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Mapping Air Pollution eMissions (MAPM) is a 2-year project whose goal is to develop a method to infer particulate matter (PM) emissions maps from in situ PM concentration measurements. Central to the functionality of MAPM is an inverse model. The input of the inverse model includes a spatially distributed prior emissions estimate and PM measurement time series from instruments distributed across the desired domain. In this proof-of-concept study, we describe the construction of this inverse model, the mathematics underlying the retrieval of the resultant posterior PM emissions maps, the way in which uncertainties are traced through the MAPM processing chain, and plans for future developments. To demonstrate the capability of the inverse model developed for MAPM, we use the PM2.5 measurements obtained during a dedicated winter field campaign in Christchurch, New Zealand, in 2019 to infer PM2.5 emissions maps on a city scale. The results indicate a systematic overestimation in the prior emissions for Christchurch of at least 40 %–60 %, which is consistent with some of the underlying assumptions used in the composition of the bottom-up emissions map used as the prior, highlighting the uncertainties in bottom-up approaches for estimating PM2.5 emissions maps.

The National Institute of Water and Atmospheric Research/Bodeker Scientific (NIWA–BS) total column ozone (TCO) database and the associated BS-filled TCO database have been updated to cover the period 1979 to 2019, bringing both to version 3.5.1 (V3.5.1). The BS-filled database builds on the NIWA–BS database by using a machine-learning algorithm to fill spatial and temporal data gaps to provide gap-free TCO fields over Antarctica. These filled TCO fields then provide a more complete picture of wintertime changes in the ozone layer over Antarctica. The BS-filled database has been used to calculate continuous, homogeneous time series of indicators of Antarctic ozone depletion from 1979 to 2019, including (i) daily values of the ozone mass deficit based on TCO below a 220 DU threshold; (ii) daily measures of the area over Antarctica where TCO levels are below 150 DU, below 220 DU, more than 30 % below 1979 to 1981 climatological means, and more than 50 % below 1979 to 1981 climatological means; (iii) the date of disappearance of 150 DU TCO values, 220 DU TCO values, values 30 % or more below 1979 to 1981 climatological means, and values 50 % or more below 1979 to 1981 climatological means, for each year; and (iv) daily minimum TCO values over the range 75 to 90∘ S equivalent latitude. Since both the NIWA–BS and BS-filled databases provide uncertainties on every TCO value, the Antarctic ozone depletion metrics are provided, for the first time, with fully traceable uncertainties. To gain insight into how the vertical distribution of ozone over Antarctica has changed over the past 36 years, ozone concentrations, combined and homogenized from several satellite-based ozone monitoring instruments as well as the global ozonesonde network, were also analysed. A robust attribution to changes in the drivers of long-term secular variability in these metrics has not been performed in this analysis. As a result, statements about the recovery of Antarctic TCO from the effects of ozone-depleting substances cannot be made. That said, there are clear indications of a change in trend in many of the metrics reported on here around the turn of the century, close to when Antarctic stratospheric concentrations of chlorine and bromine peaked.

Total column ozone (TCO) data from multiple satellite-based instruments have been combined to create a single near-global daily time series of ozone fields at 1.25∘ longitude by 1∘ latitude spanning the period 31 October 1978 to 31 December 2016. Comparisons against TCO measurements from the ground-based Dobson and Brewer spectrophotometer networks are used to remove offsets and drifts between the ground-based measurements and a subset of the satellite-based measurements. The corrected subset is then used as a basis for homogenizing the remaining data sets. The construction of this database improves on earlier versions of the database maintained first by the National Institute of Water and Atmospheric Research (NIWA) and now by Bodeker Scientific (BS), referred to as the NIWA-BS TCO database. The intention is for the NIWA-BS TCO database to serve as a climate data record for TCO, and to this end, the requirements for constructing climate data records, as detailed by GCOS (the Global Climate Observing System), have been followed as closely as possible. This new version includes a wider range of satellite-based instruments, uses updated sources of satellite data, extends the period covered, uses improved statistical methods to model the difference fields when homogenizing the data sets, and, perhaps most importantly, robustly tracks uncertainties from the source data sets through to the final climate data record which is now accompanied by associated uncertainty fields. Furthermore, a gap-free TCO database (referred to as the BS-filled TCO database) has been created and is documented in this paper. The utility of the NIWA-BS TCO database is demonstrated through an analysis of ozone trends from November 1978 to December 2016. Both databases are freely available for non-commercial purposes: the DOI for the NIWA-BS TCO database is https://doi.org/10.5281/zenodo.1346424 (Bodeker et al., 2018) and is available from https://zenodo.org/record/1346424. The DOI for the BS-filled TCO database is https://doi.org/10.5281/zenodo.3908787 (Bodeker et al., 2020) and is available from https://zenodo.org/record/3908787. In addition, both data sets are available from http://www.bodekerscientific.com/data/total-column-ozone (last access: June 2021).

>We analyse simulations performed for the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion caused by anthropogenic stratospheric chlorine and bromine. We consider a total of 155 simulations from 20 models, including a range of sensitivity studies which examine the impact of climate change on ozone recovery. For the control simulations (unconstrained by nudging towards analysed meteorology) there is a large spread (±20 DU in the global average) in the predictions of the absolute ozone column. Therefore, the model results need to be adjusted for biases against historical data. Also, the interannual variability in the model results need to be smoothed in order to provide a reasonably narrow estimate of the range of ozone return dates. Consistent with previous studies, but here for a Representative Concentration Pathway (RCP) of 6.0, these new CCMI simulations project that global total column ozone will return to 1980 values in 2049 (with a 1σ uncertainty of 2043–2055). At Southern Hemisphere mid-latitudes column ozone is projected to return to 1980 values in 2045 (2039–2050), and at Northern Hemisphere mid-latitudes in 2032 (2020–2044). In the polar regions, the return dates are 2060 (2055–2066) in the Antarctic in October and 2034 (2025–2043) in the Arctic in March. The earlier return dates in the Northern Hemisphere reflect the larger sensitivity to dynamical changes. Our estimates of return dates are later than those presented in the 2014 Ozone Assessment by approximately 5–17 years, depending on the region, with the previous best estimates often falling outside of our uncertainty range. In the tropics only around half the models predict a return of ozone to 1980 values, around 2040, while the other half do not reach the 1980 value. All models show a negative trend in tropical total column ozone towards the end of the 21st century. The CCMI models generally agree in their simulation of the time evolution of stratospheric chlorine and bromine, which are the main drivers of ozone loss and recovery. However, there are a few outliers which show that the multi-model mean results for ozone recovery are not as tightly constrained as possible. Throughout the stratosphere the spread of ozone return dates to 1980 values between models tends to correlate with the spread of the return of inorganic chlorine to 1980 values. In the upper stratosphere, greenhouse gas-induced cooling speeds up the return by about 10–20 years. In the lower stratosphere, and for the column, there is a more direct link in the timing of the return dates of ozone and chlorine, especially for the large Antarctic depletion. Comparisons of total column ozone between the models is affected by different predictions of the evolution of tropospheric ozone within the same scenario, presumably due to differing treatment of tropospheric chemistry. Therefore, for many scenarios, clear conclusions can only be drawn for stratospheric ozone columns rather than the total column. As noted by previous studies, the timing of ozone recovery is affected by the evolution of N2O and CH4. However, quantifying the effect in the simulations analysed here is limited by the few realisations available for these experiments compared to internal model variability. The large increase in N2O given in RCP 6.0 extends the ozone return globally by ∼ 15 years relative to N2O fixed at 1960 abundances, mainly because it allows tropical column ozone to be depleted. The effect in extratropical latitudes is much smaller. The large increase in CH4 given in the RCP 8.5 scenario compared to RCP 6.0 also lengthens ozone return by ∼ 15 years, again mainly through its impact in the tropics. Overall, our estimates of ozone return dates are uncertain due to both uncertainties in future scenarios, in particular those of greenhouse gases, and uncertainties in models. The scenario uncertainty is small in the short term but increases with time, and becomes large by the end of the century. There are still some model–model differences related to well-known processes which affect ozone recovery. Efforts need to continue to ensure that models used for assessment purposes accurately represent stratospheric chemistry and the prescribed scenarios of ozone-depleting substances, and only those models are used to calculate return dates. For future assessments of single forcing or combined effects of CO2, CH4, and N2O on the stratospheric column ozone return dates, this work suggests that it is more important to have multi-member (at least three) ensembles for each scenario from every established participating model, rather than a large number of individual models.

Understanding carbon dioxide (CO2) biospheric processes is of great importance because the terrestrial exchange drives the seasonal and inter-annual variability of CO2 in the atmosphere. Atmospheric inversions based on CO2 concentration measurements alone can only determine net biosphere fluxes, but not differentiate between photosynthesis (uptake) and respiration (production). Carbonyl sulfide (OCS) could provide an important additional constraint: it is also taken up by plants during photosynthesis but not emitted during respiration, and therefore is a potential mean to differentiate between these processes. Solar absorption Fourier Transform InfraRed (FTIR) spectrometry allows for the retrievals of the atmospheric concentrations of both CO2 and OCS from measured solar absorption spectra. Here, we investigate co-located and quasi-simultaneous FTIR measurements of OCS and CO2 performed at three selected sites located in the Northern Hemisphere. These measurements are compared to simulations of OCS and CO2 using a chemical transport model (GEOS-Chem). The OCS simulations are driven by different land biospheric fluxes to reproduce the seasonality of the measurements. Increasing the plant uptake of Kettle et al. (2002a) by a factor of three resulted in the best comparison with FTIR measurements. However, there are still discrepancies in the latitudinal distribution when comparing with HIPPO (HIAPER Pole-to-Pole Observations) data spanning both hemispheres. The coupled biospheric fluxes of OCS and CO2 from the simple biosphere model (SiB) are used in the study and compared to measurements. The CO2 simulation with SiB fluxes agrees with the measurements well, while the OCS simulation reproduced a weaker drawdown than FTIR measurements at selected sites, and a smaller latitudinal gradient in the Northern Hemisphere during growing season. An offset in the timing of the seasonal cycle minimum between SiB simulation and measurements is also seen. Using OCS as a photosynthesis proxy can help to understand how the biospheric processes are reproduced in models and to further understand the carbon cycle in the real world.