Testing our understanding of Arctic denitrification using MIPAS-E satellite measurements in winter 2002/2003

Davies, S.; Mann, G. W.; Carslaw, K. S.; Chipperfield, Martyn; Remedios, J. J.; Allen, Grant; Waterfall, A. M.; Spang, R.; Toon, G. C.

doi:10.5194/acp-6-3149-2006

Cited by 13 publications

(16 citation statements)

References 43 publications

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“…Although a 3D Lagrangian NAT particle sedimentation model has been employed with SLIMCAT to investigate Arctic denitrification [ Mann et al , 2002, 2003, 2005; Davies et al , 2005, 2006], none of those studies used coupled chemistry. The “standard” version of SLIMCAT used here and in most other studies of polar processing and ozone loss does not include a microphysical model.…”

Section: Measurement and Model Descriptionsmentioning

confidence: 99%

A study of stratospheric chlorine partitioning based on new satellite measurements and modeling

Santee¹,

MacKenzie²,

Manney³

et al. 2008

J. Geophys. Res.

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132

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[1] Two recent satellite instruments, the Microwave Limb Sounder (MLS) on Aura and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on SCISAT-1, provide an unparalleled opportunity to investigate stratospheric chlorine partitioning. We use measurements of ClO, HCl, ClONO 2 , and other species from MLS and ACE-FTS to study the evolution of reactive and reservoir chlorine throughout the lower stratosphere during two Arctic and two Antarctic winters characterizing both relatively cold and relatively warm and disturbed conditions in each hemisphere. At middle latitudes, and at high latitudes at the beginning of winter, HCl greatly exceeds ClONO 2 , representing $0.7-0.8 of estimated total inorganic chlorine. Nearly complete chlorine activation is seen inside the winter polar vortices. In the Arctic, chlorine recovery follows different paths in the two winters: In 2004/2005, deactivation initially takes place through reformation of ClONO 2 , then both reservoirs are produced concurrently but ClONO 2 continues to significantly exceed HCl, and finally slow repartitioning between ClONO 2 and HCl occurs; in 2005/2006, HCl and ClONO 2 rise at comparable rates in some regions. In the Antarctic, chlorine deactivation proceeds in a similar manner in both winters, with a rapid rise in HCl accompanying the decrease in ClO. The measurements are compared to customized runs of the SLIMCAT three-dimensional chemical transport model. Measured and modeled values typically agree well outside the winter polar regions. In contrast, partly because of the equilibrium scheme used to parameterize polar stratospheric clouds, the model overestimates the magnitude, spatial extent, and duration of chlorine activation inside the polar vortices.

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Section: Measurement and Model Descriptionsmentioning

confidence: 99%

A study of stratospheric chlorine partitioning based on new satellite measurements and modeling

Santee¹,

MacKenzie²,

Manney³

et al. 2008

J. Geophys. Res.

Self Cite

103

132

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“…Denitrification is observed regularly in the lower stratosphere in Antarctica and in cold winters in the Arctic (e.g. Davies et al, 2006;Santee et al, 2008;Grooß et al, 2014).…”

Section: A2 Denitrificationmentioning

confidence: 99%

The maintenance of elevated active chlorine levels in the Antarctic lower stratosphere through HCl null cycles

Müller¹,

Grooß²,

Zafar

et al. 2018

Atmos. Chem. Phys.

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Abstract. The Antarctic ozone hole arises from ozone destruction driven by elevated levels of ozone destroying ("active") chlorine in Antarctic spring. These elevated levels of active chlorine have to be formed first and then maintained throughout the period of ozone destruction. It is a matter of debate how this maintenance of active chlorine is brought about in Antarctic spring, when the rate of formation of HCl (considered to be the main chlorine deactivation mechanism in Antarctica) is extremely high. Here we show that in the heart of the ozone hole (16-18 km or 85-55 hPa, in the core of the vortex), high levels of active chlorine are maintained by effective chemical cycles (referred to as HCl null cycles hereafter). In these cycles, the formation of HCl is balanced by immediate reactivation, i.e. by immediate reformation of active chlorine. Under these conditions, polar stratospheric clouds sequester HNO 3 and thereby cause NO 2 concentrations to be low. These HCl null cycles allow active chlorine levels to be maintained in the Antarctic lower stratosphere and thus rapid ozone destruction to occur. For the observed almost complete activation of stratospheric chlorine in the lower stratosphere, the heterogeneous reaction HCl + HOCl is essential; the production of HOCl occurs via HO 2 + ClO, with the HO 2 resulting from CH 2 O photolysis. These results are important for assessing the impact of changes of the future stratospheric composition on the recovery of the ozone hole. Our simulations indicate that, in the lower stratosphere, future increased methane concentrations will not lead to enhanced chlorine deactivation (through the reaction CH 4 + Cl −→ HCl+CH 3 ) and that extreme ozone destruction to levels below ≈ 0.1 ppm will occur until mid-century.

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“…Manney et al (2003), Goutail et al (2005) and Feng et al (2007a) have shown large year-to-year variations of polar Arctic ozone loss due to different meteorological conditions. There have been extensive studies about denitrification for cold Arctic winters (e.g., Carslaw et al, 2002;Grooß et al, 2002;Kleinböhl, 2004;Jin et al, 2006;Davies et al, 2006;Schoeberl et al, 2006). Some of these studies also included the SLIMCAT model run with the equilibrium denitrification scheme or DLAPSE schemes.…”

Section: Discussionmentioning

confidence: 99%

“…Previous studies (e.g., Davies et al, , 2006Mann et al, , 2005 used the separate microphysical Denitrification by Lagrangian Particle Sedimentation (DLAPSE) model to investigate denitrification effect in Arctic winters, but only Davies et al (2006) combined this with the full SLIMCAT chemistry. These studies advected gas phase HNO 3 in SLIMCAT, interpolated to the Lagrangian particle positions, then ran the DLAPSE model to calculate the growth and sedimentation of several hundred thousand particles (more details can be found in .…”

Section: Model and Experimentsmentioning

confidence: 99%

“…These studies advected gas phase HNO 3 in SLIMCAT, interpolated to the Lagrangian particle positions, then ran the DLAPSE model to calculate the growth and sedimentation of several hundred thousand particles (more details can be found in . In Davies et al (2006), they were running two independent models (DLAPSE and SLIMCAT) and passing information between these two models. For this work, we have fully incorporated the Lagrangian particle denitrification model (DLAPSE) into the SLIMCAT model to extend the options of PSC scheme in the model.…”

Section: Model and Experimentsmentioning

confidence: 99%

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Modelling the effect of denitrification on polar ozone depletion for Arctic winter 2004/2005

et al. 2011

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Abstract. A three-dimensional (3-D) chemical transport model (CTM), SLIMCAT, has been used to quantify the effect of denitrification on ozone loss for the Arctic winter 2004/2005. The simulated HNO 3 is found to be highly sensitive to the polar stratospheric cloud (PSC) scheme used in the model. Here the standard SLIMCAT full chemistry model, which uses a thermodynamic equilibrium PSC scheme, overpredicts the ozone loss for Arctic winter 2004/2005 due to the overestimation of denitrification and stronger chlorine activation than observed. A model run with a coupled detailed microphysical denitrification scheme, DLAPSE (Denitrification by Lagrangian Particle Sedimentation), is less denitrified than the standard model run and better reproduces the observed HNO 3 as measured by Airborne SUbmillimeter Radiometer (ASUR) and Aura Microwave Limb Sounder (MLS) instruments. Overall, denitrification is responsible for a ∼30 % enhancement in O 3 depletion compared with simulations without denitrification for Arctic winter 2004/2005, which is slightly larger than the inferred impact of denitrification on Arctic ozone loss for previous winters from different CTMs simulations. The overestimated denitrification from standard SLIMCAT simulation causes ∼5-10 % more ozone loss at ∼17 km compared with the simulation using the DLAPSE PSC scheme for Arctic winter 2004/2005. The calculated partial column ozone loss from SLIMCAT using the DLAPSE scheme is about 130 DU by mid-March 2005, which compares well with the inferred column ozone loss from ozonesondes and satellite data (127±21 DU).

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Testing our understanding of Arctic denitrification using MIPAS-E satellite measurements in winter 2002/2003

Cited by 13 publications

References 43 publications

A study of stratospheric chlorine partitioning based on new satellite measurements and modeling

A study of stratospheric chlorine partitioning based on new satellite measurements and modeling

The maintenance of elevated active chlorine levels in the Antarctic lower stratosphere through HCl null cycles

Modelling the effect of denitrification on polar ozone depletion for Arctic winter 2004/2005

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