Changes In O3 Research Articles

Long‐term changes in lower tropospheric baseline ozone concentrations: Comparing chemistry‐climate models and observations at northern midlatitudes

AbstractTwo recent papers have quantified long‐term ozone (O3) changes observed at northern midlatitude sites that are believed to represent baseline (here understood as representative of continental to hemispheric scales) conditions. Three chemistry‐climate models (NCAR CAM‐chem, GFDL‐CM3, and GISS‐E2‐R) have calculated retrospective tropospheric O3 concentrations as part of the Atmospheric Chemistry and Climate Model Intercomparison Project and Coupled Model Intercomparison Project Phase 5 model intercomparisons. We present an approach for quantitative comparisons of model results with measurements for seasonally averaged O3 concentrations. There is considerable qualitative agreement between the measurements and the models, but there are also substantial and consistent quantitative disagreements. Most notably, models (1) overestimate absolute O3 mixing ratios, on average by ~5 to 17 ppbv in the year 2000, (2) capture only ~50% of O3 changes observed over the past five to six decades, and little of observed seasonal differences, and (3) capture ~25 to 45% of the rate of change of the long‐term changes. These disagreements are significant enough to indicate that only limited confidence can be placed on estimates of present‐day radiative forcing of tropospheric O3 derived from modeled historic concentration changes and on predicted future O3 concentrations. Evidently our understanding of tropospheric O3, or the incorporation of chemistry and transport processes into current chemical climate models, is incomplete. Modeled O3 trends approximately parallel estimated trends in anthropogenic emissions of NOx, an important O3 precursor, while measured O3 changes increase more rapidly than these emission estimates.

Source, transport and impacts of a heavy dust event in the Yangtze River Delta, China, in 2011

Abstract. Dust invasion is an important type of particle pollution in China. During 1 to 6 May in 2011, a dust event was observed in the Yangtze River Delta region (YRD). The highest PM10 (particles up to 10 μ in diameter) concentration reached over 1000 μg m−3 and the visibility was below 3 km. In this study, the Community Multi-scale Air Quality modeling system (CMAQ5.0) coupled with an in-line windblown dust model was used to simulate the formation, spatial and temporal characteristics of this dust event, and analyze its impacts. The threshold friction velocity for loose, fine-grained soil with low surface roughness in the dust model was revised based on Chinese data to improve the model performance. This dust storm broke out in Xinjiang and Mongolia during 28 to 30 April and arrived in the YRD region on 1 May. The transported dust particles contributed to the mean surface layer concentrations of PM10 in the YRD region 78.9% during 1 to 6 May with their impact weakening from north to south due to the removal of dust particles along the path. The dry deposition, wet deposition and total deposition of PM10 in the YRD reached 184.7 kt, 172.6 kt and 357.32 kt, respectively. The dust particles also had significant impacts on optical/radiative characteristics by absorption and scattering. In Shanghai, the largest perturbations of aerosol optical depth (AOD) and irradiance were about 0.8 DU and −130 W m−2, which could obviously influence the radiation balance in this region. The decrease of actinic fluxes impacts future photochemistry. In Shanghai, the negative effects on the NO2 and O3 photolysis could be −35% when dust particles arrived. The concentrations of O3 and OH were reduced by 1.5% and 3.1% in the whole of China, and by 9.4% and 12.1% in the YRD region, respectively. Such changes in O3 and OH levels can affect the future formation of secondary aerosols in the atmosphere by directly determining the oxidation rate of their precursors. The work of this manuscript is meaningful for understanding the dust emissions in China as well as for the application of CMAQ in Asia. It is also helpful for understanding the formation mechanism and impacts of dust pollution in the YRD.

UV Sensitivity to Changes in Ozone, Aerosols, and Clouds in Seoul, South Korea

AbstractThe total ozone (O3) and aerosol optical depth (AOD) at 320 nm have been observed from the ultraviolet (UV) measurements made at Yonsei University in Seoul, South Korea, with Dobson and Brewer spectrophotometers, respectively, during 2004–10. The daily datasets are analyzed to show the sensitivities of UV radiation to changes in O3, AOD, and cloud cover (CC) together with global solar radiation (GS), including the long-term characteristics of surface UV irradiance in Seoul. The UV sensitivities show that 1% increases of O3 and AOD relative to their reference values under all- and clear-sky conditions similarly manifest as 1–1.2% and 0.2% decreases of both daily erythemal UV (EUV) and total UV (TUV) irradiance at the ground level except for TUV sensitivity to O3 (~0.3%). Those UV sensitivities to CC and GS changes are associated with a 0.12% decrease and 0.7% increase, respectively, in fractional UV changes. The trends show that the positive trends of O3 (+7.2% decade−1), AOD (+22.4% decade−1), and CC (+52.4% decade−1) induce negative trends in EUV (−8.4% decade−1) and TUV (−2.5% decade−1), in both UV (−4.7% decade−1), and in EUV (−6.3% decade−1) and TUV (−6.8% decade−1), respectively. On the basis of the multiple linear regression analyses, it is found that UV sensitivity to O3 is relatively high in the forcing factors, but the contributions of the UV forcing factors to the daily variability and the range of UV disturbances due to the variability of the forcing factors are affected more by AOD than by O3 and CC in both UV fractional changes.

Modelling the impact of megacities on local, regional and global tropospheric ozone and the deposition of nitrogen species

Abstract. We examine the effects of ozone precursor emissions from megacities on present-day air quality using the global chemistry–climate model UM-UKCA (UK Met Office Unified Model coupled to the UK Chemistry and Aerosols model). The sensitivity of megacity and regional ozone to local emissions, both from within the megacity and from surrounding regions, is important for determining air quality across many scales, which in turn is key for reducing human exposure to high levels of pollutants. We use two methods, perturbation and tagging, to quantify the impact of megacity emissions on global ozone. We also completely redistribute the anthropogenic emissions from megacities, to compare changes in local air quality going from centralised, densely populated megacities to decentralised, lower density urban areas. Focus is placed not only on how changes to megacity emissions affect regional and global NOx and O3, but also on changes to NOy deposition and to local chemical environments which are perturbed by the emission changes. The perturbation and tagging methods show broadly similar megacity impacts on total ozone, with the perturbation method underestimating the contribution partially because it perturbs the background chemical environment. The total redistribution of megacity emissions locally shifts the chemical environment towards more NOx-limited conditions in the megacities, which is more conducive to ozone production, and monthly mean surface ozone is found to increase up to 30% in megacities, depending on latitude and season. However, the displacement of emissions has little effect on the global annual ozone burden (0.12% change). Globally, megacity emissions are shown to contribute ~3% of total NOy deposition. The changes in O3, NOx and NOy deposition described here are useful for quantifying megacity impacts and for understanding the sensitivity of megacity regions to local emissions. The small global effects of the 100% redistribution carried out in this study suggest that the distribution of emissions on the local scale is unlikely to have large implications for chemistry–climate processes on the global scale.

Optimizing the emission inventory of volatile organic compounds (VOCs) based on network observations

Hourly observations of 56 non-methane hydrocarbons (NMHCs) performed by a network of photochemical assessment monitoring stations (PAMS) at 11 locations across Taiwan were used to evaluate 56 speciated emissions and the resulting simulations of an air quality model. Based on the PAMS observations at two urban sites, emission modification was made for the 56 PAMS species in the model. To further test the applicability of this emission correction approach, the same modified emissions were subject to seven different meteorological conditions and comparison with observations of all the 11 PAMS sites. Originally there was a minimum of only 8 of 56 species showed agreement with observations for the worst of the 11 PAMS sites and 28 of 56 species for the best site. With modified emissions, the number increased to 13–52 species across the 11 PAMS sites, demonstrating that the simple urban based correction procedure has broad applicability. When applying this modification of PAMS emissions to the simulations of other air quality gases, SO2 and NOx showed small changes compared with observations (−0.27% and −2.51%, respectively), while total VOC concentrations showed significant changes (+15.28%) as a result of the adjustment in VOC emissions (+26.7%). Although VOCs are the precursor of ozone, the relatively large changes in VOC did not seem to affect ozone formation to the similar extent, only resulting in the changes of average O3 by 2.9 ppb (+9.41%). It shows that although the emission modification improves individual VOC simulations, the performance in oxidant simulation is still largely unaltered. Although the original U.S. VOC emission profiles can capture the general features of ambient VOCs, further optimization of emissions may still be needed by referencing extensive observations, so that emissions can better fit domestic conditions and accuracy in model simulations can be improved.

Crystal and Magnetic Structure in Co-Substituted BiFeO3

Ultra-high-resolution neutron diffraction studies of BiFe(0.8)Co(0.2)O3 show a transition from a cycloidal space modulated spin structure at T = 10 K to a collinear G-type antiferromagnetic structure at T = 120 K. The model of antiparallel directions of Fe(3+) and Co(3+) magnetic moments at the shared Wyckoff position describes well the observed neutron diffraction intensities. On heating above RT, the crystal structure of BiFe(0.8)Co(0.2)O3 changes from a rhombohedral R3c to a monoclinic Cm. At 573 K only the Cm phase is present. The collinear C-type antiferromagnetic structure is present in the Cm phase of BiFe(0.8)Co(0.2)O3 at RT after annealing.

Stratospheric O<sub>3</sub> changes during 2001–2010: the small role of solar flux variations in a chemical transport model

Abstract. Solar spectral fluxes (or irradiance) measured by the SOlar Radiation and Climate Experiment (SORCE) show different variability at ultraviolet (UV) wavelengths compared to other irradiance measurements and models (e.g. NRL-SSI, SATIRE-S). Some modelling studies have suggested that stratospheric/lower mesospheric O3 changes during solar cycle 23 (1996–2008) can only be reproduced if SORCE solar fluxes are used. We have used a 3-D chemical transport model (CTM), forced by meteorology from the European Centre for Medium-Range Weather Forecasts (ECMWF), to simulate middle atmospheric O3 using three different solar flux data sets (SORCE, NRL-SSI and SATIRE-S). Simulated O3 changes are compared with Microwave Limb Sounder (MLS) and Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) satellite data. Modelled O3 anomalies from all solar flux data sets show good agreement with the observations, despite the different flux variations. The off-line CTM reproduces these changes through dynamical information contained in the analyses. A notable feature during this period is a robust positive solar signal in the tropical middle stratosphere, which is due to realistic dynamical changes in our simulations. Ozone changes in the lower mesosphere cannot be used to discriminate between solar flux data sets due to large uncertainties and the short time span of the observations. Overall this study suggests that, in a CTM, the UV variations detected by SORCE are not necessary to reproduce observed stratospheric O3 changes during 2001–2010.

Health burdens of surface ozone in the UK for a range of future scenarios

Exposure to surface ozone (O3), which is influenced by emissions of precursor chemical species, meteorology and population distribution, is associated with excess mortality and respiratory morbidity. In this study, the EMEP-WRF atmospheric chemistry transport model was used to simulate surface O3 concentrations at 5km horizontal resolution over the British Isles for a baseline year of 2003, for three anthropogenic emissions scenarios for 2030, and for a +5°C increase in air temperature on the 2003 baseline. Deaths brought forward and hospitalisation burdens for 12 UK regions were calculated from population-weighted daily maximum 8-hour O3. The magnitude of changes in annual mean surface O3 over the UK for +5°C temperature (+1.0 to +1.5ppbv, depending on region) was comparable to those due to inter-annual meteorological variability (−1.5 to +1.5ppbv) but considerably less than changes due to precursor emissions changes by 2030 (−3.0 to +3.5ppbv, depending on scenario and region). Including population changes in 2030, both the ‘current legislation’ and ‘maximum feasible reduction’ scenarios yield greater O3-attributable health burdens than the ‘high’ emission scenario: +28%, +22%, and +16%, respectively, above 2003 baseline deaths brought forward (11,500) and respiratory hospital admissions (30,700), using O3 exposure over the full year and no threshold for health effects. The health burdens are greatest under the ‘current legislation’ scenario because O3 concentrations increase as a result of both increases in background O3 concentration and decreases in UK NOx emissions. For the +5°C scenario, and no threshold (and not including population increases), total UK health burden increases by 500 premature deaths (4%) relative to the 2003 baseline. If a 35ppbv threshold for O3 effects is assumed, health burdens are more sensitive to the current legislation and +5°C scenarios, although total health burdens are roughly an order of magnitude lower. In all scenarios, the assumption of a threshold increases the proportion of health burden in the south and east of the UK compared with the no threshold assumption. The study highlights that the total, and geographically-apportioned, O3-attributable health burdens in the UK are highly sensitive to the future trends of hemispheric, regional and local emissions of O3 precursors, and to the assumption of a threshold for O3 effect.

A global model study of the impact of land-use change in Borneo on atmospheric composition

Abstract. In this study, a high resolution version of the Cambridge p-TOMCAT chemical transport model is used, along with measurement data from the 2008 NERC-funded Oxidant and Particle Photochemical Processes (OP3) project, to examine the potential impact of the expansion of oil palm in Borneo on atmospheric composition. Several model emission scenarios are run for the OP3 measurement period, incorporating emissions from both global datasets and local flux measurements. Using the OP3 observed isoprene fluxes and OH recycling chemistry in p-TOMCAT substantially improves the comparison between modelled and observed isoprene and OH concentrations relative to using MEGAN isoprene emissions without OH recycling. However, a similar improvement was also achieved without using HOx recycling, by fixing boundary layer isoprene concentrations over Borneo to follow the OP3 observations. An extreme hypothetical future scenario, in which all of Borneo is converted to oil palm plantation, assessed the sensitivity of the model to changes in isoprene and NOx emissions associated with land-use change. This scenario suggested a 70% upper limit on surface ozone increases resulting from land-use change on Borneo, excluding the impact of future changes in emissions elsewhere. Although the largest changes in this scenario occurred directly over Borneo, the model also calculated notable regional changes of O3, OH and other species downwind of Borneo and in the free troposphere.

Impacts of 21st century climate change on global air pollution-related premature mortality

Climate change modulates surface concentrations of fine particulate matter (PM2.5) and ozone (O3), indirectly affecting premature mortality attributed to air pollution. We estimate the change in global premature mortality and years of life lost (YLL) associated with changes in surface O3 and PM2.5 over the 21st century as a result of climate change. We use a global coupled chemistry-climate model to simulate current and future climate and the effect of changing climate on air quality. Epidemiological concentration-response relationships are applied to estimate resulting changes in premature mortality and YLL. The effect of climate change on air quality is isolated by holding emissions of air pollutants constant while allowing climate to evolve over the 21st century according to a moderate projection of greenhouse gas emissions (A1B scenario). Resulting changes in 21st century climate alone lead to an increase in simulated PM2.5 concentrations globally, and to higher (lower) O3 concentrations over populated (remote) regions. Global annual premature mortality associated with chronic exposure to PM2.5 increases by approximately 100 thousand deaths (95 % confidence interval, CI, of 66–130 thousand) with corresponding YLL increasing by nearly 900 thousand (95 % CI, 576–1,128 thousand) years. The annual premature mortality due to respiratory disease associated with chronic O3 exposure increases by +6,300 deaths (95 % CI, 1,600–10,400). This climate penalty indicates that stronger emission controls will be needed in the future to meet current air quality standards and to avoid higher health risks associated with climate change induced worsening of air quality over populated regions.

Structures and magnetic properties of Tm1−y Y y Mn1−x Co x O3

The structure and magnetic properties of Tm1−y Y y Mn1−x Co x O3 with 0 ≦ x ≦ 0.5 and 0 ≦ y ≦ 0.3 were investigated by X-ray diffraction, specific heat and magnetization measurements. Thulium manganite TmMnO3 prepared by solid-state synthesis at ambient pressure is hexagonal and antiferromagnetic with a Nèel temperature T N of 86 K. The substitution of Y for Tm in TmMnO3 does not greatly affect the fundamental hexagonal structure. The magnetization and specific heat measurement results for Tm1−y Y y MnO3 can be qualitatively explained in terms of the dilution effect of Tm by Y. On the other hand, the structure of TmMn1−x Co x O3 changes gradually from hexagonal to orthorhombic with the substitution of Co for Mn; hexagonal and orthorhombic phases coexist in samples for x ≦ 0.3 whereas TmMn0.6Co0.4O3 is almost a single orthorhombic phase. The magnetization of TmMn0.6Co0.4O3 in a field of 250 Oe increases rapidly at about 60K with decreasing temperature. The difference between zero-field-cooled (ZFC) and field-cooled (FC) magnetizations increases remarkably at about 60 K. Moreover, the temperature dependences of the ZFC and the FC magnetizations exhibit peaks at about 40 and 30K, respectively. Thus, TmMn1−x Co x O3 exhibits complex magnetic properties.

The role of the solar irradiance variability in the evolution of the middle atmosphere during 2004–2009

AbstractRecent measurements by the Spectral Irradiance Monitor (SIM) and the Solar Stellar Irradiance Comparison Experiment (SOLSTICE) onboard the Solar Radiation and Climate Experiment satellite have revealed the spectral solar irradiance (SSI) changes in the ultraviolet between 2004 and 2009 to be several times higher than it was shown by all previous SSI measurements and reconstructions. In this paper, we simulate the O3, OH, and temperature responses to solar irradiance variability using four different SSI data sets trying to define which one gives the best agreement between the simulated and observed responses. First, we apply the 1‐D radiative‐convective model with interactive photochemistry to determine the regions of the atmosphere where the O3, OH, and temperature are most sensitive to the spectrum discrepancies between the different SSI data sets. As the comparison with observations can be only made taking into account dynamics and all known forcings of the atmosphere, we then apply the 3‐D chemistry‐climate model SOCOL to simulate the atmosphere evolution from May 2004 to February 2009. We compare the modeled OH, O3, and temperature changes with atmospheric data measured by several space instruments. Overall, the comparison shows that the atmospheric changes simulated with the 3‐D SOCOL model driven by the SIM and SOLSTICE SSI are closest to the atmospheric measurements.

Impacts of climate change on surface ozone and intercontinental ozone pollution: A multi‐model study

AbstractThe impact of climate change between 2000 and 2095 SRES A2 climates on surface ozone (O)3 and on O3 source‐receptor (S‐R) relationships is quantified using three coupled climate‐chemistry models (CCMs). The CCMs exhibit considerable variability in the spatial extent and location of surface O3 increases that occur within parts of high NOx emission source regions (up to 6 ppbv in the annual average and up to 14 ppbv in the season of maximum O3). In these source regions, all three CCMs show a positive relationship between surface O3 change and temperature change. Sensitivity simulations show that a combination of three individual chemical processes—(i) enhanced PAN decomposition, (ii) higher water vapor concentrations, and (iii) enhanced isoprene emission—largely reproduces the global spatial pattern of annual‐mean surface O3 response due to climate change (R2 = 0.52). Changes in climate are found to exert a stronger control on the annual‐mean surface O3 response through changes in climate‐sensitive O3 chemistry than through changes in transport as evaluated from idealized CO‐like tracer concentrations. All three CCMs exhibit a similar spatial pattern of annual‐mean surface O3 change to 20% regional O3 precursor emission reductions under future climate compared to the same emission reductions applied under present‐day climate. The surface O3 response to emission reductions is larger over the source region and smaller downwind in the future than under present‐day conditions. All three CCMs show areas within Europe where regional emission reductions larger than 20% are required to compensate climate change impacts on annual‐mean surface O3.

Ozone is associated with cardiopulmonary and stroke emergency hospital visits in Reykjavík, Iceland 2003–2009

BackgroundAir pollution exposure is associated with hospital admissions and emergency room visits for cardiopulmonary disease and stroke. Iceland’s capital area, Reykjavik, has generally low air pollution levels, but traffic and natural sources contribute to pollution levels. The objective of this study was to investigate temporal associations between emergency hospital visits and air pollutants ozone (O3), nitrogen dioxide (NO2), and particulate matter (PM10) in the Icelandic capital area.MethodsWe constructed a time series of the daily number of adults who visited the emergency room, or were acutely admitted for stroke or cardiorespiratory causes to Landspitali University Hospital 1 January 2003 – 31 December 2009 from the hospital in-patient register. We used generalized additive models assuming Poisson distribution, to analyze the daily emergency hospital visits as a function of the pollutant levels, and adjusted for meteorological variables, day of week, and time trend with splines.ResultsDaily emergency hospital visits increased 3.9% (95% confidence interval (CI) 1.7-6.1%) per interquartile (IQR) change in average O3 the same and two previous days. For females, the increase was 7.8% (95% CI 3.6-12.1) for elderly (70+), the increase was 3.9% (95% CI 0.6-7.3%) per IQR increase of NO2. There were no associations with PM10.ConclusionsWe found an increase in daily emergency hospital visits associated with O3, indicating that low-level exposure may trigger cardiopulmonary events or stroke.

Sensitivity of tropospheric oxidants to biomass burning emissions: implications for radiative forcing

AbstractBiomass burning is one of the largest sources of trace gases and aerosols to the atmosphere and has profound influence on tropospheric oxidants and radiative forcing. Using a fully coupled chemistry‐climate model (GFDL AM3), we find that co‐emission of trace gases and aerosol from present‐day biomass burning increases the global tropospheric ozone burden by 5.1% and decreases global mean OH by 6.3%. Gas and aerosol emissions combine to increase CH4 lifetime nonlinearly. Heterogeneous processes are shown to contribute partly to the observed lower ΔO3/ΔCO ratios in northern high latitudes versus tropical regions. The radiative forcing from biomass burning is shown to vary nonlinearly with biomass burning strength. At present‐day emission levels, biomass burning produces a net radiative forcing of −0.19 W/m2 (−0.29 from short‐lived species, mostly aerosol direct and indirect effects, +0.10 from CH4‐ and CH4‐induced changes in O3 and stratospheric H2O) but increases emissions to over 5 times present levels would result in a positive net forcing.

Tropospheric ozone changes, radiative forcing and attribution to emissions in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

Abstract. Ozone (O3) from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) has been used to calculate tropospheric ozone radiative forcings (RFs). All models applied a common set of anthropogenic emissions, which are better constrained for the present-day than the past. Future anthropogenic emissions follow the four Representative Concentration Pathway (RCP) scenarios, which define a relatively narrow range of possible air pollution emissions. We calculate a value for the pre-industrial (1750) to present-day (2010) tropospheric ozone RF of 410 mW m−2. The model range of pre-industrial to present-day changes in O3 produces a spread (±1 standard deviation) in RFs of ±17%. Three different radiation schemes were used – we find differences in RFs between schemes (for the same ozone fields) of ±10%. Applying two different tropopause definitions gives differences in RFs of ±3%. Given additional (unquantified) uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of ±30% for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (44±12%), nitrogen oxides (31 ± 9%), carbon monoxide (15 ± 3%) and non-methane volatile organic compounds (9 ± 2%); earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 42 mW m−2 DU−1, a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (mW m−2; relative to 1750) for the four future scenarios (RCP2.6, RCP4.5, RCP6.0 and RCP8.5) of 350, 420, 370 and 460 (in 2030), and 200, 300, 280 and 600 (in 2100). Models show some coherent responses of ozone to climate change: decreases in the tropical lower troposphere, associated with increases in water vapour; and increases in the sub-tropical to mid-latitude upper troposphere, associated with increases in lightning and stratosphere-to-troposphere transport. Climate change has relatively small impacts on global mean tropospheric ozone RF.

Spectral Fingerprints of Earth-like Planets Around FGK Stars

We present model atmospheres for an Earth-like planet orbiting the entire grid of main sequence FGK stars with effective temperatures ranging from Teff=4250 K to Teff=7000 K in 250 K intervals. We have modeled the remotely detectable spectra of Earth-like planets for clear and cloudy atmospheres at the 1 AU equivalent distance from the VIS to IR (0.4 to 20 μm) to compare detectability of features in different wavelength ranges in accordance with the James Webb Space Telescope and future design concepts to characterize exo-Earths. We have also explored the effect of the stellar UV levels as well as spectral energy distribution on a terrestrial atmosphere, concentrating on detectable atmospheric features that indicate habitability on Earth, namely, H2O, O3, CH4, N2O, and CH3Cl. The increase in UV dominates changes of O3, OH, CH4, N2O, and CH3Cl, whereas the increase in stellar temperature dominates changes in H2O. The overall effect as stellar effective temperatures and corresponding UV increase is a lower surface temperature of the planet due to a bigger part of the stellar flux being reflected at short wavelengths, as well as increased photolysis. Earth-like atmosphere models show more O3 and OH but less stratospheric CH4, N2O, CH3Cl, and tropospheric H2O (but more stratospheric H2O) with increasing effective temperature of main sequence stars. The corresponding detectable spectral features, on the other hand, show different detectability depending on the wavelength observed. We concentrate on directly imaged planets here as a framework to interpret future light curves, direct imaging, and secondary eclipse measurements of atmospheres of terrestrial planets in the habitable zone at varying orbital positions.

Air pollution and associated human mortality: the role of air pollutant emissions, climate change and methane concentration increases from the preindustrial period to present

Abstract. Increases in surface ozone (O3) and fine particulate matter (≤2.5 μm aerodynamic diameter, PM2.5) are associated with excess premature human mortalities. We estimate changes in surface O3 and PM2.5 from pre-industrial (1860) to present (2000) and the global present-day (2000) premature human mortalities associated with these changes. We extend previous work to differentiate the contribution of changes in three factors: emissions of short-lived air pollutants, climate change, and increased methane (CH4) concentrations, to air pollution levels and associated premature mortalities. We use a coupled chemistry-climate model in conjunction with global population distributions in 2000 to estimate exposure attributable to concentration changes since 1860 from each factor. Attributable mortalities are estimated using health impact functions of long-term relative risk estimates for O3 and PM2.5 from the epidemiology literature. We find global mean surface PM2.5 and health-relevant O3 (defined as the maximum 6-month mean of 1-h daily maximum O3 in a year) have increased by 8 ± 0.16 μg m−3 and 30 ± 0.16 ppbv (results reported as annual average ±standard deviation of 10-yr model simulations), respectively, over this industrial period as a result of combined changes in emissions of air pollutants (EMIS), climate (CLIM) and CH4 concentrations (TCH4). EMIS, CLIM and TCH4 cause global population-weighted average PM2.5 (O3) to change by +7.5 ± 0.19 μg m−3 (+25 ± 0.30 ppbv), +0.4 ± 0.17 μg m−3 (+0.5 ± 0.28 ppbv), and 0.04 ± 0.24 μg m−3 (+4.3 ± 0.33 ppbv), respectively. Total global changes in PM2.5 are associated with 1.5 (95% confidence interval, CI, 1.2–1.8) million cardiopulmonary mortalities and 95 (95% CI, 44–144) thousand lung cancer mortalities annually and changes in O3 are associated with 375 (95% CI, 129–592) thousand respiratory mortalities annually. Most air pollution mortality is driven by changes in emissions of short-lived air pollutants and their precursors (95% and 85% of mortalities from PM2.5 and O3 respectively). However, changing climate and increasing CH4 concentrations also contribute to premature mortality associated with air pollution globally (by up to 5% and 15%, respectively). In some regions, the contribution of climate change and increased CH4 together are responsible for more than 20% of the respiratory mortality associated with O3 exposure. We find the interaction between climate change and atmospheric chemistry has influenced atmospheric composition and human mortality associated with industrial air pollution. Our study highlights the benefits to air quality and human health of CH4 mitigation as a component of future air pollution control policy.

Houston’s rapid ozone increases: preconditions and geographic origins

Many of Houston's highest 8-h ozone (O3) peaks are characterised by increases in concentrations of at least 40 ppb in 1 h, or 60 ppb in 2 h. These rapid increases are called non-typical O3 changes (NTOCs). In 2004, the Texas Commission on Environmental Quality (TCEQ) developed a novel emissions control strategy aimed at eliminating NTOCs. The strategy limited routine and short-term emissions of ethene, propene, 1,3-butadiene and butene isomers, collectively called highly reactive volatile organic compounds (HRVOCs), which are released from petrochemical facilities. HRVOCs have been associated with NTOCs through field campaigns and modelling studies. This study analysed wind measurements and O3, formaldehyde (HCHO) and sulfur dioxide (SO2) concentrations from 2000 to 2011 at 25 ground monitors in Houston. NTOCs almost always occurred when monitors were downwind of petrochemical facilities. Rapid O3 increases were associated with low wind speeds; 75 % of NTOCs occurred when the 3-h average wind speed preceding the event was less than 6.5 km h-1. Statistically significant differences in HCHO concentrations were seen between days with and without NTOCs. Early afternoon HCHO concentrations were greater on NTOC days. In the morning before an observed NTOC event, however, there were no significant differences in HCHO concentrations between days with and without NTOCs. Hourly SO2 concentrations also increased rapidly, exhibiting behaviour similar to NTOCs. Oftentimes, the SO2 increases preceded a NTOC. These findings show that, despite the apparent success of targeted HRVOC emission controls, further restrictions may be needed to eliminate the remaining O3 events.

Future impact of traffic emissions on atmospheric ozone and OH based on two scenarios

Abstract. The future impact of traffic emissions on atmospheric ozone and OH has been investigated separately for the three sectors AIRcraft, maritime SHIPping and ROAD traffic. To reduce uncertainties we present results from an ensemble of six different atmospheric chemistry models, each simulating the atmospheric chemical composition in a possible high emission scenario (A1B), and with emissions from each transport sector reduced by 5% to estimate sensitivities. Our results are compared with optimistic future emission scenarios (B1 and B1 ACARE), presented in a companion paper, and with the recent past (year 2000). Present-day activity indicates that anthropogenic emissions so far evolve closer to A1B than the B1 scenario. As a response to expected changes in emissions, AIR and SHIP will have increased impacts on atmospheric O3 and OH in the future while the impact of ROAD traffic will decrease substantially as a result of technological improvements. In 2050, maximum aircraft-induced O3 occurs near 80° N in the UTLS region and could reach 9 ppbv in the zonal mean during summer. Emissions from ship traffic have their largest O3 impact in the maritime boundary layer with a maximum of 6 ppbv over the North Atlantic Ocean during summer in 2050. The O3 impact of road traffic emissions in the lower troposphere peaks at 3 ppbv over the Arabian Peninsula, much lower than the impact in 2000. Radiative forcing (RF) calculations show that the net effect of AIR, SHIP and ROAD combined will change from a marginal cooling of −0.44 ± 13 mW m−2 in 2000 to a relatively strong cooling of −32 ± 9.3 (B1) or −32 ± 18 mW m−2 (A1B) in 2050, when taking into account RF due to changes in O3, CH4 and CH4-induced O3. This is caused both by the enhanced negative net RF from SHIP, which will change from −19 ± 5.3 mW m−2 in 2000 to −31 ± 4.8 (B1) or −40 ± 9 mW m−2 (A1B) in 2050, and from reduced O3 warming from ROAD, which is likely to turn from a positive net RF of 12 ± 8.5 mW m−2 in 2000 to a slightly negative net RF of −3.1 ± 2.2 (B1) or −3.1 ± 3.4 (A1B) mW m−2 in the middle of this century. The negative net RF from ROAD is temporary and induced by the strong decline in ROAD emissions prior to 2050, which only affects the methane cooling term due to the longer lifetime of CH4 compared to O3. The O3 RF from AIR in 2050 is strongly dependent on scenario and ranges from 19 ± 6.8 (B1 ACARE) to 61 ± 14 mW m−2 (A1B). There is also a considerable span in the net RF from AIR in 2050, ranging from −0.54 ± 4.6 (B1 ACARE) to 12 ± 11 (A1B) mW m−2 compared to 6.6 ± 2.2 mW m−2 in 2000.