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- ItemMegacity and local contributions to regional air pollution: An aircraft case study over London(Katlenburg-Lindau : EGU, 2020) Ashworth, Kirsti; Bucci, Silvia; Gallimore, Peter J.; Lee, Junghwa; Nelson, Beth S.; Sanchez-Marroquín, Alberto; Schimpf, Marina B.; Smith, Paul D.; Drysdale, Will S.; Hopkins, Jim R.; Lee, James D.; Pitt, Joe R.; Di Carlo, Piero; Krejci, Radovan; McQuaid, James B.In July 2017 three research flights circumnavigating the megacity of London were conducted as a part of the STANCO training school for students and early career researchers organised by EUFAR (European Facility for Airborne Research). Measurements were made from the UK's Facility for Airborne Atmospheric Measurements (FAAM) BAe-146-301 atmospheric research aircraft with the aim to sample, characterise and quantify the impact of megacity outflow pollution on air quality in the surrounding region. Conditions were extremely favourable for airborne measurements, and all three flights were able to observe clear pollution events along the flight path. A small change in wind direction provided sufficiently different air mass origins over the 2 d such that a distinct pollution plume from London, attributable marine emissions and a double-peaked dispersed area of pollution resulting from a combination of local and transported emissions were measured. We were able to analyse the effect of London emissions on air quality in the wider region and the extent to which local sources contribute to pollution events. The background air upwind of London was relatively clean during both days; concentrations of CO were 88-95 ppbv, total (measured) volatile organic compounds (VOCs) were 1.6-1.8 ppbv and NOx was 0.7- 0.8 ppbv. Downwind of London, we encountered elevations in all species with CO>100 ppbv, VOCs 2.8-3.8 ppbv, CH4>2080 ppbv and NOx>4 ppbv, and peak concentrations in individual pollution events were higher still. Levels of O3 were inversely correlated with NOx during the first flight, with O3 concentrations of 37 ppbv upwind falling to 26 ppbv in the well-defined London plume. Total pollutant fluxes from London were estimated through a vertical plane downwind of the city. Our calculated CO2 fluxes are within the combined uncertainty of those estimated previously, but there was a greater disparity in our estimates of CH4 and CO. On the second day, winds were lighter and downwind O3 concentrations were elevated to 39-43 ppbv (from 32 to 35 ppbv upwind), reflecting the contribution of more aged pollution to the regional background. Elevations in pollutant concentrations were dispersed over a wider area than the first day, although we also encountered a number of clear transient enhancements from local sources. This series of flights demonstrated that even in a region of megacity outflow, such as the south-east of the UK, local fresh emissions and more distant UK sources of pollution can all contribute substantially to pollution events. In the highly complex atmosphere around a megacity where a high background level of pollution mixes with a variety of local sources at a range of spatial and temporal scales and atmospheric dynamics are further complicated by the urban heat island, the use of pollutant ratios to track and determine the ageing of air masses may not be valid. The individual sources must therefore all be well-characterised and constrained to understand air quality around megacities such as London. Research aircraft offer that capability through targeted sampling of specific sources and longitudinal studies monitoring trends in emission strength and profiles over time. © 2020 Copernicus GmbH. All rights reserved.
- ItemModel simulations of chemical effects of sprites in relation with observed HO2 enhancements over sprite-producing thunderstorms(Katlenburg-Lindau : European Geosciences Union, 2021) Winkler, Holger; Yamada, Takayoshi; Kasai, Yasuko; Berger, Uwe; Notholt, JustusRecently, measurements by the Superconducting Submillimeter-Wave Limb Emission Sounder (SMILES) satellite instrument have been presented which indicate an increase in mesospheric HO2 above sprite-producing thunderstorms. The aim of this paper is to compare these observations to model simulations of chemical sprite effects. A plasma chemistry model in combination with a vertical transport module was used to simulate the impact of a streamer discharge in the altitude range 70–80 km, corresponding to one of the observed sprite events. Additionally, a horizontal transport and dispersion model was used to simulate advection and expansion of the sprite air masses. The model simulations predict a production of hydrogen radicals mainly due to reactions of proton hydrates formed after the electrical discharge. The net effect is a conversion of water molecules into H+OH. This leads to increasing HO2 concentrations a few hours after the electric breakdown. Due to the modelled long-lasting increase in HO2 after a sprite discharge, an accumulation of HO2 produced by several sprites appears possible. However, the number of sprites needed to explain the observed HO2 enhancements is unrealistically large. At least for the lower measurement tangent heights, the production mechanism of HO2 predicted by the model might contribute to the observed enhancements.
- 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.
- ItemEffective CO2 lifetime and future CO2 levels based on fit function(Göttingen : Copernicus, 2013) Sonnemann, G.R.; Grygalashvyly, M.The estimated global CO2 emission rates and the measured atmospheric CO2 concentrations show that only a certain share of the emitted CO2 accumulates in the atmosphere. For given atmospheric emissions of CO2, the effective lifetime determines its accumulation in the atmosphere and, consequently, its impact on the future global warming. We found that on average the inferred effective lifetime of CO2 decreases as its atmospheric concentration increases, reducing the rate of its accumulation in the atmosphere. We derived a power function that fits the varying lifetimes. Based on this fitting function, we calculated the increase of CO2 for different scenarios of future global emission rates.
- ItemAtmospheric band fitting coefficients derived from a self-consistent rocket-borne experiment(Göttingen : Copernicus GmbH, 2019) Grygalashvyly, M.; Eberhart, M.; Hedin, J.; Strelnikov, B.; Lübken, F.-J.; Rapp, M.; Löhle, S.; Fasoulas, S.; Khaplanov, M.; Gumbel, J.; Vorobeva, E.Based on self-consistent rocket-borne measurements of temperature, the densities of atomic oxygen and neutral air, and the volume emission of the atmospheric band (762 nm), we examined the one-step and two-step excitation mechanism of O2 + b16C g for nighttime conditions. Following McDade et al. (1986), we derived the empirical fitting coefficients, which parameterize the atmospheric band emission O2 + b16C g X36 g .0;0/. This allows us to derive the atomic oxygen concentration from nighttime observations of atmospheric band emission O2 + b16C g X36 g .0; 0/. The derived empirical parameters can also be utilized for atmospheric band modeling. Additionally, we derived the fit function and corresponding coefficients for the combined (one- and two-step) mechanism. The simultaneous common volume measurements of all the parameters involved in the theoretical calculation of the observed O2 + b16C g X36 g .0; 0/ emission, i.e., temperature and density of the background air, atomic oxygen density, and volume emission rate, is the novelty and the advantage of this work. © Author(s) 2019.
- ItemGlobal annual methane emission rate derived from its current atmospheric mixing ratio and estimated lifetime(Göttingen : Copernicus, 2014) Sonnemann, G.R.; Grygalashvyly, M.We use the estimated lifetime of methane (CH4), the current methane concentration, and its annual growth rate to calculate the global methane emission rate. The upper and lower limits of the annual global methane emission rate, depending on loss of CH4 into the stratosphere and methane consuming bacteria, amounts to 648.0 Mt a-1 and 608.0 Mt a-1. These values are in reasonable agreement with satellite and with much more accurate in situ measurements of methane. We estimate a mean tropospheric and mass-weighted temperature related to the reaction rate and employ a mean OH-concentration to calculate a mean methane lifetime. The estimated atmospheric lifetime of methane amounts to 8.28 years and 8.84 years, respectively. In order to improve the analysis a realistic 3D-calculations should be performed.
- ItemRetrieval of ice-nucleating particle concentrations from lidar observations and comparison with UAV in situ measurements(Katlenburg-Lindau : EGU, 2019) Marinou, Eleni; Tesche, Matthias; Nenes, Athanasios; Ansmann, Albert; Schrod, Jann; Mamali, Dimitra; Tsekeri, Alexandra; Pikridas, Michael; Baars, Holger; Engelmann, Ronny; Voudouri, Kalliopi-Artemis; Solomos, Stavros; Sciare, Jean; Groß, Silke; Ewald, Florian; Amiridis, VassilisAerosols that are efficient ice-nucleating particles (INPs) are crucial for the formation of cloud ice via heterogeneous nucleation in the atmosphere. The distribution of INPs on a large spatial scale and as a function of height determines their impact on clouds and climate. However, in situ measurements of INPs provide sparse coverage over space and time. A promising approach to address this gap is to retrieve INP concentration profiles by combining particle concentration profiles derived by lidar measurements with INP efficiency parameterizations for different freezing mechanisms (immersion freezing, deposition nucleation). Here, we assess the feasibility of this new method for both ground-based and spaceborne lidar measurements, using in situ observations collected with unmanned aerial vehicles (UAVs) and subsequently analyzed with the FRIDGE (FRankfurt Ice nucleation Deposition freezinG Experiment) INP counter from an experimental campaign at Cyprus in April 2016. Analyzing five case studies we calculated the cloud-relevant particle number concentrations using lidar measurements (n250,dry with an uncertainty of 20 % to 40 % and Sdry with an uncertainty of 30 % to 50 %), and we assessed the suitability of the different INP parameterizations with respect to the temperature range and the type of particles considered. Specifically, our analysis suggests that our calculations using the parameterization of Ullrich et al. (2017) (applicable for the temperature range −50 to −33 ∘C) agree within 1 order of magnitude with the in situ observations of nINP; thus, the parameterization of Ullrich et al. (2017) can efficiently address the deposition nucleation pathway in dust-dominated environments. Additionally, our calculations using the combination of the parameterizations of DeMott et al. (2015, 2010) (applicable for the temperature range −35 to −9 ∘C) agree within 2 orders of magnitude with the in situ observations of INP concentrations (nINP) and can thus efficiently address the immersion/condensation pathway of dust and nondust particles. The same conclusion is derived from the compilation of the parameterizations of DeMott et al. (2015) for dust and Ullrich et al. (2017) for soot.
- ItemHydroxyl layer: trend of number density and intra-annual variability(Katlenburg, Lindau : Copernicus, 2015) Sonnemann, G.R.; Hartogh, P.; Berger, U.; Grygalashvyly, M.The layer of vibrationally excited hydroxyl (OH*) near the mesopause in Earth's atmosphere is widely used to derive the temperature at this height and to observe dynamical processes such as gravity waves. The concentration of OH* is controlled by the product of atomic hydrogen, with ozone creating a layer of enhanced concentration in the mesopause region. However, the basic influences on the OH* layer are atomic oxygen and temperature. The long-term monitoring of this layer provides information on a changing atmosphere. It is important to know which proportion of a trend results from anthropogenic impacts on the atmosphere and which proportion reflects natural variations. In a previous paper (Grygalashvyly et al., 2014), the trend of the height of the layer and the trend in temperature were investigated particularly in midlatitudes on the basis of our coupled dynamic and chemical transport model LIMA (Leibniz Institute Middle Atmosphere). In this paper we consider the trend for the number density between the years 1961 and 2009 and analyze the reason of the trends on a global scale. Further, we consider intra-annual variations. Temperature and wind have the strongest impacts on the trend. Surprisingly, the increase in greenhouse gases (GHGs) has no clear influence on the chemistry of OH*. The main reason for this lies in the fact that, in the production term of OH*, if atomic hydrogen increases due to increasing humidity of the middle atmosphere by methane oxidation, ozone decreases. The maximum of the OH* layer is found in the mesopause region and is very variable. The mesopause region is a very intricate domain marked by changeable dynamics and strong gradients of all chemically active minor constituents determining the OH* chemistry. The OH* concentration responds, in part, very sensitively to small changes in these parameters. The cause for this behavior is given by nonlinear reactions of the photochemical system being a nonlinear enforced chemical oscillator driven by the diurnal-periodic solar insolation. At the height of the OH* layer the system operates in the vicinity of chemical resonance. The solar cycle is mirrored in the data, but the long-term behavior due to the trend in the Lyman-α radiation is very small. The number density shows distinct hemispheric differences. The calculated OH* values show sometimes a step around a certain year. We introduce a method to find out the date of this step and discuss a possible reason for such behavior.