ALBERT

Description: Lightning is one of the major natural sources of NOx in the atmosphere. A suite of time slice experiments using a stratosphere-resolving configuration of the Unified Model (UM), containing the United Kingdom Chemistry and Aerosols sub-model (UKCA), has been performed to investigate the impact of climate change on emissions of NOx from lightning (LNOx) and to highlight its critical impacts on photochemical ozone production and the oxidising capacity of the troposphere. Two Representative Concentration Pathway (RCP) scenarios (RCP4.5 and RCP8.5) are explored. LNOx is simulated to increase in a year-2100 climate by 33% (RCP4.5) and 78% (RCP8.5), primarily as a result of increases in the depth of convection. The total tropospheric chemical odd oxygen production (P(Ox)) increases linearly with increases in total LNOx and consequently, tropospheric ozone burdens of 29 ± 4 Tg(O3) (RCP4.5) and 46 ± 4 Tg(O3) (RCP8.5) are calculated here. By prescribing a uniform surface boundary concentration for methane in these simulations, methane-driven feedbacks are essentially neglected. A simple estimate of the contribution of the feedback reduces the increase in ozone burden to 24 and 33 Tg(O3), respectively. We thus show that, through changes in LNOx, the effects of climate change counteract the simulated mitigation of the ozone burden, which results from reductions in ozone precursor emissions as part of air quality controls projected in the RCP scenarios. Without the driver of increased LNOx, our simulations suggest that the net effect of climate change would be to lower free tropospheric ozone. In addition, we identify large climate-change-induced enhancements in the concentration of the hydroxyl radical (OH) in the tropical upper troposphere (UT), particularly over the Maritime Continent, primarily as a consequence of greater LNOx. The OH enhancement in the tropics increases oxidation of both methane (with feedbacks onto chemistry and climate) and very short-lived substances (VSLS) (with implications for stratospheric ozone depletion). We emphasise that it is important to improve our understanding of LNOx in order to gain confidence in model projections of composition change under future climate.

Description: It has been shown previously that one member of the Met Office Hadley Centre single-parameter perturbed physics ensemble – the so-called "low entrainment parameter" member – has a much higher climate sensitivity than other individual parameter perturbations. Here we show that the concentration of stratospheric water vapour in this member is over three times higher than observations, and, more importantly for climate sensitivity, increases significantly when climate warms. The large surface temperature response of this ensemble member is more consistent with stratospheric humidity change, rather than upper tropospheric clouds as has been previously suggested. The direct relationship between the bias in the control state (elevated stratospheric humidity) and the cause of the high climate sensitivity (a further increase in stratospheric humidity) lends further doubt as to the realism of this particular integration. This, together with other evidence, lowers the likelihood that the climate system's physical sensitivity is significantly higher than the likely upper range quoted in the Intergovernmental Panel on Climate Change's Fourth Assessment Report.

Description: It has been shown previously that one member of the Met Office Hadley Centre single-parameter perturbed physics ensemble – the so-called "low entrainment parameter" member – has a much higher climate sensitivity than other individual parameter perturbations. Here we show that the concentration of stratospheric water vapour in this member is over three times higher than observations, and, more importantly for climate sensitivity, increases significantly when climate warms. The large surface temperature response of this ensemble member is more consistent with a feedback associated with the stratospheric humidity change, rather than high clouds as has been previously suggested. The direct relationship between the bias in the control state (elevated stratospheric humidity) and the cause of the high climate sensitivity (a further increase in stratospheric humidity) lends further doubt as to the realism of this particular integration. This, together with other evidence, lowers the likelihood that the climate system's physical sensitivity might be significantly higher than the likely upper range quoted in the Intergovernmental Panel on Climate Change's fourth assessment report.

Description: A stratosphere-resolving configuration of the Met Office's Unified Model (UM) with the United Kingdom Chemistry and Aerosols (UKCA) scheme is used to investigate the atmospheric response to changes in (a) greenhouse gases and climate, (b) ozone-depleting substances (ODSs) and (c) non-methane ozone precursor emissions. A suite of time-slice experiments show the separate, as well as pairwise, impacts of these perturbations between the years 2000 and 2100. Sensitivity to uncertainties in future greenhouse gases and aerosols is explored through the use of the Representative Concentration Pathway (RCP) 4.5 and 8.5 scenarios. The results highlight an important role for the stratosphere in determining the annual mean tropospheric ozone response, primarily through stratosphere–troposphere exchange of ozone (STE). Under both climate change and reductions in ODSs, increases in STE offset decreases in net chemical production, leading to overall increases in the tropospheric ozone burden. This opposes the effects of projected decreases in ozone precursors through measures to improve air quality, which act to reduce the ozone burden. The global tropospheric lifetime of ozone (τO3) does not change significantly under climate change at RCP4.5, but it decreases at RCP8.5. This opposes the increases in τO3 simulated under reductions in both ODSs and ozone precursor emissions. The additivity of the changes in ozone is examined by comparing the sum of the responses in the single-forcing experiments to those from equivalent combined-forcing experiments. Whilst the ozone responses to most forcing combinations are found to be approximately additive, non-additive changes are found in both the stratosphere and troposphere when a large climate forcing (RCP8.5) is combined with the effects of ODSs.

Description: Lightning is one of the major natural sources of NOx in the atmosphere. A suite of time-slice experiments using a stratosphere-resolving configuration of the Unified Model (UM), containing the UK Chemistry and Aerosols sub-model (UKCA), have been performed to investigate the impact of climate change on lightning produced NOx (LNOx) and to highlight its critical impacts on photochemical ozone production and the oxidising capacity of the troposphere. Two Representative Concentration Pathway (RCP) scenarios (RCP4.5 and RCP8.5) are explored. LNOx emissions are simulated to increase in a year-2100 climate by 33% (RCP4.5) and 78% (RCP8.5) in response to changes in convection. The total tropospheric chemical odd oxygen production (P(Ox)) increases linearly with total LNOx emissions and consequently, the tropospheric ozone burden also increases by 29 ± 4 Tg(O3) (RCP4.5) and 46 ± 4 Tg(O3) (RCP8.5). We thus show that, through changes in LNOx, the effects of climate change counteract the simulated mitigation of the ozone burden, which results from reductions in ozone precursor emissions as part of air quality controls projected in the RCP scenarios. Without the driver of increased LNOx, our simulations suggest that the net effect of climate change would be to lower free tropospheric ozone. In addition, we identify large climate-change induced enhancements in the concentration of the hydroxyl radical (OH) in the tropical upper troposphere (UT), particularly over the Maritime Continent, primarily as a consequence of larger LNOx emissions. The OH enhancement in the tropics increases oxidation of both methane (with feedbacks onto chemistry and climate) and very short-lived substances (VSLS) (with implications for stratospheric ozone depletion). We emphasise that it is important to improve our understanding of LNOx in order to gain confidence in model projections of future climate.

Description: Trends in the vertical distribution of ozone are reported and compared for a number of new and recently revised datasets. The amount of ozone-depleting compounds in the stratosphere (as measured by Equivalent Effective Stratospheric Chlorine – EESC) maximised in the second half of the 1990s. We therefore examine the trends in the periods before and after that peak to see if any change in trend is discernible in the ozone record. Prior to 1998, trends in the upper stratosphere (~ 45 km, 4 hPa) are found to be −5 to −10% per decade at mid-latitudes and closer to −5% per decade in the tropics. No trends are found in the mid-stratosphere (28 km, 30 hPa). Negative trends are seen in the lower stratosphere at mid-latitudes in both hemispheres and in the deep tropics. However it is hard to be categorical about the trends in the lower stratosphere for three reasons: (i) there are fewer measurements, (ii) the data quality is poorer, and (iii) the measurements in the 1990s are perturbed by aerosols from the Mt. Pinatubo eruption in 1991. These findings are similar to those reported previously even though the measurements for the two main satellite instruments (SBUV and SAGE II) and the ground-based Umkehr and ozonesonde stations have been revised. There is no sign of a continued negative trend in the upper stratosphere since 1998: instead there is a hint of an average positive trend of ~ 2% per decade in mid-latitudes and ~ 3% per decade in the tropics. The significance of these upward trends is investigated using different assumptions of the independence of the trend estimates found from different datasets. The averaged upward trends are significant if the trends derived from various datasets are assumed to be independent, but are generally not significant if the trends are not independent. This arises because many of the underlying measurement records are used in more than one merged dataset. At this point it is not possible to say which assumption is best. Including an estimate of the drift of the overall ozone observing system decreases the significance of the trends. The significance will become clearer as (i) more years are added to the observational record, (ii) further improvements are made to the historic ozone record (e.g. through algorithm development), and (iii) the data merging techniques are refined, particularly through a more rigorous treatment of uncertainties.

Description: Future trends in Arctic springtime total column ozone, and its chemical and dynamical drivers, are assessed using a 7 member ensemble from the Met Office Unified Model with United Kingdom Chemistry and Aerosols (UM-UKCA) simulating the period 1960-2100. The Arctic mean March total column ozone increases throughout the 21st century at a rate of ~11.5 DU decade-1, and is projected to return to the 1980 level in the late 2030s. However, the integrations show that even past 2060 springtime Arctic ozone can episodically drop by ~50-100 DU below the long-term mean to near present day values. Consistent with the global decline in inorganic chlorine (Cly) over the century, the estimated mean halogen induced chemical ozone loss in the Arctic lower atmosphere in spring decreases by around a factor of two between 1981-2000 and 2061-2080. However, in the presence of a cold and strong polar vortex elevated halogen losses well above the long-term mean continue to occur in the simulations into the second part of the century. The ensemble shows a radiatively-driven cooling trend modelled in the Arctic winter mid- and upper stratosphere, but there is less consistency across the seven ensemble members in the lower stratosphere (100-50 hPa). This is partly due to an increase in downwelling over the Arctic polar cap in winter, which increases transport of ozone into the polar region as well as drives adiabatic warming that partly offsets the radiatively-driven stratospheric cooling. However, individual years characterised by significantly suppressed downwelling, reduced transport and low temperatures continue into the future. We conclude that despite the future long-term recovery of Arctic ozone, the large interannual dynamical variability is expected to continue thereby facilitating episodic reductions in springtime ozone columns. Whilst our results suggest that the relative role of dynamical processes for determining Arctic springtime ozone will increase in the future, halogen chemistry will remain a smaller but non-negligible contributor for many decades.

Description: The impact of changes in incoming solar ultraviolet irradiance on stratospheric ozone forms an important part of the climate response to solar variability. To realistically simulate the climate response to solar variability using climate models, a minimum requirement is that they should include a solar cycle ozone component that has a realistic amplitude and structure, and which varies with season. For climate models that do not include interactive ozone chemistry, this component must be derived from observations and/or chemistry–climate model simulations and included in an externally prescribed ozone database that also includes the effects of all major external forcings. Part 1 of this two part study presents the solar-ozone responses in a number of updated satellite datasets for the period 1984–2004, including the Stratospheric Aerosol and Gas Experiment (SAGE) II version 6.2 and version 7.0 data, and the Solar Backscatter Ultraviolet Instrument (SBUV) version 8.0 and version 8.6 data. A number of combined datasets, which have extended SAGE II using more recent satellite measurements, are also analysed for the period 1984–2011. It is shown that SAGE II derived solar-ozone signals are sensitive to the independent temperature measurements used to convert ozone number density to mixing ratio units. A change in these temperature measurements in the recent SAGE II v7.0 data leads to substantial differences in the mixing ratio solar-ozone response compared to the previous v6.2, particularly in the tropical upper stratosphere. We also show that alternate satellite ozone datasets have issues (e.g., sparse spatial and temporal sampling, low vertical resolution, and shortness of measurement record), and that the methods of accounting for instrument offsets and drifts in merged satellite datasets can have a substantial impact on the solar cycle signal in ozone. For example, the magnitude of the solar-ozone response varies by around a factor of two across different versions of the SBUV VN8.6 record, which appears to be due to the methods used to combine the separate SBUV timeseries. These factors make it difficult to extract more than an annual-mean solar-ozone response from the available satellite observations. It is therefore unlikely that satellite ozone measurements alone can be applied to estimate the necessary solar cycle ozone component of the prescribed ozone database for future coupled model intercomparison projects (e.g., CMIP6).

Description: Trends in the vertical distribution of ozone are reported and compared for a number of new and recently revised data sets. The amount of ozone-depleting compounds in the stratosphere (as measured by equivalent effective stratospheric chlorine – EESC) was maximised in the second half of the 1990s. We examine the periods before and after the peak to see if any change in trend is discernible in the ozone record that might be attributable to a change in the EESC trend, though no attribution is attempted. Prior to 1998, trends in the upper stratosphere (~ 45 km, 4 hPa) are found to be −5 to −10 % per decade at mid-latitudes and closer to −5 % per decade in the tropics. No trends are found in the mid-stratosphere (28 km, 30 hPa). Negative trends are seen in the lower stratosphere at mid-latitudes in both hemispheres and in the deep tropics. However, it is hard to be categorical about the trends in the lower stratosphere for three reasons: (i) there are fewer measurements, (ii) the data quality is poorer, and (iii) the measurements in the 1990s are perturbed by aerosols from the Mt Pinatubo eruption in 1991. These findings are similar to those reported previously even though the measurements for the main satellite and ground-based records have been revised. There is no sign of a continued negative trend in the upper stratosphere since 1998: instead there is a hint of an average positive trend of ~ 2 % per decade in mid-latitudes and ~ 3 % per decade in the tropics. The significance of these upward trends is investigated using different assumptions of the independence of the trend estimates found from different data sets. The averaged upward trends are significant if the trends derived from various data sets are assumed to be independent (as in Pawson et al., 2014) but are generally not significant if the trends are not independent. This occurs because many of the underlying measurement records are used in more than one merged data set. At this point it is not possible to say which assumption is best. Including an estimate of the drift of the overall ozone observing system decreases the significance of the trends. The significance will become clearer as (i) more years are added to the observational record, (ii) further improvements are made to the historic ozone record (e.g. through algorithm development), and (iii) the data merging techniques are refined, particularly through a more rigorous treatment of uncertainties.