scholarly journals The impact of lightning on tropospheric ozone chemistry using a new global parametrisation

2016 ◽  
Author(s):  
D. L. Finney ◽  
R. M. Doherty ◽  
O. Wild ◽  
N. L. Abraham
Keyword(s):  
Frequency Distribution ◽  
Tropospheric Ozone ◽  
Climate Model ◽  
Upper Troposphere ◽  
Temporal Correlations ◽  
The Uk ◽  
Cloud Ice ◽  
The Impact ◽  
No Emissions ◽  
Tropical Upper Troposphere

Abstract. A lightning parametrisation based on upward cloud ice flux is implemented in a chemistry-climate model (CCM) for the first time. The UK Chemistry and Aerosols model is used to study the impact of these lightning nitric oxide (NO) emissions on ozone. Comparisons are then made between the new ice flux parametrisation and the commonly-used, cloud-top height parametrisation. The ice flux approach improves the simulation of lightning and the temporal correlations with ozone sonde measurements in the middle and upper troposphere. Peak values of ozone in these regions are attributed to high lightning NO emissions. The ice flux approach reduces the overestimation of tropical lightning apparent in this CCM when using the cloud-top approach. This results in less emission in the tropical upper troposphere and more in the extratropics when using the ice flux scheme. In the tropical upper troposphere the reduction in ozone concentration is around 5–10 %. Surprisingly, there is only a small reduction in tropospheric ozone burden when using the ice flux approach. The greatest absolute change in ozone burden is found in the lower stratosphere suggesting that much of the ozone produced in the upper troposphere is transported to higher altitudes. Major differences in the frequency distribution of flash rates for the two approaches are found. The cloud-top height scheme has lower maximum flash rates and more mid-range flash rates than the ice flux scheme. The initial Ox (odd oxygen species) production associated with the frequency distribution of continental lightning is analysed to show that higher flash rates are less efficient at producing Ox – low flash rates produce around 10 times more Ox per flash than high-end flash rates. We find that the newly implemented lightning scheme performs favourably compared to the cloud-top scheme with respect to simulation of lightning and tropospheric ozone. This alternative lightning scheme shows spatial and temporal differences in ozone chemistry which may have implications for comparison on models and observations and for simulation of future changes in tropospheric ozone.

scholarly journals The impact of lightning on tropospheric ozone chemistry using a new global lightning parametrisation

2016 ◽  
Vol 16 (12) ◽  
pp. 7507-7522 ◽  
Author(s):  
D. L. Finney ◽  
R. M. Doherty ◽  
O. Wild ◽  
N. L. Abraham
Keyword(s):  
Frequency Distribution ◽  
Tropospheric Ozone ◽  
Climate Model ◽  
Upper Troposphere ◽  
Temporal Correlations ◽  
The Uk ◽  
Cloud Ice ◽  
The Impact ◽  
No Emissions ◽  
Tropical Upper Troposphere

Abstract. A lightning parametrisation based on upward cloud ice flux is implemented in a chemistry–climate model (CCM) for the first time. The UK Chemistry and Aerosols model is used to study the impact of these lightning nitric oxide (NO) emissions on ozone. Comparisons are then made between the new ice flux parametrisation and the commonly used, cloud-top height parametrisation. The ice flux approach improves the simulation of lightning and the temporal correlations with ozone sonde measurements in the middle and upper troposphere. Peak values of ozone in these regions are attributed to high lightning NO emissions. The ice flux approach reduces the overestimation of tropical lightning apparent in this CCM when using the cloud-top approach. This results in less NO emission in the tropical upper troposphere and more in the extratropics when using the ice flux scheme. In the tropical upper troposphere the reduction in ozone concentration is around 5–10 %. Surprisingly, there is only a small reduction in tropospheric ozone burden when using the ice flux approach. The greatest absolute change in ozone burden is found in the lower stratosphere, suggesting that much of the ozone produced in the upper troposphere is transported to higher altitudes. Major differences in the frequency distribution of flash rates for the two approaches are found. The cloud-top height scheme has lower maximum flash rates and more mid-range flash rates than the ice flux scheme. The initial Ox (odd oxygen species) production associated with the frequency distribution of continental lightning is analysed to show that higher flash rates are less efficient at producing Ox; low flash rates initially produce around 10 times more Ox per flash than high-end flash rates. We find that the newly implemented lightning scheme performs favourably compared to the cloud-top scheme with respect to simulation of lightning and tropospheric ozone. This alternative lightning scheme shows spatial and temporal differences in ozone chemistry which may have implications for comparison between models and observations, as well as for simulation of future changes in tropospheric ozone.

scholarly journals Radiative Cooling, Latent Heating, and Cloud Ice in the Tropical Upper Troposphere

2021 ◽  
pp. 1-39
Keyword(s):  
Heating Rate ◽  
Radiative Cooling ◽  
Convective Heating ◽  
Tropospheric Temperature ◽  
Latent Heating ◽  
Upper Troposphere ◽  
Eddy Heat Flux ◽  
Cloud Ice ◽  
The Impact ◽  
Tropical Upper Troposphere

Abstract The radiative cooling rate in the tropical upper troposphere is expected to increase as climate warms. Since the tropics are approximately in radiative-convective equilibrium (RCE), this implies an increase in the convective heating rate, which is the sum of the latent heating rate and the eddy heat flux convergence. We examine the impact of these changes on the vertical profile of cloud ice amount in cloud-resolving simulations of RCE. Three simulations are conducted: a control run, a warming run, and an experimental run in which there is no warming but a temperature forcing is imposed to mimic the warming-induced increase in radiative cooling. Surface warming causes a reduction in cloud fraction at all upper tropospheric temperature levels but an increase in the ice mixing ratio within deep convective cores. The experimental run has more cloud ice than the warming run at fixed temperature despite the fact that their latent heating rates are equal, which suggests that the efficiency of latent heating by cloud ice increases with warming. An analytic expression relating the ice-related latent heating rate to a number of other factors is derived and used to understand the model results. This reveals that the increase in latent heating efficiency is driven mostly by 1) the migration of isotherms to lower pressure and 2) a slight warming of the top of the convective layer. These physically robust changes act to reduce the residence time of ice along at any particular temperature level, which tempers the response of the mean cloud ice profile to warming.

scholarly journals Modelling the impact of megacities on local, regional and global tropospheric ozone and the deposition of nitrogen species

2013 ◽  
Vol 13 (24) ◽  
pp. 12215-12231 ◽  
Author(s):  
Z. S. Stock ◽  
M. R. Russo ◽  
T. M. Butler ◽  
A. T. Archibald ◽  
M. G. Lawrence ◽  
...  
Keyword(s):  
Air Quality ◽  
Urban Areas ◽  
Climate Model ◽  
Surface Ozone ◽  
Global Scale ◽  
Chemical Environment ◽  
Ozone Production ◽  
The Uk ◽  
The Impact ◽  
Local Emissions

Abstract. We examine the effects of ozone precursor emissions from megacities on present-day air quality using the global chemistry–climate model UM-UKCA (UK Met Office Unified Model coupled to the UK Chemistry and Aerosols model). The sensitivity of megacity and regional ozone to local emissions, both from within the megacity and from surrounding regions, is important for determining air quality across many scales, which in turn is key for reducing human exposure to high levels of pollutants. We use two methods, perturbation and tagging, to quantify the impact of megacity emissions on global ozone. We also completely redistribute the anthropogenic emissions from megacities, to compare changes in local air quality going from centralised, densely populated megacities to decentralised, lower density urban areas. Focus is placed not only on how changes to megacity emissions affect regional and global NOx and O3, but also on changes to NOy deposition and to local chemical environments which are perturbed by the emission changes. The perturbation and tagging methods show broadly similar megacity impacts on total ozone, with the perturbation method underestimating the contribution partially because it perturbs the background chemical environment. The total redistribution of megacity emissions locally shifts the chemical environment towards more NOx-limited conditions in the megacities, which is more conducive to ozone production, and monthly mean surface ozone is found to increase up to 30% in megacities, depending on latitude and season. However, the displacement of emissions has little effect on the global annual ozone burden (0.12% change). Globally, megacity emissions are shown to contribute ~3% of total NOy deposition. The changes in O3, NOx and NOy deposition described here are useful for quantifying megacity impacts and for understanding the sensitivity of megacity regions to local emissions. The small global effects of the 100% redistribution carried out in this study suggest that the distribution of emissions on the local scale is unlikely to have large implications for chemistry–climate processes on the global scale.

scholarly journals Chemistry–climate interactions of aerosol nitrate from lightning

2017 ◽  
Vol 17 (2) ◽  
pp. 1125-1142 ◽  
Author(s):  
Holger Tost
Keyword(s):  
Climate Model ◽  
Statistical Significance ◽  
Aerosol Particles ◽  
Internal Variability ◽  
Aerosol Size Distribution ◽  
Upper Troposphere ◽  
Uncertainty Range ◽  
Mixing Ratios ◽  
Microphysical Properties ◽  
The Impact

Abstract. Lightning represents one of the dominant emission sources for NOx in the troposphere. The direct release of oxidised nitrogen in the upper troposphere does not only affect ozone formation, but also chemical and microphysical properties of aerosol particles in this region. This study investigates the direct impact of LNOx emissions on upper-tropospheric nitrate using a global chemistry climate model. The simulation results show a substantial influence of the lightning emissions on the mixing ratios of nitrate aerosol in the upper troposphere of more than 50 %. In addition to the impact on nitrate, lightning substantially affects the oxidising capacity of the atmosphere with substantial implications for gas-phase sulfate formation and new particle formation in the upper troposphere. In conjunction with the condensation of nitrates, substantial differences in the aerosol size distribution occur in the upper troposphere as a consequence of lightning. This has implications for the extinction properties of the aerosol particles and for the cloud optical properties. While the extinction is generally slightly enhanced due to the LNOx emissions, the response of the clouds is ambiguous due to compensating effects in both liquid and ice clouds. Resulting shortwave flux perturbations are of   ∼ −100 mW m−2 as determined from several sensitivity scenarios, but an uncertainty range of almost 50 % has to be defined due to the large internal variability of the system and the uncertainties in the multitude of involved processes. Despite the clear statistical significance of the influence of lightning on the nitrate concentrations, the robustness of the findings gradually decreases towards the determination of the radiative flux perturbations.

scholarly journals Impact of biogenic hydrocarbons on tropospheric chemistry: results from a global chemistry-climate model

2005 ◽  
Vol 5 (5) ◽  
pp. 10517-10612 ◽  
Author(s):  
G. A. Folberth ◽  
D. A. Hauglustaine ◽  
J. Lathière ◽  
F. Brocheton
Keyword(s):  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Climate Model ◽  
Primary Source ◽  
Tropospheric Chemistry ◽  
Secondary Source ◽  
Peroxy Radicals ◽  
Substantial Impact ◽  
The Impact ◽  
Global Mean

Abstract. We present a description and evaluation of LMDz-INCA, a global three-dimensional chemistry-climate model, pertaining to its recently developed NMHC version. In this substantially extended version of the model a comprehensive representation of the photochemistry of non-methane hydrocarbons (NMHC) and volatile organic compounds (VOC) from biogenic, anthropogenic, and biomass-burning sources has been included. The tropospheric annual mean methane (9.2 years) and methylchloroform (5.5 years) chemical lifetimes are well within the range of previous modelling studies and are in excellent agreement with estimates established by means of global observations. The model provides a reasonable simulation of the horizontal and vertical distribution and seasonal cycle of CO and key non-methane VOC, such as acetone, methanol, and formaldehyde as compared to observational data from several ground stations and aircraft campaigns. LMDz-INCA in the NMHC version reproduces tropospheric ozone concentrations fairly well throughout most of the troposphere. The model is applied in several sensitivity studies of the biosphere-atmosphere photochemical feedback. The impact of surface emissions of isoprene, acetone, and methanol is studied. These experiments show a substantial impact of isoprene on tropospheric ozone and carbon monoxide concentrations revealing an increase in surface O3 and CO levels of up to 30 ppbv and 60 ppbv, respectively. Isoprene also appears to significantly impact the global OH distribution resulting in a decrease of the global mean tropospheric OH concentration by approximately 0.9×105 molecules cm−3 or roughly 10% and an increase in the global mean tropospheric methane lifetime by approximately four months. A global mean ozone net radiative forcing due to the isoprene induced increase in the tropospheric ozone burden of 0.09W m−2 is found. The key role of isoprene photooxidation in the global tropospheric redistribution of NOx is demonstrated. LMDz-INCA calculates an increase of PAN surface mixing ratios ranging from 75 to 750 pptv and 10 to 250 pptv during northern hemispheric summer and winter, respectively. Acetone and methanol are found to play a significant role in the upper troposphere/lower stratosphere (UT/LS) budget of peroxy radicals. Calculations with LMDz-INCA show an increase in HOx concentrations region of 8 to 15% and 10 to 15% due to methanol and acetone biogenic surface emissions, respectively. The model has been used to estimate the global tropospheric CO budget. A global CO source of 3019 TgCO yr−1 is estimated. This source divides into a primary source of 1533 TgCO yr−1 and secondary source of 1489 TgCO yr−1 deriving from VOC photooxidation. Global VOC-to-CO conversion efficiencies of 90% for methane and between 20 and 45% for individual VOC are calculated by LMDz-INCA.

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 Transport of aerosol pollution in the UTLS during Asian summer monsoon as simulated by ECHAM5-HAMMOZ model

2012 ◽  
Vol 12 (11) ◽  
pp. 30081-30117 ◽  
Author(s):  
S. Fadnavis ◽  
K. Semeniuk ◽  
L. Pozzoli ◽  
M. G. Schultz ◽  
S. D. Ghude ◽  
...  
Keyword(s):  
Summer Monsoon ◽  
Asian Summer Monsoon ◽  
Indian Subcontinent ◽  
Aerosol Layer ◽  
Anthropogenic Aerosols ◽  
Upper Troposphere ◽  
Aerosol Pollution ◽  
Asian Summer ◽  
Cloud Ice ◽  
The Impact

Abstract. An eight member ensemble of ECHAM5-HAMMOZ simulations for the year 2003 is analyzed to study the transport of aerosols in the Upper Troposphere and Lower Stratosphere (UTLS) during the Asian Summer Monsoon (ASM). Simulations show persistent maxima in black carbon, organic carbon, sulfate, and mineral dust aerosols within the anticyclone in the UTLS throughout the ASM (period from July to September) when convective activity over the Indian subcontinent is highest. Model simulations indicate boundary layer aerosol pollution as the source of this UTLS aerosol layer and identify ASM convection as the dominant transport process. Evidence of ASM transport of aerosols into the stratosphere is observed in HALogen Occultation Experiment (HALOE) and Stratospheric Aerosol and Gas Experiment (SAGE) II aerosol extinction. The impact of aerosols in the UTLS region is analyzed by evaluating the differences between simulations with (CTRL) and without aerosol (HAM-off) loading. The transport of anthropogenic aerosols in the UTLS increases cloud ice, water vapour and temperature, indicating that aerosols play an important role in enhancement of cloud ice in the Upper-Troposphere (UT). Aerosol induced circulation changes include a weakening of the main branch of the Hadley circulation and increased vertical transport around the southern flank of the Himalayas and reduction in monsoon precipitation over the India region.

scholarly journals A description and evaluation of an air quality model nested within global and regional composition-climate models using MetUM

2017 ◽  
Author(s):  
Lucy S. Neal ◽  
Mohit Dalvi ◽  
Gerd Folberth ◽  
Rachel N. McInnes ◽  
Paul Agnew ◽  
...  
Keyword(s):  
Air Quality ◽  
Spatial Resolution ◽  
Climate Models ◽  
Climate Model ◽  
Air Quality Model ◽  
Nested Models ◽  
Modelling Framework ◽  
Resolution Model ◽  
The Uk ◽  
The Impact

Abstract. There is a clear need for the development of modelling frameworks for both climate change and air quality to help inform policies for addressing these issues. This paper presents an initial attempt to develop a single modelling framework, by introducing a greater degree of consistency in the modelling framework by using a two-step, one-way nested configuration of models, from a global composition-climate model (GCCM) (140 km resolution) to a regional composition-climate model covering Europe (RCCM) (50 km resolution) and finally to a high (12 km) resolution model over the UK (AQUM). The latter model is used to produce routine air quality forecasts for the UK. All three models are based on the Met Office's Unified Model (MetUM). In order to better understand the impact of resolution on the downscaling of projections of future climate and air quality, we have used this nest of models to simulate a five year period using present-day emissions and under present-day climate conditions. We also consider the impact of running the higher resolution model with higher spatial resolution emissions, rather than simply regridding emissions from the RCCM. We present an evaluation of the models compared to in situ air quality observations over the UK, plus a comparison against an independent 1 km resolution gridded dataset, derived from a combination of modelling and observations. We show that using a high resolution model over the UK has some benefits in improving air quality modelling, but that the use of higher spatial resolution emissions is important to capture local variations in concentrations, particularly for primary pollutants such as nitrogen dioxide and sulphur dioxide. For secondary pollutants such as ozone and the secondary component of PM10, the benefits of a higher resolution nested model are more limited and reasons for this are discussed. This study confirms that the resolution of models is not the only factor in determining model performance - consistency between nested models is also important.

scholarly journals Process-oriented analysis of aircraft soot-cirrus interactions constrains the climate impact of aviation

2021 ◽  
Vol 2 (1) ◽  
Author(s):  
Bernd Kärcher ◽  
Fabian Mahrt ◽  
Claudia Marcolli
Keyword(s):  
Radiative Forcing ◽  
Large Scale ◽  
Climate Models ◽  
Climate Model ◽  
Global Climate ◽  
Climate Impact ◽  
Global Climate Models ◽  
Soot Particles ◽  
Cloud Ice ◽  
The Impact

AbstractFully accounting for the climate impact of aviation requires a process-level understanding of the impact of aircraft soot particle emissions on the formation of ice clouds. Assessing this impact with the help of global climate models remains elusive and direct observations are lacking. Here we use a high-resolution cirrus column model to investigate how aircraft-emitted soot particles, released after ice crystals sublimate at the end of the lifetime of contrails and contrail cirrus, perturb the formation of cirrus. By allying cloud simulations with a measurement-based description of soot-induced ice formation, we find that only a small fraction (<1%) of the soot particles succeeds in forming cloud ice alongside homogeneous freezing of liquid aerosol droplets. Thus, soot-perturbed and homogeneously-formed cirrus fundamentally do not differ in optical depth. Our results imply that climate model estimates of global radiative forcing from interactions between aircraft soot and large-scale cirrus may be overestimates. The improved scientific understanding reported here provides a process-based underpinning for improved climate model parametrizations and targeted field observations.

Sign in / Sign up

Export Citation Format

Share Document