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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.

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).

Due to its remote location and extreme weather conditions, atmospheric in situ measurements are rare in the Southern Ocean. As a result, aerosol–cloud interactions in this region are poorly understood and remain a major source of uncertainty in climate models. This, in turn, contributes substantially to persistent biases in climate model simulations such as the well-known positive shortwave radiation bias at the surface, as well as biases in numerical weather prediction models and reanalyses. It has been shown in previous studies that in situ and ground-based remote sensing measurements across the Southern Ocean are critical for complementing satellite data sets due to the importance of boundary layer and low-level cloud processes. These processes are poorly sampled by satellite-based measurements and are often obscured by multiple overlying cloud layers. Satellite measurements also do not constrain the aerosol–cloud processes very well with imprecise estimation of cloud condensation nuclei. In this work, we present a comprehensive set of ship-based aerosol and meteorological observations collected on the 6-week Southern Ocean Ross Sea Marine Ecosystem and Environment voyage (TAN1802) voyage of RV Tangaroa across the Southern Ocean, from Wellington, New Zealand, to the Ross Sea, Antarctica. The voyage was carried out from 8 February to 21 March 2018. Many distinct, but contemporaneous, data sets were collected throughout the voyage. The compiled data sets include measurements from a range of instruments, such as (i) meteorological conditions at the sea surface and profile measurements; (ii) the size and concentration of particles; (iii) trace gases dissolved in the ocean surface such as dimethyl sulfide and carbonyl sulfide; (iv) and remotely sensed observations of low clouds. Here, we describe the voyage, the instruments, and data processing, and provide a brief overview of some of the data products available. We encourage the scientific community to use these measurements for further analysis and model evaluation studies, in particular, for studies of Southern Ocean clouds, aerosol, and their interaction. The data sets presented in this study are publicly available at https://doi.org/10.5281/zenodo.4060237 (Kremser et al., 2020).

MAPM (Mapping Air Pollution eMissions) is a project whose goal is to develop a method to infer airborne particulate matter (PM) emissions maps from in situ PM concentration measurements. In support of MAPM, a winter field campaign was conducted in New Zealand in 2019 (June to September) to obtain the measurements required to test and validate the MAPM methodology. Two different types of instruments measuring PM were deployed: ES-642 remote dust monitors (17 instruments) and Outdoor Dust Information Nodes (ODINs; 50 instruments). The measurement campaign was bracketed by two intercomparisons where all instruments were co-located, with a permanently installed tapered element oscillating membrane (TEOM) instrument, to determine any instrument biases. Changes in biases between the pre- and post-campaign intercomparisons were used to determine instrument drift over the campaign period. Once deployed, each ES-642 was co-located with an ODIN. In addition to the PM measurements, meteorological variables (temperature, pressure, wind speed, and wind direction) were measured at three automatic weather station (AWS) sites established as part of the campaign, with additional data being sourced from 27 further AWSs operated by other agencies. Vertical profile measurements were made with 12 radiosondes during two 24 h periods and complimented measurements made with a mini micropulse lidar and ceilometer. Here we present the data collected during the campaign and discuss the correction of the measurements made by various PM instruments. We find that when compared to measurements made with a simple linear correction, a correction based on environmental conditions improves the quality of measurements retrieved from ODINs but results in over-fitting and increases the uncertainties when applied to the more sophisticated ES-642 instruments. We also compare PM2.5 and PM10 measured by ODINs which, in some cases, allows us to identify PM from natural and anthropogenic sources. The PM data collected during the campaign are publicly available from https://doi.org/10.5281/zenodo.4542559 (Dale et al., 2020b), and the data from other instruments are available from https://doi.org/10.5281/zenodo.4536640 (Dale et al., 2020a).

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.

High-quality satellite-based measurements are crucial to the assessment of global stratospheric composition change. The Stratospheric Aerosol and Gas Experiment II (SAGE II) provides the longest, continuous data set of vertically resolved ozone and aerosol extinction coefficients to date and therefore remains a cornerstone of understanding and detecting long-term ozone variability and trends in the stratosphere. Despite its stability, SAGE II measurements must be screened for outliers that are a result of excessive aerosol emitted into the atmosphere and that degrade inferences of change. Current methods for SAGE II ozone measurement quality assurance consist of multiple ad hoc and sometimes conflicting rules, leading to too much valuable data being removed or outliers being missed. In this work, the SAGE II ozone data set version 7.00 is used to develop and present a new set of screening recommendations and to compare the output to the screening recommendations currently used. Applying current recommendations to SAGE II ozone leads to unexpected features, such as removing ozone values around zero if the relative error is used as a screening criterion, leading to biases in monthly mean zonal mean ozone concentrations. Most of these current recommendations were developed based on “visual inspection”, leading to inconsistent rules that might not be applicable at every altitude and latitude. Here, a set of new screening recommendations is presented that take into account the knowledge of how the measurements were made. The number of screening recommendations is reduced to three, which mainly remove ozone values that are affected by high aerosol loading and are therefore not reliable measurements. More data remain when applying these new recommendations compared to the rules that are currently being used, leading to more data being available for scientific studies. The SAGE II ozone data set used here is publicly available at https://doi.org/10.5281/zenodo.3710518 (Kremser et al., 2020). The complete SAGE II version 7.00 data set, which includes other variables in addition to ozone, is available at https://eosweb.larc.nasa.gov/project/sage2/sage2_v7_table (last access: December 2019), https://doi.org/10.5067/ERBS/SAGEII/SOLAR_BINARY_L2-V7.0 (SAGE II Science Team, 2012; Damadeo et al., 2013).

Carbonyl sulfide (OCS) and carbon disulfide (CS2) are volatile sulfur gases that are naturally formed in seawater and exchanged with the atmosphere. OCS is the most abundant sulfur gas in the atmosphere, and CS2 is its most important precursor. They have attracted increased interest due to their direct (OCS) or indirect (CS2 via oxidation to OCS) contribution to the stratospheric sulfate aerosol layer. Furthermore, OCS serves as a proxy to constrain terrestrial CO2 uptake by vegetation. Oceanic emissions of both gases contribute a major part to their atmospheric concentration. Here we present a database of previously published and unpublished (mainly shipborne) measurements in seawater and the marine boundary layer for both gases, available at https://doi.org/10.1594/PANGAEA.905430 (Lennartz et al., 2019). The database contains original measurements as well as data digitalized from figures in publications from 42 measurement campaigns, i.e., cruises or time series stations, ranging from 1982 to 2019. OCS data cover all ocean basins except for the Arctic Ocean, as well as all months of the year, while the CS2 dataset shows large gaps in spatial and temporal coverage. Concentrations are consistent across different sampling and analysis techniques for OCS. The database is intended to support the identification of global spatial and temporal patterns and to facilitate the evaluation of model simulations.

With low concentrations of tropospheric aerosol, the Southern Ocean offers a “natural laboratory” for studies of aerosol–cloud interactions. Aerosols over the Southern Ocean are produced from biogenic activity in the ocean, which generates sulfate aerosol via dimethylsulfide (DMS) oxidation, and from strong winds and waves that lead to bubble bursting and sea spray emission. Here, we evaluate the representation of Southern Ocean aerosols in the Hadley Centre Global Environmental Model version 3, Global Atmosphere 7.1 (HadGEM3-GA7.1) chemistry–climate model. Compared with aerosol optical depth (AOD) observations from two satellite instruments (the Moderate Resolution Imaging Spectroradiometer, MODIS-Aqua c6.1, and the Multi-angle Imaging Spectroradiometer, MISR), the model simulates too-high AOD during winter and too-low AOD during summer. By switching off DMS emission in the model, we show that sea spray aerosol is the dominant contributor to AOD during winter. In turn, the simulated sea spray aerosol flux depends on near-surface wind speed. By examining MODIS AOD as a function of wind speed from the ERA-Interim reanalysis and comparing it with the model, we show that the sea spray aerosol source function in HadGEM3-GA7.1 overestimates the wind speed dependency. We test a recently developed sea spray aerosol source function derived from measurements made on a Southern Ocean research voyage in 2018. In this source function, the wind speed dependency of the sea spray aerosol flux is less than in the formulation currently implemented in HadGEM3-GA7.1. The new source function leads to good agreement between simulated and observed wintertime AODs over the Southern Ocean; however, it reveals partially compensating errors in DMS-derived AOD. While previous work has tested assumptions regarding the seawater climatology or sea–air flux of DMS, we test the sensitivity of simulated AOD, cloud condensation nuclei and cloud droplet number concentration to three atmospheric sulfate chemistry schemes. The first scheme adds DMS oxidation by halogens and the other two test a recently developed sulfate chemistry scheme for the marine troposphere; one tests gas-phase chemistry only, while the second adds extra aqueous-phase sulfate reactions. We show how simulated sulfur dioxide and sulfuric acid profiles over the Southern Ocean change as a result and how the number concentration and particle size of the soluble Aitken, accumulation and coarse aerosol modes are affected. The new DMS chemistry scheme leads to a 20 % increase in the number concentration of cloud condensation nuclei and cloud droplets, which improves agreement with observations. Our results highlight the importance of atmospheric chemistry for simulating aerosols and clouds accurately over the Southern Ocean.

When computing climatological averages of atmospheric trace-gas mixing ratios obtained from satellite-based measurements, sampling biases arise if data coverage is not uniform in space and time. Homogeneous spatiotemporal coverage is essentially impossible to achieve. Solar occultation measurements, by virtue of satellite orbit and the requirement of direct observation of the sun through the atmosphere, result in particularly sparse spatial coverage. In this proof-of-concept study, a method is presented to adjust for such sampling biases when calculating climatological means. The method is demonstrated using carbonyl sulfide (OCS) measurements at 16 km altitude from the ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer). At this altitude, OCS mixing ratios show a steep gradient between the poles and Equator. ACE-FTS measurements, which are provided as vertically resolved profiles, and integrated stratospheric OCS columns are used in this study. The bias adjustment procedure requires no additional information other than the satellite data product itself. In particular, the method does not rely on atmospheric models with potentially unreliable transport or chemistry parameterizations, and the results can be used uncompromised to test and validate such models. It is expected to be generally applicable when constructing climatologies of long-lived tracers from sparsely and heterogeneously sampled satellite measurements. In the first step of the adjustment procedure, a regression model is used to fit a 2-D surface to all available ACE-FTS OCS measurements as a function of day-of-year and latitude. The regression model fit is used to calculate an adjustment factor that is then used to adjust each measurement individually. The mean of the adjusted measurement points of a chosen latitude range and season is then used as the bias-free climatological value. When applying the adjustment factor to seasonal averages in 30∘ zones, the maximum spatiotemporal sampling bias adjustment was 11 % for OCS mixing ratios at 16 km and 5 % for the stratospheric OCS column. The adjustments were validated against the much denser and more homogeneous OCS data product from the limb-sounding MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) instrument, and both the direction and magnitude of the adjustments were in agreement with the adjustment of the ACE-FTS data.

An updated and improved version of a global, vertically resolved, monthly mean zonal mean ozone database has been calculated – hereafter referred to as the BSVertOzone (Bodeker Scientific Vertical Ozone) database. Like its predecessor, it combines measurements from several satellite-based instruments and ozone profile measurements from the global ozonesonde network. Monthly mean zonal mean ozone concentrations in mixing ratio and number density are provided in 5° latitude bins, spanning 70 altitude levels (1 to 70 km), or 70 pressure levels that are approximately 1 km apart (878.4 to 0.046 hPa). Different data sets or tiers are provided: Tier 0 is based only on the available measurements and therefore does not completely cover the whole globe or the full vertical range uniformly; the Tier 0.5 monthly mean zonal means are calculated as a filled version of the Tier 0 database where missing monthly mean zonal mean values are estimated from correlations against a total column ozone (TCO) database. The Tier 0.5 data set includes the full range of measurement variability and is created as an intermediate step for the calculation of the Tier 1 data where a least squares regression model is used to attribute variability to various known forcing factors for ozone. Regression model fit coefficients are expanded in Fourier series and Legendre polynomials (to account for seasonality and latitudinal structure, respectively). Four different combinations of contributions from selected regression model basis functions result in four different Tier 1 data sets that can be used for comparisons with chemistry–climate model (CCM) simulations that do not exhibit the same unforced variability as reality (unless they are nudged towards reanalyses). Compared to previous versions of the database, this update includes additional satellite data sources and ozonesonde measurements to extend the database period to 2016. Additional improvements over the previous version of the database include the following: (i) adjustments of measurements to account for biases and drifts between different data sources (using a chemistry-transport model, CTM, simulation as a transfer standard), (ii) a more objective way to determine the optimum number of Fourier and Legendre expansions for the basis function fit coefficients, and (iii) the derivation of methodological and measurement uncertainties on each database value are traced through all data modification steps. Comparisons with the ozone database from SWOOSH (Stratospheric Water and OzOne Satellite Homogenized data set) show good agreement in many regions of the globe. Minor differences are caused by different bias adjustment procedures for the two databases. However, compared to SWOOSH, BSVertOzone additionally covers the troposphere. Version 1.0 of BSVertOzone is publicly available at https://doi.org/http://doi.org/10.5281/zenodo.1217184.

>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.

Upper-air measurements of essential climate variables (ECVs), such as temperature, are crucial for climate monitoring and climate change detection. Because of the internal variability of the climate system, many decades of measurements are typically required to robustly detect any trend in the climate data record. It is imperative for the records to be temporally homogeneous over many decades to confidently estimate any trend. Historically, records of upper-air measurements were primarily made for short-term weather forecasts and as such are seldom suitable for studying long-term climate change as they lack the required continuity and homogeneity. Recognizing this, the Global Climate Observing System (GCOS) Reference Upper-Air Network (GRUAN) has been established to provide reference-quality measurements of climate variables, such as temperature, pressure, and humidity, together with well-characterized and traceable estimates of the measurement uncertainty. To ensure that GRUAN data products are suitable to detect climate change, a scientifically robust instrument replacement strategy must always be adopted whenever there is a change in instrumentation. By fully characterizing any systematic differences between the old and new measurement system a temporally homogeneous data series can be created. One strategy is to operate both the old and new instruments in tandem for some overlap period to characterize any inter-instrument biases. However, this strategy can be prohibitively expensive at measurement sites operated by national weather services or research institutes. An alternative strategy that has been proposed is to alternate between the old and new instruments, so-called interlacing, and then statistically derive the systematic biases between the two instruments. Here we investigate the feasibility of such an approach specifically for radiosondes, i.e. flying the old and new instruments on alternating days. Synthetic data sets are used to explore the applicability of this statistical approach to radiosonde change management.

A method, based on climate pattern scaling, has been developed to expand a small number of projections of fields of a selected climate variable (X) into an ensemble that encapsulates a wide range of indicative model structural uncertainties. The method described in this paper is referred to as the Ensemble Projections Incorporating Climate model uncertainty (EPIC) method. Each ensemble member is constructed by adding contributions from (1) a climatology derived from observations that represents the time-invariant part of the signal; (2) a contribution from forced changes in X, where those changes can be statistically related to changes in global mean surface temperature (Tglobal); and (3) a contribution from unforced variability that is generated by a stochastic weather generator. The patterns of unforced variability are also allowed to respond to changes in Tglobal. The statistical relationships between changes in X (and its patterns of variability) and Tglobal are obtained in a training phase. Then, in an implementation phase, 190 simulations of Tglobal are generated using a simple climate model tuned to emulate 19 different global climate models (GCMs) and 10 different carbon cycle models. Using the generated Tglobal time series and the correlation between the forced changes in X and Tglobal, obtained in the training phase, the forced change in the X field can be generated many times using Monte Carlo analysis. A stochastic weather generator is used to generate realistic representations of weather which include spatial coherence. Because GCMs and regional climate models (RCMs) are less likely to correctly represent unforced variability compared to observations, the stochastic weather generator takes as input measures of variability derived from observations, but also responds to forced changes in climate in a way that is consistent with the RCM projections. This approach to generating a large ensemble of projections is many orders of magnitude more computationally efficient than running multiple GCM or RCM simulations. Such a large ensemble of projections permits a description of a probability density function (PDF) of future climate states rather than a small number of individual story lines within that PDF, which may not be representative of the PDF as a whole; the EPIC method largely corrects for such potential sampling biases. The method is useful for providing projections of changes in climate to users wishing to investigate the impacts and implications of climate change in a probabilistic way. A web-based tool, using the EPIC method to provide probabilistic projections of changes in daily maximum and minimum temperatures for New Zealand, has been developed and is described in this paper.

To simulate the impacts of volcanic eruptions on the stratosphere, chemistry–climate models that do not include an online aerosol module require temporally and spatially resolved aerosol size parameters for heterogeneous chemistry and aerosol radiative properties as a function of wavelength. For phase 1 of the Chemistry-Climate Model Initiative (CCMI-1) and, later, for phase 6 of the Coupled Model Intercomparison Project (CMIP6) two such stratospheric aerosol data sets were compiled, whose functional capability and representativeness are compared here. For CCMI-1, the SAGE-4λ data set was compiled, which hinges on the measurements at four wavelengths of the SAGE (Stratospheric Aerosol and Gas Experiment) II satellite instrument and uses ground-based lidar measurements for gap-filling immediately after the 1991 Mt Pinatubo eruption, when the stratosphere was too optically opaque for SAGE II. For CMIP6, the new SAGE-3λ data set was compiled, which excludes the least reliable SAGE II wavelength and uses measurements from CLAES (Cryogenic Limb Array Etalon Spectrometer) on UARS, the Upper Atmosphere Research Satellite, for gap-filling following the Mt Pinatubo eruption instead of ground-based lidars. Here, we performed SOCOLv3 (Solar Climate Ozone Links version 3) chemistry–climate model simulations of the recent past (1986–2005) to investigate the impact of the Mt Pinatubo eruption in 1991 on stratospheric temperature and ozone and how this response differs depending on which aerosol data set is applied. The use of SAGE-4λ results in heating and ozone loss being overestimated in the tropical lower stratosphere compared to observations in the post-eruption period by approximately 3 K and 0.2 ppmv, respectively. However, less heating occurs in the model simulations based on SAGE-3λ, because the improved gap-filling procedures after the eruption lead to less aerosol loading in the tropical lower stratosphere. As a result, simulated tropical temperature anomalies in the model simulations based on SAGE-3λ for CMIP6 are in excellent agreement with MERRA and ERA-Interim reanalyses in the post-eruption period. Less heating in the simulations with SAGE-3λ means that the rate of tropical upwelling does not strengthen as much as it does in the simulations with SAGE-4λ, which limits dynamical uplift of ozone and therefore provides more time for ozone to accumulate in tropical mid-stratospheric air. Ozone loss following the Mt Pinatubo eruption is overestimated by up to 0.1 ppmv in the model simulations based on SAGE-3λ, which is a better agreement with observations than in the simulations based on SAGE-4λ. Overall, the CMIP6 stratospheric aerosol data set, SAGE-3λ, allows SOCOLv3 to more accurately simulate the post-Pinatubo eruption period.

We present 20 years (1996–2015) of austral springtime measurements of chlorine monoxide (ClO) over Antarctica from the Chlorine Oxide Experiment (ChlOE1) ground-based millimeter wave spectrometer at Scott Base, Antarctica, as well 12 years (2004–2015) of ClO measurements from the Aura Microwave Limb Sounder (MLS). From August onwards we observe a strong increase in lower stratospheric ClO, with a peak column amount usually occurring in early September. From mid-September onwards we observe a strong decrease in ClO. In order to study interannual differences, we focus on a 3-week period from 28 August to 17 September for each year and compare the average column ClO anomalies. These column ClO anomalies are shown to be highly correlated with the average ozone mass deficit for September and October of each year. We also show that anomalies in column ClO are strongly anti-correlated with 30 hPa temperature anomalies, both on a daily and an interannual timescale. Making use of this anti-correlation we calculate the linear dependence of the interannual variations in column ClO on interannual variations in temperature. By making use of this relationship, we can better estimate the underlying trend in the total chlorine (Cly = HCl + ClONO2 + HOCl + 2 × Cl2 + 2 × Cl2O2 + ClO + Cl). The resultant trends in Cly, which determine the long-term trend in ClO, are estimated to be −0.5 ± 0.2, −1.4 ± 0.9, and −0.6 ± 0.4 % year−1, for zonal MLS, Scott Base MLS (both 2004–2015), and ChlOE (1996–2015) respectively. These trends are within 1σ of trends in stratospheric Cly previously found at other latitudes. The decrease in ClO is consistent with the trend expected from regulations enacted under the Montreal Protocol.

Understanding carbon dioxide (CO2) biospheric processes is of great importance because the terrestrial exchange drives the seasonal and interannual 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 means 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 five 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 coupled biospheric fluxes of OCS and CO2 from the simple biosphere model (SiB) are used in the study. 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 when comparing with HIPPO (HIAPER Pole-to-Pole Observations) data spanning both hemispheres. 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.

The Global Climate Observing System (GCOS) Reference Upper Air Network (GRUAN) provides reference quality RS92 radiosonde measurements of temperature, pressure and humidity. A key attribute of reference quality measurements, and hence GRUAN data, is that each datum has a well characterized and traceable estimate of the measurement uncertainty. The long-term homogeneity of the measurement records, and their well characterized uncertainties, make these data suitable for reliably detecting changes in global and regional climate on decadal time scales. Considerable effort is invested in GRUAN operations to (i) describe and analyse all sources of measurement uncertainty to the extent possible, (ii) quantify and synthesize the contribution of each source of uncertainty to the total measurement uncertainty, and (iii) verify that the evaluated net uncertainty is within the required target uncertainty. However, if the climate science community is not sufficiently well informed on how to capitalize on this added value, the significant investment in estimating meaningful measurement uncertainties is largely wasted. This paper presents and discusses the techniques that will need to be employed to reliably quantify long-term trends in GRUAN data records. A pedagogical approach is taken whereby numerical recipes for key parts of the trend analysis process are explored. The paper discusses the construction of linear least squares regression models for trend analysis, boot-strapping approaches to determine uncertainties in trends, dealing with the combined effects of autocorrelation in the data and measurement uncertainties in calculating the uncertainty on trends, best practice for determining seasonality in trends, how to deal with co-linear basis functions, and interpreting derived trends. Synthetic data sets are used to demonstrate these concepts which are then applied to a first analysis of temperature trends in RS92 radiosonde upper air soundings at the GRUAN site at Lindenberg, Germany (52.21° N, 14.12° E).

An extremely fast model to estimate the degree of stratospheric ozone depletion during polar winters is described. It is based on a set of coupled differential equations that simulate the seasonal evolution of vortex-averaged hydrogen chloride (HCl), nitric acid (HNO3), chlorine nitrate (ClONO2), active forms of chlorine (ClOx = Cl + ClO + 2 ClOOCl) and ozone (O3) on isentropic levels within the polar vortices. Terms in these equations account for the chemical and physical processes driving the time rate of change of these species. Eight empirical fit coefficients associated with these terms are derived by iteratively fitting the equations to vortex-averaged satellite-based measurements of HCl, HNO3 and ClONO2 and observationally derived ozone loss rates. The system of differential equations is not stiff and can be solved with a time step of one day, allowing many years to be processed per second on a standard PC. The inputs required are the daily fractions of the vortex area covered by polar stratospheric clouds and the fractions of the vortex area exposed to sunlight. The resultant model, SWIFT (Semi-empirical Weighted Iterative Fit Technique), provides a fast yet accurate method to simulate ozone loss rates in polar regions. SWIFT's capabilities are demonstrated by comparing measured and modeled total ozone loss outside of the training period.

A Climate Pattern-Scaling Model (CPSM) that simulates global patterns of climate change, for a prescribed emissions scenario, is described. A CPSM works by quantitatively establishing the statistical relationship between a climate variable at a specific location (e.g. daily maximum surface temperature, Tmax) and one or more predictor time series (e.g. global mean surface temperature, Tglobal) – referred to as the "training" of the CPSM. This training uses a regression model to derive fit coefficients that describe the statistical relationship between the predictor time series and the target climate variable time series. Once that relationship has been determined, and given the predictor time series for any greenhouse gas (GHG) emissions scenario, the change in the climate variable of interest can be reconstructed – referred to as the "application" of the CPSM. The advantage of using a CPSM rather than a typical atmosphere–ocean global climate model (AOGCM) is that the predictor time series required by the CPSM can usually be generated quickly using a simple climate model (SCM) for any prescribed GHG emissions scenario and then applied to generate global fields of the climate variable of interest. The training can be performed either on historical measurements or on output from an AOGCM. Using model output from 21st century simulations has the advantage that the climate change signal is more pronounced than in historical data and therefore a more robust statistical relationship is obtained. The disadvantage of using AOGCM output is that the CPSM training might be compromised by any AOGCM inadequacies. For the purposes of exploring the various methodological aspects of the CPSM approach, AOGCM output was used in this study to train the CPSM. These investigations of the CPSM methodology focus on monthly mean fields of daily temperature extremes (Tmax and Tmin). The methodological aspects of the CPSM explored in this study include (1) investigation of the advantage gained in having five predictor time series over having only one predictor time series, (2) investigation of the time dependence of the fit coefficients and (3) investigation of the dependence of the fit coefficients on GHG emissions scenario. Key conclusions are (1) overall, the CPSM trained on simulations based on the Representative Concentration Pathway (RCP) 8.5 emissions scenario is able to reproduce AOGCM simulations of Tmax and Tmin based on predictor time series from an RCP 4.5 emissions scenario; (2) access to hemisphere average land and ocean temperatures as predictors improves the variance that can be explained, particularly over the oceans; (3) regression model fit coefficients derived from individual simulations based on the RCP 2.6, 4.5 and 8.5 emissions scenarios agree well over most regions of the globe (the Arctic is the exception); (4) training the CPSM on concatenated time series from an ensemble of simulations does not result in fit coefficients that explain significantly more of the variance than an approach that weights results based on single simulation fits; and (5) the inclusion of a linear time dependence in the regression model fit coefficients improves the variance explained, primarily over the oceans.

Two semi-empirical models were developed for the Antarctic stratosphere to relate the shift of species within total chlorine (Cly = HCl + ClONO2 + HOCl + 2 × Cl2 + 2×Cl2O2 + ClO + Cl) into the active forms (here: ClOx = 2×Cl2O2 + ClO), and to relate the rate of ozone destruction to ClOx. These two models provide a fast and computationally inexpensive way to describe the inter- and intra-annual evolution of ClOx and ozone mass deficit (OMD) in the Antarctic spring. The models are based on the underlying physics/chemistry of the system and capture the key chemical and physical processes in the Antarctic stratosphere that determine the interaction between climate change and Antarctic ozone depletion. They were developed considering bulk effects of chemical mechanisms for the duration of the Antarctic vortex period and quantities averaged over the vortex area. The model equations were regressed against observations of daytime ClO and OMD providing a set of empirical fit coefficients. Both semi-empirical models are able to explain much of the intra- and inter-annual variability observed in daily ClOx and OMD time series. This proof-of-concept paper outlines the semi-empirical approach to describing the evolution of Antarctic chlorine activation and ozone depletion.

Key kinetic parameters governing the partitioning of chlorine species in the Antarctic polar stratosphere were retrieved from 28 days of chlorine monoxide (ClO) microwave radiometer measurements made during the late winter/early spring of 2005 at Scott Base (77.85° S, 166.75° E). During day-time the loss of the ClO dimer chlorine peroxide (ClOOCl) occurs mainly by photolysis. Some time after sunrise, a photochemical equilibrium is established and the ClO/ClOOCl partitioning is determined by the ratio of the photolysis frequency, J, and the dimer formation rate, kf. The values of J and kf from laboratory studies remain uncertain to a considerable extent, and as a complement to these ongoing studies, the goal of this work is to provide a constraint on that uncertainty based on observations of ClO profiles in the Antarctic. First an optimal estimation technique was used to derive J/kf ratios for a range of Keq values. The optimal estimation forward model was a photochemical box model that takes J, kf, and Keq as inputs, together with a priori profiles of activated chlorine (ClOx = ClO+2×ClOOCl), profiles of ozone, temperature, and pressure. JPL06 kinetics are used as a priori in the optimal estimation and for all other chemistry in the forward model. Using the more recent JPL09 kinetics results in insignificant differences in the retrieved value of J/kf. A complementary approach was used to derive the optimal kinetic parameters; the full parameter space of J, kf, Keq and ClOx was sampled to find the minimum in differences between measured and modelled ClO profiles. Furthermore, values of Keq up to 2.0 times larger than recommended by JPL06 were explored to test the sensitivity of the J/kf ratio to changes in Keq. The results show that the retrieved J/kf ratios bracket the range of 1.23 to 1.97 times the J/kf value recommended by JPL06 over the range of Keq values considered. The retrieved J/kf ratios lie in the lower half of the large uncertainty range of J/kf recommended by JPL06 and towards the upper portion of the smaller uncertainty range recommended by JPL09.

Establishing sharp and correctly positioned boundaries in spatial gene expression patterns is a central task in both developmental and synthetic biology. We consider situations where a global morphogen gradient provides positional information to cells but is insufficient to ensure the required boundary precision, due to different types of noise in the system. In a conceptual model, we quantitatively compare three mechanisms, which combine the global signal with local signaling between neighboring cells, to enhance the boundary formation process. These mechanisms differ with respect to the way in which they combine the signals by following either an AND, an OR, or a SUM rule. Within our model, we analyze the dynamics of the boundary formation process, and the fuzziness of the resulting boundary. Furthermore, we consider the tunability of the boundary position and its scaling with system size. We find that all three mechanisms produce less fuzzy boundaries than the purely gradient-based reference mechanism, even in the regime of high noise in the local signals relative to the noise in the global signal. Among the three mechanisms, the SUM rule produces the most accurate boundary. However, in contrast to the other two mechanisms, it requires noise to exit metastable states and rapidly reach the stable boundary pattern.

The antibody Fv module which binds antigen consists of the variable domains V L and V H . These exhibit a conserved ß-sheet structure and comprise highly variable loops (CDRs). Little is known about the contributions of the framework residues and CDRs to their association. We exchanged conserved interface residues as well as CDR loops and tested the effects on two Fvs interacting with moderate affinities (K D s of ~2.5 µM and ~6 µM). While for the rather instable domains, almost all mutations had a negative effect, the more stable domains tolerated a number of mutations of conserved interface residues. Of particular importance for Fv association are V L P44 and V H L45. In general, the exchange of conserved residues in the V L /V H interface did not have uniform effects on domain stability. Furthermore, the effects on association and antigen binding do not strictly correlate. In addition to the interface, the CDRs modulate the variable domain framework to a significant extent as shown by swap experiments. Our study reveals a complex interplay of domain stability, association and antigen binding including an unexpected strong mutual influence of the domain framework and the CDRs on stability/association on the one side and antigen binding on the other side.