scholarly journals Wintertime radiative effects of black carbon (BC) over Indo-Gangetic Plain as modelled with new BC emission inventoriesin CHIMERE

2020 ◽  
Author(s):  
Sanhita Ghosh ◽  
Shubha Verma ◽  
Jayanarayanan Kuttippurath ◽  
Laurent Menut
Keyword(s):  
Black Carbon ◽  
Climate Model ◽  
Transport Model ◽  
Indian Subcontinent ◽  
Chemical Transport Model ◽  
Surface Cooling ◽  
Gangetic Plain ◽  
Bottom Up ◽  
Radiative Perturbation ◽  
Indo Gangetic Plain

Abstract. To reduce the uncertainty in the black carbon (BC) induced climatic impacts from the global and regional aerosol-climate model simulations, it is a foremost requirement to improve the prediction of modelled BC distribution. And that specifically, over the regions where the atmosphere is loaded with a large amount of BC, e.g., the Indo-Gangetic plain (IGP) in the Indian subcontinent. Here we present the wintertime radiative perturbation due to BC with an efficiently modelled BC distribution over the IGP in a high-resolution (0.1° × 0.1°) chemical transport model, CHIMERE, implementing new BC emission inventories. The model efficiency in simulating the observed BC distribution was examined executing five simulations: Constrained and bottomup (Smog, Cmip, Edgar, Pku) implementing respectively, the recently estimated India-based constrained BC emission and the latest bottom-up BC emissions (India-based: Smog-India, and global: Coupled Model Intercomparison Project phase 6 (CMIP6), Emission Database for Global Atmospheric Research-V4 (EDGAR-V4) and Peking University BC Inventory (PKU)). A low estimated value of the normalised mean bias (NMB) and root mean square error (RMSE) from Constrained estimated BC concentration (NMB: < 17 %) and aerosol optical depth due to BC (BC-AOD) (NMB: 11 %) indicated that simulation with constrained BC emissions in CHIMERE could simulate the distribution of BC pollution over the IGP more efficiently than with the bottom-up. The large BC pollution covering the IGP region comprised of wintertime all-day (daytime) monthly mean BC concentration and BC-AOD from the Constrained, respectively, in the range 14–25 (6–8) µg m−3 and 0.04–0.08, with a strong correlation between the variance in BC emission and simulated BC mass concentration or BC-AOD. Five main hotspot locations were identified in and around Delhi (northern-IGP), Prayagraj (or Allahabad)-Varanasi (central-IGP), Patna-Palamu (upper/lower mideastern-IGP), and Kolkata (eastern-IGP). The wintertime radiative perturbation due to BC aerosols from the Constrained included a wide-spread enhancement in atmospheric radiative warming by 2–3 times and a reduction in surface cooling by 10 %–20 %, with net warming at the top of atmosphere (TOA) of 10–15 W m−2, compared to the atmosphere without BC, for which, a net cooling at the TOA was, although, exhibited. These perturbations were spotted being the strongest around megacities (Kolkata and Delhi), and were inferred as 30 %–50 % lower from the bottomup than the Constrained.

scholarly journals Wintertime direct radiative effects due to black carbon (BC) over the Indo-Gangetic Plain as modelled with new BC emission inventories in CHIMERE

2021 ◽  
Vol 21 (10) ◽  
pp. 7671-7694
Author(s):  
Sanhita Ghosh ◽  
Shubha Verma ◽  
Jayanarayanan Kuttippurath ◽  
Laurent Menut
Keyword(s):  
Black Carbon ◽  
Transport Model ◽  
Eastern Coast ◽  
Emission Inventories ◽  
Surface Cooling ◽  
Gangetic Plain ◽  
Bottom Up ◽  
Bc Aerosols ◽  
Radiative Perturbation ◽  
Indo Gangetic Plain

Abstract. To reduce the uncertainty in climatic impacts induced by black carbon (BC) from global and regional aerosol–climate model simulations, it is a foremost requirement to improve the prediction of modelled BC distribution, specifically over the regions where the atmosphere is loaded with a large amount of BC, e.g. the Indo-Gangetic Plain (IGP) in the Indian subcontinent. Here we examine the wintertime direct radiative perturbation due to BC with an efficiently modelled BC distribution over the IGP in a high-resolution (0.1∘ × 0.1∘) chemical transport model, CHIMERE, implementing new BC emission inventories. The model efficiency in simulating the observed BC distribution was assessed by executing five simulations: Constrained and bottomup (bottomup includes Smog, Cmip, Edgar, and Pku). These simulations respectively implement the recently estimated India-based observationally constrained BC emissions (Constrainedemiss) and the latest bottom-up BC emissions (India-based: Smog-India; global: Coupled Model Intercomparison Project phase 6 – CMIP6, Emission Database for Global Atmospheric Research-V4 – EDGAR-V4, and Peking University BC Inventory – PKU). The mean BC emission flux from the five BC emission inventory databases was found to be considerably high (450–1000 kg km−2 yr−1) over most of the IGP, with this being the highest (> 2500 kg km−2 yr−1) over megacities (Kolkata and Delhi). A low estimated value of the normalised mean bias (NMB) and root mean square error (RMSE) from the Constrained estimated BC concentration (NMB: < 17 %) and aerosol optical depth due to BC (BC-AOD) (NMB: 11 %) indicated that simulations with Constrainedemiss BC emissions in CHIMERE could simulate the distribution of BC pollution over the IGP more efficiently than with bottom-up emissions. The high BC pollution covering the IGP region comprised a wintertime all-day (daytime) mean BC concentration and BC-AOD respectively in the range 14–25 µg m−3 (6–8 µg m−3) and 0.04–0.08 µg m−3 from the Constrained simulation. The simulated BC concentration and BC-AOD were inferred to be primarily sensitive to the change in BC emission strength over most of the IGP (including the megacity of Kolkata), but also to the transport of BC aerosols over megacity Delhi. Five main hotspot locations were identified in and around Delhi (northern IGP), Prayagraj–Allahabad–Varanasi (central IGP), Patna–Palamu (upper, lower, and mideastern IGP), and Kolkata (eastern IGP). The wintertime direct radiative perturbation due to BC aerosols from the Constrained simulation estimated the atmospheric radiative warming (+30 to +50 W m−2) to be about 50 %–70 % larger than the surface cooling. A widespread enhancement in atmospheric radiative warming due to BC by 2–3 times and a reduction in surface cooling by 10 %–20 %, with net warming at the top of the atmosphere (TOA) of 10–15 W m−2, were noticed compared to the atmosphere without BC, for which a net cooling at the TOA was exhibited. These perturbations were the strongest around megacities (Kolkata and Delhi), extended to the eastern coast, and were inferred to be 30 %–50% lower from the bottomup than the Constrained simulation.

Evaluation of emission strength efficacy in simulating black carbon burden with CHIMERE: estimating wintertime radiative effect over Indo-Gangetic Plain

2020 ◽  
Author(s):  
Sanhita Ghosh ◽  
Shubha Verma ◽  
Jayanarayanan Kuttippurath
Keyword(s):  
Black Carbon ◽  
Transport Model ◽  
Indian Subcontinent ◽  
Chemical Transport ◽  
Climate Impacts ◽  
Eastern Coast ◽  
Spatial And Temporal Patterns ◽  
Gangetic Plain ◽  
Bc Aerosols ◽  
Indo Gangetic Plain

&lt;p&gt;Black carbon (BC) aerosols over the Indian subcontinent have been represented inadequately so-far in chemical transport models restricting the accurate assessment of BC-induced climate impacts. The divergence between simulated and measured BC concentration has specifically been reported to be large over the Indo-Gangetic Plain (IGP) during winter when a large BC burden is observed. In this study, we evaluate the BC transport simulations over the IGP in a high resolution (0.1&amp;#186; &amp;#215; 0.1&amp;#186; ) chemical transport model, CHIMERE. We examine the model efficiency to simulate the observed BC distribution executing five sets of simulation experiments: &lt;em&gt;Constrained &lt;/em&gt;and&lt;em&gt; bottomup&lt;/em&gt; (&lt;em&gt;Smog, Pku, Edgar, Cmip&lt;/em&gt;) implementing respectively, the recently estimated India-based constrained BC emission and the latest bottom-up BC emissions (India-based: Smog-India, and global: Coupled Model Intercomparison Project phase 6 (CMIP6), Emission Database for Global Atmospheric Research-V4 (EDGAR-V4) and Peking University BC Inventory (PKU)). The mean BC emission flux over most of the IGP from the five emission datasets is considerably high (450&amp;#8211;1000 kg km&lt;sup&gt;-2&lt;/sup&gt; y&lt;sup&gt;-1&lt;/sup&gt;) with a relatively low divergence obtained for the eastern and upper-mideastern IGP. Evaluation of BC transport simulations shows that the spatial and temporal gradient in the simulated BC concentration from the &lt;em&gt;Constrained &lt;/em&gt;was equivalent to that from the &lt;em&gt;bottomup&lt;/em&gt; and also to that from observations. This indicates that the spatial and temporal patterns of BC concentration are consistently simulated by the model processes. However, the efficacy to simulate BC distribution is commendable for the estimates from &lt;em&gt;Constrained&lt;/em&gt; for which the lowest normalised mean bias (NMB, &lt; 20%) is obtained in comparison to that from the &lt;em&gt;bottomup&lt;/em&gt; (37&amp;#8211;52%). 75&amp;#8211;100% of the observed all-day (daytime) mean BC concentration is simulated most of the times (&gt;80% of the number of stations data) for &lt;em&gt;Constrained&lt;/em&gt;, whereas, this being less frequent (&lt;50%) for the &lt;em&gt;Pku, Smog, Edgar&lt;/em&gt; and poor for &lt;em&gt;Cmip&lt;/em&gt;. The BC-AOD (0.04&amp;#8211;0.08) estimated from the &lt;em&gt;Constrained&lt;/em&gt; is 20&amp;#8211;50% higher than the &lt;em&gt;Pku&lt;/em&gt; and &lt;em&gt;Smog&lt;/em&gt;. Three main hotspot locations comprising of a large value of BC load are identified over the eastern, mideastern, and northern IGP. Assessment of the effect of BC burden on the wintertime radiative perturbation over the IGP shows that the presence of BC aerosols in the atmosphere enhances atmospheric heating by 2&amp;#8211;3 times more compared to that considering atmosphere without BC. Also, a net warming at the top of the atmosphere (TOA) by 10&amp;#8211;17 W m&lt;sup&gt;-&lt;/sup&gt;&lt;sup&gt;2&lt;/sup&gt; is noticed from the &lt;em&gt;Constrained&lt;/em&gt;, with the largest value estimated in and around megacities (Kolkata and Delhi) that extends to the eastern coast. This value is higher by 10&amp;#8211;20% than that from &lt;em&gt;Cmip&lt;/em&gt; over the IGP and by 2&amp;#8211;10% than that from &lt;em&gt;Smog&lt;/em&gt; over Delhi and eastern part of the IGP.&lt;/p&gt;

scholarly journals A global 3-D CTM evaluation of black carbon in the Tibetan Plateau

2014 ◽  
Vol 14 (13) ◽  
pp. 7091-7112 ◽  
Author(s):  
C. He ◽  
Q. B. Li ◽  
K. N. Liou ◽  
J. Zhang ◽  
L. Qi ◽  
...  
Keyword(s):  
Tibetan Plateau ◽  
Black Carbon ◽  
Transport Model ◽  
The Tibetan Plateau ◽  
Emission Inventories ◽  
Chemical Transport Model ◽  
Central Plateau ◽  
Gangetic Plain ◽  
Rural Sites ◽  
Indo Gangetic Plain

Abstract. We systematically evaluate the black carbon (BC) simulations for 2006 over the Tibetan Plateau by a global 3-D chemical transport model (CTM) (GEOS-Chem) driven by GEOS-5 assimilated meteorological fields, using in situ measurements of BC in surface air, BC in snow, and BC absorption aerosol optical depth (AAOD). Using improved anthropogenic BC emission inventories for Asia that account for rapid technology renewal and energy consumption growth (Zhang et al., 2009; Lu et al., 2011) and improved global biomass burning emission inventories that account for small fires (van der Werf et al., 2010; Randerson et al., 2012), we find that model results of both BC in surface air and in snow are statistically in good agreement with observations (biases < 15%) away from urban centers. Model results capture the seasonal variations of the surface BC concentrations at rural sites in the Indo-Gangetic Plain, but the observed elevated values in winter are absent. Modeled surface-BC concentrations are within a factor of 2 of the observations at remote sites. Part of the discrepancy is explained by the deficiencies of the meteorological fields over the complex Tibetan terrain. We find that BC concentrations in snow computed from modeled BC deposition and GEOS-5 precipitation are spatiotemporally consistent with observations (r = 0.85). The computed BC concentrations in snow are a factor of 2–4 higher than the observations at several Himalayan sites because of excessive BC deposition. The BC concentrations in snow are biased low by a factor of 2 in the central plateau, which we attribute to the absence of snow aging in the CTM and strong local emissions unaccounted for in the emission inventories. Modeled BC AAOD is more than a factor of 2 lower than observations at most sites, particularly to the northwest of the plateau and along the southern slopes of the Himalayas in winter and spring, which is attributable in large part to underestimated emissions and the assumption of external mixing of BC aerosols in the model. We find that assuming a 50% increase of BC absorption associated with internal mixing reduces the bias in modeled BC AAOD by 57% in the Indo-Gangetic Plain and the northeastern plateau and to the northeast of the plateau, and by 16% along the southern slopes of the Himalayas and to the northwest of the plateau. Both surface BC concentration and AAOD are strongly sensitive to anthropogenic emissions (from China and India), while BC concentration in snow is especially responsive to the treatment of BC aerosol aging. We find that a finer model resolution (0.5° × 0.667° nested over Asia) reduces the bias in modeled surface-BC concentration from 15 to 2%. The large range and non-homogeneity of discrepancies between model results and observations of BC across the Tibetan Plateau undoubtedly undermine current assessments of the climatic and hydrological impact of BC in the region and thus warrant imperative needs for more extensive measurements of BC, including its concentration in surface air and snow, AAOD, vertical profile and deposition.

scholarly journals A global 3-D CTM evaluation of black carbon in the Tibetan Plateau

2014 ◽  
Vol 14 (6) ◽  
pp. 7305-7354
Author(s):  
C. He ◽  
Q. B. Li ◽  
K. N. Liou ◽  
J. Zhang ◽  
L. Qi ◽  
...  
Keyword(s):  
Tibetan Plateau ◽  
Black Carbon ◽  
Transport Model ◽  
The Tibetan Plateau ◽  
Chemical Transport Model ◽  
Gangetic Plain ◽  
Remote Sites ◽  
Rural Sites ◽  
Indo Gangetic Plain ◽  
Good Agreement

Abstract. We evaluate the black carbon (BC) simulations for 2006 over the Tibetan Plateau by a global 3-D chemical transport model using surface observations of BC in surface air and in snow and BC absorption aerosol optical depth (AAOD). Using updated Asian anthropogenic BC emissions (Lu et al., 2011; Zhang et al., 2009) and global biomass burning emissions (Randerson et al., 2012; van der Werf et al., 2010), model results of both surface BC and BC in snow are statistically in good agreement with observations (biases < 15%). Model results capture the seasonal variation of surface BC concentration, but the observed wintertime high values at rural sites in the Indo-Gangetic Plain are absent in the model. Model results are in general agreement with observations (within a factor of two) at remote sites. Model simulated BC concentrations in snow are spatiotemporally consistent with observations at most sites. We find that modeled BC AAOD are significantly lower than observations to the northwest of the Plateau and along the southern slopes of the Himalayas during winter and spring, reflecting model deficiencies in emissions, topography and BC mixing state. We find that anthropogenic emissions strongly affect surface BC concentration and AAOD, while the BC aging mainly affects BC in snow over the Plateau.

Black carbon sanitary burden in the Indo-Gangetic plain: exposures, risks and mitigation

2020 ◽  
Author(s):  
Shubha Verma ◽  
Sanhita Ghosh ◽  
Olivier Boucher ◽  
Rong Wang ◽  
Laurent Menut ◽  
...  
Keyword(s):  
Black Carbon ◽  
Urban Area ◽  
Transport Model ◽  
Thermal Power ◽  
Surface Concentration ◽  
Population Exposure ◽  
Chemical Transport Model ◽  
Modeling Framework ◽  
Gangetic Plain ◽  
Indo Gangetic Plain

Abstract A large discrepancy between simulated and observed black carbon (BC) surface concentrations over the densely populated Indo-Gangetic plain (IGP) has so far limited our ability to assess the magnitude of BC sanitary impacts in terms of population exposure, morbidity, and mortality. We evaluate these impacts using an integrated modeling framework, including a successfully predicted BC surface concentration in a high-resolution chemical transport model CHIMERE with observationally-constrained BC emissions, combined with consistent health functions for BC. Population exposure to BC is noteworthy, with more than 60 million people identified living over hotspots of BC concentration (wintertime mean > 20 μg m−3). A fraction of 62% of the total cardiovascular diseases mortality (CVM) burden for the megacity is found attributable to wintertime BC exposure. The semi-urban area has 50% of the CVM burden attributable to BC exposure in the total population over the IGP. More than 400 thousand lives can potentially be saved from CVM annually, by implementing prioritized emission reduction from the combustion of domestic biofuel in the semi-urban area, and diesel oil in transportation and coal in thermal power plant and brick kiln industries in megacities.

scholarly journals Sunset–sunrise difference in solar occultation ozone measurements (SAGE II, HALOE, and ACE–FTS) and its relationship to tidal vertical winds

2015 ◽  
Vol 15 (2) ◽  
pp. 829-843 ◽  
Author(s):  
T. Sakazaki ◽  
M. Shiotani ◽  
M. Suzuki ◽  
D. Kinnison ◽  
J. M. Zawodny ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Seasonal Variations ◽  
Climate Model ◽  
Transport Model ◽  
Stratospheric Aerosol ◽  
Data Sets ◽  
Chemical Transport Model ◽  
Latitude Range ◽  
Solar Occultation ◽  
Vertical Winds

Abstract. This paper contains a comprehensive investigation of the sunset–sunrise difference (SSD, i.e., the sunset-minus-sunrise value) of the ozone mixing ratio in the latitude range of 10° S–10° N. SSD values were determined from solar occultation measurements based on data obtained from the Stratospheric Aerosol and Gas Experiment (SAGE) II, the Halogen Occultation Experiment (HALOE), and the Atmospheric Chemistry Experiment–Fourier transform spectrometer (ACE–FTS). The SSD was negative at altitudes of 20–30 km (−0.1 ppmv at 25 km) and positive at 30–50 km (+0.2 ppmv at 40–45 km) for HALOE and ACE–FTS data. SAGE II data also showed a qualitatively similar result, although the SSD in the upper stratosphere was 2 times larger than those derived from the other data sets. On the basis of an analysis of data from the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) and a nudged chemical transport model (the specified dynamics version of the Whole Atmosphere Community Climate Model: SD–WACCM), we conclude that the SSD can be explained by diurnal variations in the ozone concentration, particularly those caused by vertical transport by the atmospheric tidal winds. All data sets showed significant seasonal variations in the SSD; the SSD in the upper stratosphere is greatest from December through February, while that in the lower stratosphere reaches a maximum twice: during the periods March–April and September–October. Based on an analysis of SD–WACCM results, we found that these seasonal variations follow those associated with the tidal vertical winds.

scholarly journals Sunset–sunrise difference in solar occultation ozone measurements (SAGE II, HALOE, and ACE–FTS) and its relationship to tidal vertical winds

2014 ◽  
Vol 14 (11) ◽  
pp. 16043-16083
Author(s):  
T. Sakazaki ◽  
M. Shiotani ◽  
M. Suzuki ◽  
D. Kinnison ◽  
J. M. Zawodny ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Seasonal Variations ◽  
Climate Model ◽  
Transport Model ◽  
Stratospheric Aerosol ◽  
Chemical Transport Model ◽  
Latitude Range ◽  
Solar Occultation ◽  
Vertical Winds ◽  
Chemistry Experiment

Abstract. This paper contains a comprehensive investigation of the sunset–sunrise difference (SSD; i.e., the sunset-minus-sunrise value) of the ozone mixing ratio in the latitude range of 10° S–10° N. SSD values were determined from solar occultation measurements based on data obtained from the Stratospheric Aerosol and Gas Experiment (SAGE) II, the Halogen Occultation Experiment (HALOE), and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). The SSD was negative at altitudes of 20–30 km (–0.1 ppmv at 25 km) and positive at 30–50 km (+0.2 ppmv at 40–45 km) for HALOE and ACE–FTS data. SAGE II data also showed a qualitatively similar result, although the SSD in the upper stratosphere was two times larger than those derived from the other datasets. On the basis of an analysis of data from the Superconducting Submillimeter Limb Emission Sounder (SMILES), and a nudged chemical-transport model (the Specified Dynamics version of the Whole Atmosphere Community Climate Model: SD–WACCM), we conclude that the SSD can be explained by diurnal variations in the ozone concentration, particularly those caused by vertical transport by the atmospheric tidal winds. All datasets showed significant seasonal variations in the SSD; the SSD in the upper stratosphere is greatest from December through February, while that in the lower stratosphere reaches a maximum twice: during the periods March–April and September–October. Based on an analysis of SD–WACCM results, we found that these seasonal variations follow those associated with the tidal vertical winds.

scholarly journals Black Carbon physical and optical properties across northern India during pre-monsoon and monsoon seasons

2019 ◽  
Author(s):  
James Brooks ◽  
Dantong Liu ◽  
James D. Allan ◽  
Paul I. Williams ◽  
Jim Haywood ◽  
...  
Keyword(s):  
Physical Properties ◽  
Black Carbon ◽  
Mixing State ◽  
Atmospheric Measurements ◽  
Core Diameter ◽  
Gangetic Plain ◽  
North West ◽  
North East ◽  
Northern India ◽  
Indo Gangetic Plain

Abstract. Black carbon (BC) is known to have major impacts on both climate and human health, so is therefore of global importance, particularly so in regions close to large populations that have strong sources. The physical properties and mixing state of black carbon containing particles are important determinants in these effects but information is often lacking, particularly in some of the most important regions of the globe. Detailed analysis into the vertical and horizontal BC optical and physical properties across northern India has been carried out using airborne in-situ measurements. The size-resolved mixing state of BC-containing particles was characterised using a single particle soot photometer (SP2). The study focusses on the Indo-Gangetic Plain during the pre-monsoon and monsoon seasons. Data presented are from the UK Facility for Airborne Atmospheric Measurements BAe-146 research aircraft that performed flights during the pre-monsoon (11th and 12th June) and monsoon (30th June to 11th July) seasons of 2016. Over the Indo-Gangetic Plain, BC mass concentrations were greater (1.95 µg/m3) compared to north-west India (1.50 µg/m3) and north-east India (0.70 µg/m3) during the pre-monsoon. Across northern India, two distinct BC modes were recorded; a mode of small BC particles (core diameter 

scholarly journals Attribution of recent increases in atmospheric methane through 3-D inverse modelling

2018 ◽  
Author(s):  
Joe McNorton ◽  
Chris Wilson ◽  
Manuel Gloor ◽  
Rob Parker ◽  
Hartmut Boesch ◽  
...  
Keyword(s):  
Growth Rate ◽  
Transport Model ◽  
Energy Sector ◽  
Total Carbon ◽  
Sensitivity Analyses ◽  
Northern Eurasia ◽  
Atmospheric Methane ◽  
Chemical Transport Model ◽  
Bottom Up ◽  
Source And Sink

Abstract. The atmospheric methane (CH4) growth rate has varied considerably in recent decades. Unexplained renewed growth after 2006 followed seven years of stagnation and coincided with an isotopic trend toward CH4 more depleted in 13C, suggesting changes in sources and/or sinks. Using surface observations of both CH4 and the isotopologue ratio value (δ13CH4) to constrain a global 3D chemical transport model (CTM), we have performed a synthesis inversion for source and sink attribution. Our method extends on previous studies by providing monthly and regional attribution of emissions from 6 different sectors and changes in atmospheric sinks for the extended 2003–2015 period. Regional evaluation of the model CH4 tracer with independent column observations from the Greenhouse gases Observing SATellite (GOSAT) shows improved performance when using posterior fluxes (R = 0.94–0.96, RMSE = 8.3–16.5 ppb), relative to prior fluxes (R = 0.60–0.92, RMSE = 48.6–64.6 ppb). Further independent validation with data from the Total Carbon Column Observing Network (TCCON) shows a similar improvement in the posterior fluxes (R = 0.90, RMSE = 21.4 ppb) compared to the prior (R = 0.71, RMSE = 55.3 ppb). Based on these improved posterior fluxes, the inversion results suggest the most likely cause of the renewed methane growth is a post-2006 1.8 ± 0.4 % decrease in mean OH, a 12.9 ± 2.7 % increase in energy sector emissions, mainly from Africa/Middle East and Southern Asia/Oceania, and a 2.6 ± 1.8 % increase in wetland emissions, mainly from Northern Eurasia. The posterior wetland increases are in general agreement with bottom-up estimates, but the energy sector growth is greater than estimated by bottom-up methods. The model results are consistent across a range of sensitivity analyses performed. When forced to assume a constant (annually repeating) OH distribution, the inversion requires a greater increase in energy sector (13.6 ± 2.7 %) and wetland (3.6 ± 1.8 %) emissions but also introduces an 11.5 ± 3.8 % decrease in biomass burning emissions. Assuming no prior trend in sources and sinks slightly reduces the posterior growth rate in energy sector and wetland emissions and further increases the amplitude of the negative OH trend. We find that possible tropospheric Cl variations do not to influence δ13CH4 and CH4 trends, although we suggest further work on Cl variability is required to fully diagnose this contribution. While the study provides quantitative insight into possible emissions variations which may explain the observed trends, uncertainty in prior source and sink estimates and a paucity of δ13CH4 observations limit the accuracy of the posterior estimates.

Impacts of stratospheric dynamical variability on total inorganic fluorine from observations and models constrained by state-of-the-art reanalyses

2020 ◽  
Author(s):  
Maxime Prignon ◽  
Peter F. Bernath ◽  
Simon Chabrillat ◽  
Martyn P. Chipperfield ◽  
Sandip S. Dhomse ◽  
...  
Keyword(s):  
Time Series ◽  
Fourier Transform ◽  
Atmospheric Chemistry ◽  
Climate Model ◽  
Transport Model ◽  
State Of The Art ◽  
Chemical Transport Model ◽  
Common Time ◽  
Good Proxy ◽  
Circulation Changes

&lt;p&gt;Man-made halogenated compounds emitted from the Earth&amp;#8217;s surface ultimately reach the stratosphere where they undergo photolysis, leading to three main fluorine reservoirs: hydrogen fluoride (HF), carbonyl fluoride (COF&lt;sub&gt;2&lt;/sub&gt;) and carbonyl chloride fluoride (COClF). This process is directly influenced by the strength of the mean meridional circulation of the stratosphere, the Brewer-Dobson Circulation (BDC). The BDC is projected to speed-up with the greenhouse gases induced global warming. However, studies have highlighted a multiyear variability in the strength of the BDC resulting in hemispheric asymmetries in observed and modelled trends of age of air and long-lived tracers.&lt;/p&gt;&lt;p&gt;Total inorganic fluorine (F&lt;sub&gt;y&lt;/sub&gt;, the fluorine weighted sum of HF, COF&lt;sub&gt;2&lt;/sub&gt; and COClF) is used here as a tracer of the stratospheric circulation changes. We perform an analysis and interpretation of Fourier transform infrared (FTIR) multidecadal time-series of HF and COF&lt;sub&gt;2&lt;/sub&gt; from the Jungfraujoch (Switzerland, 46.55&amp;#176;N) and Lauder (New-Zealand, 45.03&amp;#176;S) stations and from the space-borne Atmospheric Chemistry Experiment - Fourier Transform Spectrometer (ACE-FTS). Indeed, the summation of HF and COF&lt;sub&gt;2&lt;/sub&gt; is a very good proxy of F&lt;sub&gt;y &lt;/sub&gt;as we determine, from ACE-FTS and the chemical-transport model (CTM) TOMCAT, that COClF is only accounting for less than 5% of the total F&lt;sub&gt;y &lt;/sub&gt;budget.&lt;/p&gt;&lt;p&gt;The kinematic CTM BASCOE (Belgian assimilation system for chemical observations) is used here to assess the representation of the investigated circulation changes in four state-of-the-art meteorological reanalyses, i.e., ERA-Interim, JRA-55, MERRA and MERRA-2. We also investigate if WACCM4 (Whole Atmosphere Community Climate Model version 4) is able to reproduce these changes through a free-running simulation.&lt;/p&gt;&lt;p&gt;The ground-based and satellite FTIR time-series of COF&lt;sub&gt;2&lt;/sub&gt; show contrasting results over their common time period (2004-2019), with a positive total column trend above the Jungfraujoch, and a non-significant (ground-based) or decreasing trend (ACE-FTS) above Lauder. We find large discrepancies between the BASCOE-CTM simulations, with MERRA-2 inducing overly large simulated F&lt;sub&gt;y&lt;/sub&gt; total columns which could confirm the weaker tropical upwelling highlighted in previous age of air studies.&lt;/p&gt;

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