Peroxy radicals and ozone photochemistry in air masses undergoing long-range transport

Concentrations of peroxy radicals (HO2+ΣiRiO2) in addition to other trace gases were measured onboard the UK Meteorological Office/Natural Environment Research Council British Aerospace 146-300 atmospheric research aircraft during the Intercontinental Transport of Ozone and Precursors (ITOP) campaign based at Horta Airport, Faial, Azores (38.58° N, 28.72° W) in July/August 2004. The overall peroxy radical altitude profile displays an increase with altitude that is likely to have been impacted by the effects of long-range transport. The peroxy radical altitude profile for air classified as of marine origin shows no discernable altitude profile. A range of air-masses were intercepted with varying source signatures, including those with aged American and Asian signatures, air-masses of biomass burning origin, and those that originated from the east coast of the United States. Enhanced peroxy radical concentrations have been observed within this range of air-masses indicating that long-range transported air-masses traversing the Atlantic show significant photochemical activity. The net ozone production at clear sky limit is in general negative, and as such the summer mid-Atlantic troposphere is at limit net ozone destructive. However, there is clear evidence of positive ozone production even at clear sky limit within air masses undergoing long-range transport, and during ITOP especially between 5 and 5.5 km, which in the main corresponds to a flight that extensively sampled air with a biomass burning signature. Ozone production was NOx limited throughout ITOP, as evidenced by a good correlation (r2=0.72) between P(O3) and NO. Strong positive net ozone production has also been seen in varying source signature air-masses undergoing long-range transport, including but not limited to low-level export events, and export from the east coast of the United States.

Stratospheric temperature and radiative forcing response to 11-year solar cycle changes in irradiance and ozone

The 11-yr solar cycle temperature response to spectrally resolved solar irradiance changes and associated ozone changes is calculated using a fixed dynamical heating (FDH) model. Imposed ozone changes are from satellite observations, in contrast to some earlier studies. A maximum of 1.6 K is found in the equatorial upper stratosphere and a secondary maximum of 0.4 K in the equatorial lower stratosphere, forming a double peak in the vertical. The upper maximum is primarily due to the irradiance changes while the lower maximum is due to the imposed ozone changes. The results compare well with analyses using the 40-yr ECMWF Re-Analysis (ERA-40) and NCEP/NCAR datasets. The equatorial lower stratospheric structure is reproduced even though, by definition, the FDH calculations exclude dynamically driven temperature changes, suggesting an important role for an indirect dynamical effect through ozone redistribution. The results also suggest that differences between the Stratospheric Sounding Unit (SSU)/Microwave Sounding Unit (MSU) and ERA-40 estimates of the solar cycle signal can be explained by the poor vertical resolution of the SSU/MSU measurements. The adjusted radiative forcing of climate change is also investigated. The forcing due to irradiance changes was 0.14 W m−2, which is only 78% of the value obtained by employing the standard method of simple scaling of the total solar irradiance (TSI) change. The difference arises because much of the change in TSI is at wavelengths where ozone absorbs strongly. The forcing due to the ozone change was only 0.004 W m−2 owing to strong compensation between negative shortwave and positive longwave forcings.

Stratospheric temperature trends: impact of ozone variability and the QBO

In most climate simulations used by the Intergovernmental Panel on Climate Change 2007 fourth assessment report, stratospheric processes are only poorly represented. For example, climatological or simple specifications of time-varying ozone concentrations are imposed and the quasi-biennial oscillation (QBO) of equatorial stratospheric zonal wind is absent. Here we investigate the impact of an improved stratospheric representation using two sets of perturbed simulations with the Hadley Centre coupled ocean atmosphere model HadGEM1 with natural and anthropogenic forcings for the 1979–2003 period. In the first set of simulations, the usual zonal mean ozone climatology with superimposed trends is replaced with a time series of observed zonal mean ozone distributions that includes interannual variability associated with the solar cycle, QBO and volcanic eruptions. In addition to this, the second set of perturbed simulations includes a scheme in which the stratospheric zonal wind in the tropics is relaxed to appropriate zonal mean values obtained from the ERA-40 re-analysis, thus forcing a QBO. Both of these changes are applied strictly to the stratosphere only. The improved ozone field results in an improved simulation of the stepwise temperature transitions observed in the lower stratosphere in the aftermath of the two major recent volcanic eruptions. The contribution of the solar cycle signal in the ozone field to this improved representation of the stepwise cooling is discussed. The improved ozone field and also the QBO result in an improved simulation of observed trends, both globally and at tropical latitudes. The Eulerian upwelling in the lower stratosphere in the equatorial region is enhanced by the improved ozone field and is affected by the QBO relaxation, yet neither induces a significant change in the upwelling trend.

Radiative forcing since preindustrial times due to ozone change in the troposphere and the lower stratosphere

Changes in atmospheric ozone have occurred since the preindustrial era as a result of increasing anthropogenic emissions. Within ACCENT, a European Network of Excellence, ozone changes between 1850 and 2000 are assessed for the troposphere and the lower stratosphere ( up to 30 km) by a variety of seven chemistry-climate models and three chemical transport models. The modeled ozone changes are taken as input for detailed calculations of radiative forcing. When only changes in chemistry are considered ( constant climate) the modeled global-mean tropospheric ozone column increase since preindustrial times ranges from 7.9 DU to 13.8 DU among the ten participating models, while the stratospheric column reduction lies between 14.1 DU and 28.6 DU in the models considering stratospheric chemistry. The resulting radiative forcing is strongly dependent on the location and altitude of the modeled ozone change and varies between 0.25 Wm(-2) and 0.45 Wm(-2) due to ozone change in the troposphere and - 0.123 Wm(-2) and + 0.066 Wm(-2) due to the stratospheric ozone change. Changes in ozone and other greenhouse gases since preindustrial times have altered climate. Six out of the ten participating models have performed an additional calculation taking into account both chemical and climate change. In most models the isolated effect of climate change is an enhancement of the tropospheric ozone column increase, while the stratospheric reduction becomes slightly less severe. In the three climate-chemistry models with detailed tropospheric and stratospheric chemistry the inclusion of climate change increases the resulting radiative forcing due to tropospheric ozone change by up to 0.10 Wm(-2), while the radiative forcing due to stratospheric ozone change is reduced by up to 0.034 Wm(-2). Considering tropospheric and stratospheric change combined, the total ozone column change is negative while the resulting net radiative forcing is positive.

An observing system simulation experiment to evaluate the scientific merit of wind and ozone measurements from the future SWIFT instrument

(from author) One of the first papers in the peer-review literature to discuss an OSSE to evaluate future wind observations in the stratosphere. Provides key evidence to justify the construction of the SWIFT instrument (currently planned to be built by the Canadian Space Agency for launch on ~ 2010).

Assimilation of stratospheric ozone from MIPAS into a global general-circulation model: The September 2002 vortex split

Ozone and temperature profiles from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) have been assimilated, using three-dimensional variational assimilation, into a stratosphere troposphere version of the Met Office numerical weather-prediction system. Analyses are made for the month of September 2002, when there was an unprecedented split in the southern hemisphere polar vortex. The analyses are validated against independent ozone observations from sondes, limb-occultation and total column ozone satellite instruments. Through most of the stratosphere, precision varies from 5 to 15%, and biases are 15% or less of the analysed field. Problems remain in the vortex and below the 60 hPa. level, especially at the tropopause where the analyses have too much ozone and poor agreement with independent data. Analysis problems are largely a result of the model rather than the data, giving confidence in the MIPAS ozone retrievals, though there may be a small high bias in MIPAS ozone in the lower stratosphere. Model issues include an excessive Brewer-Dobson circulation, which results both from known problems with the tracer transport scheme and from the data assimilation of dynamical variables. The extreme conditions of the vortex split reveal large differences between existing linear ozone photochemistry schemes. Despite these issues, the ozone analyses are able to successfully describe the ozone hole split and compare well to other studies of this event. Recommendations are made for the further development of the ozone assimilation system.