical and scanning electron microscopy were utilized to analyze aerosol and ice particle replicas between 0.1 micrometer and several 100 micrometer diameter. In first approximation, the combined aerosol-cloud particle spectrum in several clouds followed a power law N alpha D(sup -2.5). Thus, large cloud particles carried most of the condensate mass, while small cloud and aerosol particles determined the surface area. The mechanism of formation of small particles is growth of (hygroscopic, possibly ocean-derived) aerosol particles along the Kohler curves. The concentration of small particles is higher and less variable in space and time, and their tropospheric residence time is longer, than those of large cloud particles because of lower sedimentation velocities. Small particles shift effective cloud particle radii to sizes much smaller than the mean diameter of the cloud particles. This causes an increase in shortwave reflectivity and IR emissivity, and a decrease in transmissivity. Occasionally, the cloud reflectivity increased with altitude (decreasing temperature) stronger than did cloud emissivity, yielding enhanced radiative cooling at higher altitudes. Thus, cirrus produced by deep convection in the tropics may be critical in controlling processes whereby energy from warm tropical oceans is injected to different levels in the atmosphere to subsequently influence not only tropical but mid-latitude climate.

Pueschel, R. F.↗

NASA NTRSDate not supplied

Atmospheric Escape Processes and Planetary Atmospheric Evolution: From Misconceptions to Challenges

The recent discoveries of telluric exoplanets in the habitable zone of different stars have led to questioning the nature of their atmosphere, which is required to determine their habitability. Atmospheric escape is one of the challenging problems to be solved: simply adapting what is currently observed in the solar system is doomed to fail due to the large variations in the conditions encountered around other stars. A better strategy is to evaluate the different processes that shaped planetary atmosphere and to evaluate their importance depending upon the stellar conditions. We reviewed the different escape mechanisms and their magnitude in function of different conditions [Gronoff et al. 2020]. This led us to discuss the importance of a magnetic field in protecting an atmosphere. The importance of the thermal escape, of polar wind, and of the transport of plasma within the magnetosphere are typically forgotten when claiming that magnetic fields are protecting planetary atmospheres and leading to their habitability. Overall, the habitability of a planet should not be claimed only on by its location in the habitable zone but also after careful analysis of the interaction between its atmosphere and its parent star . Gronoff, G., Arras, P., Baraka, S., Bell, J. M., Cessateur, G., Cohen, O., et al. ( 2020). Atmospheric Escape Processes and Planetary Atmospheric Evolution. Journal of Geophysical Research: Space Physics, 125, e2019JA027639. https://doi.org/10.1029/2019JA027639

G Gronoff↗

DOE OSTI2019

Effects of Sea Spray on Microphysics and Intensity of Deep Convective Clouds Under Strong Winds

Deep convective clouds similar to those arising in the tropical cyclone eyewall are simulated using a parcel model and 2–D slab symmetric cloud model with spectral bin microphysics (the Hebrew University Cloud Model). The size distribution of sea spray particles (SSPs) at cloud base is calculated using the Lagrangian–Eulerian bin microphysics model. The model describes the SSP production, advection, and formation of the size distribution of SSP in the hurricane atmospheric boundary layer at different strong wind speeds. The SSP distributions calculated by the Lagrangian–Eulerian bin microphysics model are used in the parcel model and the Hebrew University Cloud Model to investigate the microphysical and dynamical effects of SSP on clouds. The SSPs ascending in cloud updrafts dramatically increase the number concentration of cloud drops within a wide range of drop sizes. As a result, sea spray creates clouds with unique property combinations of both maritime and continental types. These clouds have droplet size distributions characterized by a high drop concentration and a low effective radius, as in continental clouds. At the same time, the presence of SSP of a few hundred microns in radii triggers intense rain just above the cloud base, which is typical of extreme maritime clouds. In the presence of large sea spray drops, the smallest cloud condensational nuclei, including the smallest SSP, are activated, giving rise to the permanent in–cloud nucleation of small droplets, which produce a high concentration of small ice crystals above the level of homogeneous freezing. We showed that the SSP substantially increased the maximum vertical velocity, cloud water content, and mass contents of ice particles. Here, the results are compared with available observed data.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Product distribution, kinetics, and aerosol formation from the OH oxidation of dimethyl sulfide under different RO 2 regimes

Abstract. The atmospheric oxidation of dimethyl sulfide (DMS) represents a major natural source of atmospheric sulfate aerosols. However, there remain large uncertainties in our understanding of the underlying chemistry that governs the product distribution and sulfate yield from DMS oxidation. Here, chamber experiments were conducted to simulate gas-phase OH-initiated oxidation of DMS under a range of reaction conditions. Most importantly, the bimolecular lifetime (τbi) of the peroxy radical CH3SCH2OO was varied over several orders of magnitude, enabling the examination of the role of peroxy radical isomerization reactions on product formation. An array of analytical instruments was used to measure nearly all sulfur-containing species in the reaction mixture, and results were compared with a near-explicit chemical mechanism. When relative humidity was low, “sulfur closure” was achieved under both high-NO (τbi<0.1 s) and low-NO (τbi>10 s) conditions, though product distributions were substantially different in the two cases. Under high-NO conditions, approximately half the product sulfur was in the particle phase, as methane sulfonic acid (MSA) and sulfate, with most of the remainder as SO2 (which in the atmosphere would eventually oxidize to sulfate or be lost to deposition). Under low-NO conditions, hydroperoxymethyl thioformate (HPMTF, HOOCH2SCHO), formed from CH3SCH2OO isomerization, dominates the sulfur budget over the course of the experiment, suppressing or delaying the formation of SO2 and particulate matter. The isomerization rate constant of CH3SCH2OO at 295 K is found to be 0.13±0.03 s−1, in broad agreement with other recent laboratory measurements. The rate constants for the OH oxidation of key first-generation oxidation products (HPMTF and methyl thioformate, MTF) were also determined (kOH+HPMTF=2.1×10-11 cm3 molec.−1 s−1, kOH+MTF=1.35×10-11 cm3 molec.−1 s−1). Product measurements agree reasonably well with mechanistic predictions in terms of total sulfur distribution and concentrations of most individual species, though the mechanism overpredicts sulfate and underpredicts MSA under high-NO conditions. Lastly, results from high-relative-humidity conditions suggest efficient heterogenous loss of at least some gas-phase products.

Ye, Qing (ORCID:0000000337978988)↗

NASA NTRS1997

Laboratory Evaluation and Application of Microwave Absorption Properties Under Simulated Conditions for Planetary Atmospheres

Radio absorptivity data for planetary atmospheres obtained from spacecraft radio occultation experiments and earth-based radio astronomical observations can be used to infer abundances of microwave absorbing constituents in those atmospheres, as long as reliable information regarding the microwave absorbing properties of potential constituents is available. The use of theoretically-derived microwave absorption properties for such atmospheric constituents, or using laboratory measurements of such properties under environmental conditions which are significantly different than those of the planetary atmosphere being studied, often leads to significant misinterpretation of available opacity data. Laboratory measurements completed under this grant (NAGW-533), have shown that the opacity from, SO2 under simulated Venus conditions is best described by a different lineshape than was previously used in theoretical predictions. The recognition of the need to make such laboratory measurements of simulated planetary atmospheres over a range of temperatures and pressures which correspond to the altitudes probed by both radio occultation experiments and radio astronomical observations, and over a range of frequencies which correspond to those used in both radio occultation experiments and radio astronomical observations, has led to the development of a facility at Georgia Tech which is capable of making such measurements. It has been the goal of this investigation to conduct such measurements and to apply the results to a wide range of planetary observations, both spacecraft and earth-based, in order to determine the identity and abundance profiles of constituents in those planetary atmospheres.

Steffes, Paul G.↗

NASA NTRS1965

The ionosphere.

Atmospheric ionization, discussing formation of different ionospheric regions

SOLAR ACTIVITY↗

DOE OSTI2017

Estimating Trends and Variation of Net Biome Productivity in India for 1980–2012 Using a Land Surface Model

In this paper we explore the trend in net biome productivity (NBP) over India for the period 1980–2012 and quantify the impact of different environmental factors, including atmospheric CO 2 concentrations ([CO 2 ]), land use and land cover change, climate, and nitrogen deposition on carbon fluxes using a land surface model, Integrated Science Assessment Model. Results show that terrestrial ecosystems of India have been a carbon sink for this period. Driven by a strong CO 2 fertilization effect, magnitude of NBP increased from 27.17 TgC/yr in the 1980s to 34.39 TgC/yr in the 1990s but decreased to 23.70 TgC/yr in the 2000s due to change in climate. Adoption of forest conservation, management, and reforestation policies in the past decade has promoted carbon sequestration in the ecosystems, but this effect has been offset by loss of carbon from ecosystems due to rising temperatures and decrease in precipitation.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

Air turbulence characteristics at multiple sites in and above the Amazon rainforest canopy

Atmospheric turbulence characteristics within and above rain forest canopies are investigated at several sites located in the Amazon region of Brazil. Turbulence data provided by bi- and three-dimensional sonic anemometers, which were deployed at heights ranging from near the forest floor to about 80 m, are analyzed to describe the principal features of atmospheric turbulence, sensible heat flux (H), and components of the turbulent kinetic energy (TKE) budget equation. The analyses focused on weak (WW) and strong (SW) wind conditions to achieve the research objectives of evaluating the turbulence structure above and below the rain forest canopy and estimating the degree of coupling between air layers above the forest and deep in the canopy. Turbulence statistical moments show that atmospheric eddies, generated above the canopy, hardly penetrate the region below 0.5h (h is the canopy height). Forest-atmosphere exchanges of heat differ depending on the observed wind regimes. Sensible heat fluxes decrease with canopy depth for SW conditions and are approximately constant with the height for WW above the canopy. Sensible heat flux profiles reveal a transition layer (around 0.6h) which sometimes exchanges heat with the upper and sometimes with the lower forest canopy, depending on time of day and weather conditions. TKE balance results show that during the daytime period in SW conditions the shear production is at least an order of magnitude greater than the buoyancy above the forest canopy. This turbulence, however, is practically all dissipated in the region above 0.5h. Thus, the air layer from the soil surface to 0.5h is largely decoupled from the upper part of the forest canopy. This feature of having the bottom of the canopy mostly decoupled from the air aloft in the dense and tall rain forest can exert control on the residence times and turbulent transport of plant-emitted gases out of the forest canopy.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

In-situ hydrogenation of bio-oil/bio-oil phenolic compounds with secondary alcohols over a synthesized mesoporous Ni/CeO 2 catalyst

Mesoporous ceria, which was synthesized under supercritical conditions, was found to be an effective support material of Ni catalyst for the in-situ hydrogenation of m-cresol (a representative compound of bio-oil) using secondary alcohols of 2-propanol (2-PrOH) and 2-butanol (2-BuOH) as a hydrogen source (H-donor) to produce 3-methylcyclohexanol, 3-methylcyclohexene, and methylcyclohexane under a H2 gas-free atmosphere. The activities of different metal catalysts (Ni, Cu, and Co) for the in-situ hydrogenation of m-cresol were examined using 2-PrOH as a H-donor. Total and effective conversion of m-cresol achieved only over Ni/CeO 2 because of its fair catalytic properties, as determined by N2 adsorption-desorption, hydrogen temperature-programmed reduction, ammonia temperature-programmed desorption, X-ray diffraction, and transmission electron microscopy. The dependence of Ni/CeO2 performance on the reaction time (4-6 h) and Ni loading (3-9 wt%) was examined from the in-situ hydrogenation of m-cresol with 2-PrOH. The deactivation test of Ni/CeO 2 was performed by reusing the spent catalyst, which was then regenerated through successive oxidation and reduction, several times in the m-cresol transformation employing 2-PrOH as a H-donor. In addition to m-cresol, other phenolic model compounds of bio-oil, such as anisole, phenol, and guaiacol, were also treated by in-situ hydrogenation with 2-PrOH over Ni/CeO 2 . Although this catalyst was effective for phenol and guaiacol transformation, it was relatively ineffective for anisole conversion. The in-situ hydrogenation of crude bio-oil with 2-PrOH and 2-BuOH was accomplished over the Ni/CeO 2 catalyst, resulting in a refined bio-oil with a 37.5-38.9% lower oxygen content and a high heating value (HHV) of up to 25 MJ/kg.

09 BIOMASS FUELS↗

DOE OSTI2025

Influence of temperature, oxygen partial pressure, and microstructure on the high-temperature oxidation behavior of the SiC Layer of TRISO particles

Tristructural isotropic (TRISO)-coated fuel particles are designed for use in high-temperature gas-cooled nuclear reactors, featuring a structural SiC layer that may be exposed to oxygen-rich environments over 1000 °C. Surrogate TRISO particles were tested in 0.2–20 kPa O 2 atmospheres to observe the differences in oxidation behavior. Oxide growth mechanisms remained consistent from 1200–1600 °C for each P O$_2$ , with activation energies of 228 ± 7 kJ/mol for 20 kPa O 2 and 188 ± 8 kJ/mol for 0.2 kPa O 2 . At 1600 °C, kinetic analysis revealed a change in oxide growth mechanisms between 0.2 and 6 kPa O2. In 0.2 kPa O 2 , oxidation produced raised oxide nodules on pockets with nanocrystalline SiC. Oxidation mechanisms were determined using Atom probe tomography. Active SiC oxidation occurred in C-rich grain boundaries with low P O$_2$ , leading to SiO 2 buildup in porous nodules. Here, this phenomenon was not observed at any temperature in 20 kPa O 2 environments.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2017

Uncertainty propagation through an aeroelastic wind turbine model using polynomial surrogates

Polynomial surrogates are used to characterize the energy production and lifetime equivalent fatigue loads for different components of the DTU 10 MW reference wind turbine under realistic atmospheric conditions. The variability caused by different turbulent inflow fields are captured by creating independent surrogates for the mean and standard deviation of each output with respect to the inflow realizations. A global sensitivity analysis shows that the turbulent inflow realization has a bigger impact on the total distribution of equivalent fatigue loads than the shear coefficient or yaw miss-alignment. The methodology presented extends the deterministic power and thrust coefficient curves to uncertainty models and adds new variables like damage equivalent fatigue loads in different components of the turbine. These surrogate models can then be implemented inside other work-flows such as: estimation of the uncertainty in annual energy production due to wind resource variability and/or robust wind power plant layout optimization. It can be concluded that it is possible to capture the global behavior of a modern wind turbine and its uncertainty under realistic inflow conditions using polynomial response surfaces. In conclusion, the surrogates are a way to obtain power and load estimation under site specific characteristics without sharing the proprietary aeroelastic design.

17 WIND ENERGY↗

DOE OSTI2017

Cross-biome assessment of gross soil nitrogen cycling in California ecosystems

Microbial transformations of nitrogen (N) largely determine whether N is retained in ecosystems via net primary productivity or lost via gaseous emissions and leaching. The controls on soil N cycling are often studied at single locales, making it difficult to predict N cycling at regional to global scales. We hypothesized that contemporary soil properties exhibit consistent relationships with instantaneous gross N cycling rates across diverse biomes that create a continuum in these properties. We measured ex situ gross N cycling rates and soil properties at 33 study sites representing five biome classifications in California including deserts, grasslands, shrublands, forest, and wetlands. Desert soils had significantly lower total N, organic carbon (C), microbial biomass N, and soil moisture as well as higher pH than all other biomes, whereas forests and wetlands had significantly lower soil nitrate ($NO_3^-$) concentrations (P < 0.001 for all). Gross mineralization rates were best predicted by the combination of soil moisture and soil C:N ratios (R 2 = 0.46), which exerted positive and negative controls, respectively. Grasslands exhibited marginally higher gross mineralization than all other biomes, whereas deserts had the lowest rates due to low soil moisture (P = 0.09). Gross nitrification rates were positively correlated to soil $NO_3^-$ concentrations (R 2 = 0.34) and negatively correlated to soil C:N ratios (R 2 = 0.31). The negative relationship between gross nitrification and soil C:N ratios was driven by forest soils, which had significantly higher C:N ratios and lower gross nitrification than all other biomes (P < 0.05). Dissimilatory $NO_3^-$- reduction to $NH_4^+$ (DNRA) occurred in soils from all biomes. The strong positive correlation between DNRA rates and soil $NO_3^-$ (R 2 = 0.41) suggests $NO_3^-$ limitation of DNRA. Predictable patterns in gross N cycling across biomes in California suggest that contemporary soil properties are important drivers of instantaneous soil N cycling rates that integrate over differences in vegetation type, atmospheric N deposition rates, and local climate.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Gas-Phase Temperature Mapping of Evaporating Microdroplets

Evaporation is a ubiquitous and complex phenomenon of importance to many natural and industrial systems. Evaporation occurs when molecules near the free interface overcome intermolecular attractions with the bulk liquid. As molecules escape the liquid phase, heat is removed, causing evaporative cooling. The influence of evaporative cooling on inducing a temperature difference with the surrounding atmosphere as well as within the liquid is poorly understood. Here, we develop a technique to overcome past difficulties encountered during the study of heterogeneous droplet evaporation by coupling a piezo-driven droplet generation mechanism to a controlled micro-thermocouple to probe microdroplet evaporation. The technique allowed us to probe the gas-phase temperature distribution using a micro-thermocouple (50 μm) in the vicinity of the liquid–vapor interface with high spatial (±10 μm) and temporal (±100 ms) resolution. We experimentally map the temperature gradient formed surrounding sessile water droplets having varying curvature dictated by the apparent advancing contact angle (100° ≲ θ ≲ 165°). The experiments were carried out at temperatures below and above ambient for a range of fixed droplet radii (130 μm ≲ R ≲ 330 μm). Our results provide a primary validation of the centuries-old theoretical framework underpinning heterogeneous droplet evaporation mediated by the working fluid, substrate, and gas thermophysical properties, droplet apparent contact angle, and droplet size. We show that microscale droplets residing on low-thermal-conductivity substrates such as glass absorb up to 8× more heat from the surrounding gas compared to droplets residing on high-thermal-conductivity substrates such as copper. Finally, our work not only develops an experimental understanding of the heat transfer mechanisms governing droplet evaporation but also presents a powerful platform for the study and characterization of liquid–vapor transport at curved interfaces wetting and nonwetting advanced functional surfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2018

Locally Enhanced Aerosols Over a Shipping Lane Produce Convective Invigoration but Weak Overall Indirect Effects in Cloud-Resolving Simulations

The effect of aerosol emissions from an active shipping lane in the Indian Ocean is simulated using an idealized framework in a cloud-resolving model. Increased aerosol concentrations over the modeled shipping lane lead to increased cloud droplet number, cloud liquid mass, ice hydrometeor mass, and simulated radar reflectivity. The invigoration of deep convection induces mesoscale uplift and increased precipitation over the shipping lane. A predicted increase in the prevalence of both strong updrafts and radar echoes aloft is suggestive of enhanced lightning activity over the shipping lane, as observed in a recent study. Cloud radiative effects, both shortwave and longwave, are intensified over the shipping lane, but the change in the net radiative flux at top of atmosphere is not significantly different from zero.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Tropical Cirrus in Global Storm-Resolving Models. Part II: Cirrus Life Cycle and Top-of-Atmosphere Radiative Fluxes

Cirrus clouds of various thicknesses and radiative characteristics extend over much of the tropics, especially around deep convection. They are difficult to observe due to their high altitude and sometimes small optical depths. They are also difficult to simulate in conventional global climate models, which have coarse grid spacings and simplified parameterizations of deep convection and cirrus formation. We investigate the representation of tropical cirrus in global storm-resolving models (GSRMs), which have higher spatial resolution and explicit convection and could more accurately represent cirrus cloud processes. This study uses GSRMs from the DYnamics of the Atmospheric general circulation Modeled On Non-hydrostatic Domains (DYAMOND) project. The aggregate life cycle of tropical cirrus is analyzed using joint albedo and outgoing longwave radiation (OLR) histograms to assess the fidelity of models in capturing the observed cirrus cloud populations over representative tropical ocean and land regions. The proportions of optically-thick deep convection, anvils, and cirrus vary across models and are portrayed in the vertical distribution of cloud cover and top-of-atmosphere radiative fluxes. Model differences in cirrus populations, likely driven by subgrid processes such as ice microphysics, dominate over regional differences between convectively-active tropical land and ocean locations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

The Potential Benefits of Handling Mixture Statistics via a Bi-Gaussian EnKF: Tests With All-Sky Satellite Infrared Radiances

The meteorological characteristics of cloudy atmospheric columns can be very different from their clear counterparts. Thus, when a forecast ensemble is uncertain about the presence/absence of clouds at a specific atmospheric column (i.e., some members are clear while others are cloudy), that column's ensemble statistics will contain a mixture of clear and cloudy statistics. Such mixtures are inconsistent with the ensemble data assimilation algorithms currently used in numerical weather prediction. Hence, ensemble data assimilation algorithms that can handle such mixtures can potentially outperform currently used algorithms. In this study, we demonstrate the potential benefits of addressing such mixtures through a bi-Gaussian extension of the ensemble Kalman filter (BGEnKF). The BGEnKF is compared against the commonly used ensemble Kalman filter (EnKF) using perfect model observing system simulated experiments (OSSEs) with a realistic weather model (the Weather Research and Forecast model). Synthetic all-sky infrared radiance observations are assimilated in this study. In these OSSEs, the BGEnKF outperforms the EnKF in terms of the horizontal wind components, temperature, specific humidity, and simulated upper tropospheric water vapor channel infrared brightness temperatures. This study is one of the first to demonstrate the potential of a Gaussian mixture model EnKF with a realistic weather model. Our results thus motivate future research toward improving numerical Earth system predictions though explicitly handling mixture statistics.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Increased Asian Sulfate Aerosol Emissions Remarkably Enhance Sahel Summer Precipitation

Observational evidence shows that Sahel summer precipitation has experienced a considerable increase since the 1980s, coinciding with significant diverging trends of increased sulfate emissions in Asia and decreased emissions in Europe (dipole pattern of aerosols between Asia and Europe). The decrease in European sulfate aerosols has substantial effects on the Sahel summer precipitation increase, but the corresponding effect of increased Asian sulfate is unknown. Multi-model simulations in the Precipitation Driver and Response Model Intercomparison Project (PDRMIP) show, compared to decreased European aerosols, that increased Asian aerosols similarly enhance the Sahel summer precipitation but with different large-scale atmospheric circulation changes. Further analysis of the Sixth Coupled Model Intercomparison Project (CMIP6) simulations under historical attribution and various emission scenarios reinforces the results about the climate impacts of anthropogenic aerosols and suggests that in future scenarios with strong international cooperation and rapid climate mitigations (SSP2-45), the Sahel drought will be intensified likely due to the decline in Asian aerosol emissions. Our results suggest that Asian anthropogenic aerosols are likely a non-negligible driver of the recent recovery in Sahel precipitation amounts

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Arctic Ocean annual high in ${{\boldsymbol{p}}}_{{{\bf{CO}}}_{{\bf{2}}}}$ could shift from winter to summer

Long-term stress on marine organisms from ocean acidification will differ between seasons. As atmospheric carbon dioxide (CO 2 ) increases, so do seasonal variations of ocean CO 2 partial pressure (p co 2 ), causing summer and winter long-term trends to diverge. Trends may be further influenced by an unexplored factor—changes in the seasonal timing of p co 2 . In Arctic Ocean surface waters, the observed timing is typified by a winter high and summer low because biological effects dominate thermal effects. Here we show that 27 Earth system models simulate similar timing under historical forcing but generally project that the summer low, relative to the annual mean, eventually becomes a high across much of the Arctic Ocean under mid-to-high-level CO 2 emissions scenarios. Often the greater increase in summer p co 2 , although gradual, abruptly inverses the chronological order of the annual high and low, a phenomenon not previously seen in climate-related variables. The main cause is the large summer sea surface warming from earlier retreat of seasonal sea ice. Warming and changes in other drivers enhance this century’s increase in extreme summer p co 2 by 29 ± 9 per cent compared with no change in driver seasonalities. Thus the timing change worsens summer ocean acidification, which in turn may lower the tolerance of endemic marine organisms to increasing summer temperatures.

54 ENVIRONMENTAL SCIENCES↗