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- ItemSensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics(Göttingen : Copernicus GmbH, 2009) Kawa, S.R.; Stolarski, R.S.; Newman, P.A.; Douglass, A.R.; Rex, M.; Hofmann, D.J.; Santee, M.L.; Frieler, K.The impact and significance of uncertainties in model calculations of stratospheric ozone loss resulting from known uncertainty in chemical kinetics parameters is evaluated in trajectory chemistry simulations for the Antarctic and Arctic polar vortices. The uncertainty in modeled ozone loss is derived from Monte Carlo scenario simulations varying the kinetic (reaction and photolysis rate) parameters within their estimated uncertainty bounds. Simulations of a typical winter/spring Antarctic vortex scenario and Match scenarios in the Arctic produce large uncertainty in ozone loss rates and integrated seasonal loss. The simulations clearly indicate that the dominant source of model uncertainty in polar ozone loss is uncertainty in the Cl2O 2 photolysis reaction, which arises from uncertainty in laboratory-measured molecular cross sections at atmospherically important wavelengths. This estimated uncertainty in JCl 2O2 from laboratory measurements seriously hinders our ability to model polar ozone loss within useful quantitative error limits. Atmospheric observations, however, suggest that the Cl2O2 photolysis uncertainty may be less than that derived from the lab data. Comparisons to Match, South Pole ozonesonde, and Aura Microwave Limb Sounder (MLS) data all show that the nominal recommended rate simulations agree with data within uncertainties when the Cl2O2 photolysis error is reduced by a factor of two, in line with previous in situ ClOx measurements. Comparisons to simulations using recent cross sections from Pope et al. (2007) are outside the constrained error bounds in each case. Other reactions producing significant sensitivity in polar ozone loss include BrO + ClO and its branching ratios. These uncertainties challenge our confidence in modeling polar ozone depletion and projecting future changes in response to changing halogen emissions and climate. Further laboratory, theoretical, and possibly atmospheric studies are needed.
- ItemMass analysis of charged aerosol particles in NLC and PMSE during the ECOMA/MASS campaign(München : European Geopyhsical Union, 2009) Robertson, S.; Horányi, M.; Knappmiller, S.; Sternovsky, Z.; Holzworth, R.; Shimogawa, M.; Friedrich, M.; Torkar, K.; Gumbel, J.; Megner, L.; Baumgarten, G.; Latteck, R.; Rapp, M.; Hoppe, U.-P.; Hervig, M.E.MASS (Mesospheric Aerosol Sampling Spectrometer) is a multichannel mass spectrometer for charged aerosol particles, which was flown from the Andøya Rocket Range, Norway, through NLC and PMSE on 3 August 2007 and through PMSE on 6 August 2007. The eight-channel analyzers provided for the first time simultaneous measurements of the charge density residing on aerosol particles in four mass ranges, corresponding to ice particles with radii <0.5 nm (including ions), 0.5–1 nm, 1–2 nm, and >3 nm (approximately). Positive and negative particles were recorded on separate channels. Faraday rotation measurements provided electron density and a means of checking charge density measurements made by the spectrometer. Additional complementary measurements were made by rocket-borne dust impact detectors, electric field booms, a photometer and ground-based radar and lidar. The MASS data from the first flight showed negative charge number densities of 1500–3000 cm−3 for particles with radii >3 nm from 83–88 km approximately coincident with PMSE observed by the ALWIN radar and NLC observed by the ALOMAR lidar. For particles in the 1–2 nm range, number densities of positive and negative charge were similar in magnitude (~2000 cm−3) and for smaller particles, 0.5–1 nm in radius, positive charge was dominant. The occurrence of positive charge on the aerosol particles of the smallest size and predominately negative charge on the particles of largest size suggests that nucleation occurs on positive condensation nuclei and is followed by collection of negative charge during subsequent growth to larger size. Faraday rotation measurements show a bite-out in electron density that increases the time for positive aerosol particles to be neutralized and charged negatively. The larger particles (>3 nm) are observed throughout the NLC region, 83–88 km, and the smaller particles are observed primarily at the high end of the range, 86–88 km. The second flight into PMSE alone at 84–88 km, found only small number densities (~500 cm−3) of particles >3 nm in a narrow altitude range, 86.5–87.5 km. Both positive (~2000 cm−3) and negative (~4500 cm−3) particles with radii 1–2 nm were detected from 85–87.5 km.
- ItemA case study of a sporadic sodium layer observed by the ALOMAR Weber Na lidar(München : European Geopyhsical Union, 2008) Nesse, H.; Heinrich, D.; Williams, B.; Hoppe, U.-P.; Stadsnes, J.; Rietveld, M.; Singer, W.; Blum, U.; Sandanger, M.I.; Trondsen, E.Simultaneous measurements of temperature and polar mesosphere summer echoes (PMSE) were performed at the polar cap (78° N) during summer 2001 and 2003. In summer time the mesopause region is characterized by extremely low temperatures around 120 K. It is remarkable that PMSE are practically never observed above 92 km although temperatures are low enough to allow the existence of ice particles. In this case study we compare the PMSE topside with temperatures measured by the potassium lidar and with frost point temperatures using water-vapor mixing ratios from models. We find striking discrepancies with our current understanding of ice particles and temperature in this region. In this case study we find that the temperature can be more than 20 K lower than the frost point temperature but no PMSE is observed above 92 km altitude. We show that the lack of PMSE does not necessarily imply that the temperature is too high.
- ItemThe contribution of sulphuric acid to atmospheric particle formation and growth: A comparison between boundary layers in Northern and Central Europe(München : European Geopyhsical Union, 2005) Fiedler, V.; Dal Maso, M.; Boy, M.; Aufmhoff, H.; Hoffmann, J.; Schuck, T.; Birmili, W.; Hanke, M.; Uecker, J.; Arnold, F.; Kulmala, M.Atmospheric gaseous sulphuric acid was measured and its influence on particle formation and growth was investigated building on aerosol data. The measurements were part of the EU-project QUEST and took place at two different measurement sites in Northern and Central Europe (Hyytiälä, Finland, March-April 2003 and Heidelberg, Germany, March-April 2004). From a comprehensive data set including sulphuric acid, particle number size distributions and meteorological data, particle growth rates, particle formation rates and source rates of condensable vapors were inferred. Growth rates were determined in two different ways, from particle size distributions as well as from a so-called timeshift analysis. Moreover, correlations between sulphuric acid and particle number concentration between 3 and 6 nm were examined and the influence of air masses of different origin was investigated. Measured maximum concentrations of sulphuric acid were in the range from 1x106 to 16x106cm-3. The gaseous sulphuric acid lifetime with respect to condensation on aerosol particles ranged from 2 to 33min in Hyytiälä and from 0.5 to 8 min in Heidelberg. Most calculated values (growth rates, formation rates, vapor source rates) were considerably higher in Central Europe (Heidelberg), due to the more polluted air and higher preexistent aerosol concentrations. Close correlations between H2SO4 and nucleation mode particles (size range: 3-6 nm) were found on most days at both sites. The percentage contribution of sulphuric acid to particle growth was below 10% at both places and to initial growth below 20%. An air mass analysis indicated that at Heidelberg new particles were formed predominantly in air advected from southwesterly directions.
- ItemLong-term behavior of the concentration of the minor constituents in the mesosphere-a model study(Göttingen : Copernicus, 2009) Grygalashvyly, M.; Sonnemann, G.R.; Hartogh, P.We investigate the influence the rising concentrations of methane, nitrous oxide and carbon dioxide which have occurred since the pre-industrial era, have had on the chemistry of the mesosphere. For this investigation we use our global 3-D-model COMMA-IAP which was designed for the exploration of the MLT-region and in particular the extended mesopause region. Assumptions and approximations for the trends in the Lyman-flux (needed for the water vapor dissociation rate), methane and the water vapor mixing ratio at the hygropause are necessary to accomplish this study. To approximate the solar Lyman-α flux back to the pre-industrial time, we derived a quadratic fit using the sunspot number record which extends back to 1749 and is the only solar proxy available for the Lyman-α flux prior to 1947. We assume that methane increases with a constant growth rate from the pre-industrial era to the present. An unsolved problem for the model calculations consists of how the water vapor mixing ratio at the hygropause should be specified during this period. We assume that the hygropause was dryer during pre-industrial times than the present. As a consequence of methane oxidation, the model simulation indicates that the middle atmosphere has become more humid as a result of the rising methane concentration, but with some dependence on height and with a small time delay of few years. The solar influence on the water vapor mixing ratio is insignificant below about 80 km in summer high latitudes, but becomes increasingly more important above this altitude. The enhanced water vapor concentration increasesthe hydrogen radical concentration and reduces the mesospheric ozone. A second region of stronger ozone decrease is located in the vicinity of the stratopause. Increases in CO2 concentration enhance slightly the concentration of CO in the mesosphere. However, its influence upon the chemistry is small and its main effect is connected with a cooling of the upper atmosphere. The long-term behavior of water vapor is discussed in particular with respect to its impact on the NLC region.
- ItemLarge mesospheric ice particles at exceptionally high altitudes(München : European Geopyhsical Union, 2009) Megner, L.; Khaplanov, M.; Baumgarten, G.; Gumbel, J.; Stegman, J.; Strelnikov, B.; Robertson, S.We here report on the characteristics of exceptionally high Noctilucent clouds (NLC) that were detected with rocket photometers during the ECOMA/MASS campaign at Andøya, Norway 2007. The results from three separate flights are shown and discussed in connection to lidar measurements. Both the lidar measurements and the large difference between various rocket passages through the NLC show that the cloud layer was inhomogeneous on large scales. Two passages showed a particularly high, bright and vertically extended cloud, reaching to approximately 88 km. Long time series of lidar measurements show that NLC this high are very rare, only one NLC measurement out of thousand reaches above 87 km. The NLC is found to consist of three distinct layers. All three were bright enough to allow for particle size retrieval by phase function analysis, even though the lowest layer proved too horizontally inhomogeneous to obtain a trustworthy result. Large particles, corresponding to an effective radius of 50 nm, were observed both in the middle and top of the NLC. The present cloud does not comply with the conventional picture that NLC ice particles nucleate near the temperature minimum and grow to larger sizes as they sediment to lower altitudes. Strong up-welling, likely caused by gravity wave activity, is required to explain its characteristics.
- ItemThe ECOMA 2007 campaign: Rocket observations and numerical modelling of aerosol particle charging and plasma depletion in a PMSE/NLC layer(München : European Geopyhsical Union, 2009) Brattli, A.; Lie-Svendsen, Ø.; Svenes, K.; Hoppe, U.-P.; Strelnikova, I.; Rapp, M.; Latteck, R.; Torkar, K.; Gumbel, J.; Megner, L.; Baumgarten, G.The ECOMA series of rocket payloads use a set of aerosol particle, plasma, and optical instruments to study the properties of aerosol particles and their interaction with the ambient plasma environment in the polar mesopause region. In August 2007 the ECOMA-3 payload was launched into a region with Polar Mesosphere Summer Echoes (PMSE) and noctilucent clouds (NLC). An electron depletion was detected in a broad region between 83 and 88 km, coincident with enhanced density of negatively charged aerosol particles. We also find evidence for positive ion depletion in the same region. Charge neutrality requires that a population of positively charged particles smaller than 2 nm and with a density of at least 2×108 m−3 must also have been present in the layer, undetected by the instruments. A numerical model for the charging of aerosol particles and their interaction with the ambient plasma is used to analyse the results, showing that high aerosol particle densities are required in order to explain the observed ion density depletion. The model also shows that a very high photoionisation rate is required for the particles smaller than 2 nm to become positively charged, indicating that these may have a lower work function than pure water ice.
- ItemThe noctilucent cloud (NLC) display during the ECOMA/MASS sounding rocket flights on 3 August 2007: Morphology on global to local scales(München : European Geopyhsical Union, 2009) Baumgarten, G.; Fiedler, J.; Fricke, K.H.; Gerding, M.; Hervig, M.; Hoffmann, P.; Müller, N.; Pautet, P.-D.; Rapp, M.; Robert, C.; Rusch, D.; von Savigny, C.; Singer, W.During the ECOMA/MASS rocket campaign large scale NLC/PMC was observed by satellite, lidar and camera from polar to mid latitudes. We examine the observations from different instruments to investigate the morphology of the cloud. Satellite observations show a planetary wave 2 structure. Lidar observations from Kühlungsborn (54° N), Esrange (68° N) and ALOMAR (69° N) show a highly dynamic NLC layer. Under favorable solar illumination the cloud is also observable by ground-based cameras. The cloud was detected by cameras from Trondheim (63° N), Juliusruh (55° N) and Kühlungsborn. We investigate planetary scale morphology and local scale gravity wave structures, important for the interpretation of the small scale rocket soundings. We compare in detail the lidar observations with the NLC structure observed by the camera in Trondheim. The ALOMAR RMR-lidar observed only a faint NLC during the ECOMA launch window, while the camera in Trondheim showed a strong NLC display in the direction of ALOMAR. Using the high resolution camera observations (t~30 s, Δx<5 km) and the wind information from the meteor radar at ALOMAR we investigate the formation and destruction of NLC structures. We observe that the NLC brightness is reduced by a factor of 20–40 within 100 s which can be caused by a temperature about 15 K above the frostpoint temperature. A horizontal temperature gradient of more than 3 K/km is estimated.
- ItemOccurrence of polar mesosphere summer echoes at very high latitudes(München : European Geopyhsical Union, 2009) Zecha, M.; Röttger, J.Observations of polar mesosphere summer echoes (PMSE) have been carried out during the summer periodes 1999–2001 and 2003–2004 at the very high latitude of 78° N using the SOUSY Svalbard Radar (53.5 MHz) at Longyearbyen. Although the measurements could not be done continuously in these seasons, PMSE have been detected over more than 6600 h of 9300 h of observation time overall. Using this data base, particular PMSE occurrence characteristics have been determined. PMSE at Svalbard appear from the middle of May to the end of August with an almost permanent total occurrence in June and July. Diurnal variations are observable in the height-depend occurrence rates and in PMSE thickness, they show a maximum around 09:00–10:00 UTC and a minimum around 21:00–22:00 UTC. PMSE occur nearly exclusively between a height of 80 km and 92 km with a maximum near 85 km. However, PMSE appear not simultaneously over the entire height range, the mean vertical PMSE extension is around 4–6 km in June and July. Furthermore, typically PMSE are separated into several layers, and only 30% of all PMSE are single layers. The probability of multiple layers is greater in June and July than at the beginning and the end of the PMSE season and shows a marked 5-day-variation. The same variation is noticeable in the seasonal dependence of the PMSE occurrence and the PMSE thickness. We finally discuss potential geophysical processes to explain our observational results.
- ItemOn the two-day oscillations and the day-to-day variability in global 3-D-modeling of the chemical system of the upper mesosphere/mesopause region(Göttingen : Copernicus GmbH, 2005) Sonnemann, G.R.; Grygalashvyly, M.The integration of the photochemical system of the upper mesosphere/ mesopause region brought evidence that the system is able to respond in a nonlinear manner under certain conditions. Under the action of the diurnallyperiodic insolation, the system creates subharmonic oscillations or chaos if disregarding strong diffusion, and under special conditions it possesses multiple solutions. The models used in the past were simplified and idealized in view of the number of dimensions and the consideration of the full dynamics. On the basis of our global 3-D-model of the dynamics and chemistry of the middle atmosphere (COMMAIAP), we also found a nonlinear response in the photochemistry under realistic conditions. The model under consideration is not yet self-consistent, but the chemical model uses the dynamical fields calculated by the dynamic model. From our calculations we got period-2 oscillations of the photochemical system within confined latitudinal regions around the solstices but not during the equinoxes. The consequence of the period-2 oscillation of the chemical active minor constituents is that a marked two-day variation of the chemical heating rates is an important thermal pumping mechanism. We discuss these findings particularly in terms of the influence of realistic dynamics on the creation of nonlinear effects.