scholarly journals Maintenance of polar stratospheric clouds in a moist stratosphere

2008 ◽  
Vol 4 (1) ◽  
pp. 69-78 ◽  
Author(s):  
D. B. Kirk-Davidoff ◽  
J.-F. Lamarque

Abstract. Previous work has shown that polar stratospheric clouds (PSCs) could have acted to substantially warm high latitude regions during past warm climates such as the Eocene (55 Ma). Using a simple model of stratospheric water vapor transport and polar stratospheric cloud (PSC) formation, we investigate the dependence of PSC optical depth on tropopause temperature, cloud microphysical parameters, stratospheric overturning, and tropospheric methane. We show that PSC radiative effects can help slow removal of water from the stratosphere via self-heating. However, we also show that the ability of PSCs to have a substantial impact on climate depends strongly on the PSC particle number density and the strength of the overturning circulation. Thus even a large source of stratospheric water vapor (e.g. from methane oxidation) will not result in substantial PSC radiative effects unless PSC ice crystal number density is high compared to most current observations, and stratospheric overturning (which modulates polar stratospheric temperatures) is low. These results are supported by analysis of a series of runs of the NCAR WACCM model with methane concentrations varying up to one thousand times present levels.

2007 ◽  
Vol 3 (4) ◽  
pp. 935-960 ◽  
Author(s):  
D. B. Kirk-Davidoff ◽  
J.-F. Lamarque

Abstract. Previous work has shown that polar stratospheric clouds (PSCs) could have acted to substantially warm high latitude regions during past warm climates such as the Eocene (55 Ma). Using a simple model of stratospheric water vapor transport and polar stratospheric cloud (PSC) formation, we investigate the dependence of PSC optical depth on tropopause temperature, cloud microphysical parameters, stratospheric overturning, and tropospheric methane. We show that PSC radiative effects can help slow removal of water from the stratosphere via self-heating. However, we also show that the ability of PSCs to have a substantial impact on climate depends strongly on the PSC particle number density and the strength of the overturning circulation. Thus even a large source of stratospheric water vapor (e.g. from methane oxidation) will not result in substantial PSC radiative effects unless PSC ice crystal number density is high, and stratospheric overturning (which modulates polar stratospheric temperatures) is low. These results are supported by analysis of a series of runs of the NCAR WACCM model with methane concentrations varying up to one thousand times present levels.


2020 ◽  
Author(s):  
Michael Steiner ◽  
Beiping Luo ◽  
Thomas Peter ◽  
Michael C. Pitts ◽  
Andrea Stenke

Abstract. Polar Stratospheric Clouds (PSCs) contribute to catalytic ozone destruction by providing surfaces for the conversion of inert chlorine species into active forms and by denitrification of the stratosphere. Therefore, an accurate representation of PSCs in chemistry-climate models (CCMs) is of great importance to correctly simulate polar ozone concentrations. Here, we evaluate PSCs as simulated by the CCM SOCOLv3.1 for the Antarctic winter 2007 by comparison with backscatter measurements by CALIOP onboard the CALIPSO satellite. The model considers supercooled ternary solution (STS) droplets, nitric acid trihydrate (NAT) particles, water ice particles, and mixtures thereof. PSCs are parametrized in terms of temperature and partial pressures of HNO3 and H2O, assuming equilibrium between gas and particulate phase. We use the CALIOP measurements to optimize three prescribed microphysical parameters of the PSC scheme, namely ice number density, NAT particle radius and maximum NAT number density. The choice of the prescribed value of the ice number density affects simulated optical properties and dehydration, while modifying the maximum NAT number density or the NAT particle radius impacts stratospheric composition by enhancing the HNO3-uptake and denitrification. Best agreement with the CALIOP optical properties and observed denitrification was for this case study found with the ice number density increased from the hitherto used value of 0.01 to 0.05 cm−3 and the maximum NAT number density from 5×10−4 to 1×10−3 cm−3. The NAT radius was kept at the original value of 5 µm. The new parametrization reflects the higher importance attributed to heterogeneous nucleation of ice and NAT particles, e.g. on meteoric dust, following recent new data evaluations of the state-of-the-art CALIOP measurements. A cold temperature bias in the polar lower stratosphere results in an overestimated PSC areal coverage in SOCOLv3.1 by up to 100 %. Furthermore, the occurrence of mountain-wave induced ice, as observed mainly over the Antarctic Peninsula, is continuously underestimated in the model due to the coarse model resolution and the fixed ice number density. However, overall we find a good temporal and spatial agreement between modeled and observed PSC occurrence and composition, as well as reasonable modeled denitrification and ozone loss. Based on constraining three important parameters by means of the CALIOP measurements, this work demonstrates that also a simplified PSC scheme, which describes STS, NAT, ice and mixtures thereof with equilibrium assumptions and avoids nucleation and growth calculations in sophisticated, but time-consuming microphysical process models, may achieve good approximations of fundamental properties of PSCs needed in CCMs.


2021 ◽  
Vol 14 (2) ◽  
pp. 935-959
Author(s):  
Michael Steiner ◽  
Beiping Luo ◽  
Thomas Peter ◽  
Michael C. Pitts ◽  
Andrea Stenke

Abstract. Polar stratospheric clouds (PSCs) contribute to catalytic ozone destruction by providing surfaces for the conversion of inert chlorine species into active forms and by denitrification. The latter describes the removal of HNO3 from the stratosphere by sedimenting PSC particles, which hinders chlorine deactivation by the formation of reservoir species. Therefore, an accurate representation of PSCs in chemistry–climate models (CCMs) is of great importance to correctly simulate polar ozone concentrations. Here, we evaluate PSCs as simulated by the CCM SOCOLv3.1 for the Antarctic winters 2006, 2007 and 2010 by comparison with backscatter measurements by CALIOP on board the CALIPSO satellite. The year 2007 represents a typical Antarctic winter, while 2006 and 2010 are characterized by above- and below-average PSC occurrence. The model considers supercooled ternary solution (STS) droplets, nitric acid trihydrate (NAT) particles, water ice particles and mixtures thereof. PSCs are parameterized in terms of temperature and partial pressures of HNO3 and H2O, assuming equilibrium between the gas and particulate phase. The PSC scheme involves a set of prescribed microphysical parameters, namely ice number density, NAT particle radius and maximum NAT number density. In this study, we test and optimize the parameter settings through several sensitivity simulations. The choice of the value for the ice number density affects simulated optical properties and dehydration, while modifying the NAT parameters impacts stratospheric composition via HNO3 uptake and denitrification. Depending on the NAT parameters, reasonable denitrification can be modeled. However, its impact on ozone loss is minor. The best agreement with the CALIOP optical properties and observed denitrification was for this case study found with the ice number density increased from the hitherto used value of 0.01 to 0.05 cm−3 and the maximum NAT number density from 5×10-4 to 1×10-3 cm−3. The NAT radius was kept at the original value of 5 µm. The new parameterization reflects the higher importance attributed to heterogeneous nucleation of ice and NAT particles following recent new data evaluations of the state-of-the-art CALIOP measurements. A cold temperature bias in the polar lower stratosphere results in an overestimated PSC areal coverage in SOCOLv3.1 by up to 40 %. Offsetting this cold bias by +3 K delays the onset of ozone depletion by about 2 weeks, which improves the agreement with observations. Furthermore, the occurrence of mountain-wave-induced ice, as observed mainly over the Antarctic Peninsula, is continuously underestimated in the model due to the coarse model resolution (T42L39) and the fixed ice number density. Nevertheless, we find overall good temporal and spatial agreement between modeled and observed PSC occurrence and composition. This work confirms previous studies indicating that simplified PSC schemes, which avoid nucleation and growth calculations in sophisticated but time-consuming microphysical process models, may also achieve good approximations of the fundamental properties of PSCs needed in CCMs.


2019 ◽  
Author(s):  
David R. Hanson ◽  
Hussein Abdullahi ◽  
Seakh Menheer ◽  
Joaquin Vences ◽  
Michael R. Alves ◽  
...  

Abstract. Size distributions of particles formed from sulfuric acid (H2SO4) and water vapor in a Photolytic Flow Reactor (PhoFR) were measured with a nano-particle mobility sizing system. Experiments with added ammonia and dimethylamine were also performed. H2SO4(g) was synthesized from HONO, sulfur dioxide, and water vapor, initiating OH oxidation by HONO photolysis. For standard reactant flows and conditions, 296 K, 52 % relative humidity, and a ~ 40 s residence time, the calculated concentration of H2SO4 peaked at 1.2 × 1010 cm−3, measured particle mean diameter was ~ 6 nm and total number density was ~ 104 cm−3. Measured distributions were influenced by molecular clusters at small sizes, less than or equal to 2 nm diameter, but were generally dominated by large particles that are roughly log-normal with mean diameters ranging up to 12 nm and a relatively constant lnσ of ~ 0.3. Particle number density and their mean size depended on relative humidity, HONO concentration, illumination, and SO2 level. Particle formation conditions were stable over many months. Addition of single-digit pmol/mol mixing ratios of dimethylamine led to very large increases in number density. Ammonia at levels up to 2000 pmol/mol showed that NH3 is less effective than dimethylamine at producing particles. A two-dimensional simulation of PhoFR reveals that H2SO4 scales with HONO and its level builds along the length of the flow reactor. Experimentally, particle growth scaled with HONO, in accord with model-predicted H2SO4 levels. Additional comparison between experiment and model indicates that reaction of HO2 with SO2 could be a significant source of H2SO4 in this experiment. The effects of potential contaminants on particle formation rates near room temperature are addressed and provide context in comparisons with previous experiments. The added-base experimental results provide support for previously published dimethylamine-H2SO4 cluster thermodynamics but do not support previously published ammonia-sulfuric acid thermodynamics.


1990 ◽  
Vol 17 (4) ◽  
pp. 373-376 ◽  
Author(s):  
S. Kinne ◽  
O. B. Toon

2018 ◽  
Author(s):  
Javier Vaquero-Martínez

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