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.

2018-9-20, Giono, Gabriel, Strelnikov, Boris, Asmus, Heiner, Staszak, Tristan, Ivchenko, Nickolay, Lübken, Franz-Josef

Characterising the photoelectron current induced by the Sun's UV radiation is crucial to ensure accurate daylight measurements from particle detectors. This article lays out the methodology used to address this problem in the case of the meteoric smoke particle detectors (MSPDs), developed by the Leibniz Institute of Atmospheric Physics in Kühlungsborn (IAP) and flown on board the PMWEs (Polar Mesosphere Winter Echoes) sounding rockets in April 2018. The methodology focuses on two complementary aspects: modelling and experimental measurements. A detailed model of the MSPD photocurrent was created based on the expected solar UV flux, the atmospheric UV absorption as a function of height by molecular oxygen and ozone, the photoelectric yield of the material coating the MSPD as a function of wavelength, the index of refraction of these materials as a function of wavelength and the angle of incidence of the illumination onto the MSPD. Due to its complex structure, composed of a central electrode shielded by two concentric grids, extensive ray-tracing calculations were conducted to obtain the incidence angles of the illumination on the central electrode, and this was done for various orientations of the MSPD in respect to the Sun. Results of the modelled photocurrent at different heights and for different materials, as well as for different orientations of the detector, are presented. As a pre-flight confirmation, the model was used to reproduce the experimental measurements conducted by Robertson et al. (2014) and agrees within an order of magnitude. An experimental setup for the calibration of the MSPD photocurrent is also presented. The photocurrent induced by the Lyman-alpha line from a deuterium lamp was recorded inside a vacuum chamber using a narrowband filter, while a UV-sensitive photodiode was used to monitor the UV flux. These measurements were compared with the model prediction, and also matched within an order of magnitude. Although precisely modelling the photocurrent is a challenging task, this article quantitatively improved the understanding of the photocurrent on the MSPD and discusses possible strategies to untangle the meteoric smoke particles (MSPs) current from the photocurrent recorded in-flight.

2010, Lee, J.D., McFiggans, G., Allan, J.D., Baker, A.R., Ball, S.M., Benton, A.K., Carpenter, L.J., Commane, R., Finley, B.D., Evans, M., Fuentes, E., Furneaux, K., Goddard, A., Good, N., Hamilton, J.F., Heard, D.E., Herrmann, H., Hollingsworth, A., Hopkins, J.R., Ingham, T., Irwin, M., Jones, C.E., Jones, R.L., Keene, W.C., Lawler, M.J., Lehmann, S., Lewis, A.C., Long, M.S., Mahajan, A., Methven, J., Moller, S.J., Müller, K., Müller, T., Niedermeier, N., O'Doherty, S., Oetjen, H., Plane, J.M.C., Pszenny, A.A.P., Read, K.A., Saiz-Lopez, A., Saltzman, E.S., Sander, R., von Glasow, R., Whalley, L., Wiedensohler, A., Young, D.

The NERC UK SOLAS-funded Reactive Halogens in the Marine Boundary Layer (RHaMBLe) programme comprised three field experiments. This manuscript presents an overview of the measurements made within the two simultaneous remote experiments conducted in the tropical North Atlantic in May and June 2007. Measurements were made from two mobile and one ground-based platforms. The heavily instrumented cruise D319 on the RRS Discovery from Lisbon, Portugal to São Vicente, Cape Verde and back to Falmouth, UK was used to characterise the spatial distribution of boundary layer components likely to play a role in reactive halogen chemistry. Measurements onboard the ARSF Dornier aircraft were used to allow the observations to be interpreted in the context of their vertical distribution and to confirm the interpretation of atmospheric structure in the vicinity of the Cape Verde islands. Long-term ground-based measurements at the Cape Verde Atmospheric Observatory (CVAO) on São Vicente were supplemented by long-term measurements of reactive halogen species and characterisation of additional trace gas and aerosol species during the intensive experimental period. This paper presents a summary of the measurements made within the RHaMBLe remote experiments and discusses them in their meteorological and chemical context as determined from these three platforms and from additional meteorological analyses. Air always arrived at the CVAO from the North East with a range of air mass origins (European, Atlantic and North American continental). Trace gases were present at stable and fairly low concentrations with the exception of a slight increase in some anthropogenic components in air of North American origin, though NOx mixing ratios during this period remained below 20 pptv (note the non-IUPAC adoption in this manuscript of pptv and ppbv, equivalent to pmol mol−1 and nmol mol−1 to reflect common practice). Consistency with these air mass classifications is observed in the time series of soluble gas and aerosol composition measurements, with additional identification of periods of slightly elevated dust concentrations consistent with the trajectories passing over the African continent. The CVAO is shown to be broadly representative of the wider North Atlantic marine boundary layer; measurements of NO, O3 and black carbon from the ship are consistent with a clean Northern Hemisphere marine background. Aerosol composition measurements do not indicate elevated organic material associated with clean marine air. Closer to the African coast, black carbon and NO levels start to increase, indicating greater anthropogenic influence. Lower ozone in this region is possibly associated with the increased levels of measured halocarbons, associated with the nutrient rich waters of the Mauritanian upwelling. Bromide and chloride deficits in coarse mode aerosol at both the CVAO and on D319 and the continuous abundance of inorganic gaseous halogen species at CVAO indicate significant reactive cycling of halogens. Aircraft measurements of O3 and CO show that surface measurements are representative of the entire boundary layer in the vicinity both in diurnal variability and absolute levels. Above the inversion layer similar diurnal behaviour in O3 and CO is observed at lower mixing ratios in the air that had originated from south of Cape Verde, possibly from within the ITCZ. ECMWF calculations on two days indicate very different boundary layer depths and aircraft flights over the ship replicate this, giving confidence in the calculated boundary layer depth.

2011, Mikkonen, S., Romakkaniemi, S., Smith, J.N., Korhonen, H., Petäjä, T., Plass-Duelmer, C., Boy, M., McMurry, P.H., Lehtinen, K.E.J., Joutsensaari, J., Hamed, A., Mauldin III, R.L., Birmili, W., Spindler, G., Arnold, F., Kulmala, M., Laaksonen, A.

Gaseous sulphuric acid is a key precursor for new particle formation in the atmosphere. Previous experimental studies have confirmed a strong correlation between the number concentrations of freshly formed particles and the ambient concentrations of sulphuric acid. This study evaluates a body of experimental gas phase sulphuric acid concentrations, as measured by Chemical Ionization Mass Spectrometry (CIMS) during six intensive measurement campaigns and one long-term observational period. The campaign datasets were measured in Hyytiälä, Finland, in 2003 and 2007, in San Pietro Capofiume, Italy, in 2009, in Melpitz, Germany, in 2008, in Atlanta, Georgia, USA, in 2002, and in Niwot Ridge, Colorado, USA, in 2007. The long term data were obtained in Hohenpeissenberg, Germany, during 1998 to 2000. The measured time series were used to construct proximity measures ("proxies") for sulphuric acid concentration by using statistical analysis methods. The objective of this study is to find a proxy for sulfuric acid that is valid in as many different atmospheric environments as possible. Our most accurate and universal formulation of the sulphuric acid concentration proxy uses global solar radiation, SO2 concentration, condensation sink and relative humidity as predictor variables, yielding a correlation measure (R) of 0.87 between observed concentration and the proxy predictions. Interestingly, the role of the condensation sink in the proxy was only minor, since similarly accurate proxies could be constructed with global solar radiation and SO2 concentration alone. This could be attributed to SO2 being an indicator for anthropogenic pollution, including particulate and gaseous emissions which represent sinks for the OH radical that, in turn, is needed for the formation of sulphuric acid.

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.

2006, Hellmuth, O.

In Paper I of four papers, a revised columnar high-order model to investigate gas-aerosol-turbulence interactions in the convective boundary layer (CBL) was proposed. In Paper II, the model capability to predict first-, second- and third-order moments of meteorological variables in the CBL was demonstrated using available observational data. In the present Paper III, the high-order modelling concept is extended to sulphur and ammonia chemistry as well as to aerosol dynamics. Based on the previous CBL simulation, a feasibility study is performed using two "clean air mass" scenarios with an emission source at the ground but low aerosol background concentration. Such scenarios synoptically correspond to the advection of fresh post-frontal air in an anthropogenically influenced region. The aim is to evaluate the time-height evolution of ultrafine condensation nuclei (UCNs) and to elucidate the interactions between meteorological and physicochemical variables in a CBL column. The scenarios differ in the treatment of new particle formation (NPF), whereas homogeneous nucleation according to the classical nucleation theory (CNT) is considered. The first scenario considers nucleation of a binary system consisting of water vapour and sulphuric acid (H2SO4) vapour, the second one nucleation of a ternary system additionally involving ammonia (NH3). Here, the two synthetic scenarios are discussed in detail, whereas special attention is payed to the role of turbulence in the formation of the typical UCN burst behaviour, that can often be observed in the surface layer. The intercomparison of the two scenarios reveals large differences in the evolution of the UCN number concentration in the surface layer as well as in the time-height cross-sections of first-order moments and double correlation terms. Although in both cases the occurrence of NPF bursts could be simulated, the burst characteristics and genesis of the bursts are completely different. It is demonstrated, that observations from the surface layer alone are not conclusive to elucidate the origin of newly formed particles. This is also true with respect to the interpretation of box modelling studies. The binary and ternary NPF bursts observed in the surface layer differ with respect to burst amplitude and phase. New particles simulated in the binary scenario are formed in the forenoon in the upper part of the growing CBL, followed by turbulence-induced top-down transport. Hence, with respect to the burst observation site in the surface layer, new particles are formed ex situ. In opposite to this, the ternary case reveals a much more complex pattern. Here, NPF is initiated in the early morning hours in the surface layer, when temperature (T) is low and relative humidity (RH), sulphur dioxide (SO2) and NH3 concentrations are high, hence new particles are formed in situ. Shortly after that, ex situ NPF in the free troposphere sets in, followed by entrainment and top-down diffusion of newly formed particles into the surface layer. Altogether, these processes mainly contribute to the formation of a strong burst in the morning hours in the ternary scenario. While the time-height cross-section of the binary nucleation rate resembles a "blob"-like evolution pattern, the ternary one resembles a "sucking tube"-like pattern. The time-height cross-sections of the flux pattern and double correlations could be plausibly interpreted in terms of CBL turbulence and entrainment/detrainment processes both in the binary and in the ternary case. Although the present approach is a pure conceptual one, it shows the feasibility to simulate gas-aerosol-turbulence interactions in the CBL. Prior to a dedicated verification/validation study, further attempts are necessary to consider a more advanced description of the formation and activation of thermodynamically stable clusters according to modern concepts proposed by Kulmala et al. (2000), Kulmala (2003) and Kulmala et al. (2004a).

2011, Hartmann, S., Niedermeier, D., Voigtländer, J., Clauss, T., Shaw, R.A., Wex, H., Kiselev, A., Stratmann, F.

At the Leipzig Aerosol Cloud Interaction Simulator (LACIS) experiments investigating homogeneous and heterogeneous nucleation of ice (particularly immersion freezing in the latter case) have been carried out. Here both the physical LACIS setup and the numerical model developed to design experiments at LACIS and interpret their results are presented in detail. Combining results from the numerical model with experimental data, it was found that for the experimental parameter space considered, classical homogeneous ice nucleation theory is able to predict the freezing behavior of highly diluted ammonium sulfate solution droplets, while classical heterogeneous ice nucleation theory, together with the assumption of a constant contact angle, fails to predict the immersion freezing behavior of surrogate mineral dust particles (Arizona Test Dust, ATD). The main reason for this failure is the compared to experimental data apparently overly strong temperature dependence of the nucleation rate coefficient. Assuming, in the numerical model, Classical Nucleation Theory (CNT) for homogeneous ice nucleation and a CNT-based parameterization for the nucleation rate coefficient in the immersion freezing mode, recently published by our group, it was found that even for a relatively effective ice nucleating agent such as pure ATD, there is a temperature range where homogeneous ice nucleation is dominant. The main explanation is the apparently different temperature dependencies of the two freezing mechanisms. Finally, reviewing the assumptions made during the derivation of the CNT-based parameterization for immersion freezing, it was found that the assumption of constant temperature during ice nucleation and the chosen ice nucleation time were justified, underlining the applicability of the method to determine the fitting coefficients in the parameterization equation.

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.

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.

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.