scholarly journals The influence of deep convection on HCHO and H<sub>2</sub>O<sub>2</sub> in the upper troposphere over Europe

2017 ◽  
Vol 17 (19) ◽  
pp. 11835-11848 ◽  
Author(s):  
Heiko Bozem ◽  
Andrea Pozzer ◽  
Hartwig Harder ◽  
Monica Martinez ◽  
Jonathan Williams ◽  
...  

Abstract. Deep convection is an efficient mechanism for vertical trace gas transport from Earth's surface to the upper troposphere (UT). The convective redistribution of short-lived trace gases emitted at the surface typically results in a C-shaped profile. This redistribution mechanism can impact photochemical processes, e.g. ozone and radical production in the UT on a large scale due to the generally longer lifetimes of species like formaldehyde (HCHO) and hydrogen peroxide (H2O2), which are important HOx precursors (HOx =  OH + HO2 radicals). Due to the solubility of HCHO and H2O2 their transport may be suppressed as they are efficiently removed by wet deposition. Here we present a case study of deep convection over Germany in the summer of 2007 within the framework of the HOOVER II project. Airborne in situ measurements within the in- and outflow regions of an isolated thunderstorm provide a unique data set to study the influence of deep convection on the transport efficiency of soluble and insoluble trace gases. Comparing the in- and outflow indicates an almost undiluted transport of insoluble trace gases from the boundary layer to the UT. The ratios of out : inflow of CO and CH4 are 0.94 ± 0.04 and 0.99 ± 0.01, respectively. For the soluble species HCHO and H2O2 these ratios are 0.55 ± 0.09 and 0.61 ± 0.08, respectively, indicating partial scavenging and washout. Chemical box model simulations show that post-convection secondary formation of HCHO and H2O2 cannot explain their enhancement in the UT. A plausible explanation, in particular for the enhancement of the highly soluble H2O2, is degassing from cloud droplets during freezing, which reduces the retention coefficient.

2017 ◽  
Author(s):  
Heiko Bozem ◽  
Andrea Pozzer ◽  
Hartwig Harder ◽  
Monica Martinez ◽  
Jonathan Williams ◽  
...  

Abstract. Deep convection is an efficient mechanism for vertical trace gas transport from the Earth's surface to the upper troposphere (UT). The convective redistribution of short-lived trace gases emitted at the surface typically results in a C-shaped profile. This redistribution mechanism can impact photochemical processes, e.g. ozone and radical production in the UT on a large scale due to the generally longer lifetimes of species like formaldehyde (HCHO) and hydrogen peroxide (H2O2), which are important HOx precursors (HOx = OH + HO2 radicals). Due to the solubility of HCHO and H2O2 their transport may be suppressed as they are efficiently removed by wet deposition. Here we present a case study of deep convection over Germany in the summer of 2007 within the framework of the HOOVER II project. Airborne in-situ measurements within the in- and outflow regions of an isolated thunderstorm provide a unique data set to study the influence of deep convection on the transport efficiency of soluble and insoluble trace gases. Comparing the in- and outflow indicates almost undiluted transport of insoluble trace gases from the boundary layer to the UT. The ratios of out/inflow of CO and CH4 are 0.94 ± 0.04 and 0.99 ± 0.01, respectively. For the soluble species HCHO and H2O2 these ratios are 0.55 ± 0.09 and 0.61 ± 0.08, respectively, indicating partial scavenging and washout. Chemical box model simulations show that post-convection secondary formation of HCHO and H2O2 cannot explain their enhancement in the UT. A plausible explanation, in particular for the enhancement of the highly soluble H2O2, is degassing from cloud droplets during freezing, which reduces the retention coefficient.


2004 ◽  
Vol 17 (23) ◽  
pp. 4541-4563 ◽  
Author(s):  
Zhengzhao Luo ◽  
William B. Rossow

Abstract Tropical cirrus evolution and its relation to upper-tropospheric water vapor (UTWV) are examined in the paper by analyzing satellite-derived cloud data, UTWV data from infrared and microwave measurements, and the NCEP–NCAR reanalysis wind field. Building upon the existing International Satellite Cloud Climatology Project (ISCCP) data and the Television and Infrared Observation Satellite (TIROS) Operational Vertical Sounder (TOVS) product, a global (except polar region), 6-hourly cirrus dataset is developed from two infrared radiance measurements at 11 and 12 μm. The UTWV is obtained in both clear and cloudy locations by developing a combined satellite infrared and microwave-based retrieval. The analysis in this study is conducted in a Lagrangian framework. The Lagrangian trajectory analysis shows that the decay of deep convection is immediately followed by the growth of cirrostratus and cirrus, and then the decay of cirrostratus is followed by the continued growth of cirrus. Cirrus properties continuously evolve along the trajectories as they gradually thin out and move to the lower levels. Typical tropical cirrus systems last for 19–30 ± 16 h. This is much longer than cirrus particle lifetimes, suggesting that other processes (e.g., large-scale lifting) replenish the particles to maintain tropical cirrus. Consequently, tropical cirrus can advect over large distances, about 600–1000 km, during their lifetimes. For almost all current GCMs, this distance spans more than one grid box, requiring that the water vapor and cloud water budgets include an advection term. Based on their relationship to convective systems, detrainment cirrus are distinguished from in situ cirrus. It is found that more than half of the tropical cirrus are formed in situ well away from convection. The interaction between cirrus and UTWV is explored by comparing the evolution of the UTWV along composite clear trajectories and trajectories with cirrus. Cirrus are found to be associated with a moister upper troposphere and a slower rate of decrease of UTWV. Moreover, the elevated UTWV has a longer duration than cirrus. The amount of water in cirrus is too small for evaporation of cirrus ice particles to moisten the upper troposphere significantly (but cirrus may be an important water vapor sink). Rather, it is likely that the same transient motions that produce the cirrus also transport water vapor upward to maintain a larger UTWV.


2008 ◽  
Vol 8 (1) ◽  
pp. 403-452
Author(s):  
M. Salzmann ◽  
M. G. Lawrence ◽  
V. T. J. Phillips ◽  
L. J. Donner

Abstract. A cloud system resolving model including photo-chemistry (CSRMC) has been developed based on a prototype version of the Weather Research and Forecasting (WRF) model and is used to study influences of deep convection on chemistry in the TOGA COARE/CEPEX region. Lateral boundary conditions for trace gases are prescribed from global chemistry-transport simulations, and the vertical advection of trace gases by large scale dynamics, which is not reproduced in a limited area cloud system resolving model, is taken into account. The influences of in situ lightning and other processes on NOx, O3, and HOx(=HO2+OH), in the vicinity of the deep convective systems are investigated in a 7-day 3-D 248×248 km2 horizontal domain simulation and several 2-D sensitivity runs with a 500 km horizontal domain. The fraction of NOx chemically lost within the domain varies between 20 and 24% in the 2-D runs, but is negligible in the 3-D run, in agreement with a lower average NOx concentration in the 3-D run despite a greater number of flashes. In all runs, in situ lightning is found to have only minor impacts on the local O3 budget. Mid-tropospheric entrainment is more important on average for the upward transport of O3 in the 3-D run than in the 2-D runs, but at the same time undiluted O3-poor air from the marine boundary layer reaches the upper troposphere more frequently in the 3-D run than in the 2-D runs, indicating the presence of undiluted convective cores. Near zero O3 volume mixing ratios due to the reaction with lightning-produced NO are only simulated in a 2-D sensitivity run with an extremely high number of NO molecules per flash, which is outside the range of current estimates. Stratosphere to troposphere transport of O3 is simulated to occur episodically in thin filaments, but on average net upward transport of O3 from below ~16 km is simulated in association with mean large scale ascent in the region. Ozone profiles in the TOGA COARE/CEPEX region are suggested to be strongly influenced by the intra-seasonal (Madden-Julian) oscillation.


2006 ◽  
Vol 6 (2) ◽  
pp. 283-301 ◽  
Author(s):  
A. Engel ◽  
H. Bönisch ◽  
D. Brunner ◽  
H. Fischer ◽  
H. Franke ◽  
...  

Abstract. During SPURT (Spurenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region) we performed measurements of a wide range of trace gases with different lifetimes and sink/source characteristics in the northern hemispheric upper troposphere (UT) and lowermost stratosphere (LMS). A large number of in-situ instruments were deployed on board a Learjet 35A, flying at altitudes up to 13.7 km, at times reaching to nearly 380 K potential temperature. Eight measurement campaigns (consisting of a total of 36 flights), distributed over all seasons and typically covering latitudes between 35° N and 75° N in the European longitude sector (10° W–20° E), were performed. Here we present an overview of the project, describing the instrumentation, the encountered meteorological situations during the campaigns and the data set available from SPURT. Measurements were obtained for N2O, CH4, CO, CO2, CFC12, H2, SF6, NO, NOy, O3 and H2O. We illustrate the strength of this new data set by showing mean distributions of the mixing ratios of selected trace gases, using a potential temperature-equivalent latitude coordinate system. The observations reveal that the LMS is most stratospheric in character during spring, with the highest mixing ratios of O3 and NOy and the lowest mixing ratios of N2O and SF6. The lowest mixing ratios of NOy and O3 are observed during autumn, together with the highest mixing ratios of N2O and SF6 indicating a strong tropospheric influence. For H2O, however, the maximum concentrations in the LMS are found during summer, suggesting unique (temperature- and convection-controlled) conditions for this molecule during transport across the tropopause. The SPURT data set is presently the most accurate and complete data set for many trace species in the LMS, and its main value is the simultaneous measurement of a suite of trace gases having different lifetimes and physical-chemical histories. It is thus very well suited for studies of atmospheric transport, for model validation, and for investigations of seasonal changes in the UT/LMS, as demonstrated in accompanying and elsewhere published studies.


2005 ◽  
Vol 5 (4) ◽  
pp. 5081-5126
Author(s):  
A. Engel ◽  
H. Bönisch ◽  
D. Brunner ◽  
H. Fischer ◽  
H. Franke ◽  
...  

Abstract. During SPURT (Spurenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region) we performed measurements of a wide range of trace gases with different lifetimes and sink/source characteristics in the northern hemispheric upper troposphere (UT) and lowermost stratosphere (LMS). A large number of in-situ instruments were deployed on board a Learjet 35A, flying at altitudes up to 13.7 km, at times reaching to nearly 380 K potential temperature. Eight measurement campaigns (consisting of a total of 36 flights), distributed over all seasons and typically covering latitudes between 35° N and 75° N in the European longitude sector (10° W–20° E), were performed. Here we present an overview of the project, describing the instrumentation, the encountered meteorological situations during the campaigns and the data set available from SPURT. Measurements were obtained for N2O, CH4, CO, CO2, CFC12, H2, SF6, NO, NOy, O3 and H2O. We illustrate the strength of this new data set by showing mean distributions of the mixing ratios of selected trace gases, using a potential temperature – equivalent latitude coordinate system. The observations reveal that the LMS is most stratospheric in character during spring, with the highest mixing ratios of O3 and NOy and the lowest mixing ratios of N2O and SF6. The lowest mixing ratios of NOy and O3 are observed during autumn, together with the highest mixing ratios of N2O and SF6 indicating a strong tropospheric influence. For H2O, however, the maximum concentrations in the LMS are found during summer, suggesting unique (temperature- and convection-controlled) conditions for this molecule during transport across the tropopause. The SPURT data set is presently the most accurate and complete data set for many trace species in the LMS, and its main value is the simultaneous measurement of a suite of trace gases having different lifetimes and physical-chemical histories. It is thus very well suited for studies of atmospheric transport, for model validation, and for investigations of seasonal changes in the UT/LMS, as demonstrated in accompanying and elsewhere published studies.


2020 ◽  
Author(s):  
Philipp Reutter ◽  
Patrick Neis ◽  
Susanne Rohs ◽  
Bastien Sauvage ◽  
Peter Spichtinger ◽  
...  

&lt;p&gt;Cirrus clouds and their potential formation regions, so-called ice-supersaturated regions (ISSRs) occur frequently in the tropopause region.&amp;#160;It is assumed that ISSRs and cirrus clouds&amp;#160;can change the tropopause structure by diabatic processes, driven by latent heating due to phase transitions and interaction with radiation.&amp;#160;These effects may also alter the distribution of potential vorticity (PV) in the upper troposphere, thus leading to changes in large scale dynamics and stratosphere-to-troposphere exchange.&amp;#160;&amp;#160;&lt;/p&gt;&lt;p&gt;The measurement of water vapour at the tropopause level is not trivial. Beside radiosonde data the most important in-situ dataset is provided by in-service passenger airplanes.&amp;#160;The European Research Infrastructure &amp;#8217;In-service Aircraft for a Global Observing System&amp;#8217; (IAGOS) (Petzold et al., 2015) provides long-term in-situ measurements on board commercial passenger aircraft. Along its flight track every aircraft is monitoring the chemical composition of the surrounding air and atmospheric state parameters by compact instruments.&amp;#160;Especially in the upper troposphere/lowermost stratosphere (UTLS) these&amp;#160;measurements&amp;#160;are&amp;#160;very valuable as most flight tracks are situated in heights between&amp;#160;9&amp;#160;to&amp;#160;13 km, depending on the actual weather conditions,&amp;#160;seasons and geographic region.&amp;#160;&lt;/p&gt;&lt;p&gt;However, for many research questions a three-dimensional picture&amp;#160;including a&amp;#160;sufficient&amp;#160;temporal resolution of the water vapour fields in the UTLS region&amp;#160;is&amp;#160;required.&amp;#160;Hence, in our study we use the&amp;#160;in-situ data from IAGOS&amp;#160;to quantify the quality of the&amp;#160;established and often used ERA-Interim data set. The underlying IFS-model of this reanalysis data&amp;#160;allows explicitly&amp;#160;ice-supersaturation&amp;#160;in cloud free conditions&amp;#160;and is therefore&amp;#160;suitable for comparison.&amp;#160;For instance,&amp;#160;we&amp;#160;compare&amp;#160;properties&amp;#160;such as&amp;#160;the seasonal cycle of the vertical distribution&amp;#160;of water vapour mixing ratio, relative humidity&amp;#160;and the fraction of ice-supersaturated regions.&amp;#160;&lt;/p&gt;


Author(s):  
Arndt Wiessner ◽  
Jochen A. Müller ◽  
Peter Kuschk ◽  
Uwe Kappelmeyer ◽  
Matthias Kästner ◽  
...  

The large scale of the contamination by the former carbo-chemical industry in Germany requires new and often interdisciplinary approaches for performing an economically sustainable remediation. For example, a highly toxic and dark-colored phenolic wastewater from a lignite pyrolysis factory was filled into a former open-cast pit, forming a large wastewater disposal pond. This caused an extensive environmental pollution, calling for an ecologically and economically acceptable strategy for remediation. Laboratory-scale investigations and pilot-scale tests were carried out. The result was the development of a strategy for an implementation of full-scale enhanced in situ natural attenuation on the basis of separate habitats in a meromictic pond. Long-term monitoring of the chemical and biological dynamics of the pond demonstrates the metamorphosis of a former highly polluted industrial waste deposition into a nature-integrated ecosystem with reduced danger for the environment, and confirmed the strategy for the chosen remediation management.


2017 ◽  
Author(s):  
Florian Berkes ◽  
Patrick Neis ◽  
Martin G. Schultz ◽  
Ulrich Bundke ◽  
Susanne Rohs ◽  
...  

Abstract. Despite several studies on temperature trends in the tropopause region, a comprehensive understanding of the evolution of temperatures in this climate-sensitive region of the atmosphere remains elusive. Here we present a unique global-scale, long-term data set of high-resolution in-situ temperature data measured aboard passenger aircraft within the European Research Infrastructure IAGOS (In-service Aircraft for a Global Observing System, www.iagos.org). This data set is used to investigate temperature trends within the global upper troposphere and lowermost stratosphere (UTLS) for the period 1995 to 2012 in different geographical regions and vertical layers of the UTLS. The largest amount of observations is available over the North Atlantic. Here, a neutral temperature trend is found within the lowermost stratosphere. This contradicts the temperature trend in the European Centre for Medium Range Weather Forecast (ECMWF) ERA-Interim reanalysis, where a significant (95 % confidence) temperature increase of +0.56 K/decade is obtained. Differences between trends derived from observations and reanalysis data can be traced back to changes in the temperature bias between observation and model data over the studied period. This study demonstrates the value of the IAGOS temperature observations as anchor point for the evaluation of reanalyses and its suitability for independent trend analyses.


2018 ◽  
Author(s):  
Franz Slemr ◽  
Andreas Weigelt ◽  
Ralf Ebinghaus ◽  
Johannes Bieser ◽  
Carl A. M. Brenninkmeijer ◽  
...  

Abstract. Mercury was measured onboard the IAGOS-CARIBIC passenger aircraft since May 2005 until February 2016 during nearly monthly sequences of mostly four intercontinental flights from Germany to destinations in North and South America, Africa, and South and East Asia. Most of these mercury data were obtained using an internal default signal integration procedure of the Tekran instrument but since April 2014 more precise and accurate data were obtained using post-flight manual integration of the instrument raw signal. In this paper we use the latter data. Elevated upper tropospheric total mercury (TM) concentrations due to large scale biomass burning were observed in the upper troposphere (UT) at the equator and southern latitudes during the flights to Latin America and South Africa in boreal autumn (SON) and boreal winter (DJF). TM concentrations in the lowermost stratosphere (LMS) decrease with altitude above the thermal tropopause but the gradient is less steep than reported before. Seasonal variation of the vertical TM distribution in the UT and LMS is similar to that of other trace gases with surface sources and stratospheric sinks. Using speciation experiments, we show that nearly identical TM and gaseous elementary mercury (GEM) concentrations exist at and below the tropopause. Above the thermal tropopause GEM concentrations are almost always smaller than those of TM and the TM – GEM (i.e. Hg2+) difference increases up to ~ 40 % of TM at ~ 2 km and more above the thermal tropopause. Correlations with N2O as a reference tracer suggest stratospheric lifetimes of 72 ± 37 and 74 ± 27 yr for TM and GEM, respectively, comparable to the stratospheric lifetime of COS. This coincidence, combined with pieces of evidence from us and other researchers, corroborates the hypothesis that Hg2+ formed by oxidation in the stratosphere attaches to sulfate particles formed mainly by oxidation of COS and is removed with them from the stratosphere by air mass exchange, gravitational sedimentation, and cloud scavenging processes.


2021 ◽  
pp. 1-49
Author(s):  
Claude Frankignoul ◽  
Elodie Kestenare ◽  
Gilles Reverdin

AbstractMonthly sea surface salinity (SSS) fields are constructed from observations, using objective mapping on a 1°x1° grid in the Atlantic between 30°S and 50°N in the 1970-2016 period in an update of the data set of Reverdin et al. (2007). Data coverage is heterogeneous, with increased density in 2002 when Argo floats become available, high density along Voluntary Observing Ship lines, and low density south of 10°S. Using lag correlation, the seasonal reemergence of SSS anomalies is investigated between 20°N and 50°N in 5°x5° boxes during the 1993-2016 period, both locally and remotely following the displacements of the deep mixed-layer waters estimated from virtual float trajectories derived from the daily AVISO surface geostrophic currents. Although SSS data are noisy, local SSS reemergence is detected in about half of the boxes, notably in the northeast and southeast, while little reemergence is seen in the central and part of the eastern subtropical gyre. In the same period, sea surface temperature (SST) reemergence is found only slightly more frequently, reflecting the short data duration. However, taking geostrophic advection into account degrades the detection of remote SSS and even SST reemergence. When anomalies are averaged over broader areas, robust evidence of a second and third SSS reemergence peak is found in the northeastern and southeastern parts of the domain, indicating long cold-season persistence of large-scale SSS anomalies, while only a first SST reemergence is seen. An oceanic reanalysis is used to confirm that the correlation analysis indeed reflects the reemergence of subsurface salinity anomalies.


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