ALBERT

Description: We present consistent annual mean atmospheric histories and growth rates for the mainly anthropogenic halogenated compounds HCFC-22, HCFC-141b, HCFC-142b, HFC-134a, HFC-125, HFC-23, PFC-14 and PFC-116, which are all potentially useful oceanic transient tracers (tracers of water transport within the ocean), for the Northern and Southern Hemisphere with the aim of providing input histories of these compounds for the equilibrium between the atmosphere and surface ocean. We use observations of these halogenated compounds made by the Advanced Global Atmospheric Gases Experiment (AGAGE), the Scripps Institution of Oceanography (SIO), the Commonwealth Scientific and Industrial Research Organization (CSIRO), the National Oceanic and Atmospheric Administration (NOAA) and the University of East Anglia (UEA). Prior to the direct observational record, we use archived air measurements, firn air measurements and published model calculations to estimate the atmospheric mole fraction histories. The results show that the atmospheric mole fractions for each species, except HCFC-141b and HCFC-142b, have been increasing since they were initially produced. Recently, the atmospheric growth rates have been decreasing for the HCFCs (HCFC-22, HCFC-141b and HCFC-142b), increasing for the HFCs (HFC-134a, HFC-125, HFC-23) and stable with little fluctuation for the PFCs (PFC-14 and PFC-116) investigated here. The atmospheric histories (source functions) and natural background mole fractions show that HCFC-22, HCFC-141b, HCFC-142b, HFC-134a, HFC-125 and HFC-23 have the potential to be oceanic transient tracers for the next few decades only because of the recently imposed bans on production and consumption. When the atmospheric histories of the compounds are not monotonically changing, the equilibrium atmospheric mole fraction (and ultimately the age associated with that mole fraction) calculated from their concentration in the ocean is not unique, reducing their potential as transient tracers. Moreover, HFCs have potential to be oceanic transient tracers for a longer period in the future than HCFCs as the growth rates of HFCs are increasing and those of HCFCs are decreasing in the background atmosphere. PFC-14 and PFC-116, however, have the potential to be tracers for longer periods into the future due to their extremely long lifetimes, steady atmospheric growth rates and no explicit ban on their emissions. In this work, we also derive solubility functions for HCFC-22, HCFC-141b, HCFC-142b, HFC-134a, HFC-125, HFC-23, PFC-14 and PFC-116 in water and seawater to facilitate their use as oceanic transient tracers. These functions are based on the Clark–Glew–Weiss (CGW) water solubility function fit and salting-out coefficients estimated by the poly-parameter linear free-energy relationships (pp-LFERs). Here we also provide three methods of seawater solubility estimation for more compounds. Even though our intention is for application in oceanic research, the work described in this paper is potentially useful for tracer studies in a wide range of natural waters, including freshwater and saline lakes, and, for the more stable compounds, groundwaters.

Description: Nitrous oxide (N2O) is a long-lived potent greenhouse gas and stratospheric ozone-depleting substance, which has been accumulating in the atmosphere since the pre-industrial period. The mole fraction of atmospheric N2O has increased by nearly 25 % from 270 parts per billion (ppb) in 1750 to 336 ppb in 2022, with the fastest annual growth rate since 1980 of more than 1.3 ppb yr-1 in both 2020 and 2021. As a core component of our global greenhouse gas assessments coordinated by the Global Carbon Project (GCP), we present a global N2O budget that incorporates both natural and anthropogenic sources and sinks, and accounts for the interactions between nitrogen additions and the biochemical processes that control N2O emissions. We use Bottom-Up (BU: inventory, statistical extrapolation of flux measurements, process-based land and ocean modelling) and Top-Down (TD: atmospheric measurement-based inversion) approaches. We provide a comprehensive quantification of global N2O sources and sinks in 21 natural and anthropogenic categories in 18 regions between 1980 and 2020. We estimate that total annual anthropogenic N2O emissions increased 40 % (or 1.9 Tg N yr-1) in the past four decades (1980–2020). Direct agricultural emissions in 2020, 3.9 Tg N yr−1 (best estimate) represent the large majority of anthropogenic emissions, followed by other direct anthropogenic sources (including ‘Fossil fuel and industry’, ‘Waste and wastewater’, and ‘Biomass burning’ (2.1 Tg N yr−1), and indirect anthropogenic sources (1.3 Tg N yr−1). For the year 2020, our best estimate of total BU emissions for natural and anthropogenic sources was 18.3 (lower-upper bounds: 10.5–27.0) Tg N yr-1, close to our TD estimate of 17.0 (16.6–17.4) Tg N yr-1. For the period 2010–2019, the annual BU decadal-average emissions for natural plus anthropogenic sources were 18.1 (10.4–25.9) Tg N yr-1 and TD emissions were 17.4 (15.8–19.20 Tg N yr-1. The once top emitter Europe has reduced its emissions since the 1980s by 31 % while those of emerging economies have grown, making China the top emitter since the 2010s. The observed atmospheric N2O concentrations in recent years have exceeded projected levels under all scenarios in the Coupled Model Intercomparison Project Phase 6 (CMIP6), underscoring the urgency to reduce anthropogenic N2O emissions. To evaluate mitigation efforts and contribute to the Global Stocktake of the United Nations Framework Convention on Climate Change, we propose establishing a global network for monitoring and modeling N2O from the surface through the stratosphere. The data presented in this work can be downloaded from https://doi.org/10.18160/RQ8P-2Z4R (Tian et al. 2023).