Laura E. Revell

The effectiveness of N2O in depleting stratospheric ozone

Recently, it was shown that of the ozone-depleting substances currently emitted, N2O emissions (the primary source of stratospheric NOx) dominate, and are likely to do so throughout the 21st century. To investigate the links between N2O and NOx concentrations, and the effects of NOx on ozone in a changing climate, the evolution of stratospheric ozone from 1960 to 2100 was simulated using the NIWA-SOCOL chemistry-climate model. The yield of NOx from N2O is reduced due to stratospheric cooling and a strengthening of the Brewer-Dobson circulation. After accounting for the reduced NOx yield, additional weakening of the primary NOx cycle is attributed to reduced availability of atomic oxygen, due to a) stratospheric cooling decreasing the atomic oxygen/ozone ratio, and b) enhanced rates of chlorine-catalyzed ozone loss cycles around 2000 and enhanced rates of HOx-induced ozone depletion. Our results suggest that the effects of N2O on ozone depend on both the radiative and chemical environment of the upper stratosphere, specifically CO2-induced cooling of the stratosphere and elevated CH4 emissions which enhance HOx-induced ozone loss and remove the availability of atomic oxygen to participate in NOx ozone loss cycles.

The changing ozone depletion potential of N2O in a future climate

Nitrous oxide (N2O), which decomposes in the stratosphere to form nitrogen oxides (NOx), is currently the dominant anthropogenic ozone-depleting substance emitted. Ozone depletion potentials (ODPs) of specific compounds, commonly evaluated for present-day conditions, were developed for long-lived halocarbons and are used by policymakers to inform decision-making around protection of the ozone layer. However, the effect of N2O on ozone will evolve in the future due to changes in stratospheric dynamics and chemistry induced by rising levels of greenhouse gases. Despite the fact that NOx-induced ozone loss slows with increasing concentrations of CO2 and CH4, we show that ODPN2O for year 2100 varies under different scenarios and is mostly larger than ODPN2O for year 2000. This occurs because the traditional ODP approach is tied to ozone depletion induced by CFC-11, which is also sensitive to CO2 and CH4. We therefore suggest that a single ODP for N2O is of limited use.

The influence of absorbed solar radiation by Saharan dust on hurricane genesis

To date, the radiative impact of dust and the Saharan air layer (SAL) on North Atlantic hurricane activity is not yet known. According to previous studies, dust stabilizes the atmosphere due to absorption of solar radiation but thus shifts convection to regions more conducive for hurricane genesis. Here we analyze differences in hurricane genesis and frequency from ensemble sensitivity simulations with radiatively active and inactive dust in the aerosol-climate model ECHAM6-HAM. We investigate dust burden and other hurricane-related variables and determine their influence on disturbances which develop into hurricanes (developing disturbances, DDs) and those which do not (nondeveloping disturbances, NDDs). Dust and the SAL are found to potentially have both inhibiting and supporting influences on background conditions for hurricane genesis. A slight southward shift of DDs is determined when dust is active as well as a significant warming of the SAL, which leads to a strengthening of the vertical circulation associated with the SAL. The dust burden of DDs is smaller in active dust simulations compared to DDs in simulations with inactive dust, while NDDs contain more dust in active dust simulations. However, no significant influence of radiatively active dust on other variables in DDs and NDDs is found. Furthermore, no substantial change in the DD and NDD frequency due to the radiative effects of dust can be detected.

The representation of solar cycle signals in stratospheric ozone. Part II: Analysis of global models

Monthly and zonal mean coefficients for the 11 year solar cycle effect on stratospheric ozone derived from the CMIP6 ozone dataset. The coefficients are provided on a 3-D (latitude-pressure-month) grid and are derived using multiple linear regression of ozone against either: (1) the F10.7cm solar radio flux (cmip6_solar-o3_coeffs_per_SFU.nc); and (2) the 200-320 nm integrated spectral solar irradiance (cmip6_solar-o3_coeffs_per_Wm-2.nc) for the period 1960-2011. The coefficients are provided in terms of both % and mol mol-1 of ozone change. Also included are p-values for the ozone coefficients as a function of latitude-pressure-month. The dataset is provided in NetCDF format.

Stratospheric ozone loss over the Eurasian continent induced by the polar vortex shift

The Montreal Protocol has succeeded in limiting major ozone-depleting substance emissions, and consequently stratospheric ozone concentrations are expected to recover this century. However, there is a large uncertainty in the rate of regional ozone recovery in the Northern Hemisphere. Here we identify a Eurasia-North America dipole mode in the total column ozone over the Northern Hemisphere, showing negative and positive total column ozone anomaly centres over Eurasia and North America, respectively. The positive trend of this mode explains an enhanced total column ozone decline over the Eurasian continent in the past three decades, which is closely related to the polar vortex shift towards Eurasia. Multiple chemistry-climate-model simulations indicate that the positive Eurasia-North America dipole trend in late winter is likely to continue in the near future. Our findings suggest that the anticipated ozone recovery in late winter will be sensitive not only to the ozone-depleting substance decline but also to the polar vortex changes, and could be substantially delayed in some regions of the Northern Hemisphere extratropics.Climate change can exert a significant effect on the ozone recovery. Here, the authors show that the Arctic polar vortex shift associated with Arctic sea-ice loss could slow down ozone recovery over the Eurasian continent.

On the aliasing of the solar cycle in the lower stratospheric tropical temperature

The double-peaked response of the tropical stratospheric temperature profile to the 11-year solar cycle (SC) has been well documented. However, there are concerns about the origin of the lower peak due to potential aliasing with volcanic eruptions or the El Nino Southern Oscillation (ENSO) detected using multiple linear regression (MLR) analysis. We confirm the aliasing using the results of the chemistry-climate model (CCM) SOCOLv3 obtained in the framework of the IGAC/SPAR Chemistry-Climate Model Initiative phase 1 (CCMI-1). We further show that, even without major volcanic eruptions included in transient simulations, the lower stratospheric response exhibits a residual peak when historical sea surface temperatures (SST)/sea ice coverage (SIC) are used. Only the use of climatological SSTs/SICs in addition to background stratospheric aerosols removes volcanic and ENSO signals and results in an almost complete disappearance of the modeled solar signal in the lower stratospheric temperature. We demonstrate that the choice of temporal sub-period considered for the regression analysis has a large impact on the estimated profile signal in the lower stratosphere: at least 45 consecutive years are needed to avoid the large aliasing effect of SC maxima with volcanic eruptions in 1982 and 1991 in historical simulations, reanalyses and observations. The application of volcanic forcing compiled for phase 6 of the Coupled Model Intercomparison Project (CMIP6) in the CCM SOCOLv3 reduces the warming overestimation in the tropical lower stratosphere and the volcanic aliasing of the temperature response to the SC, although it does not eliminate it completely.

Stratospheric Injection of Brominated Very Short‐Lived Substances: Aircraft Observations in the Western Pacific and Representation in Global Models

We quantify the stratospheric injection of brominated very short‐lived substances (VSLS) based on aircraft observations acquired in winter 2014 above the Tropical Western Pacific during the CONvective TRansport of Active Species in the Tropics (CONTRAST) and the Airborne Tropical TRopopause EXperiment (ATTREX) campaigns. The overall contribution of VSLS to stratospheric bromine was determined to be 5.0 ± 2.1 ppt, in agreement with the 5 ± 3 ppt estimate provided in the 2014 World Meteorological Organization (WMO) Ozone Assessment report (WMO 2014), but with lower uncertainty. Measurements of organic bromine compounds, including VSLS, were analyzed using CFC‐11 as a reference stratospheric tracer. From this analysis, 2.9 ± 0.6 ppt of bromine enters the stratosphere via organic source gas injection of VSLS. This value is two times the mean bromine content of VSLS measured at the tropical tropopause, for regions outside of the Tropical Western Pacific, summarized in WMO 2014. A photochemical box model, constrained to CONTRAST observations, was used to estimate inorganic bromine from measurements of BrO collected by two instruments. The analysis indicates that 2.1 ± 2.1 ppt of bromine enters the stratosphere via inorganic product gas injection. We also examine the representation of brominated VSLS within 14 global models that participated in the Chemistry‐Climate Model Initiative. The representation of stratospheric bromine in these models generally lies within the range of our empirical estimate. Models that include explicit representations of VSLS compare better with bromine observations in the lower stratosphere than models that utilize longer‐lived chemicals as a surrogate for VSLS.

Formaldehyde in the Tropical Western Pacific: Chemical Sources and Sinks, Convective Transport, and Representation in CAM-Chem and the CCMI Models

Formaldehyde (HCHO) directly affects the atmospheric oxidative capacity through its effects on HOx. In remote marine environments, such as the Tropical Western Pacific (TWP), it is particularly important to understand the processes controlling the abundance of HCHO because model output from these regions is used to correct satellite retrievals of HCHO. Here, we have used observations from the CONTRAST field campaign, conducted during January and February 2014, to evaluate our understanding of the processes controlling the distribution of HCHO in the TWP as well as its representation in chemical transport/climate models. Observed HCHO mixing ratios varied from ~500 pptv near the surface to ~75 pptv in the upper troposphere. Recent convective transport of near surface HCHO and its precursors, acetaldehyde and possibly methyl hydroperoxide, increased upper tropospheric HCHO mixing ratios by ~33% (22 pptv); this air contained roughly 60% less NO than more aged air. Output from the CAM-Chem chemistry transport model (2014 meteorology) as well as nine chemistry climate models from the Chemistry-Climate Model Initiative (free-running meteorology) are found to uniformly underestimate HCHO columns derived from in situ observations by between 4 and 50%. This underestimate of HCHO likely results from a near factor of two underestimate of NO in most models, which strongly suggests errors in NOx emissions inventories and/or in the model chemical mechanisms. Likewise, the lack of oceanic acetaldehyde emissions and potential errors in the model acetaldehyde chemistry lead to additional underestimates in modeled HCHO of up to 75 pptv (~15%) in the lower troposphere.

Revisiting the Mystery of Recent Stratospheric Temperature Trends

Simulated stratospheric temperatures over the period 1979-2016 in models from the Chemistry-Climate Model Initiative (CCMI) are compared with recently updated and extended satellite observations. The multi-model mean global temperature trends over 1979- 2005 are -0.88 ± 0.23, -0.70 ± 0.16, and -0.50 ± 0.12 K decade-1 for the Stratospheric Sounding Unit (SSU) channels 3 (~40-50 km), 2 (~35-45 km), and 1 (~25-35 km), respectively. These are within the uncertainty bounds of the observed temperature trends from two reprocessed satellite datasets. In the lower stratosphere, the multi-model mean trend in global temperature for the Microwave Sounding Unit channel 4 (~13-22 km) is -0.25 ± 0.12 K decade-1 over 1979-2005, consistent with estimates from three versions of this satellite record. The simulated stratospheric temperature trends in CCMI models over 1979-2005 agree with the previous generation of chemistry-climate models. The models and an extended satellite dataset of SSU with the Advanced Microwave Sounding Unit-A show weaker global stratospheric cooling over 1998-2016 compared to the period of intensive ozone depletion (1979-1997). This is due to the reduction in ozone-induced cooling from the slow-down of ozone trends and the onset of ozone recovery since the late 1990s. In summary, the results show much better consistency between simulated and satellite observed stratospheric temperature trends than was reported by Thompson et al. (2012) for the previous versions of the SSU record and chemistry-climate models. The improved agreement mainly comes from updates to the satellite records; the range of simulated trends is comparable to the previous generation of models.

Tropospheric ozone in CCMI models and Gaussian emulation to understand biases in the SOCOLv3 chemistry-climate model

Previous multi-model intercomparisons have shown that chemistry-climate models exhibit significant biases in tropospheric ozone compared with observations. We investigate annual-mean tropospheric column ozone in 15 models participating in the SPARC/IGAC (Stratosphere-troposphere Processes and their Role in Climate/International Global Atmospheric Chemistry) Chemistry-Climate Model Initiative (CCMI). These models exhibit a positive bias, on average, of up to 40–50% in the Northern Hemisphere compared with observations derived from the Ozone Monitoring Instrument and Microwave Limb 5 Sounder (OMI/MLS), and a negative bias of up to ∼30% in the Southern Hemisphere. SOCOLv3.0 (version 3 of the SolarClimate Ozone Links CCM), which participated in CCMI, simulates global-mean tropospheric ozone columns of 40.2 DU – approximately 33% larger than the CCMI multi-model mean. Here we introduce an updated version of SOCOLv3.0, “SO1 Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-615 Manuscript under review for journal Atmos. Chem. Phys. Discussion started: 26 June 2018 c