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The goal of the Sea2Cloud project is to study the interplay between surface ocean biogeochemical and physical properties, fluxes to the atmosphere, and ultimately their impact on cloud formation under minimal direct anthropogenic influence. Here we present an interdisciplinary approach, combining atmospheric physics and chemistry with marine biogeochemistry, during a voyage between 41° and 47°S in March 2020. In parallel to ambient measurements of atmospheric composition and seawater biogeochemical properties, we describe semicontrolled experiments to characterize nascent sea spray properties and nucleation from gas-phase biogenic emissions. The experimental framework for studying the impact of the predicted evolution of ozone concentration in the Southern Hemisphere is also detailed. After describing the experimental strategy, we present the oceanic and meteorological context including provisional results on atmospheric thermodynamics, composition, and flux measurements. In situ measurements and flux studies were carried out on different biological communities by sampling surface seawater from subantarctic, subtropical, and frontal water masses. Air–Sea-Interface Tanks (ASIT) were used to quantify biogenic emissions of trace gases under realistic environmental conditions, with nucleation observed in association with biogenic seawater emissions. Sea spray continuously generated produced sea spray fluxes of 34% of organic matter by mass, of which 4% particles had fluorescent properties, and which size distribution resembled the one found in clean sectors of the Southern Ocean. The goal of Sea2Cloud is to generate realistic parameterizations of emission flux dependences of trace gases and nucleation precursors, sea spray, cloud condensation nuclei, and ice nuclei using seawater biogeochemistry, for implementation in regional atmospheric models. This research received funding from the European Research Council (ERC) under the Horizon 2020 research and innovation programme (Grant Agreement 771369), the Centre National des Etudes Spatiales (CNES), and was supported by NIWA SSIF funding to the Ocean-Climate Interactions, and Flows and Productivity Programmes. The Sea2Cloud project is endorsed by SOLAS. We acknowledge the support and expertise of the Officers and Crew of the R/V Tangaroa and NIWA Vessel Services. PJD and KAM acknowledge the U.S. National Science Foundation Grant AGS1660486, and KAM was additionally supported by an NSF Graduate Research Fellowship under Grant 006784. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the author(s) and do not necessarily reflect the views of the National Science Foundation. 27 pags. 17 figs. -- All atmospheric and ocean datasets are accessible at https://sea2cloud. data-terra.org/en/catalogue/. -- This paper is dedicated to Mike Harvey, who played a leading role in the Sea2Cloud campaign and whose scientific contribution and collaboration in this and other research will be sadly missed. Peer reviewed

Long-term changes in the life history and behaviour of seabirds during the non-breeding season can reflect shifts in environmental conditions. However, long-term marine studies are scarce, particularly on southern hemisphere seabirds. Here, we used moult scores from 86 Brown Skuas (Stercorarius antarcticus lonnbergi), a large predatory seabird breeding on the Chatham Islands, Aotearoa/New Zealand to model both the timing and duration of primary feather moult. In addition, we analysed stable isotope values (δ13C and δ15N) from 62 modern (2014–16) and ten museum tail feathers. These data provide insights into the non-breeding behaviour of Brown Skua. Interestingly, our results show that the primary feather moult occurred prior to birds departing the colony, starting on average on 2 January ± 5 days (SE). The average start of primary feather moult occurred five days prior to the end of breeding (7 January ± 10 days (SD)) and 42 days before the birds departed the colony (13 February ± 11 days (SD)). The average duration of primary feather moult was 189 ± 14 days (SE). Importantly, low δ13C values in four females suggested that tail feather moult might also occur while skuas are at the colony. There was no difference in tail feather δ13C and δ15N values between any pairwise comparison of modern and museum years. However, values of δ15N from tail feathers sampled in 2014 were different from those sampled in 2015 and 2016. This large annual variation in δ15N values from tail feathers over such a short period makes long-term comparisons difficult to interpret, particularly between years with low sample sizes. While the stable isotope analyses of tail feathers are informative, we recommend future studies of skuas sample the primary coverts rather than tail feathers.

To limit global warming to 1.5 °C, vast amounts of CO2 will have to be removed from the atmosphere via Carbon Dioxide Removal (CDR). Enhancing the CO2 sequestration of ecosystems will require not just one approach but a portfolio of CDR options, including so-called nature-based approaches alongside CDR options that are perceived as more technical. Creating a CDR “supply curve” would however imply that all carbon removals are considered to be perfect substitutes. The various co-benefits of nature-based CDR approaches militate against this. We discuss this aspect of nature-based solutions in connection with the enhancement of blue carbon ecosystems (BCE) such as mangrove or seagrass habitats. Enhancing BCEs can indeed contribute to CO2 sequestration, but the value of their carbon storage is low compared to the overall contribution of their ecosystem services to wealth. Furthermore, their property rights are often unclear, i.e. not comprehensively defined or not enforced. Hence, payment schemes that only compensate BCE carbon sequestration could create tradeoffs at the expense of other important, often local, ecosystem services and might not result in socially optimal outcomes. Accordingly, one chance for preserving and restoring BCEs lies in the consideration of all services in potential compensation schemes for local communities. Also, local contexts, management structures, and benefit-sharing rules are crucial factors to be taken into account when setting up international payment schemes to support the use of BCEs and other nature- or ecosystem-based CDR. However, regarding these options as the only hope of achieving more CDR will very probably not bring about the desired outcome, either for climate mitigation or for ecosystem preservation. Unhalted degradation, in turn, will make matters worse due to the large amounts of stored carbon that would be released. Hence, countries committed to climate mitigation in line with the Paris targets should not hide behind vague pledges to enhance natural sinks for removing atmospheric CO2 but commit to scaling up engineered CDR.

The potential biogeochemical and ecological impacts of ocean alkalinity enhancement were tested in a 5-weeks mesocosm experiment conducted in the subtropical, oligotrophic waters off Gran Canaria in September/October 2021. In the nine mesocosms, each with a volume of about 10 m3 inhabiting a natural plankton community, alkalinity enhancement was achieved through addition of a mix of sodium bicarbonate and sodium carbonate, simulating CO2-equilibrated alkalinization in a gradient from control up to twice the natural alkalinity. The response of the enclosed plankton community to the alkalinity addition was monitored in over 50 parameters which were sampled or measured in situ daily or every second day. In addition to the mesocosm experiment, a series of side experiments were conducted, focusing on individual aspects of mineral dissolution, secondary precipitation and biological responses at the primary producer level. This campaign, in which 47 scientists from 6 nations participated, generated the most comprehensive data set collected so far on the ecological and biogeochemical impacts of ocean alkalinity enhancement.

Detailed geochemical and mineralogical insights into some of the richest rare earth elements and yttrium (REY)-containing bioapatites from ocean-floor sediments have been provided by combining laser ablation inductively coupled plasma diffraction analysis, and Ce L3-edge high energy-resolution X-ray absorption near edge structure (HR-XANES) spectroscopy. Bioapatites at 1.94 and 4.70 m below the seafloor (mbsf) of the Clarion-Clipperton Zone (CCZ) of the Pacific Ocean have 26,600 (RSD = 15.7%, n = 20) and 30,300 (RSD = 14.6%, n = 10) mg/kg (mg/kg) total REY, respectively, and bioapatites at 2.28 and 6.95 mbsf of the Peru Basin have 15,500 (RSD = 15.6%, n = 20) and 15,700 (RSD = 17.8%, n = 29) mg/kg total REY, respectively. All bioapatite specimens have a variety of isomorphic substitutions in all atomic positions of the crystallographic structure. The average crystallochemical formula of bioapatites at 6.95 mbsf of the Peru Basin is [(PO4)2.71(SiO4)0.04(CO3,SO4)0.25][Ca4.57Na0.29Y0.04][F0.87Cl0.21]. All other substituents are below 0.04 atoms per formula unit. HR-XANES provides the first direct evidence for trivalent Ce in sediment apatites. The strong negative geochemical anomaly of Ce in fossil bioapatites is well explained by the occurrence of four valent Ce-MnO2 and CeO2 within the sediment and in seafloor ferromanganese nodules.