Divergence of sun-rays by atmospheric refraction at large solar zenith angles

International audienceFor the determination of photolysis rates at large zenith angles it has been demonstrated that refraction by the earth's atmosphere must be taken into account. In fact, due to the modified optical path the optical transmittance is thereby increased in most instances. Here we show that in addition the divergence of sun-rays, which is also caused by refraction but which reduces the direct solar irradiance, should not be neglected. Our calculations are based on a spherically symmetric atmosphere and include extinction by Rayleigh scattering, ozone, and background aerosol. For rays with 10km tangent altitude the divergence yields a reduction of about 10% to 40% at solar zenith angles of 91° to 96°. Moreover, we find that the divergence effect can completely cancel the relative enhancement caused by the increase of transmittance

The H Lyman-<b>a</b> actinic flux in the middle atmosphere

International audienceThe penetration of solar H Lyman-a radiation into the terrestrial middle atmosphere is studied in detail. The Lyman-a actinic flux is calculated with a Monte Carlo approach including multiple resonance scattering of Lyman-a photons within the terrestrial atmosphere and a temperature dependent absorption cross section of molecular oxygen. The dependence of the actinic flux on the temperature profile is significant for O2 column densities greater than about 1024 m-2. For column densities greater than about 5 · 1024 m-2 resonance scattering becomes important at solar zenith angles > 60°. The O(1D) quantum yield of the O2 dissociation by Lyman-a photons is found to decrease from 0.58 in the lower thermosphere to 0.48 in the lower mesosphere. Parameterisations for Lyman-a actinic flux, mean O2 absorption cross section and O(1D) quantum yield including temperature dependence and resonance scattering are given valid up to a O2 column density of about 1025 m-2

Observation of mesospheric air inside the arctic stratospheric polar vortex in early 2003

During several balloon flights inside the Arctic polar vortex in early 2003, unusual trace gas distributions were observed, which indicate a strong influence of mesospheric air in the stratosphere. The tuneable diode laser (TDL) instrument SPIRALE (Spectroscopie InFrarouge par Absorption de Lasers Embarqués) measured unusually high CO values (up to 600 ppb) on 27 January at about 30 km altitude. The cryosampler BONBON sampled air masses with very high molecular Hydrogen, extremely low SF6 and enhanced CO values on 6 March at about 25 km altitude. Finally, the MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) Fourier Transform Infra-Red (FTIR) spectrometer showed NOy values which are significantly higher than NOy* (the NOy derived from a correlation between N2O and NOy under undisturbed conditions), on 21 and 22 March in a layer centred at 22 km altitude. Thus, the mesospheric air seems to have been present in a layer descending from about 30 km in late January to 25 km altitude in early March and about 22 km altitude on 20 March. We present corroborating evidence from a model study using the KASIMA (KArlsruhe Simulation model of the Middle Atmosphere) model that also shows a layer of mesospheric air, which descended into the stratosphere in November and early December 2002, before the minor warming which occurred in late December 2002 lead to a descent of upper stratospheric air, cutting of a layer in which mesospheric air is present. This layer then descended inside the vortex over the course of the winter. The same feature is found in trajectory calculations, based on a large number of trajectories started in the vicinity of the observations on 6 March. Based on the difference between the mean age derived from SF6 (which has an irreversible mesospheric loss) and from CO2 (whose mesospheric loss is much smaller and reversible) we estimate that the fraction of mesospheric air in the layer observed on 6 March, must have been somewhere between 35% and 100%

Subtropical trace gas profiles determined by ground-based FTIR spectroscopy at Izaña (28° N, 16° W): Five-year record, error analysis, and comparison with 3-D CTMs

International audienceWithin the framework of the NDSC (Network for the Detection of Stratospheric Change) ground-based FTIR solar absorption spectra have been routinely recorded at Izaña Observatory (28° N, 16° W) on Tenerife Island since March 1999. By analyzing the shape of the absorption lines, and their different temperature sensitivities, the vertical distribution of the absorbers can be retrieved. Unique time series of subtropical profiles of O3, HCl, HF, N2O, and CH4 are presented. The effects of both dynamical and chemical annually varying cycles can be seen in the retrieved profiles. These include enhanced upwelling and photochemistry in summer and a more disturbed atmosphere in winter, which are typical of the subtropical stratosphere. A detailed error analysis has been performed for each profile. The output from two different three-dimensional (3-D) chemical transport models (CTMs), which are forced by ECMWF analyses, are compared to the measured profiles. Both models agree well with the measurements in tracking abrupt variations in the atmospheric structure, e.g. due to tropical streamers, in particular for the lower stratosphere. Simulated and measured profiles also reflect similar dynamical and chemical annual cycles. However, the differences between their mixing ratios clearly exceed the error bars estimated for the measured profiles. Possible reasons for this are discussed

The impact of an extreme solar event on the middle atmosphere: a case study

A possible impact of an extreme solar particle event (ESPE) on the middle atmosphere is studied for present-day climate and geomagnetic conditions. We consider an ESPE with an occurrence probability of about 1 per millennium. In addition, we assume that the ESPE is followed by an extreme geomagnetic storm (GMS), and we compare the contribution of the two extreme events. The strongest known and best-documented ESPE of 774/5 CE is taken as a reference example and established estimates of the corresponding ionization rates are applied. The ionization rates due to the energetic particle precipitation (EPP) during an extreme GMS are upscaled from analyzed distributions of electron energy spectra of observed GMSs. The consecutive buildup of NOx and HOx by ionization is modeled in the high-top 3D chemistry circulation model KArlsruhe SImulation Model of the middle Atmosphere (KASIMA), using specified dynamics from ERA-Interim analyses up to the stratopause. A specific dynamical situation was chosen that includes an elevated stratosphere event during January and maximizes the vertical coupling between the northern polar mesosphere–lower thermosphere region and the stratosphere; it therefore allows us to estimate a maximum possible impact. The particle event initially produces about 65 Gmol of NOy, with 25 Gmol of excess NOy even after 1 year. The related ozone loss reaches up to 50 % in the upper stratosphere during the first weeks after the event and slowly descends to the mid-stratosphere. After about 1 year, 20 % ozone loss is still observed in the northern stratosphere. The GMS causes strong ozone reduction in the mesosphere but plays only a minor role in the reduction in total ozone. In the Southern Hemisphere (SH), the long-lived NOy in the polar stratosphere, which is produced almost solely by the ESPE, is transported into the Antarctic polar vortex, where it experiences strong denitrification into the troposphere. For this special case, we estimate a NO3 washout that could produce a measurable signal in ice cores. The reduction in total ozone causes an increase of the UV erythema dose of less than 5 %, which maximizes in spring for northern latitudes of 30∘ and in summer for northern latitudes of about 60∘.</p

HOCl chemistry in the Antarctic stratospheric vortex 2002, as observed with the Michelson interferometer for passive atmospheric sounding (MIPAS)

In the 2002 Antarctic polar vortex enhanced HOCl mixing ratios were detected by the Michelson Interferometer for Passive Atmospheric Sounding both at altitudes of around 35 km (1000K potential temperature), where HOCl abundances are ruled by gas phase chemistry and at around 18–24 km (475–625 K), which belongs to the altitude domain where heterogeneous chlorine chemistry is relevant. At altitudes of 33 to 40 km polar vortex HOCl mixing ratios were found to be around 0.14 ppbv as long as the polar vortex was intact, centered at the pole, and thus received relatively little sunlight. This is the altitude region where in midlatitudinal and tropic atmospheres peak HOCl mixing ratios significantly above 0.2 ppbv (in terms of daily mean values) are observed. After deformation and displacement of the polar vortex in the course of a major warming, ClO-rich vortex air was more exposed to sunlight, where enhanced HOx abundances led to largely increased HOCl mixing ratios (up to 0.3 ppbv), exceeding typical midlatitudinal and tropical amounts significantly. The HOCl increase was preceded by an increase of ClO. Model runs could reproduce these measurements only when the Stimpfle et al. (1979) rate constant for the reaction ClO+HO2→HOCl+O2 was used but not with the current JPL recommendation. At an altitude of 24 km, HOCl mixing ratios of up to 0.15 ppbv were detected. This HOCl enhancement, which is already visible in 18 September data, is attributed to heterogeneous chemistry, which is in agreement with observations of polar stratospheric clouds. The measurements were compared to a model run where no polar stratospheric clouds appeared during the observation period. The fact that HOCl still was produced in the model run suggests that a significant part of HOCl was generated from ClO rather than directly via heterogeneous reaction. Excess ClO, lower ClONO2 and earlier loss of HOCl in the measurements are attributed to ongoing heterogeneous chemistry which is not reproduced by the model. On 11 October, polar vortex mean daytime mixing ratios were only 0.03 ppbv

Global stratospheric hydrogen peroxide distribution from MIPAS-Envisat full resolution spectra compared to KASIMA model results

MIPAS-ENVISAT full resolution spectra were analyzed to obtain a global distribution of hydrogen peroxide (H&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;2&lt;/sub&gt;) in the stratosphere. H&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;2&lt;/sub&gt; acts as reservoir gas for the HO&lt;sub&gt;x&lt;/sub&gt; family (= H+OH+HO&lt;sub&gt;2&lt;/sub&gt;) and thus, observations of H&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;2&lt;/sub&gt; provide a better understanding of the HO&lt;sub&gt;x&lt;/sub&gt; chemistry in the atmosphere. A retrieval approach based on constrained least squares fitting was developed and applied to small dedicated spectral analysis windows with maximum H&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;2&lt;/sub&gt; information and minimum contribution of interfering gases. Due to a low signal to noise ratio in the measured spectra single profiles cannot be used for scientific interpretation and about 100 profiles have to be averaged temporally or spatially. Our retrievals of H&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;2&lt;/sub&gt; from MIPAS measurements provide meaningful results between approximately 20 and 60 km. A possible impact by the high uncertainty of the reaction rate constant for HO&lt;sub&gt;2&lt;/sub&gt; + HO&lt;sub&gt;2&lt;/sub&gt;→H&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;2&lt;/sub&gt; + O&lt;sub&gt;2&lt;/sub&gt; in our 3D-CTM KASIMA is discussed. We find best agreement between model and observations for applying rate constants according to Christensen et al. (2002) however, a mismatch in vertical profile shape remains. The observations were compared to the model results of KASIMA focusing on low to mid latitudes. Good agreement in spatial distribution and in temporal evolution was found. Highest vmr of H&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;2&lt;/sub&gt; in the stratosphere were observed and modeled in low latitudes shortly after equinox at about 30 km. The modelled diurnal cycle with lowest vmr shortly after sunrise and highest vmr in the afternoon is confirmed by the MIPAS observations