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A modelling study of the impact of cirrus clouds on the moisture budget of the upper troposphere

We present a modelling study of the effect of cirrus clouds on the moisture budget of the layer wherein the cloud formed. Our framework simplifies many aspects of cloud microphysics and collapses the problem of sedimentation onto a 0-dimensional box model, but retains essential feedbacks between saturation mixing ratio, particle growth, and water removal through particle sedimentation. The water budget is described by two coupled first-order differential equations for dimensionless particle number density and saturation point temperature, where the parameters defining the system (layer depth, reference temperature, amplitude and time scale of temperature perturbation and inital particle number density, which may or may not be a function of reference temperature and cooling rate) are encapsulated in a single coefficient. This allows us to scale the results to a broad range of atmospheric conditions, and to test sensitivities. Results of the moisture budget calculations are presented for a range of atmospheric conditions (T: 238–205 K; p: 325–180 hPa) and a range of time scales τT of the temperature perturbation that induces the cloud formation. The cirrus clouds are found to efficiently remove water for τT longer than a few hours, with longer perturbations (τT≳10 h) required at lower temperatures (T≲210 K). Conversely, we find that temperature perturbations of duration order 1 h and less (a typical timescale for e.g., gravity waves) do not efficiently dehydrate over most of the upper troposphere. A consequence is that (for particle densities typical of current cirrus clouds) the assumption of complete dehydration to the saturation mixing ratio may yield valid predictions for upper tropospheric moisture distributions if it is based on the large scale temperature field, but this assumption is not necessarily valid if it is based on smaller scale temperature fields.
Screening the ESA ATSR-2 World Fire Atlas (1997–2002)

We screened the algorithm 2 (308 K threshold) European Space Agency (ESA) World Fire Atlas (WFA), for the period 1997–2002, using ancillary land cover, night-lights and volcanic activity datasets, combined with statistical techniques to detect the occurrence of space-time clusters of anomalous observations. The WFA is built using night time data from the Along Track Scanning Radiometer (ATSR) onboard the Second European Remote-Sensing Satellite (ERS-2). The spatial resolution of the data is 1 km and the satellite revisiting period is 3 days at the equator. The WFA is the first and longest archive of global fire observations and has been used in numerous biomass burning studies. Known limitations of the WFA are the inclusion of warm surfaces, gas flares, and city lights, and an underestimation of actual global fire activity, due to the time of satellite overpass. Nevertheless, it has been considered that the WFA contains a relatively small proportion of observations that do not correspond to vegetation fires, which is not corroborated by our findings. During the study period, the annual percentage of false alarms and non-vegetation fires varied from a minimum value of 20.6% in 1997 to a maximum of 27.9% in 1998. Gas flares and hot bare soils are the major sources of false alarms and non-vegetation fires.
Mixing height determination by ceilometer

A novel method for estimating the mixing height based on ceilometer measurements is described and tested against commonly used methods for determining mixing height. In this method an idealised backscatter profile is fitted to the observed backscatter profile. The mixing height is one of the idealised backscatter profile parameters. An extensive amount of ceilometer data and vertical soundings data from the Helsinki area in 2002 is utilized to test the applicability of the ceilometer for mixing height determination. The results, including 71 convective and 38 stable cases, show that in clear sky conditions the mixing heights determined from ceilometer based aerosol profiles and BL-height estimates based on sounding data are in a good agreement. Rejected outlier cases corresponded to very low aerosol concentrations in the mixed layer leading to a very weak aerosol backscatter signal in the lowest layer.
A group contribution method for estimating the vapour pressures of α-pinene oxidation products

A prediction method based on group contribution principles is proposed for estimating the vapour pressure of α-pinene oxidation products. Temperature dependent contributions are provided for the following chemical groups: carbonyl, nitrate, hydroxy, hydroperoxy, acyl peroxy nitrate and carboxy. On the basis of observed vapour pressure differences between isomers of diols and dinitrates, a simple refinement is introduced in the method to account for the influence of substitutions on the vapour pressure for alcohols and nitrates. The vapour pressures predicted with this new method have been compared with the predictions from UNIFAC (Asher et al., 2002). Given the large uncertainties of the vapour pressure data for the least volatile compounds, further experimental studies of subcooled vapour pressures of multifunctional compounds at ambient temperatures are required for better parameterizations. Among the α-pinene products identified to date, pinic acid and hydroxy pinonic acid are predicted to be the least volatile compounds, with estimated vapour pressures of 3×10−6 torr and 6×10−7 torr, respectively. The vapour pressure of the other primary products range from 10−5 to 10−3 torr, with hydroxy hydroperoxides presenting the lowest values. Noting that multifunctional carboxylic acids, in particular pinic acid, are believed to be mostly present as dimers in laboratory conditions, we suggest that the partial vapour pressure of the pinic acid dimer should be close to the experimental subcooled vapour pressure for pinic acid (estimated at ~10−6 torr) due to its large contribution to the total concentration (dimer+monomer) in experimental conditions.
Sub-continental transport mechanisms and pathways during two ozone episodes in northern Spain

Two ozone episodes (occurring in June 2001 and June 2003) in the air quality monitoring network of the Basque Country (BC) are analyzed. The population information threshold was exceeded in many stations (urban, urban-background and rural). During this type of episodes, forced by a blocking anticyclone over the British Isles, ozone background concentrations over the area increase after the import of pollution from both, the continental Europe and the western Mediterranean areas (Gangoiti et al., 2002). For the present analysis, emphasis is made in the search for transport mechanisms, pathways and area sources contributing to the build-up of the episodes. Contributions from a selection of 17 urban and industrial conglomerates in the western European Atlantic (WEA) and the western Mediterranean (WM) are shown after the results of a coupled RAMS-HYPACT modelling system. Meteorological simulations are tested against both the high-resolution wind data recorded at the BC coastal area by a boundary layer wind-profiler radar (Alonso et al., 1998) and the wind soundings reported by the National Centres of Meteorology at a selection of European and north-African sites. Results show that during the accumulation phase of the episodes, background ozone concentrations increase in the whole territory as a consequence of transport from the Atlantic coast of France and the British Channel. For the peak phase, intrusions from new sources, located at the Western Mediterranean, Southern France, Ebro Valley, and, occasionally, the area of Madrid are added, resulting in a further increase in the ozone concentrations. Direct day and night transport within the north-easterly winds over the sea from the WEA source region, and night-time transport within the residual layer over continental areas (southern France, the Ebro Valley, and central Iberia) modulate the import sequence of pollutants and the local increase of ozone concentrations. The alternative direct use of low resolution meteorological data for the estimation of back-trajectories shows a more simple transport scheme with no contributions neither from the Western Mediterranean nor from the Madrid area.
The origin of ozone

Highest atmospheric ozone production rates can be found at around 30 km in the tropical stratosphere, leading to ozone mixing ratios of about 10 ppmv. Those stratospheric air masses are then transported to extra-tropical latitudes via the Brewer-Dobson circulation. This is considered the main mechanism to generate mid- and high latitude ozone. By applying the climate-chemistry models E39/C and MAECHAM4/CHEM, this view is investigated in more detail. The origin of ozone in the troposphere and stratosphere is analysed, by incorporating a diagnostics ("marked ozone origin tracers") into the models, which allows to identify the origin of ozone. In most regions the simulated local ozone concentration is dominated by local ozone production, i.e. less than 50% of the ozone at higher latitudes of the stratosphere is produced in the tropics, which conflicts with the idea that the tropics are the global source for stratospheric ozone. Although episodic stratospheric intrusions occur basically everywhere, the main ozone stratosphere-to-troposphere exchange is connected to exchange processes at the sub-tropical jet-stream. The simulated tropospheric influx of ozone amounts to 420 Tg per year, and originates in the Northern Hemisphere from the extra-tropical stratosphere, whereas in the Southern Hemisphere a re-circulation of tropical tropospheric ozone contributes most to the influx of ozone into the troposphere. In the model E39/C, the upper troposphere of both hemispheres is clearly dominated by tropical tropospheric ozone (40%–50%) except for northern summer hemisphere, where the tropospheric contribution (from the tropics as well as from the Northern Hemisphere) does not exceed 20%.
Measurements and modelling of I2, IO, OIO, BrO and NO3 in the mid-latitude marine boundary layer

Time series observations of molecular iodine (I2), iodine oxides (IO, OIO), bromine oxide (BrO), and the nitrate radical (NO3) in the mid-latitude coastal marine boundary layer (MBL) are reported. Measurements were made using a new long-path DOAS instrument during a summertime campaign at Mace Head on the B3Π(0+u)-X1Σ+g electronic transition between 535 and 575 nm. The I2 mixing ratio was found to vary from below the detection limit (~5 ppt) up to a nighttime maximum of 93 ppt. Along with I2, observations of IO, OIO and NO3 were also made during the night. Surprisingly, IO and OIO were detected at mixing ratios up to 2.5 and 10.8 ppt, respectively. A model is employed to show that the reaction between I2 and NO3 is the likely nighttime source of these radicals. The BrO mixing ratio varied from below the detection limit at night (~1 ppt) to a maximum of 6 ppt in the first hours after sunrise. A bromine chemistry model is used to simulate the diurnal behaviour of the BrO radical, demonstrating the importance of halogen recycling through sea-salt aerosol. In the same campaign a zenith sky DOAS was employed to determine the column density variation of NO3 as a function of solar zenith angle (SZA) during sunrise, from which vertical profiles of NO3 through the troposphere were obtained. On several occasions a positive gradient of NO3 was observed over the first 2 km, possibly due to dimethyl sulphide (DMS) removing NO3 at the ocean surface.
Impact of aircraft NOx emissions on the atmosphere – tradeoffs to reduce the impact

Within the EU-project TRADEOFF, the impact of NOx (=NO+NO2) emissions from subsonic aviation upon the chemical composition of the atmosphere has been calculated with focus on changes in reactive nitrogen and ozone. We apply a 3-D chemical transport model that includes comprehensive chemistry for both the troposphere and the stratosphere and uses various aircraft emission scenarios developed during TRADEOFF for the year 2000. The environmental effects of enhanced air traffic along polar routes and of possible changes in cruising altitude are investigated, taking into account effects of flight route changes on fuel consumption and emissions. In a reference case including both civil and military aircraft the model predicts aircraft-induced maximum increases of zonal-mean NOy (=total reactive nitrogen) between 156 pptv (August) and 322 pptv (May) in the tropopause region of the Northern Hemisphere. Resulting maximum increases in zonal-mean ozone vary between 3.1 ppbv in September and 7.7 ppbv in June. Enhanced use of polar routes implies substantially larger zonal-mean ozone increases in high Northern latitudes during summer, while the effect is negligible in winter. Lowering the flight altitude leads to smaller ozone increases in the lower stratosphere and upper troposphere, and to larger ozone increases at altitudes below. Regarding total ozone change, the degree of cancellation between these two effects depends on latitude and season, but annually and globally averaged the contribution from higher altitudes dominates, mainly due to washout of NOy in the troposphere, which weakens the tropospheric increase. Raising flight altitudes increases the ozone burden both in the troposphere and the lower stratosphere, primarily due to a more efficient accumulation of pollutants in the stratosphere.
Evaluation of MIPAS ozone fields assimilated using a new algorithm constrained by isentropic tracer advection

A new data assimilation algorithm, using the isentropic advection equation, is applied to MIPAS and SBUV measurements of stratospheric ozone. The system is solved separately on each isentropic level, with neither vertical advection nor chemical reactions represented. The results are validated against HALOE, POAM III, SAGE II & III, OSIRIS and ozone sonde data. The new assimilation algorithm has the accuracy of the Kalman smoother but is, for the systems studied here with up to 200 000 variables per time step and 61 million control variables in total, many orders of magnitude less computationally expensive. The analysis produced minimises a single penalty function evaluated over an analysis window of over one month. The cost of the analysis is found to increase nearly linearly with the number of control variables. Compared with over 800 profiles from Electrochemical Concentration Cell sondes at 29 sites the analysis is found to be merely 0.1% high at 420 K, rising to 0.4% at 650 K. Comparison against the other satellites imply that the bias remains small up to 1250 K (38 km) and then increases to around −10% at 1650 K (44 km). Between 20 and 35 km the root-mean-square difference relative to HALOE, SAGE II & III, and POAM is in the 5 to 10% range, with larger discrepancies relative to other instruments. Outside this height range rms differences are generally larger, though agreement with HALOE remains good up to 50 km. The assimilation has closer agreement to independent observations than found in direct near-neighbour comparisons between profiles, demonstrating that the assimilation can add value to the observations.
Modelling study of the impact of deep convection on the utls air composition - Part I: Analysis of ozone precursors

The aim of this work is to study the local impact on the upper troposphere/lower stratosphere air composition of an extreme deep convective system. For this purpose, we performed a simulation of a convective cluster composed of many individual deep convective cells that occurred near Bauru (Brazil). The simulation is performed using the 3-D mesoscale model RAMS coupled on-line with a chemistry model. The comparisons with meteorological measurements show that the model produces meteorological fields generally consistent with the observations. The present paper (part I) is devoted to the analysis of the ozone precursors (CO, NOx and non-methane volatile organic compounds) and HOx in the UTLS. The simulation results show that the distribution of CO with altitude is closely related to the upward convective motions and consecutive outflow at the top of the convective cells leading to a bulge of CO between 7 km altitude and the tropopause (around 17 km altitude). The model results for CO are consistent with satellite-borne measurements at 700 hPa. The simulation also indicates enhanced amounts of NOx up to 2 ppbv in the 7–17 km altitude layer mainly produced by the lightning associated with the intense convective activity. For insoluble non-methane volatile organic compounds, the convective activity tends to significantly increase their amount in the 7–17 km layer by dynamical effects. During daytime in the presence of lightning NOx, this bulge is largely reduced in the upper part of the layer for reactive species (e.g. isoprene, ethene) because of their reactions with OH that is increased on average during daytime. Lightning NOx also impacts on the oxydizing capacity of the upper troposphere by reducing on average HOx, HO2, H2O2 and organic hydroperoxides. During the simulation time, the impact of convection on the air composition of the lower stratosphere is negligible for all ozone precursors although several of the simulated convective cells nearly reach the tropopause. There is no significant transport from the upper troposphere to the lower stratosphere, the isentropic barrier not being crossed by convection. The impact of the increase of ozone precursors and HOx in the upper troposphere on the ozone budget in the LS is discussed in part II of this series of papers.