Redistribution of nitric acid in the Arctic lower stratosphere during the winter of 1996-1997

2001 ◽  
Vol 106 (D19) ◽  
pp. 23139-23150 ◽  
Author(s):  
H. Irie ◽  
M. Koike ◽  
Y. Kondo ◽  
G. E. Bodeker ◽  
M. Y. Danilin ◽  
...  
2015 ◽  
Vol 15 (4) ◽  
pp. 4973-5029 ◽  
Author(s):  
G. L. Manney ◽  
Z. D. Lawrence ◽  
M. L. Santee ◽  
N. J. Livesey ◽  
A. Lambert ◽  
...  

Abstract. A sudden stratospheric warming (SSW) in early January 2013 caused the polar vortex to split. After the lower stratospheric vortex split on 8 January, the two offspring vortices – one over Canada and the other over Siberia – remained intact, well-confined, and largely at latitudes that received sunlight until they reunited at the end of January. As the SSW began, temperatures abruptly rose above chlorine activation thresholds throughout the lower stratosphere. The vortex was very disturbed prior to the SSW, and was exposed to much more sunlight than usual in December 2012 and January 2013. Aura Microwave Limb Sounder (MLS) nitric acid (HNO3) data and observations from CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) indicate extensive polar stratospheric cloud (PSC) activity, with evidence of PSCs containing solid nitric acid trihydrate particles during much of December 2012. Consistent with the sunlight exposure and PSC activity, MLS observations show that chlorine monoxide (ClO) became enhanced early in December. Despite the cessation of PSC activity with the onset of the SSW, enhanced vortex ClO persisted until mid-February, indicating lingering chlorine activation. The smaller Canadian offspring vortex had lower temperatures, lower HNO3, lower hydrogen chloride (HCl), and higher ClO in late January than the Siberian vortex. Chlorine deactivation began later in the Canadian than in the Siberian vortex. HNO3 remained depressed within the vortices after temperatures rose above the PSC existence threshold, and passive transport calculations indicate vortex-averaged denitrification of about 4 ppbv; the resulting low HNO3 values persisted until the vortex dissipated in mid-February. Consistent with the strong chlorine activation and exposure to sunlight, MLS measurements show rapid ozone loss commencing in mid-December and continuing through January. Lagrangian transport estimates suggest ~ 0.7–0.8 ppmv (parts per million by volume) vortex-averaged chemical ozone loss by late January near 500 K (~ 21 km), with substantial loss occurring from ~ 450 to 550 K. The surface area of PSCs in December 2012 was larger than that in any other December observed by CALIPSO. As a result of denitrification, HNO3 abundances in 2012/13 were among the lowest in the MLS record for the Arctic. ClO enhancement was much greater in December 2012 through mid-January 2013 than that at the corresponding time in any other Arctic winter observed by MLS. Furthermore, reformation of HCl appeared to play a greater role in chlorine deactivation than in more typical Arctic winters. Ozone loss in December 2012 and January 2013 was larger than any previously observed in those months. This pattern of exceptional early winter polar processing and ozone loss resulted from the unique combination of dynamical conditions associated with the early January 2013 SSW, namely unusually low temperatures in December 2012 and offspring vortices that remained well-confined and largely in sunlit regions for about a month after the vortex split.


Atmosphere ◽  
2021 ◽  
Vol 12 (4) ◽  
pp. 454
Author(s):  
Andrew R. Jakovlev ◽  
Sergei P. Smyshlyaev ◽  
Vener Y. Galin

The influence of sea-surface temperature (SST) on the lower troposphere and lower stratosphere temperature in the tropical, middle, and polar latitudes is studied for 1980–2019 based on the MERRA2, ERA5, and Met Office reanalysis data, and numerical modeling with a chemistry-climate model (CCM) of the lower and middle atmosphere. The variability of SST is analyzed according to Met Office and ERA5 data, while the variability of atmospheric temperature is investigated according to MERRA2 and ERA5 data. Analysis of sea surface temperature trends based on reanalysis data revealed that a significant positive SST trend of about 0.1 degrees per decade is observed over the globe. In the middle latitudes of the Northern Hemisphere, the trend (about 0.2 degrees per decade) is 2 times higher than the global average, and 5 times higher than in the Southern Hemisphere (about 0.04 degrees per decade). At polar latitudes, opposite SST trends are observed in the Arctic (positive) and Antarctic (negative). The impact of the El Niño Southern Oscillation phenomenon on the temperature of the lower and middle atmosphere in the middle and polar latitudes of the Northern and Southern Hemispheres is discussed. To assess the relative influence of SST, CO2, and other greenhouse gases’ variability on the temperature of the lower troposphere and lower stratosphere, numerical calculations with a CCM were performed for several scenarios of accounting for the SST and carbon dioxide variability. The results of numerical experiments with a CCM demonstrated that the influence of SST prevails in the troposphere, while for the stratosphere, an increase in the CO2 content plays the most important role.


2016 ◽  
Author(s):  
Marianne T. Lund ◽  
Terje K. Berntsen ◽  
Bjørn H. Samset

Abstract. Despite recent improvements, significant uncertainties in global modeling of black carbon (BC) aerosols persist, posing important challenges for the design and evaluation of effective climate mitigation strategies targeted at BC emission reductions. Here we investigate the sensitivity of BC concentrations in the chemistry-transport model OsloCTM2 with the microphysical aerosol parameterization M7 (OsloCTM2-M7) to parameters controlling aerosol aging and scavenging. We focus on Arctic surface concentrations and remote region BC vertical profiles, and introduce a novel treatment of condensation of nitric acid on BC. The OsloCTM2-M7 underestimates annual averaged BC surface concentrations, with a mean normalized bias of −0.55. The seasonal cycle and magnitude of Arctic BC surface concentrations is improved compared to previous OsloCTM2 studies, but model-measurement discrepancies during spring remain. High-altitude BC over the Pacific is overestimated compared with measurements from the HIPPO campaigns. We find that a shorter global BC lifetime improves the agreement with HIPPO, in line with other recent studies. Several processes can achieve this, including allowing for convective scavenging of hydrophobic BC and reducing the amount of soluble material required for aging. Simultaneously, the concentrations in the Arctic are reduced, resulting in poorer agreement with measurements in part of the region. A first step towards inclusion of aging by nitrate in OsloCTM2-M7 is made by allowing for condensation of nitric acid on BC. This results in a faster aging and reduced lifetime, and in turn to a better agreement with the HIPPO measurements. On the other hand, model-measurement discrepancies in the Arctic are exacerbated. Work to further improve this parameterization is needed. The impact on global mean radiative forcing (RF) and surface temperature response (TS) in our experiments is estimated. Compared to the baseline, decreases in global mean direct RF on the order of 10–30 % of the total pre-industrial to present BC direct RF is estimated for the experiments that result in the largest changes in BC concentrations. We show that globally tuning parameters related to BC aging and scavenging can improve the representation of BC vertical profiles in the OsloCTM2-M7 compared with observations. Our results also show that such improvements can result from changes in several processes and often depend on assumptions about uncertain parameters such as the BC ice nucleating efficiency and the change in hygroscopicity with aging. It is also important to be aware of potential tradeoffs in model performance between different regions. Other important sources of uncertainty, particularly for Arctic BC, such as model resolution has not been investigated here. Our results underline the importance of more observations and experimental data to improve process understanding and thus further constrain models.


2015 ◽  
Vol 15 (16) ◽  
pp. 22291-22329 ◽  
Author(s):  
C. E. Sioris ◽  
J. Zou ◽  
D. A. Plummer ◽  
C. D. Boone ◽  
C. T. McElroy ◽  
...  

Abstract. Seasonal and monthly zonal medians of water vapour in the upper troposphere and lower stratosphere (UTLS) are calculated for both Atmospheric Chemistry Experiment (ACE) instruments for the northern and southern high-latitude regions (60–90 and 60–90° S). Chosen for the purpose of observing high-latitude processes, the ACE orbit provides sampling of both regions in eight of 12 months of the year, with coverage in all seasons. The ACE water vapour sensors, namely MAESTRO (Measurements of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation) and the Fourier Transform Spectrometer (ACE-FTS) are currently the only satellite instruments that can probe from the lower stratosphere down to the mid-troposphere to study the vertical profile of the response of UTLS water vapour to the annular modes. The Arctic oscillation (AO), also known as the northern annular mode (NAM), explains 64 % (r = −0.80) of the monthly variability in water vapour at northern high-latitudes observed by ACE-MAESTRO between 5 and 7 km using only winter months (January to March 2004–2013). Using a seasonal timestep and all seasons, 45 % of the variability is explained by the AO at 6.5 ± 0.5 km, similar to the 46 % value obtained for southern high latitudes at 7.5 ± 0.5 km explained by the Antarctic oscillation or southern annular mode (SAM). A large negative AO event in March 2013 produced the largest relative water vapour anomaly at 5.5 km (+70 %) over the ACE record. A similarly large event in the 2010 boreal winter, which was the largest negative AO event in the record (1950–2015), led to > 50 % increases in water vapour observed by MAESTRO and ACE-FTS at 7.5 km.


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.


2020 ◽  
Vol 20 (6) ◽  
pp. 3663-3668
Author(s):  
Ellis Remsberg ◽  
V. Lynn Harvey ◽  
Arlin Krueger ◽  
Larry Gordley ◽  
John C. Gille ◽  
...  

Abstract. The Nimbus 7 Limb Infrared Monitor of the Stratosphere (LIMS) instrument operated from 25 October 1978 through 28 May 1979. This note focuses on its Version 6 (V6) data and indications of ozone loss in the lower stratosphere of the Southern Hemisphere subpolar region during the last week of October 1978. We provide profiles and maps that show V6 ozone values of only 2 to 3 ppmv at 46 hPa within the edge of the polar vortex near 60∘ S from late October through mid-November 1978. There are also low values of V6 nitric acid (∼3 to 6 ppbv) and nitrogen dioxide (< 1 ppbv) at the same locations, indicating that conditions were suitable for a chemical loss of Antarctic ozone some weeks earlier. These “first light” LIMS observations provide the earliest space-based view of conditions within the lower stratospheric ozone layer of the southern polar region in springtime.


2014 ◽  
Vol 14 (19) ◽  
pp. 10785-10801 ◽  
Author(s):  
S. Molleker ◽  
S. Borrmann ◽  
H. Schlager ◽  
B. Luo ◽  
W. Frey ◽  
...  

Abstract. In January 2010 and December 2011, synoptic-scale polar stratospheric cloud (PSC) fields were probed during seven flights of the high-altitude research aircraft M-55 Geophysica within the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interaction) and the ESSenCe (ESSenCe: ESA Sounder Campaign) projects. Particle size distributions in a diameter range between 0.46 and 40μm were recorded by four different optical in situ instruments. Three of these particle instruments are based on the detection of forward-scattered light by single particles. The fourth instrument is a grayscale optical array imaging probe. Optical particle diameters of up to 35μm were detected with particle number densities and total particle volumes exceeding previous Arctic measurements. Also, gas-phase and particle-bound NOy was measured, as well as water vapor concentrations. The optical characteristics of the clouds were measured by the remote sensing lidar MAL (Miniature Aerosol Lidar) and by the in situ backscatter sonde MAS (Multiwavelength Aerosol Scatterometer), showing the synoptic scale of the encountered PSCs. The particle mode below 2μm in size diameter has been identified as supercooled ternary solution (STS) droplets. The PSC particles in the size range above 2μm in diameter are considered to consist of nitric acid hydrates, and the particles' high HNO3 content was confirmed by the NOy instrument. Assuming a particle composition of nitric acid trihydrate (NAT), the optically measured size distributions result in particle-phase HNO3 mixing ratios exceeding available stratospheric values. Therefore the measurement uncertainties concerning probable overestimations of measured particle sizes and volumes are discussed in detail. We hypothesize that either a strong asphericity or an alternate particle composition (e.g., water ice coated with NAT) could explain our observations. In particular, with respect to the denitrification by sedimentation of large HNO3-containing particles, generally considered to be NAT, our new measurements raise questions concerning composition, shape and nucleation pathways. Answering these would improve the numerical simulation of PSC microphysical processes like cloud particle formation, growth and denitrification, which is necessary for better predictions of future polar ozone losses, especially under changing global climate conditions. Generally, it seems that the occurrence of large NAT particles – sometimes termed "NAT rocks" – are a regular feature of synoptic-scale PSCs in the Arctic.


2006 ◽  
Vol 6 (8) ◽  
pp. 2355-2366 ◽  
Author(s):  
G. Dufour ◽  
R. Nassar ◽  
C. D. Boone ◽  
R. Skelton ◽  
K. A. Walker ◽  
...  

Abstract. From January to March 2005, the Atmospheric Chemistry Experiment high resolution Fourier transform spectrometer (ACE-FTS) on SCISAT-1 measured many of the changes occurring in the Arctic (50–80° N) lower stratosphere under very cold winter conditions. Here we focus on the partitioning between the inorganic chlorine reservoirs HCl and ClONO2 and their activation into ClO. The simultaneous measurement of these species by the ACE-FTS provides the data needed to follow chlorine activation during the Arctic winter and the recovery of the Cl-reservoir species ClONO2 and HCl. The time evolution of HCl, ClONO2 and ClO as well as the partitioning between the two reservoir molecules agrees well with previous observations and with our current understanding of chlorine activation during Arctic winter. The results of a chemical box model are also compared with the ACE-FTS measurements and are generally consistent with the measurements.


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