scholarly journals Microphysical simulations of new particle formation in the upper troposphere and lower stratosphere

2011 ◽  
Vol 11 (17) ◽  
pp. 9303-9322 ◽  
Author(s):  
J. M. English ◽  
O. B. Toon ◽  
M. J. Mills ◽  
F. Yu
Keyword(s):  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
General Circulation ◽  
Lower Stratosphere ◽  
Three Dimensional ◽  
Circulation Model ◽  
Number Concentration ◽  
Aerosol Formation ◽  
Upper Troposphere ◽  
Microphysical Processes

Abstract. Using a three-dimensional general circulation model with sulfur chemistry and sectional aerosol microphysics (WACCM/CARMA), we studied aerosol formation and microphysics in the upper troposphere and lower stratosphere (UTLS) as well as the middle and upper stratosphere based on three nucleation schemes (two binary homogeneous schemes and an ion-mediated scheme related to one of the binary schemes). Simulations suggest that ion-mediated nucleation rates in the UTLS are 25 % higher than its related binary scheme, but that the rates predicted by the two binary schemes vary by two orders of magnitude. None of the nucleation schemes is superior at matching the limited observations available at the smallest sizes. However, it is found that coagulation, not nucleation, controls number concentration at sizes greater than approximately 10 nm. Therefore, based on this study, processes relevant to atmospheric chemistry and radiative forcing in the UTLS are not sensitive to the choice of nucleation schemes. The dominance of coagulation over other microphysical processes in the UTLS is consistent with other recent work using microphysical models. Simulations using all three nucleation schemes compare reasonably well to observations of size distributions, number concentration across latitude, and vertical profiles of particle mixing ratio in the UTLS. Interestingly, we find that we need to include Van der Waals forces in our coagulation scheme to match the UTLS aerosol concentrations. We conclude that this model can reasonably represent sulfate microphysical processes in the UTLS, and that the properties of particles at atmospherically relevant sizes appear to be insensitive to the details of the nucleation scheme. We also suggest that micrometeorites, which are not included in this model, dominate the aerosol properties in the upper stratosphere above about 30 km.

scholarly journals Microphysical simulations of new particle formation in the upper troposphere and lower stratosphere

2011 ◽  
Vol 11 (4) ◽  
pp. 12441-12486 ◽  
Author(s):  
J. M. English ◽  
O. B. Toon ◽  
M. J. Mills ◽  
F. Yu
Keyword(s):  
General Circulation ◽  
Lower Stratosphere ◽  
Three Dimensional ◽  
Circulation Model ◽  
Number Concentration ◽  
Aerosol Formation ◽  
Upper Troposphere ◽  
Particle Mixing ◽  
Microphysical Processes ◽  
Atmospherically Relevant

Abstract. Using a three-dimensional general circulation model with sulfur chemistry and sectional aerosol microphysics (WACCM/CARMA), we studied aerosol formation and microphysics in the tropical upper troposphere and lower stratosphere (UTLS) based on three nucleation schemes (two binary homogeneous schemes and an ion-mediated scheme). Simulations suggest that ion-mediated nucleation rates in the UTLS are 25% higher than binary rates, but that the rates predicted by the two binary schemes vary by two orders of magnitude. However, it is found that coagulation, not nucleation, controls number concentration at sizes greater than approximately 10 nm. Therefore, based on this study, atmospherically relevant processes in the UTLS are not sensitive to the choice of nucleation schemes. The dominance of coagulation over other microphysical processes is consistent with other recent work using microphysical models. Simulations using all three nucleation schemes compare reasonably well to observations of size distributions, number concentration across latitude, and vertical profiles of particle mixing ratio in the UTLS. Interestingly, we find we need to include Van der Waals forces in our coagulation scheme to match the UTLS aerosol concentrations. We conclude that this model can accurately represent sulfate microphysical processes in the UTLS, and that the properties of particles at atmospherically relevant sizes are not sensitive to the details of the nucleation scheme. We also suggest that micrometeorites, which are not included in this model, dominate the aerosol properties in the upper stratosphere above about 30 km.

scholarly journals A new radiation infrastructure for the Modular Earth Submodel System (MESSy, based on version 2.51)

2016 ◽  
Author(s):  
Simone Dietmüller ◽  
Patrick Jöckel ◽  
Holger Tost ◽  
Markus Kunze ◽  
Cathrin Gellhorn ◽  
...  
Keyword(s):  
Optical Properties ◽  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
General Circulation ◽  
Circulation Model ◽  
Shortwave Radiation ◽  
Aerosol Optical Properties ◽  
On Line ◽  
User Friendly ◽  
Radiation Scheme

Abstract. The Modular Earth Submodel System (MESSy) provides an interface to couple submodels to a basemodel via a highly flexible data management facility (Jöckel et al., 2010). In the present paper we present the four new radiation related submodels RAD, AEROPT, CLOUDOPT and ORBIT. The submodel RAD (with shortwave radiation scheme RAD_FUBRAD) simulates the radiative transfer, the submodel AEROPT calculates the aerosol optical properties, the submodel CLOUDOPT calculates the cloud optical properties, and the submodel ORBIT is responsible for Earth orbit calculations. These submodels are coupled via the standard MESSy infrastructure and are largely based on the original radiation scheme of the general circulation model ECHAM5, however, expanded with additional features. These features comprise, among others, user-friendly and flexibly controllable (by namelists) on-line radiative forcing calculations by multiple diagnostic calls of the radiation routines. With this, it is now possible to calculate radiative forcing (instantaneous as well as stratosphere adjusted) of various greenhouse gases simultaneously in only one simulation, as well as the radiative forcing of cloud perturbations. Examples of on-line radiative forcing calculations in the ECHAM/MESSy Atmospheric Chemistry (EMAC) model are presented.

scholarly journals Characterising the seasonal and geographical variability in tropospheric ozone, stratospheric influence and recent changes

2019 ◽  
Vol 19 (6) ◽  
pp. 3589-3620 ◽  
Author(s):  
Ryan S. Williams ◽  
Michaela I. Hegglin ◽  
Brian J. Kerridge ◽  
Patrick Jöckel ◽  
Barry G. Latter ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Lower Stratosphere ◽  
Climate Model ◽  
Stratospheric Ozone ◽  
Data Availability ◽  
Ozone Production ◽  
Upper Troposphere ◽  
The World

Abstract. The stratospheric contribution to tropospheric ozone (O3) has been a subject of much debate in recent decades but is known to have an important influence. Recent improvements in diagnostic and modelling tools provide new evidence that the stratosphere has a much larger influence than previously thought. This study aims to characterise the seasonal and geographical distribution of tropospheric ozone, its variability, and its changes and provide quantification of the stratospheric influence on these measures. To this end, we evaluate hindcast specified-dynamics chemistry–climate model (CCM) simulations from the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) model and the Canadian Middle Atmosphere Model (CMAM), as contributed to the International Global Atmospheric Chemistry – Stratosphere-troposphere Processes And their Role in Climate (IGAC-SPARC) (IGAC–SPARC) Chemistry Climate Model Initiative (CCMI) activity, together with satellite observations from the Ozone Monitoring Instrument (OMI) and ozone-sonde profile measurements from the World Ozone and Ultraviolet Radiation Data Centre (WOUDC) over a period of concurrent data availability (2005–2010). An overall positive, seasonally dependent bias in 1000–450 hPa (∼0–5.5 km) sub-column ozone is found for EMAC, ranging from 2 to 8 Dobson units (DU), whereas CMAM is found to be in closer agreement with the observations, although with substantial seasonal and regional variation in the sign and magnitude of the bias (∼±4 DU). Although the application of OMI averaging kernels (AKs) improves agreement with model estimates from both EMAC and CMAM as expected, comparisons with ozone-sondes indicate a positive ozone bias in the lower stratosphere in CMAM, together with a negative bias in the troposphere resulting from a likely underestimation of photochemical ozone production. This has ramifications for diagnosing the level of model–measurement agreement. Model variability is found to be more similar in magnitude to that implied from ozone-sondes in comparison with OMI, which has significantly larger variability. Noting the overall consistency of the CCMs, the influence of the model chemistry schemes and internal dynamics is discussed in relation to the inter-model differences found. In particular, it is inferred that CMAM simulates a faster and shallower Brewer–Dobson circulation (BDC) compared to both EMAC and observational estimates, which has implications for the distribution and magnitude of the downward flux of stratospheric ozone over the most recent climatological period (1980–2010). Nonetheless, it is shown that the stratospheric influence on tropospheric ozone is significant and is estimated to exceed 50 % in the wintertime extratropics, even in the lower troposphere. Finally, long-term changes in the CCM ozone tracers are calculated for different seasons. An overall statistically significant increase in tropospheric ozone is found across much of the world but particularly in the Northern Hemisphere and in the middle to upper troposphere, where the increase is on the order of 4–6 ppbv (5 %–10 %) between 1980–1989 and 2001–2010. Our model study implies that attribution from stratosphere–troposphere exchange (STE) to such ozone changes ranges from 25 % to 30 % at the surface to as much as 50 %–80 % in the upper troposphere–lower stratosphere (UTLS) across some regions of the world, including western Eurasia, eastern North America, the South Pacific and the southern Indian Ocean. These findings highlight the importance of a well-resolved stratosphere in simulations of tropospheric ozone and its implications for the radiative forcing, air quality and oxidation capacity of the troposphere.

scholarly journals Microphysical simulations of sulfur burdens from stratospheric sulfur geoengineering

2012 ◽  
Vol 12 (10) ◽  
pp. 4775-4793 ◽  
Author(s):  
J. M. English ◽  
O. B. Toon ◽  
M. J. Mills
Keyword(s):  
Radiative Forcing ◽  
General Circulation ◽  
Climate Model ◽  
Three Dimensional ◽  
Circulation Model ◽  
Injection Rate ◽  
Sulfur Chemistry ◽  
Aerosol Mass ◽  
Tropospheric Aerosol ◽  
So2 Gas

Abstract. Recent microphysical studies suggest that geoengineering by continuous stratospheric injection of SO2 gas may be limited by the growth of the aerosols. We study the efficacy of SO2, H2SO4 and aerosol injections on aerosol mass and optical depth using a three-dimensional general circulation model with sulfur chemistry and sectional aerosol microphysics (WACCM/CARMA). We find increasing injection rates of SO2 in a narrow band around the equator to have limited efficacy while broadening the injecting zone as well as injecting particles instead of SO2 gas increases the sulfate burden for a given injection rate, in agreement with previous work. We find that injecting H2SO4 gas instead of SO2 does not discernibly alter sulfate size or mass, in contrast with a previous study using a plume model with a microphysical model. However, the physics and chemistry in aircraft plumes, which are smaller than climate model grid cells, need to be more carefully considered. We also find significant perturbations to tropospheric aerosol for all injections studied, particularly in the upper troposphere and near the poles, where sulfate burden increases by up to 100 times. This enhanced burden could have implications for tropospheric radiative forcing and chemistry. These results highlight the need to mitigate greenhouse gas emissions rather than attempt to cool the planet through geoengineering, and to further study geoengineering before it can be seriously considered as a climate intervention option.

scholarly journals Evaluation of CLaMS, KASIMA and ECHAM5/MESSy1 simulations in the lower stratosphere using observations of Odin/SMR and ILAS/ILAS-II

2009 ◽  
Vol 9 (1) ◽  
pp. 1977-2020
Author(s):  
F. Khosrawi ◽  
R. Müller ◽  
M. H. Proffitt ◽  
R. Ruhnke ◽  
O. Kirner ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
General Circulation ◽  
Lower Stratosphere ◽  
Climate Model ◽  
Middle Atmosphere ◽  
Circulation Model ◽  
Lagrangian Model ◽  
Data Sets ◽  
Data Set ◽  
The Impact

Abstract. 1-year data sets of monthly averaged nitrous oxide (N2O) and ozone (O3) derived from satellite measurements were used as a tool for the evaluation of atmospheric photochemical models. Two 1-year data sets, one derived from the Improved Limb Atmospheric Spectrometer (ILAS and ILAS-II) and one from the Odin Sub-Millimetre Radiometer (Odin/SMR) were employed. Here, these data sets are used for the evaluation of two Chemical Transport Models (CTMs), the Karlsruhe Simulation Model of the Middle Atmosphere (KASIMA) and the Chemical Lagrangian Model of the Stratosphere (CLaMS) as well as for one Chemistry-Climate Model (CCM), the atmospheric chemistry general circulation model ECHAM5/MESSy1 (E5M1) in the lower stratosphere with focus on the Northern Hemisphere. Since the Odin/SMR measurements cover the entire hemisphere, the evaluation is performed for the entire hemisphere as well as for the low latitudes, midlatitudes and high latitudes using the Odin/SMR 1-year data set as reference. To assess the impact of using different data sets for such an evaluation study we repeat the evaluation for the polar lower stratosphere using the ILAS/ILAS-II data set. Only small differences were found using ILAS/ILAS-II instead of Odin/SMR as a reference, thus, showing that the results are not influenced by the particular satellite data set used for the evaluation. The evaluation of CLaMS, KASIMA and E5M1 shows that all models are in good agreement with Odin/SMR and ILAS/ILAS-II. Differences are generally in the range of ±20%. Larger differences (up to −40%) are found in all models at 500±25 K for N2O mixing ratios greater than 200 ppb. Generally, the largest differences were found for the tropics and the lowest for the polar regions. However, an underestimation of polar winter ozone loss was found both in KASIMA and E5M1 both in the Northern and Southern Hemisphere.

scholarly journals Simulation of organics in the atmosphere: evaluation of EMACv2.54 with the Mainz Organic Mechanism (MOM) coupled to the ORACLE (v1.0) submodel

2021 ◽  
Author(s):  
Andrea Pozzer ◽  
Simon Reifenberg ◽  
Vinod Kumar ◽  
Bruno Franco ◽  
Domenico Taraborrelli ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
General Circulation ◽  
Circulation Model ◽  
Organic Aerosol ◽  
Efficient Estimation ◽  
Chemical Degradation ◽  
Aerosol Formation ◽  
Organic Species ◽  
Volatile Organic ◽  
Good Agreement

Abstract. An updated and expanded representation of organics in the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) has been evaluated. First, the comprehensive Mainz Organic Mechanism (MOM) in the submodel MECCA (Module Efficiently Calculating the Chemistry of the Atmosphere) was activated with explicit degradation of organic species up to five carbon atoms and a simplified mechanism for larger molecules. Second, the ORACLE submodel (version 1.0) considers now condensation on aerosols for all organics in the mechanism. Parameterizations for aerosol yields are used only for the lumped species that are not included in the explicit mechanism. The simultaneous usage of MOM and ORACLE allows an efficient estimation, not only of the chemical degradation of the simulated volatile organic compounds, but also of the contribution of organics to the growth and fate of (organic) aerosol, with a complexity of the mechanism largely increased compared to EMAC simulations with more simplified chemistry. The model evaluation presented here reveals that the OH concentration is well reproduced globally, while significant biases for observed oxygenated organics are present. We also investigate the general properties of the aerosols and their composition, showing that the more sophisticated and process-oriented secondary aerosol formation does not degrade the good agreement of previous model configurations with observations at the surface, allowing further research in the field of gas-aerosol interactions.

scholarly journals The impact of the 1783–1784 AD Laki eruption on global aerosol formation processes and cloud condensation nuclei

2010 ◽  
Vol 10 (2) ◽  
pp. 3189-3228
Author(s):  
A. Schmidt ◽  
K. S. Carslaw ◽  
G. W. Mann ◽  
B. M. Wilson ◽  
T. J. Breider ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Northern Hemisphere ◽  
General Circulation ◽  
Cloud Condensation Nuclei ◽  
General Circulation Models ◽  
Aerosol Formation ◽  
Condensation Nuclei ◽  
Upper Troposphere ◽  
Microphysical Processes ◽  
The Impact

Abstract. The 1783–1784 AD Laki flood lava eruption commenced on 8 June 1783 and released 122 Tg of sulphur dioxide gas over the course of 8 months into the upper troposphere and lower stratosphere above Iceland. Previous studies have examined the impact of the Laki eruption on sulphate aerosol and climate using general circulation models. Here, we study the impact on aerosol microphysical processes, including the nucleation of new particles and their growth to cloud condensation nuclei (CCN) using a comprehensive Global Model of Aerosol Processes (GLOMAP). Total particle concentrations in the free troposphere increase by a factor ~16 over large parts of the Northern Hemisphere in the 3 months following the onset of the eruption. Particle concentrations in the boundary layer increase by a factor 2 to 5 in regions as far away as North America, the Middle East and Asia due to long-range transport of nucleated particles. CCN concentrations (at 0.22% supersaturation) increase by a factor 65 in the upper troposphere with maximum changes in 3-month zonal mean concentrations of ~1400 cm−3 at high northern latitudes. 3-month zonal mean CCN concentrations in the boundary layer at the latitude of the eruption increase by up to a factor 26, and averaged over the Northern Hemisphere, the eruption caused a factor 4 increase in CCN concentrations at low-level cloud altitude. The simulations show that the Laki eruption would have completely dominated as a source of CCN in the pre-industrial atmosphere. The model also suggests an impact of the eruption in the Southern Hemisphere, where CCN concentrations are increased by up to a factor 1.4 at 20° S. Our model simulations suggest that the impact of an equivalent wintertime eruption on upper tropospheric CCN concentrations is only about one-third of that of a summertime eruption. The simulations show that the microphysical processes leading to the growth of particles to CCN sizes are fundamentally different after an eruption when compared to the unperturbed atmosphere, underlining the importance of using a fully coupled microphysics model when studying long-lasting, high-latitude eruptions.

scholarly journals Forcing of the Upper-Tropospheric Monsoon Anticyclones

2019 ◽  
Vol 76 (7) ◽  
pp. 1937-1954 ◽  
Author(s):  
Leong Wai Siu ◽  
Kenneth P. Bowman
Keyword(s):  
General Circulation ◽  
Asian Monsoon ◽  
Lower Stratosphere ◽  
Warm Season ◽  
Circulation Model ◽  
Western Hemisphere ◽  
North American Monsoon ◽  
Upper Troposphere ◽  
Forcing Mechanisms ◽  
Good Agreement

Abstract During the boreal warm season (May–September), the circulation in the upper troposphere and lower stratosphere is dominated by two large anticyclones: the Asian monsoon anticyclone (AMA) and North American monsoon anticyclone (NAMA). The existence of the AMA has long been linked to Asian monsoon precipitation using the Matsuno–Gill framework, but the origin of the NAMA has not been clearly understood. Here the forcing mechanisms of the NAMA are investigated using a simplified dry general circulation model. The simulated anticyclones are in good agreement with observations when the model is forced by a zonally symmetric meridional temperature gradient plus a realistic geographical distribution of heating based on observed tropical and subtropical precipitation in the Northern Hemisphere. Model experiments show that the AMA and NAMA are largely independent of one another, and the NAMA is not a downstream response to the Asian monsoon. The primary forcing of the NAMA is precipitation in the longitude sector between 60° and 120°W, with the largest contribution coming from the subtropical latitudes within that sector. Experiments with idealized regional heating distributions reveal that the extratropical response to tropical and subtropical precipitation depends approximately linearly on the magnitude of the forcing but nonlinearly on its latitude. The AMA is stronger than the NAMA, primarily because precipitation in the subtropics over Asia is much heavier than at similar latitudes in the Western Hemisphere.

scholarly journals Stratospheric SO<sub>2</sub> and sulphate aerosol, model simulations and satellite observations

2013 ◽  
Vol 13 (4) ◽  
pp. 11395-11425 ◽  
Author(s):  
C. Brühl ◽  
J. Lelieveld ◽  
M. Höpfner ◽  
H. Tost
Keyword(s):  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
General Circulation ◽  
Middle Atmosphere ◽  
Lower Boundary ◽  
Circulation Model ◽  
Volcanic Eruptions ◽  
Satellite Observations ◽  
Quasi Biennial Oscillation ◽  
Tropospheric Aerosol

Abstract. A multiyear study with the atmospheric chemistry general circulation model EMAC with the aerosol module GMXe at high altitude resolution demonstrates that the sulfur gases COS and SO2, the latter from low-latitude volcanic eruptions, predominantly control the formation of stratospheric aerosol. The model consistently uses the same parameters in the troposphere and stratosphere for 7 aerosol modes applied. Lower boundary conditions for COS and other long-lived trace gases are taken from measurement networks, while estimates of volcanic SO2 emissions are based on satellite observations. We show comparisons with satellite data for aerosol extinction (e.g. SAGE) and SO2 in the middle atmosphere (MIPAS on ENVISAT). This corroborates the interannual variability induced by the Quasi-Biennial Oscillation, which is internally generated by the model. The model also realistically simulates the radiative effects of stratospheric and tropospheric aerosol including the effects on the model dynamics. The medium strength volcanic eruptions of 2005 and 2006 exerted a nonnegligible radiative forcing of up to −0.6 W m−2 in the tropics, while the large Pinatubo eruption caused a maximum though short term tropical forcing of about −10 W m−2. The study also shows that observed upper stratospheric SO2 can be simulated accurately only when a sulphur sink on meteoritic dust is included and the photolysis of gaseous H2SO4 in the near infrared is higher than assumed previously.

scholarly journals Sensitivity of Global Modeling Initiative chemistry and transport model simulations of radon-222 and lead-210 to input meteorological data

2005 ◽  
Vol 5 (4) ◽  
pp. 5325-5372 ◽  
Author(s):  
D. B. Considine ◽  
D. J. Bergmann ◽  
H. Liu
Keyword(s):  
General Circulation Model ◽  
General Circulation ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Meteorological Data ◽  
Circulation Model ◽  
Convective Transport ◽  
Global Modeling ◽  
Upper Troposphere ◽  
Lead 210

Abstract. We have used the Global Modeling Initiative chemistry and transport model to simulate the radionuclides radon-222 and lead-210 using three different sets of input meteorological information: 1. Output from the Goddard Space Flight Center Global Modeling and Assimilation Office GEOS-STRAT assimilation; 2. Output from the Goddard Institute for Space Studies GISS II′ general circulation model; and 3. Output from the National Center for Atmospheric Research MACCM3 general circulation model. We intercompare these simulations with observations to determine the variability resulting from the different meteorological data used to drive the model, and to assess the agreement of the simulations with observations at the surface and in the upper troposphere/lower stratosphere region. The observational datasets we use are primarily climatologies developed from multiple years of observations. In the upper troposphere/lower stratosphere region, climatological distributions of lead-210 were constructed from ~25 years of aircraft and balloon observations compiled into the US Environmental Measurements Laboratory RANDAB database. Taken as a whole, no simulation stands out as superior to the others. However, the simulation driven by the NCAR MACCM3 meteorological data compares better with lead-210 observations in the upper troposphere/lower stratosphere region. Comparisons of simulations made with and without convection show that the role played by convective transport and scavenging in the three simulations differs substantially. These differences may have implications for evaluation of the importance of very short-lived halogen-containing species on stratospheric halogen budgets.

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