scholarly journals Nitrification of the lowermost stratosphere during the exceptionally cold Arctic winter 2015/16

Author(s):  
Marleen Braun ◽  
Jens-Uwe Grooß ◽  
Wolfgang Woiwode ◽  
Sören Johansson ◽  
Michael Höpfner ◽  
...  

Abstract. The Arctic winter 2015/16 was characterized by exceptionally cold stratospheric temperatures, favouring the formation of polar stratospheric clouds (PSCs) from mid-December until the end of February down to low stratospheric altitudes. Observations by GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) on HALO (High Altitude and LOng range research aircraft) during the PGS (POLSTRACC/GW-LCYLCE II/SALSA) campaign from December 2015 to March 2016 allow an investigation of the influence of denitrification on the lowermost stratosphere (LMS) with a high spatial resolution. For the first time vertical cross-sections of nitric acid (HNO3) along the flight track and tracer-tracer correlations derived from the GLORIA observations document detailed pictures of wide-spread nitrification of the Arctic LMS during the course of an entire winter. GLORIA observations show large-scale structures and local fine structures with strongly enhanced absolute HNO3 volume mixing ratios reaching up to 11 ppbv at altitudes of 11 km in January and nitrified filaments persisting until the middle of March. Narrow streaks of enhanced HNO3, observed in mid-January, are interpreted as regions recently nitrified by sublimating HNO3-containing particles. Overall, a nitrification of the LMS between 5.0 ppbv and 7.0 ppbv at potential temperature levels between 350 and 380 K is estimated. This extent of nitrification has never been observed before in the Arctic lowermost stratosphere. The GLORIA observations are compared with CLaMS (Chemical Lagrangian Model of the Stratosphere) simulations. The fundamental structures observed by GLORIA are well reproduced, but differences in the fine structures are diagnosed. Further, CLaMS predominantly underestimates the spatial extent of maximum HNO3 mixing ratios derived from the GLORIA observations as well as the enhancement at lower altitudes. Sensitivity simulations with CLaMS including (i) enhanced sedimentation rates in case of ice supersaturation (to resemble ice nucleation on NAT), (ii) a global temperature offset, (iii) modified growth rates (to resemble aspherical particles with larger surfaces) and (iv) temperature fluctuations (to resemble the impact of small-scale mountain waves) mostly improve the agreement with the GLORIA observations. The sensitivity simulations suggest that details of particle microphysics play a significant role for simulated LMS nitrification in January, while air subsidence, transport and mixing become increasingly important towards the end of the winter.

2019 ◽  
Vol 19 (21) ◽  
pp. 13681-13699 ◽  
Author(s):  
Marleen Braun ◽  
Jens-Uwe Grooß ◽  
Wolfgang Woiwode ◽  
Sören Johansson ◽  
Michael Höpfner ◽  
...  

Abstract. The Arctic winter 2015–2016 was characterized by exceptionally low stratospheric temperatures, favouring the formation of polar stratospheric clouds (PSCs) from mid-December until the end of February down to low stratospheric altitudes. Observations by GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) on HALO (High Altitude and LOng range research aircraft) during the PGS (POLSTRACC–GW-LCYCLE II–SALSA) campaign from December 2015 to March 2016 allow the investigation of the influence of denitrification on the lowermost stratosphere (LMS) with a high spatial resolution. Two-dimensional vertical cross sections of nitric acid (HNO3) along the flight track and tracer–tracer correlations derived from the GLORIA observations document detailed pictures of wide-spread nitrification of the Arctic LMS during the course of an entire winter. GLORIA observations show large-scale structures and local fine structures with enhanced absolute HNO3 volume mixing ratios reaching up to 11 ppbv at altitudes of 13 km in January and nitrified filaments persisting until the middle of March. Narrow coherent structures tilted with altitude of enhanced HNO3, observed in mid-January, are interpreted as regions recently nitrified by sublimating HNO3-containing particles. Overall, extensive nitrification of the LMS between 5.0 and 7.0 ppbv at potential temperature levels between 350 and 380 K is estimated. The GLORIA observations are compared with CLaMS (Chemical Lagrangian Model of the Stratosphere) simulations. The fundamental structures observed by GLORIA are well reproduced, but differences in the fine structures are diagnosed. Further, CLaMS predominantly underestimates the spatial extent of HNO3 maxima derived from the GLORIA observations as well as the overall nitrification of the LMS. Sensitivity simulations with CLaMS including (i) enhanced sedimentation rates in case of ice supersaturation (to resemble ice nucleation on nitric acid trihydrate (NAT)), (ii) a global temperature offset, (iii) modified growth rates (to resemble aspherical particles with larger surfaces) and (iv) temperature fluctuations (to resemble the impact of small-scale mountain waves) slightly improved the agreement with the GLORIA observations of individual flights. However, no parameter could be isolated which resulted in a general improvement for all flights. Still, the sensitivity simulations suggest that details of particle microphysics play a significant role for simulated LMS nitrification in January, while air subsidence, transport and mixing become increasingly important for the simulated HNO3 distributions towards the end of the winter.


2013 ◽  
Vol 13 (21) ◽  
pp. 10859-10871 ◽  
Author(s):  
C. Kalicinsky ◽  
J.-U. Grooß ◽  
G. Günther ◽  
J. Ungermann ◽  
J. Blank ◽  
...  

Abstract. The CRISTA-NF (Cryogenic Infrared Spectrometers and Telescope for the Atmosphere – New Frontiers) instrument is an airborne infrared limb sounder operated aboard the Russian research aircraft M55-Geophysica. The instrument successfully participated in a large Arctic aircraft campaign within the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions) project in Kiruna (Sweden) from January to March 2010. This paper concentrates on the measurements taken during one flight of the campaign, which took place on 2 March in the vicinity of the polar vortex. We present two-dimensional cross-sections of derived volume mixing ratios for the trace gases CFC-11, O3, and ClONO2 with an unprecedented vertical resolution of about 500 to 600 m for a large part of the observed altitude range (≈ 6–19 km) and a dense horizontal sampling along flight direction of ≈ 15 km. The trace gas distributions show several structures, for example a part of the polar vortex and a vortex filament, which can be identified by means of O3–CFC-11 tracer–tracer correlations. The observations made during this flight are interpreted using the chemistry and transport model CLaMS (Chemical Lagrangian Model of the Stratosphere). Comparisons of the observations with the model results are used to assess the performance of the model with respect to advection, mixing, and the chemistry in the polar vortex. These comparisons confirm the capability of CLaMS to reproduce even very small-scale structures in the atmosphere, which partly have a vertical extent of only 1 km. Based on the good agreement between simulation and observation, we use artificial (passive) tracers, which represent different air mass origins (e.g. vortex, tropics), to further analyse the CRISTA-NF observations in terms of the composition of air mass origins. These passive tracers clearly illustrate the observation of filamentary structures that include tropical air masses. A characteristic of the Arctic winter 2009/10 was a sudden stratospheric warming in December that led to a split of the polar vortex. The vortex re-established at the end of December. Our passive tracer simulations suggest that large parts of the re-established vortex consisted to about 45% of high- and mid-latitude air.


2013 ◽  
Vol 13 (4) ◽  
pp. 10463-10498 ◽  
Author(s):  
C. Kalicinsky ◽  
J.-U. Grooß ◽  
G. Günther ◽  
J. Ungermann ◽  
J. Blank ◽  
...  

Abstract. The CRISTA-NF (Cryogenic Infrared Spectrometers and Telescope for the Atmosphere – New Frontiers) instrument is an airborne infrared limb sounder operated aboard the Russian research aircraft M55-Geophysica. The instrument successfully participated in a large Arctic aircraft campaign within the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions) project from January to March 2010 in Kiruna, Sweden. This paper concentrates on the measurements during one flight of the campaign, which took place on 2 March in the vicinity of the polar vortex. We present two-dimensional cross-sections of volume mixing ratios for the trace gases CFC-11, O3, and ClONO2 with an unprecedented vertical resolution of about 500 to 600 m for a large part of the observed altitude range and a dense horizontal sampling along flight direction of ≈ 15 km. The trace gas distributions show several structures like the polar vortex and filaments composed of air masses of different origin. The situation during the analysed flight is simulated by the chemistry and transport model CLaMS (Chemical Lagrangian Model of the Stratosphere) and compared with the measurements to assess the performance of the model with respect to advection, mixing, and the chemistry in the polar vortex. These comparisons confirm the capability of CLaMS to reproduce even very small-scale structures in the atmosphere. Based on the good agreement between simulation and observation, we use a model concept utilising artificial tracers to further analyse the CRISTA-NF observations in terms of air mass origin. A characteristic of the Arctic winter 2009/10 was a sudden stratospheric warming in early December that led to a split of the polar vortex. The vortex re-established at the end of December. Our passive tracer simulations suggest that large parts of the re-established vortex consisted to about 45% of high- and mid-latitude air.


2003 ◽  
Vol 3 (2) ◽  
pp. 395-402 ◽  
Author(s):  
J.-U. Grooß ◽  
R. Müller

Abstract. Current stratospheric chemical model simulations underestimate substantially the large ozone loss rates that are derived for the Arctic from ozone sondes for January of some years. Until now, no explanation for this discrepancy has been found. Here, we examine the influence of intrusions of mid-latitude air into the polar vortex on these ozone loss estimates. This study focuses on the winter 1991/92, because during this winter the discrepancy between simulated and experimentally derived ozone loss rates is reported to be the largest. Also during the considered period the vortex was disturbed by a strong warming event with large-scale intrusions of mid-latitude air into the polar vortex, which is quite unusual for this time of the year. The study is based on simulations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). Two methods for determination the ozone loss are investigated, the so-called vortex average approach and the Match method. The simulations for January 1992 show that the intrusions induce a reduction of vortex average ozone mixing ratio corresponding to a systematic offset of the ozone loss rate of about 12 ppb per day. This should be corrected for in the vortex average method. The simulations further suggest, that these intrusions do not cause a significant bias for the Match method due to effective quality control measures in the Match technique.


2004 ◽  
Vol 4 (5) ◽  
pp. 6185-6212
Author(s):  
F. Khosrawi ◽  
J.-U. Grooß ◽  
R. Müller ◽  
P. Konopka ◽  
W. Kouker ◽  
...  

Abstract. During the CRISTA-1 mission three pronounced fingerlike structures reaching from the lower latitudes to the mid-latitudes, so-called streamers, were observed in the measurements of several trace gases in early November 1994. A simulation of these streamers in previous studies employing the KASIMA (Karlsruhe Simulation Model of the Middle Atmosphere) and ROSE (Research on Ozone in the Stratosphere and its Evolution) model, both being Eulerian models, show that their formation is due to adiabatic transport processes. Here, the impact of mixing on the development of these streamers is investigated. These streamers were simulated with the CLaMS model (Chemical Lagrangian Model of the Stratosphere), a Lagrangian model, using N2O as long-lived tracer. Using several different initialisations the results were compared to the KASIMA simulations and CRISTA (Cryogenic Infrared Spectrometer and Telescope for the Atmosphere) observations. Further, since the KASIMA model was employed to derive a 9-year climatology, the quality of the reproduction of streamers from such a study was tested by the comparison of the KASIMA results with CLaMS and CRISTA. The streamers are reproduced well for the Northern Hemisphere in the simulations of CLaMS and KASIMA for the 6 November 1994. However, in the CLaMS simulation a stronger filamentation is found while larger discrepancies between KASIMA and CRISTA were found especially for the Southern Hemisphere. Further, compared to the CRISTA observations the mixing ratios of N2O are in general underestimated in the KASIMA simulations. An improvement of the simulations with KASIMA was obtained for a simulation time according to the length of the CLaMS simulation. To quantify the differences between the simulations with CLaMS and KASIMA, and the CRISTA observations, the probability density function technique (PDF) is used to interpret the tracer distributions. While in the PDF of the KASIMA simulation the small scale structures observed by CRISTA are smoothed out due to the numerical diffusion in the model, the PDFs derived from CRISTA observations can be reproduced by CLaMS by optimizing the mixing parameterisation. Further, this procedure gives information on small-scale variabilities not resolved by the CRISTA observations.


2003 ◽  
Vol 3 (3) ◽  
pp. 839-849 ◽  
Author(s):  
P. Konopka ◽  
J.-U. Grooß ◽  
S. Bausch ◽  
R. Müller ◽  
D. S. McKenna ◽  
...  

Abstract. High-resolution simulations of the chemical composition of the Arctic stratosphere during late spring 1997 and 2000 were performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulations were performed for the entire northern hemisphere on two isentropic levels 450 K (~18 km) and 585 K (~24 km). The spatial distribution and the lifetime of the vortex remnants formed after the vortex breakup in May 1997 display different behavior above and below 20 km. Above 20 km, vortex remnants propagate southward (up to 40°N) and are "frozen in'' in the summer circulation without significant mixing. Below 20 km the southward propagation of the remnants is bounded by the subtropical jet. Their lifetime is shorter by a factor of 2 than that above 20 km, owing to significant stirring below this altitude. The behavior of vortex remnants formed in March 2000 is similar but, due to an earlier vortex breakup, dominated during the first 6 weeks after the vortex breakup by westerly winds, even above 20 km. Vortex remnants formed in May 1997 are characterized by large mixing ratios of HCl indicating negligible, halogen-induced ozone loss. In contrast, mid-latitude ozone loss in late boreal spring 2000 is dominated, until mid-April, by halogen-induced ozone destruction within the vortex remnants, and subsequent transport of the ozone-depleted polar air masses (dilution) into the mid-latitudes. By varying the intensity of mixing in CLaMS, the impact of mixing on the formation of ClONO2 and ozone depletion is investigated. We find that the photochemical decomposition of HNO3 and not mixing with NOx-rich mid-latitude air is the main source of NOx within the vortex remnants in March and April 2000. Ozone depletion in the remnants is driven by ClOx photolytically formed from ClONO2. At the end of May 1997, the halogen-induced ozone deficit at 450 K poleward of 30°N amounts to ~12% with ~10% in the polar vortex and ~2% in well-isolated vortex remnants after the vortex breakup.


2005 ◽  
Vol 5 (1) ◽  
pp. 85-95 ◽  
Author(s):  
F. Khosrawi ◽  
J.-U. Grooß ◽  
R. Müller ◽  
P. Konopka ◽  
W. Kouker ◽  
...  

Abstract. During the CRISTA-1 mission three pronounced fingerlike structures reaching from the lower latitudes to the mid-latitudes, so-called streamers, were observed in the measurements of several trace gases in early November 1994. A simulation of these streamers in previous studies employing the KASIMA (Karlsruhe Simulation Model of the Middle Atmosphere) and ROSE (Research on Ozone in the Stratosphere and its Evolution) model, both being Eulerian models, show that their formation is due to adiabatic transport processes. Here, the impact of mixing on the development of these streamers is investigated. These streamers were simulated with the CLaMS model (Chemical Lagrangian Model of the Stratosphere), a Lagrangian model, using N2O as long-lived tracer. Using several different initialisations the results were compared to the KASIMA simulations and CRISTA (Cryogenic Infrared Spectrometer and Telescope for the Atmosphere) observations. Further, since the KASIMA model was employed to derive a 9-year climatology, the quality of the reproduction of streamers from such a study was tested by the comparison of the KASIMA results with CLaMS and CRISTA. The streamers are reproduced well for the Northern Hemisphere in the simulations of CLaMS and KASIMA for the 6 November 1994. However, in the CLaMS simulation a stronger filamentation is found while larger discrepancies between KASIMA and CRISTA were found especially for the Southern Hemisphere. Further, compared to the CRISTA observations the mixing ratios of N2O are in general underestimated in the KASIMA simulations. An improvement of the simulations with KASIMA was obtained for a simulation time according to the length of the CLaMS simulation. To quantify the differences between the simulations with CLaMS and KASIMA, and the CRISTA observations, the probability density function technique (PDF) is used to interpret the tracer distributions. While in the PDF of the KASIMA simulation the small scale structures observed by CRISTA are smoothed out due to the numerical diffusion in the model, the PDFs derived from CRISTA observations can be reproduced by CLaMS by optimising the mixing parameterisation. Further, this procedure gives information on small-scale variabilities not resolved by the CRISTA observations.


2003 ◽  
Vol 3 (1) ◽  
pp. 1051-1080 ◽  
Author(s):  
P. Konopka ◽  
J.-U. Grooß ◽  
S. Bausch ◽  
R. Müller ◽  
D. S. McKenna ◽  
...  

Abstract. High resolution simulations of the chemical composition of the Arctic stratosphere during late spring 1997 and 2000 have been conducted with the Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulations were performed for the entire northern hemisphere on two isentropic levels 450 K (~18 km) and 585 K (~24 km). The spatial distribution and the lifetime of the vortex remnants formed after the vortex breakup in May 1997 show a completely different behavior above and below 20 km. Above 20 km, vortex remnants effectively propagate southward (up to 40° N) and are "frozen'' in the summer circulation without significant mixing. Below 20 km the southward propagation of the remnants is bounded by the subtropical jet near 55° N. Their lifetime is shorter by a factor of 2 than above 20 km, owing to significant stirring below this altitude. The behavior of vortex remnants formed in March 2000 is similar but, due to an earlier vortex breakup, dominated until mid of May by westerly winds, even above 20 km. Vortex remnants formed in May 1997 are characterized by large mixing ratios of HCl indicating a negligible contribution of the halogen-induced ozone loss. In contrast, mid-latitude ozone loss in late boreal spring 2000 is dominated by an irreversible transport of the ozone-depleted polar air masses (dilution) and, until mid of April, by halogen-induced ozone destruction within the vortex remnants. By varying the effective diffusivity of CLaMS, the impact of mixing on the formation of ClONO2 and ozone depletion is considered. In particular, the photochemical decomposition of HNO3 and not mixing with NOx-rich mid-latitude air is the main source of NOx within the vortex remnants in March and April 2000. Ozone depletion in the remnants is driven by ClOx photolytically formed from ClONO2 and can be properly resolved for CLaMS spatial resolution better then 100\\,km. At 450 K, ozone loss in the vortex remnants contributes by ~2% to the ozone deficit poleward of 30° N.


2016 ◽  
Author(s):  
Mike J. Newland ◽  
Patricia Martinerie ◽  
Emmanuel Witrant ◽  
Detlev Helmig ◽  
David R. Worton ◽  
...  

Abstract. The NOX (NO and NO2) and HOX (OH and HO2) budgets of the atmosphere exert a major influence on atmospheric composition, controlling removal of primary pollutants and formation of a wide range of secondary products, including ozone, that can influence human health and climate. However, there remain large uncertainties in the changes to these budgets over recent decades. Due to their short atmospheric lifetimes, NOX and HOX are highly variable in space and time, and so the measurements of these species are of very limited value for examining long term, large scale changes to their budgets. Here, we take an alternative approach by examining long-term atmospheric trends of alkyl nitrates, the formation of which is dependent on the atmospheric NO / HO2 ratio. We derive long term trends in the alkyl nitrates from measurements in firn air from the NEEM site, Greenland. Their mixing ratios increased by a factor of 4–5 between the 1970s and 1990s. This was followed by a steep decline to the sampling date of 2008. Moreover, we examine how the trends in the alkyl nitrates compare to similarly derived trends in their parent alkanes (i.e. the alkanes which, when oxidised in the presence of NOX, lead to the formation of the alkyl nitrates). The ratios of the alkyl nitrates to their parent alkanes increase from around 1970 to the late 1990's consistent with large changes to the [NO] / [HO2] ratio in the northern hemisphere atmosphere during this period. These could represent historic changes to NOX sources and sinks. Alternatively, they could represent changes to concentrations of the hydroxyl radical, OH, or to the transport time of the air masses from source regions to the Arctic.


2017 ◽  
Vol 10 (3) ◽  
pp. 1383-1402 ◽  
Author(s):  
Paolo Davini ◽  
Jost von Hardenberg ◽  
Susanna Corti ◽  
Hannah M. Christensen ◽  
Stephan Juricke ◽  
...  

Abstract. The Climate SPHINX (Stochastic Physics HIgh resolutioN eXperiments) project is a comprehensive set of ensemble simulations aimed at evaluating the sensitivity of present and future climate to model resolution and stochastic parameterisation. The EC-Earth Earth system model is used to explore the impact of stochastic physics in a large ensemble of 30-year climate integrations at five different atmospheric horizontal resolutions (from 125 up to 16 km). The project includes more than 120 simulations in both a historical scenario (1979–2008) and a climate change projection (2039–2068), together with coupled transient runs (1850–2100). A total of 20.4 million core hours have been used, made available from a single year grant from PRACE (the Partnership for Advanced Computing in Europe), and close to 1.5 PB of output data have been produced on SuperMUC IBM Petascale System at the Leibniz Supercomputing Centre (LRZ) in Garching, Germany. About 140 TB of post-processed data are stored on the CINECA supercomputing centre archives and are freely accessible to the community thanks to an EUDAT data pilot project. This paper presents the technical and scientific set-up of the experiments, including the details on the forcing used for the simulations performed, defining the SPHINX v1.0 protocol. In addition, an overview of preliminary results is given. An improvement in the simulation of Euro-Atlantic atmospheric blocking following resolution increase is observed. It is also shown that including stochastic parameterisation in the low-resolution runs helps to improve some aspects of the tropical climate – specifically the Madden–Julian Oscillation and the tropical rainfall variability. These findings show the importance of representing the impact of small-scale processes on the large-scale climate variability either explicitly (with high-resolution simulations) or stochastically (in low-resolution simulations).


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