scholarly journals Bias corrections for speciated and source-resolved PM2.5 chemical transport model simulations using a geographically weighted regression

Author(s):  
Carlos Hernandez ◽  
Ksakousti Skyllakou ◽  
Pablo Garcia Rivera ◽  
Brian Dinkelacker ◽  
Julian Marshall ◽  
...  
2012 ◽  
Vol 12 (15) ◽  
pp. 7073-7085 ◽  
Author(s):  
J. Kuttippurath ◽  
S. Godin-Beekmann ◽  
F. Lefèvre ◽  
G. Nikulin ◽  
M. L. Santee ◽  
...  

Abstract. We present a detailed discussion of the chemical and dynamical processes in the Arctic winters 1996/1997 and 2010/2011 with high resolution chemical transport model (CTM) simulations and space-based observations. In the Arctic winter 2010/2011, the lower stratospheric minimum temperatures were below 195 K for a record period of time, from December to mid-April, and a strong and stable vortex was present during that period. Simulations with the Mimosa-Chim CTM show that the chemical ozone loss started in early January and progressed slowly to 1 ppmv (parts per million by volume) by late February. The loss intensified by early March and reached a record maximum of ~2.4 ppmv in the late March–early April period over a broad altitude range of 450–550 K. This coincides with elevated ozone loss rates of 2–4 ppbv sh−1 (parts per billion by volume/sunlit hour) and a contribution of about 30–55% and 30–35% from the ClO-ClO and ClO-BrO cycles, respectively, in late February and March. In addition, a contribution of 30–50% from the HOx cycle is also estimated in April. We also estimate a loss of about 0.7–1.2 ppmv contributed (75%) by the NOx cycle at 550–700 K. The ozone loss estimated in the partial column range of 350–550 K exhibits a record value of ~148 DU (Dobson Unit). This is the largest ozone loss ever estimated in the Arctic and is consistent with the remarkable chlorine activation and strong denitrification (40–50%) during the winter, as the modeled ClO shows ~1.8 ppbv in early January and ~1 ppbv in March at 450–550 K. These model results are in excellent agreement with those found from the Aura Microwave Limb Sounder observations. Our analyses also show that the ozone loss in 2010/2011 is close to that found in some Antarctic winters, for the first time in the observed history. Though the winter 1996/1997 was also very cold in March–April, the temperatures were higher in December–February, and, therefore, chlorine activation was moderate and ozone loss was average with about 1.2 ppmv at 475–550 K or 42 DU at 350–550 K, as diagnosed from the model simulations and measurements.


2011 ◽  
Vol 11 (24) ◽  
pp. 12773-12786 ◽  
Author(s):  
S. Dhomse ◽  
M. P. Chipperfield ◽  
W. Feng ◽  
J. D. Haigh

Abstract. We have used an off-line 3-D chemical transport model (CTM) to investigate the 11-yr solar cycle response in tropical stratospheric ozone. The model is forced with European Centre for Medium-Range Weather Forecasts (ECMWF) (re)analysis (ERA-40/operational and ERA-Interim) data for the 1979–2005 time period. We have compared the modelled solar response in ozone to observation-based data sets that are constructed using satellite instruments such as Total Ozone Mapping Spectrometer (TOMS), Solar Backscatter UltraViolet instrument (SBUV), Stratospheric Aerosol and Gas Experiment (SAGE) and Halogen Occultation Experiment (HALOE). A significant difference is seen between simulated and observed ozone during the 1980s, which is probably due to inhomogeneities in the ERA-40 reanalyses. In general, the model with ERA-Interim dynamics shows better agreement with the observations from 1990 onwards than with ERA-40. Overall both standard model simulations are partially able to simulate a "double peak"-structured ozone solar response with a minimum around 30 km, and these are in better agreement with HALOE than SAGE-corrected SBUV (SBUV/SAGE) or SAGE-based data sets. In the tropical lower stratosphere (TLS), the modelled solar response with time-varying aerosols is amplified through aliasing with a volcanic signal, as the model overestimates ozone loss during high aerosol loading years. However, the modelled solar response with fixed dynamics and constant aerosols shows a positive signal which is in better agreement with SBUV/SAGE and SAGE-based data sets in the TLS. Our model simulations suggests that photochemistry contributes to the ozone solar response in this region. The largest model-observation differences occur in the upper stratosphere where SBUV/SAGE and SAGE-based data show a significant (up to 4%) solar response whereas the standard model and HALOE do not. This is partly due to a positive solar response in the ECMWF upper stratospheric temperatures which reduces the modelled ozone signal. The large positive upper stratospheric solar response seen in SBUV/SAGE and SAGE-based data can be reproduced in model runs with fixed dynamical fields (i.e. no inter-annual meteorological changes). As these runs effectively assume no long-term temperature changes (solar-induced or otherwise), it should provide an upper limit of the ozone solar response. Overall, full quantification of the solar response in stratospheric ozone is limited by differences in the observed data sets and by uncertainties in the solar response in stratospheric temperatures.


2010 ◽  
Vol 10 (11) ◽  
pp. 26361-26410 ◽  
Author(s):  
H. Sodemann ◽  
M. Pommier ◽  
S. R. Arnold ◽  
S. A. Monks ◽  
K. Stebel ◽  
...  

Abstract. During the POLARCAT summer campaign in 2008, two episodes (2–5 July and 7–10 July 2008) occurred where low-pressure systems traveled from Siberia across the Arctic Ocean towards the North Pole. The two cyclones had extensive smoke plumes embedded in their associated air masses, creating an excellent opportunity to use satellite and aircraft observations to validate the performance of atmospheric transport models in the Arctic, which is a challenging model domain due to numerical and other complications. Here we compare transport simulations of carbon monoxide (CO) from the Lagrangian transport model FLEXPART, the Eulerian chemical transport model TOMCAT, and for numerical aspects the limited-area chemical transport model WRF-Chem. Retrievals of total column CO from the IASI passive infrared sensor onboard the MetOp-A satellite are used as a total column CO reference for the two simulations. Main aspect of the comparison is how realistic horizontal and vertical structures are represented in the model simulations. Analysis of CALIPSO lidar curtains and in situ aircraft measurements provide further independent reference points to assess how reliable the model simulations are and what the main limitations are. The horizontal structure of mid-latitude pollution plumes agrees well between the IASI total column CO and the model simulations. However, finer-scale structures are too quickly diffused in the Eulerian models. Aircraft data suggest that the satellite data are biased high, while TOMCAT and WRF-Chem are biased low. FLEXPART fits the aircraft data rather well, but due to added background concentrations the simulation is not independent from observations. The multi-data, multi-model approach allows separating the influences of meteorological fields, model realisation, and grid type on the plume structure. In addition to the very good agreement between simulated and observed total column CO fields, the results also highlight the difficulty to identify a data set that most realistically represents the actual state of the atmosphere.


2012 ◽  
Vol 12 (3) ◽  
pp. 6877-6908
Author(s):  
J. Kuttippurath ◽  
S. Godin-Beekmann ◽  
F. Lefèvre ◽  
G. Nikulin ◽  
M. L. Santee ◽  
...  

Abstract. We present a detailed discussion of the chemical and dynamical processes in the Arctic winters 1996/1997 and 2010/2011 with high resolution chemical transport model (CTM) simulations and space-based observations. In the Arctic winter 2010/2011, the lower stratospheric minimum temperatures were below 195 K for a record period, from December to mid-April, and a strong and stable vortex was present during that period. Analyses with the Mimosa-Chim CTM simulations show that the chemical ozone loss started by early January and progressed slowly to 1 ppmv (parts per million by volume) by late February. The loss intensified by early March and reached a record maximum of ~2.4 ppmv in the late March–early April period over a broad altitude range of 450–550 K. This coincides with elevated ozone loss rates of 2–4 ppbv sh−1 (parts per billion by volume/sunlit hour) and a contribution of about 40% from the ClO–ClO cycle and about 35–40% from the ClO-BrO cycle in late February and March, and about 30–50% from the HOx cycle in April. We also estimate a loss of around 0.7–1.2 ppmv contributed (75%) by the NOx cycle at 550–700 K. The ozone loss estimated in the partial column range of 350–550 K also exhibits a record value of ~148 DU (Dobson Unit). This is the largest ozone loss ever estimated in the Arctic and is consistent with the remarkable chlorine activation and strong denitrification (40–50%) during the winter, as the modeled ClO shows ~1.8 ppbv in early January and ~1 ppbv in March at 450–550 K. These model results are in excellent agreement with those found from the Aura Microwave Limb Sounder observations. Our analyses also show that the ozone loss in 2010/2011 is close to that found in some Antarctic winters, for the first time in the observed history. Though the winter 1996/1997 was also very cold in March–April, the temperatures were higher in December–February, and, therefore, chlorine activation was moderate and ozone loss was average with about 1.2 ppmv at 475–550 K or 42 DU at 350–550 K, as diagnosed from the model simulations and measurements.


Urban Climate ◽  
2019 ◽  
Vol 27 ◽  
pp. 293-313 ◽  
Author(s):  
Dirce Maria Pellegatti Franco ◽  
Maria de Fatima Andrade ◽  
Rita Yuri Ynoue ◽  
Jason Ching

2004 ◽  
Vol 4 (1) ◽  
pp. 507-532 ◽  
Author(s):  
J. Ma ◽  
J. A. van Aardenne

Abstract. The importance of emission inventory uncertainty on the simulation of summertime tropospheric Ozone over China has been analyzed using a regional chemical transport model. Three independent emissions inventories, that are (i) emission estimates from the Emission Database for Global Atmospheric Research (EDGAR) for the year 1995, (ii) a regional emission inventory used in the Transport and Chemical Evolution over the Pacific (TRACE-P) program with emissions for the year 2000 and (iii) a national emission inventory used in the China Ozone Research Program (CORP) with emission estimates for the year 1995, are used for model simulation over a summer period. Methods used for the development of the inventories are discussed and differences in simulated ozone and its precursors with these emission inventories are analyzed. Comparison of the emission inventories revealed large differences in the emission estimates (up to 50% for NOx, ~100% for NMVOC and ~1000% for CO). Application of the different emission inventories in three model simulations showed minor differences in both surface O3 in rather unpolluted areas in China and at higher altitudes (500 mbar). In polluted areas, differences in surface O3 are 30-50% between the different model simulations which seems rather small taking into account the large differences in the emission inventories. Additional sensitivity runs showed that the difference in NOx emissions as well NMVOC emissions is a dominant factor which controls the differences in simulated O3 concentrations while the impact of differences in CO emissions is relatively small. Although the CO emission estimate by CORP seems to be underestimated, there is no confidence to highlight one emission inventory better than the others.


2008 ◽  
Vol 8 (5) ◽  
pp. 17581-17629
Author(s):  
N. Theys ◽  
M. Van Roozendael ◽  
Q. Errera ◽  
F. Hendrick ◽  
F. Daerden ◽  
...  

Abstract. A new climatology of stratospheric BrO profiles based on dynamical and chemical indicators has been developed, with the aim to apply it to the retrieval of tropospheric BrO columns from space nadir measurements. The suitability of the adopted parameterization is evaluated based on three years of output data from the 3-D chemistry transport model BASCOE. The impact of the atmospheric dynamics on the stratospheric BrO distribution is treated by means of Bry/ozone correlations build from 3-D-CTM model results, while photochemical effects are taken into account using stratospheric NO2 columns as an indicator of the BrO/Bry ratio. The model simulations have been optimized for bromine chemistry and budget, and validated through comparisons using an extensive data set of ground-based, balloon-borne and satellite limb (SCIAMACHY) stratospheric BrO observations.


Sign in / Sign up

Export Citation Format

Share Document