ALBERT

Description: Acetone is one of the most abundant oxygenated volatile organic compounds (VOCs) in the atmosphere. The oceans impose a strong control on atmospheric acetone, yet the oceanic fluxes of acetone remain poorly constrained. In this work, the global budget of acetone is evaluated using two global models: CAM‐chem and GEOS‐Chem. CAM‐chem uses an online air‐sea exchange framework to calculate the bidirectional oceanic acetone fluxes, which is coupled to a data‐oriented machine‐learning approach. The machine‐learning algorithm is trained using a global suite of seawater acetone measurements. GEOS‐Chem uses a fixed surface seawater concentration of acetone to calculate the oceanic fluxes. Both model simulations are compared to airborne observations from a recent global‐scale, multiseasonal campaign, the NASA Atmospheric Tomography Mission (ATom). We find that both CAM‐chem and GEOS‐Chem capture the measured acetone vertical distributions in the remote atmosphere reasonably well. The combined observational and modeling analysis suggests that (i) the ocean strongly regulates the atmospheric budget of acetone. The tropical and subtropical oceans are mostly a net source of acetone, while the high‐latitude oceans are a net sink. (ii) CMIP6 anthropogenic emission inventory may underestimate acetone and/or its precursors in the Northern Hemisphere. (iii) The MEGAN biogenic emissions model may overestimate acetone and/or its precursors, and/or the biogenic oxidation mechanisms may overestimate the acetone yields. (iv) The models consistently overestimate acetone in the upper troposphere‐lower stratosphere over the Southern Ocean in austral winter. (v) Acetone contributes up to 30–40% of hydroxyl radical production in the tropical upper troposphere/lower stratosphere.

Description: The air-sea gas transfer velocity (K-660) is typically assessed as a function of the 10-m neutral wind speed (U-10n), but there remains substantial uncertainty in this relationship. Here K-660 of CO2 derived with the eddy covariance (EC) technique from eight datasets (11 research cruises) are reevaluated with consistent consideration of solubility and Schmidt number and inclusion of the ocean cool skin effect. K-660 shows an approximately linear dependence with the friction velocity (u*) in moderate winds, with an overall relative standard deviation (relative standard error) of about 20% (7%). The largest relative uncertainty in K-660 occurs at low wind speeds, while the largest absolute uncertainty in K-660 occurs at high wind speeds. There is an apparent regional variation in the steepness of the K-660-u* relationships: North Atlantic 〉= Southern Ocean 〉 other regions (Arctic, Tropics). Accounting for sea state helps to collapse some of this regional variability in K-660 using the wave Reynolds number in very large seas and the mean squared slope of the waves in small to moderate seas. The grand average of EC-derived K-660 ( - 1.47 + 76.67 u * + 20.48 u *(2) o r 0.36 + 1.203 U-10n + 0.167 U (2)(10n) ) is similar at moderate to high winds to widely used dual tracer-based K-660 parametrization, but consistently exceeds the dual tracer estimate in low winds, possibly in part due to the chemical enhancement in air-sea CO2 exchange. Combining the grand average of EC-derived K-660 with the global distribution of wind speed yields a global average transfer velocity that is comparable with the global radiocarbon (C-14) disequilibrium, but is similar to 20% higher than what is implied by dual tracer parametrizations. This analysis suggests that CO2 fluxes computed using a U-10n (2) dependence with zero intercept (e.g., dual tracer) are likely underestimated at relatively low wind speeds.