Improving ozone forecasts over Europe by synergistic use of the LOTOS-EUROS chemical transport model and in-situ measurements

2012 ◽  
Vol 60 ◽  
pp. 217-226 ◽  
Author(s):  
R.L. Curier ◽  
R. Timmermans ◽  
S. Calabretta-Jongen ◽  
H. Eskes ◽  
A. Segers ◽  
...  
Keyword(s):  
Transport Model ◽  
Chemical Transport ◽  
In Situ Measurements ◽  
Chemical Transport Model

scholarly journals Retrieval of total column and surface NO<sub>2</sub> from Pandora zenith-sky measurements

2019 ◽  
Author(s):  
Xiaoyi Zhao ◽  
Debora Griffin ◽  
Vitali Fioletov ◽  
Chris McLinden ◽  
Jonathan Davies ◽  
...  
Keyword(s):  
Transport Model ◽  
Surface Concentration ◽  
In Situ Measurements ◽  
Radiative Transfer Model ◽  
Retrieval Algorithm ◽  
Transfer Model ◽  
Chemical Transport Model ◽  
High Quality ◽  
Vertical Column

Abstract. Pandora spectrometers can retrieve nitrogen dioxide (NO2) vertical column densities (VCDs) via two viewing geometries: direct-sun and zenith-sky. The direct-sun NO2 VCD measurements have high quality (0.1 DU accuracy in clear-sky conditions) and do not rely on any radiative transfer model to calculate air mass factors (AMFs); however, they are not available when the sun is obscured by clouds. To perform NO2 measurements in cloudy conditions, a simple but robust NO2 retrieval algorithm is developed for Pandora zenith-sky measurements. This algorithm derives empirical zenith-sky NO2 AMFs from coincident high-quality direct-sun NO2 observations. Moreover, the retrieved Pandora zenith-sky NO2 VCD data are converted to surface NO2 concentrations with a scaling algorithm that uses chemical-transport-model predictions and satellite measurements as inputs. NO2 VCDs and surface concentrations are retrieved from Pandora zenith-sky measurements made in Toronto, Canada, from 2015 to 2017. The retrieved Pandora zenith-sky NO2 data (VCD and surface concentration) show good agreement with both satellite and in situ measurements. The diurnal and seasonal variations of derived Pandora zenith-sky surface NO2 data also agree well with in situ measurements (diurnal difference within ±2 ppbv). Overall, this work shows that the new Pandora zenith-sky NO2 products have the potential to be used in various applications such as future satellite validation in moderate cloudy scenes and air quality monitoring.

scholarly journals On the ability of chemical transport models to simulate the vertical structure of the N<sub>2</sub>O, NO<sub>2</sub> and HNO<sub>3</sub> species in the mid-latitude stratosphere

2005 ◽  
Vol 5 (6) ◽  
pp. 12373-12401
Author(s):  
G. Berthet ◽  
N. Huret ◽  
F. Lefèvre ◽  
G. Moreau ◽  
C. Robert ◽  
...  
Keyword(s):  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Transport Models ◽  
One Dimensional ◽  
Chemical Transport Models ◽  
Dimensional Version ◽  
The Impact

Abstract. In this paper we study the impact of the modelling of N2O on the simulation of NO2 and HNO3 by comparing in situ vertical profiles measured at mid-latitudes with the results of the Reprobus 3-D CTM (Three-dimensional Chemical Transport Model) computed with the kinetic parameters from the JPL recommendation in 2002. The analysis of the measured in situ profile of N2O shows particular features indicating different air mass origins. The measured N2O, NO2 and HNO3 profiles are not satisfyingly reproduced by the CTM when computed using the current 6-hourly ECMWF operational analysis. Improving the simulation of N2O transport allows us to calculate quantities of NO2 and HNO3 in reasonable agreement with observations. This is achieved using 3-hourly winds obtained from ECMWF forecasts. The best agreement is obtained by constraining a one-dimensional version of the model with the observed N2O. This study shows that modelling the NOy partitioning with better accuracy relies at least on a correct simulation of N2O and thus of total NOy.

scholarly journals Evaluation of the LOTOS-EUROS NO<sub>2</sub> simulations using ground-based measurements and S5P/TROPOMI observations over Greece

2021 ◽  
Vol 21 (7) ◽  
pp. 5269-5288
Author(s):  
Ioanna Skoulidou ◽  
Maria-Elissavet Koukouli ◽  
Astrid Manders ◽  
Arjo Segers ◽  
Dimitris Karagkiozidis ◽  
...  
Keyword(s):  
Spatial Correlation ◽  
Extreme Values ◽  
Transport Model ◽  
Chemical Transport ◽  
Pollution Monitoring ◽  
Optical Absorption Spectroscopy ◽  
Chemical Transport Model ◽  
Night Time ◽  
Tropospheric No2

Abstract. The evaluation of chemical transport models, CTMs, is essential for the assessment of their performance regarding the physical and chemical parameterizations used. While regional CTMs have been widely used and evaluated over Europe, their validation over Greece is limited. In this study, we investigate the performance of the Long Term Ozone Simulation European Operational Smog (LOTOS-EUROS) v2.2.001 regional chemical transport model in simulating nitrogen dioxide, NO2, over Greece from June to December 2018. In situ NO2 measurements obtained from 14 stations of the National Air Pollution Monitoring Network are compared with surface simulations over the two major cities of Greece, Athens and Thessaloniki. Overall the LOTOS-EUROS NO2 surface simulations compare very well to the in situ measurements showing a mild underestimation of the measurements with a mean relative bias of ∼-10 %, a high spatial correlation coefficient of 0.86 and an average temporal correlation of 0.52. The CTM underestimates the NO2 surface concentrations during daytime by ∼-50 ± 15 %, while it slightly overestimates during night-time ∼ 10 ± 35 %. Furthermore, the LOTOS-EUROS tropospheric NO2 columns are evaluated against ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) NO2 measurements in Athens and Thessaloniki. We report that the CTM tropospheric NO2 column simulations over both urban and rural locations represent the diurnal patterns and hourly levels for both summer and winter seasons satisfactorily. The relative biases range between ∼ −2 % and −35 %, depending on season and relative NO2 load observed. Finally, the CTM was assessed also against space-borne Sentinel-5 Precursor (S5P) carrying the Tropospheric Monitoring Instrument (TROPOMI) tropospheric NO2 observations. We conclude that LOTOS-EUROS simulates extremely well the tropospheric NO2 patterns over the region with very high spatial correlation of 0.82 on average, ranging between 0.66 and 0.95, with negative biases in the summer and positive in the winter. Updated emissions for the simulations and model improvements when extreme values of boundary layer height are encountered are further suggested.

scholarly journals Retrieval of total column and surface NO<sub>2</sub> from Pandora zenith-sky measurements

2019 ◽  
Vol 19 (16) ◽  
pp. 10619-10642 ◽  
Author(s):  
Xiaoyi Zhao ◽  
Debora Griffin ◽  
Vitali Fioletov ◽  
Chris McLinden ◽  
Jonathan Davies ◽  
...  
Keyword(s):  
Transport Model ◽  
Surface Concentration ◽  
In Situ Measurements ◽  
Radiative Transfer Model ◽  
Retrieval Algorithm ◽  
Transfer Model ◽  
Chemical Transport Model ◽  
High Quality ◽  
Vertical Column

Abstract. Pandora spectrometers can retrieve nitrogen dioxide (NO2) vertical column densities (VCDs) via two viewing geometries: direct Sun and zenith sky. The direct-Sun NO2 VCD measurements have high quality (0.1 DU accuracy in clear-sky conditions) and do not rely on any radiative transfer model to calculate air mass factors (AMFs); however, they are not available when the Sun is obscured by clouds. To perform NO2 measurements in cloudy conditions, a simple but robust NO2 retrieval algorithm is developed for Pandora zenith-sky measurements. This algorithm derives empirical zenith-sky NO2 AMFs from coincident high-quality direct-Sun NO2 observations. Moreover, the retrieved Pandora zenith-sky NO2 VCD data are converted to surface NO2 concentrations with a scaling algorithm that uses chemical-transport-model predictions and satellite measurements as inputs. NO2 VCDs and surface concentrations are retrieved from Pandora zenith-sky measurements made in Toronto, Canada, from 2015 to 2017. The retrieved Pandora zenith-sky NO2 data (VCD and surface concentration) show good agreement with both satellite and in situ measurements. The diurnal and seasonal variations of derived Pandora zenith-sky surface NO2 data also agree well with in situ measurements (diurnal difference within ±2 ppbv). Overall, this work shows that the new Pandora zenith-sky NO2 products have the potential to be used in various applications such as future satellite validation in moderate cloudy scenes and air quality monitoring.

scholarly journals Contributions of the troposphere and stratosphere to CH<sub>4</sub> model biases

2017 ◽  
Vol 17 (21) ◽  
pp. 13283-13295 ◽  
Author(s):  
Zhiting Wang ◽  
Thorsten Warneke ◽  
Nicholas M. Deutscher ◽  
Justus Notholt ◽  
Ute Karstens ◽  
...  
Keyword(s):  
Latitudinal Gradient ◽  
Transport Model ◽  
In Situ Measurements ◽  
Model Bias ◽  
Chemical Transport Model ◽  
Fourier Transform Spectrometry ◽  
Model Biases ◽  
Inverse Models ◽  
Total Column

Abstract. Inverse modelling is a useful tool for retrieving CH4 fluxes; however, evaluation of the applied chemical transport model is an important step before using the inverted emissions. For inversions using column data one concern is how well the model represents stratospheric and tropospheric CH4 when assimilating total column measurements. In this study atmospheric CH4 from three inverse models is compared to FTS (Fourier transform spectrometry), satellite and in situ measurements. Using the FTS measurements the model biases are separated into stratospheric and tropospheric contributions. When averaged over all FTS sites the model bias amplitudes (absolute model to FTS differences) are 7.4 ± 5.1, 6.7 ± 4.8, and 8.1 ± 5.5 ppb in the tropospheric partial column (the column from the surface to the tropopause) for the models TM3, TM5-4DVAR, and LMDz-PYVAR, respectively, and 4.3 ± 9.9, 4.7 ± 9.9, and 6.2 ± 11.2 ppb in the stratospheric partial column (the column from the tropopause to the top of the atmosphere). The model biases in the tropospheric partial column show a latitudinal gradient for all models; however there are no clear latitudinal dependencies for the model biases in the stratospheric partial column visible except with the LMDz-PYVAR model. Comparing modelled and FTS-measured tropospheric column-averaged mole fractions reveals a similar latitudinal gradient in the model biases but comparison with in situ measured mole fractions in the troposphere does not show a latitudinal gradient, which is attributed to the different longitudinal coverage of FTS and in situ measurements. Similarly, a latitudinal pattern exists in model biases in vertical CH4 gradients in the troposphere, which indicates that vertical transport of tropospheric CH4 is not represented correctly in the models.

scholarly journals Global evaluation of ammonia bidirectional exchange and livestock diurnal variation schemes

2015 ◽  
Vol 15 (22) ◽  
pp. 12823-12843 ◽  
Author(s):  
L. Zhu ◽  
D. Henze ◽  
J. Bash ◽  
G.-R. Jeong ◽  
K. Cady-Pereira ◽  
...  
Keyword(s):  
Transport Model ◽  
In Situ Measurements ◽  
Global Evaluation ◽  
Chemical Transport Model ◽  
Southeastern China ◽  
Surface Exchange ◽  
Diurnal Variability ◽  
Fertilizer Application Rate ◽  
Bidirectional Exchange

Abstract. Bidirectional air–surface exchange of ammonia (NH3) has been neglected in many air quality models. In this study, we implement the bidirectional exchange of NH3 in the GEOS-Chem global chemical transport model. We also introduce an updated diurnal variability scheme for NH3 livestock emissions and evaluate the recently developed MASAGE_NH3 bottom-up inventory. While updated diurnal variability improves comparison of modeled-to-hourly in situ measurements in the southeastern USA, NH3 concentrations decrease throughout the globe, up to 17 ppb in India and southeastern China, with corresponding decreases in aerosol nitrate by up to 7 μg m−3. The ammonium (NH4+) soil pool in the bidirectional exchange model largely extends the NH3 lifetime in the atmosphere. Including bidirectional exchange generally increases NH3 gross emissions (7.1 %) and surface concentrations (up to 3.9 ppb) throughout the globe in July, except in India and southeastern China. In April and October, it decreases NH3 gross emissions in the Northern Hemisphere (e.g., 43.6 % in April in China) and increases NH3 gross emissions in the Southern Hemisphere. Bidirectional exchange does not largely impact NH4+ wet deposition overall. While bidirectional exchange is fundamentally a better representation of NH3 emissions from fertilizers, emissions from primary sources are still underestimated and thus significant model biases remain when compared to in situ measurements in the USA. The adjoint of bidirectional exchange has also been developed for the GEOS-Chem model and is used to investigate the sensitivity of NH3 concentrations with respect to soil pH and fertilizer application rate. This study thus lays the groundwork for future inverse modeling studies to more directly constrain these physical processes rather than tuning bulk unidirectional NH3 emissions.

scholarly journals On the ability of chemical transport models to simulate the vertical structure of the N<sub>2</sub>O, NO<sub>2</sub> and HNO<sub>3</sub> species in the mid-latitude stratosphere

2006 ◽  
Vol 6 (6) ◽  
pp. 1599-1609 ◽  
Author(s):  
G. Berthet ◽  
N. Huret ◽  
F. Lefèvre ◽  
G. Moreau ◽  
C. Robert ◽  
...  
Keyword(s):  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Transport Models ◽  
One Dimensional ◽  
Chemical Transport Models ◽  
Dimensional Version ◽  
The Impact

Abstract. In this paper we study the impact of the modelling of N2O on the simulation of NO2 and HNO3 by comparing in situ vertical profiles measured at mid-latitudes with the results of the Reprobus 3-D CTM (Three-dimensional Chemical Transport Model) computed with the kinetic parameters from the JPL recommendation in 2002. The analysis of the measured in situ profile of N2O shows particular features indicating different air mass origins. The measured N2O, NO2 and HNO3 profiles are not satisfyingly reproduced by the CTM when computed using the current 6-hourly ECMWF operational analysis. Improving the simulation of N2O transport allows us to calculate quantities of NO2 and HNO3 in reasonable agreement with observations. This is achieved using 3-hourly winds obtained from ECMWF forecasts. The best agreement is obtained by constraining a one-dimensional version of the model with the observed N2O. This study shows that the modelling of the NOy partitioning with better accuracy relies at least on a correct simulation of N2O and thus of total NOy.

scholarly journals Evaluation of modeling NO<sub>2</sub> concentrations driven by satellite-derived and bottom-up emission inventories using in situ measurements over China

2018 ◽  
Vol 18 (6) ◽  
pp. 4171-4186 ◽  
Author(s):  
Fei Liu ◽  
Ronald J. van der A ◽  
Henk Eskes ◽  
Jieying Ding ◽  
Bas Mijling
Keyword(s):  
Spatial Correlation ◽  
Rural Areas ◽  
Urban Areas ◽  
Transport Model ◽  
Chemical Transport ◽  
In Situ Measurements ◽  
Nox Emissions ◽  
Emission Inventories ◽  
Bottom Up

Abstract. Chemical transport models together with emission inventories are widely used to simulate NO2 concentrations over China, but validation of the simulations with in situ measurements has been extremely limited. Here we use ground measurements obtained from the air quality monitoring network recently developed by the Ministry of Environmental Protection of China to validate modeling surface NO2 concentrations from the CHIMERE regional chemical transport model driven by the satellite-derived DECSO and the bottom-up MIX emission inventories. We applied a correction factor to the observations to account for the interferences of other oxidized nitrogen compounds (NOz), based on the modeled ratio of NO2 to NOz. The model accurately reproduces the spatial variability in NO2 from in situ measurements, with a spatial correlation coefficient of over 0.7 for simulations based on both inventories. A negative and positive bias is found for the simulation with the DECSO (slope  =  0.74 and 0.64 for the daily mean and daytime only) and the MIX (slope  =  1.3 and 1.1) inventories, respectively, suggesting an underestimation and overestimation of NOx emissions from corresponding inventories. The bias between observed and modeled concentrations is reduced, with the slope dropping from 1.3 to 1.0 when the spatial distribution of NOx emissions in the DECSO inventory is applied as the spatial proxy for the MIX inventory, which suggests an improvement of the distribution of emissions between urban and suburban or rural areas in the DECSO inventory compared to that used in the bottom-up inventory. A rough estimate indicates that the observed concentrations, from sites predominantly placed in the populated urban areas, may be 10–40 % higher than the corresponding model grid cell mean. This reduces the estimate of the negative bias of the DECSO-based simulation to the range of −30 to 0 % on average and more firmly establishes that the MIX inventory is biased high over major cities. The performance of the model is comparable over seasons, with a slightly worse spatial correlation in summer due to the difficulties in resolving the more active NOx photochemistry and larger concentration gradients in summer by the model. In addition, the model well captures the daytime diurnal cycle but shows more significant disagreement between simulations and measurements during nighttime, which likely produces a positive model bias of about 15 % in the daily mean concentrations. This is most likely related to the uncertainty in vertical mixing in the model at night.

scholarly journals Evaluation of modelling NO<sub>2</sub> concentrations driven by satellite-derived and bottom-up emission inventories using in-situ measurements over China

2017 ◽  
Author(s):  
Fei Liu ◽  
Ronald J. van der A ◽  
Henk Eskes ◽  
Jieying Ding ◽  
Bas Mijling
Keyword(s):  
Spatial Correlation ◽  
Rural Areas ◽  
Urban Areas ◽  
Transport Model ◽  
Chemical Transport ◽  
In Situ Measurements ◽  
Nox Emissions ◽  
Emission Inventories ◽  
Bottom Up

Abstract. Chemical transport models together with emission inventories are widely used to simulate NO2 concentrations over China, but validation of the simulations with in situ measurements has been extremely limited. Here we use ground measurements obtained from the air quality monitoring network recently developed by the Ministry of Environmental Protection of China to validate modelling surface NO2 concentrations from the CHIMERE regional chemical-transport model driven by the satellite-derived DECSO and the bottom-up MIX emission inventories. We applied a correction factor to the observations to account for the interferences of other oxidized nitrogen compounds (NOz), based on the modelled ratio of NO2 to NOz. The model accurately reproduces the spatial variability of NO2 from in-situ measurements, with a spatial correlation coefficient of over 0.7 for simulations based on both inventories. A negative and positive bias is found for the simulation with the DECSO (slope = 0.74/0.64 for the daily-mean/daytime only) and the MIX (slope = 1.3/1.1) inventory respectively, suggesting an underestimation and overestimation of NOx emissions from corresponding inventories. The bias between observed and modelled concentrations is reduced with the slope dropping from 1.3 to 1.0 when the spatial distribution of NOx emissions in the DECSO inventory is applied as the spatial proxy for the MIX inventory, which suggests an improvement of the distribution of emissions between urban and suburban/rural areas in the DECSO inventory compared to that used in the bottom-up inventory. A rough estimate indicates that the observed concentrations, from sites predominantly placed in the populated urban areas, may be 10–40 % higher than the corresponding model grid-cell mean. This reduces the estimate of the negative bias of the DECSO based simulation to the range of −30 % to 0 % on average, and establishes more firmly that the MIX inventory is biased high over major cities. The performance of the model is comparable over seasons, with a slightly worse spatial correlation in summer, due to the difficulties in resolving the more active NOx photochemistry and larger concentration gradients in summer by the model. In addition, the model well captures the daytime diurnal cycle, but shows more significant disagreement between simulations and measurements during night time, which likely produces a positive model bias of about 15 % in the daily mean concentrations. This is most likely related to the uncertainty in vertical mixing in the model at night.

scholarly journals Contributions of the troposphere and stratosphere to CH<sub>4</sub> model biases

2016 ◽  
Author(s):  
Zhiting Wang ◽  
Thorsten Warneke ◽  
Nicholas Deutscher ◽  
Justus Notholt ◽  
Ute Karsten ◽  
...  
Keyword(s):  
Latitudinal Gradient ◽  
Transport Model ◽  
In Situ Measurements ◽  
Model Bias ◽  
Chemical Transport Model ◽  
Fourier Transform Spectrometry ◽  
Model Biases ◽  
Inverse Models ◽  
Total Column

Abstract. Inverse modeling is a useful tool to retrieve CH4 fluxes; however, evaluation of the applied chemical transport model is an important step before using the inverted emissions. For inversions using column data one concern is how well the model represents stratospheric and tropospheric CH4 respectively when assimilating total column measurements. In this study atmospheric CH4 from three inverse models is compared to FTS (Fourier Transform Spectrometry), satellite and in situ measurements. Using the FTS measurements the model biases are separated into stratospheric and tropospheric contributions. When averaged over all FTS sites the model bias amplitudes (absolute model to FTS differences) are 7.4 ± 5.1 ppb, 6.7 ± 4.8 ppb, and 8.1 ± 5.5 ppb in the troposphere for the models TM3, TM5-4DVAR, LMDz-PYVAR, respectively, and 4.3 ± 9.9 ppb, 4.7 ± 9.9 ppb, and 6.2 ± 11.2 ppb in the stratosphere. The tropospheric model biases show a latitudinal gradient for all models, however there are no clear latitudinal dependencies for stratospheric model biases visible except with the LMDz-PYVAR model. The latitudinal gradient is not present in a comparison with in situ measurements, which is attributed to the different longitudinal coverage of FTS and in situ measurements. Similarly, a latitudinal pattern exists in model biases in vertical CH4 gradients in the troposphere, which indicates vertical transports of tropospheric CH4 is not represented correctly in the models.

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