Summertime total ozone variations over middle and polar latitudes

The statistical relationship between springtime and summertime ozone over middle and polar latitudes is analyzed using zonally averaged total ozone data. Shortterm variations in springtime midlatitude ozone demonstrate only a modest correlation with springtime polar ozone variations. However by early summer, ozone variations throughout the extratropics are highly correlated. Analysis of correlation functions indicates that springtime midlatitude ozone, not polar ozone, is the best predictor for summertime polar ozone. Long-term total ozone trends at middle and high latitudes are also different for spring and nearly identical for summer. About 39% of the observed southern midlatitude ozone decline in December can be attributed to the polar ozone depletion up to November. In the Northern Hemisphere, the corresponding contribution is about 15%, but the error bars are too large to make an accurate estimate.

Ozone database in support of CMIP5 simulations: results and corresponding radiative forcing

A continuous tropospheric and stratospheric vertically resolved ozone time series, from 1850 to 2099, has been generated to be used as forcing in global climate models that do not include interactive chemistry. A multiple linear regression analysis of SAGE I+II satellite observations and polar ozonesonde measurements is used for the stratospheric zonal mean dataset during the well-observed period from 1979 to 2009. In addition to terms describing the mean annual cycle, the regression includes terms representing equivalent effective stratospheric chlorine (EESC) and the 11-yr solar cycle variability. The EESC regression fit coefficients, together with pre-1979 EESC values, are used to extrapolate the stratospheric ozone time series backward to 1850. While a similar procedure could be used to extrapolate into the future, coupled chemistry climate model (CCM) simulations indicate that future stratospheric ozone abundances are likely to be significantly affected by climate change, and capturing such effects through a regression model approach is not feasible. Therefore, the stratospheric ozone dataset is extended into the future (merged in 2009) with multimodel mean projections from 13 CCMs that performed a simulation until 2099 under the SRES (Special Report on Emission Scenarios) A1B greenhouse gas scenario and the A1 adjusted halogen scenario in the second round of the Chemistry-Climate Model Validation (CCMVal-2) Activity. The stratospheric zonal mean ozone time series is merged with a three-dimensional tropospheric data set extracted from simulations of the past by two CCMs (CAM3.5 and GISSPUCCINI)and of the future by one CCM (CAM3.5). The future tropospheric ozone time series continues the historical CAM3.5 simulation until 2099 following the four different Representative Concentration Pathways (RCPs). Generally good agreement is found between the historical segment of the ozone database and satellite observations, although it should be noted that total column ozone is overestimated in the southern polar latitudes during spring and tropospheric column ozone is slightly underestimated. Vertical profiles of tropospheric ozone are broadly consistent with ozonesondes and in-situ measurements, with some deviations in regions of biomass burning. The tropospheric ozone radiative forcing (RF) from the 1850s to the 2000s is 0.23Wm−2, lower than previous results. The lower value is mainly due to (i) a smaller increase in biomass burning emissions; (ii) a larger influence of stratospheric ozone depletion on upper tropospheric ozone at high southern latitudes; and possibly (iii) a larger influence of clouds (which act to reduce the net forcing) compared to previous radiative forcing calculations. Over the same period, decreases in stratospheric ozone, mainly at high latitudes, produce a RF of −0.08Wm−2, which is more negative than the central Intergovernmental Panel on Climate Change (IPCC) Fourth Assessment Report (AR4) value of −0.05Wm−2, but which is within the stated range of −0.15 to +0.05Wm−2. The more negative value is explained by the fact that the regression model simulates significant ozone depletion prior to 1979, in line with the increase in EESC and as confirmed by CCMs, while the AR4 assumed no change in stratospheric RF prior to 1979. A negative RF of similar magnitude persists into the future, although its location shifts from high latitudes to the tropics. This shift is due to increases in polar stratospheric ozone, but decreases in tropical lower stratospheric ozone, related to a strengthening of the Brewer-Dobson circulation, particularly through the latter half of the 21st century. Differences in trends in tropospheric ozone among the four RCPs are mainly driven by different methane concentrations, resulting in a range of tropospheric ozone RFs between 0.4 and 0.1Wm−2 by 2100. The ozone dataset described here has been released for the Coupled Model Intercomparison Project (CMIP5) model simulations in netCDF Climate and Forecast (CF) Metadata Convention at the PCMDI website (http://cmip-pcmdi.llnl.gov/).

Northern winter stratospheric temperature and ozone responses to ENSO inferred from an ensemble of Chemistry Climate Models

The connection between the El Ni˜no Southern Oscillation (ENSO) and the Northern polar stratosphere has been established from observations and atmospheric modeling. Here a systematic inter-comparison of the sensitivity of the modeled stratosphere to ENSO in Chemistry Climate Models (CCMs) is reported. This work uses results from a number of the CCMs included in the 2006 ozone assessment. In the lower stratosphere, the mean of all model simulations reports a warming of the polar vortex during strong ENSO events in February–March, consistent with but smaller than the estimate from satellite observations and ERA40 reanalysis. The anomalous warming is associated with an anomalous dynamical increase of column ozone north of 70� N that is accompanied by coherent column ozone decrease in the Tropics, in agreement with that deduced from the NIWA column ozone database, implying an increased residual circulation in the mean of all model simulations during ENSO. The spread in the model responses is partly due to the large internal stratospheric variability and it is shown that it crucially depends on the representation of the tropospheric ENSO teleconnection in the models.

Persistence and photochemical decay of springtime total ozone anomalies in the Canadian Middle Atmosphere Model

The persistence and decay of springtime total ozone anomalies over the entire extratropics (midlatitudes plus polar regions) is analysed using results from the Canadian Middle Atmosphere Model (CMAM), a comprehensive chemistry-climate model. As in the observations, interannual anomalies established through winter and spring persist with very high correlation coefficients (above 0.8) through summer until early autumn, while decaying in amplitude as a result of photochemical relaxation in the quiescent summertime stratosphere. The persistence and decay of the ozone anomalies in CMAM agrees extremely well with observations, even in the southern hemisphere when the model is run without heterogeneous chemistry (in which case there is no ozone hole and the seasonal cycle of ozone is quite different from observations). However in a version of CMAM with strong vertical diffusion, the northern hemisphere anomalies decay far too rapidly compared to observations. This shows that ozone anomaly persistence and decay does not depend on how the springtime anomalies are created or on their magnitude, but reflects the transport and photochemical decay in the model. The seasonality of the long-term trends over the entire extratropics is found to be explained by the persistence of the interannual anomalies, as in the observations, demonstrating that summertime ozone trends reflect winter/spring trends rather than any change in summertime ozone chemistry. However this mechanism fails in the northern hemisphere midlatitudes because of the relatively large impact, compared to observations, of the CMAM polar anomalies. As in the southern hemisphere, the influence of polar ozone loss in CMAM increases the midlatitude summertime loss, leading to a relatively weak seasonal dependence of ozone loss in the Northern Hemisphere compared to the observations.

Assessment of temperature, trace species, and ozone in chemistry-climate model simulations of the recent past

Simulations of the stratosphere from thirteen coupled chemistry-climate models (CCMs) are evaluated to provide guidance for the interpretation of ozone predictions made by the same CCMs. The focus of the evaluation is on how well the fields and processes that are important for determining the ozone distribution are represented in the simulations of the recent past. The core period of the evaluation is from 1980 to 1999 but long-term trends are compared for an extended period (1960–2004). Comparisons of polar high-latitude temperatures show that most CCMs have only small biases in the Northern Hemisphere in winter and spring, but still have cold biases in the Southern Hemisphere spring below 10 hPa. Most CCMs display the correct stratospheric response of polar temperatures to wave forcing in the Northern, but not in the Southern Hemisphere. Global long-term stratospheric temperature trends are in reasonable agreement with satellite and radiosonde observations. Comparisons of simulations of methane, mean age of air, and propagation of the annual cycle in water vapor show a wide spread in the results, indicating differences in transport. However, for around half the models there is reasonable agreement with observations. In these models the mean age of air and the water vapor tape recorder signal are generally better than reported in previous model intercomparisons. Comparisons of the water vapor and inorganic chlorine (Cly) fields also show a large intermodel spread. Differences in tropical water vapor mixing ratios in the lower stratosphere are primarily related to biases in the simulated tropical tropopause temperatures and not transport. The spread in Cly, which is largest in the polar lower stratosphere, appears to be primarily related to transport differences. In general the amplitude and phase of the annual cycle in total ozone is well simulated apart from the southern high latitudes. Most CCMs show reasonable agreement with observed total ozone trends and variability on a global scale, but a greater spread in the ozone trends in polar regions in spring, especially in the Arctic. In conclusion, despite the wide range of skills in representing different processes assessed here, there is sufficient agreement between the majority of the CCMs and the observations that some confidence can be placed in their predictions.

Ozone and climate: a review of interconnections

Stratospheric ozone has been depleted over the last 25 years following anthropogenic emissions of a number of chlorine- and bromine-containing compounds (ozone-depleting substances, ODSs), which are now regulated under the Montreal Protocol. The Protocol has been effective in controlling the net growth of these compounds in the atmosphere. As chlorine and bromine slowly decrease in the future, ozone levels are expected to increase in the coming decades, although the evolution will also depend on the changing climate system.

Seasonal persistence of midlatitude total ozone anomalies

Temporal autocorrelations of monthly mean total ozone anomalies over the 35–60°S and 35–60°N latitude bands reveal that anomalies established in the wintertime midlatitude ozone buildup persist (with photochemical decay) until the end of the following autumn, and then are rapidly erased once the next winter's buildup begins. The photochemical decay rate is found to be identical between the two hemispheres. High predictability of ozone through late summer exists based on the late-spring values. In the northern hemisphere, extending the 1979–2001 springtime ozone trend to other months through regression based on the seasonal persistence of anomalies captures the seasonality of the ozone trends remarkably well. In the southern hemisphere, the springtime trend only accounts for part of the summertime trends. There is a strong correlation between the ozone anomalies in northern hemisphere spring and those in the subsequent southern hemisphere spring, but not the converse.

Inhalation exposure to particulate matter in rooms with underfloor air distribution

This work investigated the personal exposure to indoor particulate matters using the intake fraction metric and provided a possible way to trace the particle inhaled from an indoor particle source. A turbulence model validated by the particle measurements in a room with underfloor air distribution (UFAD) system was used to predict the indoor particle concentrations. Inhalation intake fraction of indoor particles was defined and evaluated in two rooms equipped with the UFAD, i.e., the experimental room and a small office. According to the exposure characteristics and a typical respiratory rate, the intake fraction was determined in two rooms with a continuous and episodic (human cough) source of particles, respectively. The findings showed that the well-mixing assumption of indoor air failed to give an accurate estimation of inhalation exposure and the average concentration at return outlet or within the overall room could not relate well the intake fraction to the amount of particle emitted from an indoor source.

Arctic ozone depletion in 2002–2003 measured by ASUR and comparison with POAM observations

We present ozone loss estimated from airborne measurements taken during January–February and March in the Arctic winter 2002/2003. The first half of the winter was characterized by unusually cold temperatures and the second half by a major stratospheric sudden warming around 15–18 January 2003. The potential vorticity maps show a vortex split in the lower stratosphere during the major warming (MW) in late January and during the minor warming in mid-February due to wave 1 amplification. However, the warming can be termed as a vortex displacement event as there was no vortex split during the MW period at 10 hPa. Very low temperatures, large areas of polar stratospheric clouds (PSCs), and high chlorine activation triggered significant ozone loss in the early winter, as the vortex moved to the midlatitude regions. The ozone depletion derived from the ASUR measurements sampled inside the vortex, in conjunction with the Mimosa-Chim model tracer, shows a maximum of 1.3 ± 0.2 ppmv at 450–500 K by late March. The partial column loss derived from the ASUR ozone profiles reaches up to 61 ± 4 DU in 400–550 K in the same period. The evolution of ozone and ozone loss assessed from the ASUR measurements is in very good agreement with POAM observations. The reduction in ozone estimated from the POAM measurements shows a similar maximum of 1.3 ± 0.2 ppmv at 400–500 K or 63 ± 4 DU in 400–550 K in late March. Our study reveals that the Arctic winter 2002/2003 was unique as it had three minor warmings and a MW, yet showed large loss in ozone. No such feature was observed in any other Arctic winter in the 1989–2010 period. In addition, an unusually large ozone loss in December, around 0.5 ± 0.2 ppmv at 450–500 K or 12 ± 1 DU in 400–550 K, was estimated for the first time in the Arctic. A careful and detailed diagnosis with all available published results for this winter exhibits an average ozone loss of 1.5 ± 0.3 ppmv at 450–500 K or 65 ± 5 DU in 400–550 K by the end of March, which exactly matches the ozone depletion derived from the ASUR, POAM and model data. The early ozone loss together with considerable loss afterwards put the warm Arctic winter 2002/2003 amongst the moderately cold winters in terms of the significance of the ozone loss.

Comparison of polar ozone loss rates simulated by one-dimensional and three-dimensional models with Match observations in recent Antarctic and Arctic winters

Simulations of ozone loss rates using a three-dimensional chemical transport model and a box model during recent Antarctic and Arctic winters are compared with experimental loss rates. The study focused on the Antarctic winter 2003, during which the first Antarctic Match campaign was organized, and on Arctic winters 1999/2000, 2002/2003. The maximum ozone loss rates retrieved by the Match technique for the winters and levels studied reached 6 ppbv/sunlit hour and both types of simulations could generally reproduce the observations at 2-sigma error bar level. In some cases, for example, for the Arctic winter 2002/2003 at 475 K level, an excellent agreement within 1-sigma standard deviation level was obtained. An overestimation was also found with the box model simulation at some isentropic levels for the Antarctic winter and the Arctic winter 1999/2000, indicating an overestimation of chlorine activation in the model. Loss rates in the Antarctic show signs of saturation in September, which have to be considered in the comparison. Sensitivity tests were performed with the box model in order to assess the impact of kinetic parameters of the ClO-Cl2O2 catalytic cycle and total bromine content on the ozone loss rate. These tests resulted in a maximum change in ozone loss rates of 1.2 ppbv/sunlit hour, generally in high solar zenith angle conditions. In some cases, a better agreement was achieved with fastest photolysis of Cl2O2 and additional source of total inorganic bromine but at the expense of overestimation of smaller ozone loss rates derived later in the winter.

Forecast, measurement, and modeling of an unprecedented polar ozone filament event over Mauna Loa Observatory, Hawaii

In mid-March 2005 the northern lower stratospheric polar vortex experienced a severe stretching episode, bringing a large polar filament far south of Alaska toward Hawaii. This meridional intrusion of rare extent, coinciding with the polar vortex final warming and breakdown, was followed by a zonal stretching in the wake of the easterly propagating subtropical main flow. This caused polar air to remain over Hawaii for several days before diluting into the subtropics. After being successfully forecasted to pass over Hawaii by the high-resolution potential vorticity advection model Modèle Isentrope du transport Méso-échelle de l'Ozone Stratosphérique par Advection (MIMOSA), the filament was observed on isentropic surfaces between 415 K and 455 K (17–20 km) by the Jet Propulsion Laboratory stratospheric ozone lidar measurements at Mauna Loa Observatory, Hawaii, between 16 and 19 March 2005. It was materialized as a thin layer of enhanced ozone peaking at 1.6 ppmv in a region where the climatological values usually average 1.0 ppmv. These values were compared to those obtained by the three-dimensional Chemistry-Transport Model MIMOSA-CHIM. Agreement between lidar and model was excellent, particularly in the similar appearance of the ozone peak near 435 K (18.5 km) on 16 March, and the persistence of this layer at higher isentropic levels for the following three days. Passive ozone, also modeled by MIMOSA-CHIM, was at about 3–4 ppmv inside the filament while above Hawaii. A detailed history of the modeled chemistry inside the filament suggests that the air mass was still polar ozone–depleted when passing over Hawaii. The filament quickly separated from the main vortex after its Hawaiian overpass. It never reconnected and, in less than 10 days, dispersed entirely in the subtropics

Statistical analysis of eight surface ozone measurement series for various sites in Ireland

Data from various stations having different measurement record periods between 1988 and 2007 are analyzed to investigate the surface ozone concentration, long-term trends, and seasonal changes in and around Ireland. Time series statistical analysis is performed on the monthly mean data using seasonal and trend decomposition procedures and the Box-Jenkins approach (autoregressive integrated moving average). In general, ozone concentrations in the Irish region are found to have a negative trend at all sites except at the coastal sites of Mace Head and Valentia. Data from the most polluted Dublin city site have shown a very strong negative trend of −0.33 ppb/yr with a 95% confidence limit of 0.17 ppb/yr (i.e., −0.33 ± 0.17) for the period 2002−2007, and for the site near the city of Cork, the trend is found to be −0.20 ± 0.11 ppb/yr over the same period. The negative trend for other sites is more pronounced when the data span is considered from around the year 2000 to 2007. Rural sites of Wexford and Monaghan have also shown a very strong negative trend of −0.99 ± 0.13 and −0.58 ± 0.12, respectively, for the period 2000−2007. Mace Head, a site that is representative of ozone changes in the air advected from the Atlantic to Europe in the marine planetary boundary layer, has shown a positive trend of about +0.16 ± 0.04 ppb per annum over the entire period 1988−2007, but this positive trend has reduced during recent years (e.g., in the period 2001−2007). Cluster analysis for back trajectories are performed for the stations having a long record of data, Mace Head and Lough Navar. For Mace Head, the northern and western clean air sectors have shown a similar positive trend (+0.17 ± 0.02 ppb/yr for the northern sector and +0.18 ± 0.02 ppb/yr for the western sector) for the whole period, but partial analysis for the clean western sector at Mace Head shows different trends during different time periods with a decrease in the positive trend since 1988 indicating a deceleration in the ozone trend for Atlantic air masses entering Europe.

Simultaneous lidar and EOS MLS measurements, and modeling, of a rare polar ozone filament event over Mauna Loa Observatory, Hawaii

In mid-March 2005, a rare lower stratospheric polar vortex filamentation event was observed simultaneously by the JPL lidar at Mauna Loa Observatory, Hawaii, and by the EOS MLS instrument onboard the Aura satellite. The event coincided with the beginning of the spring 2005 final warming. On 16 March, the filament was observed by lidar around 0600 UT between 415 K and 455 K, and by MLS six hours earlier. It was seen on both the lidar and MLS profiles as a layer of enhanced ozone, peaking at 1.7 ppmv in a region where the climatological values are usually around or below 1 ppmv. Ozone profiles measured by lidar and MLS were compared to profiles from the Chemical Transport Model MIMOSA-CHIM. The agreement between lidar, MLS, and the model is excellent considering the difference in the sampling techniques. MLS was also able to identify the filament at another location north of Hawaii.

High resolution simulation of recent Arctic and Antarctic stratospheric chemical ozone loss compared to observations

Simulations of polar ozone losses were performed using the three-dimensional high-resolution (1∘ × 1∘) chemical transport model MIMOSA-CHIM. Three Arctic winters 1999–2000, 2001–2002, 2002–2003 and three Antarctic winters 2001, 2002, and 2003 were considered for the study. The cumulative ozone loss in the Arctic winter 2002–2003 reached around 35% at 475 K inside the vortex, as compared to more than 60% in 1999–2000. During 1999–2000, denitrification induces a maximum of about 23% extra ozone loss at 475 K as compared to 17% in 2002–2003. Unlike these two colder Arctic winters, the 2001–2002 Arctic was warmer and did not experience much ozone loss. Sensitivity tests showed that the chosen resolution of 1∘ × 1∘ provides a better evaluation of ozone loss at the edge of the polar vortex in high solar zenith angle conditions. The simulation results for ozone, ClO, HNO3, N2O, and NO y for winters 1999–2000 and 2002–2003 were compared with measurements on board ER-2 and Geophysica aircraft respectively. Sensitivity tests showed that increasing heating rates calculated by the model by 50% and doubling the PSC (Polar Stratospheric Clouds) particle density (from 5 × 10−3 to 10−2 cm−3) refines the agreement with in situ ozone, N2O and NO y levels. In this configuration, simulated ClO levels are increased and are in better agreement with observations in January but are overestimated by about 20% in March. The use of the Burkholder et al. (1990) Cl2O2 absorption cross-sections slightly increases further ClO levels especially in high solar zenith angle conditions. Comparisons of the modelled ozone values with ozonesonde measurement in the Antarctic winter 2003 and with Polar Ozone and Aerosol Measurement III (POAM III) measurements in the Antarctic winters 2001 and 2002, shows that the simulations underestimate the ozone loss rate at the end of the ozone destruction period. A slightly better agreement is obtained with the use of Burkholder et al. (1990) Cl2O2 absorption cross-sections.