scholarly journals Global evaluation of ammonia bi-directional exchange

2015 ◽  
Vol 15 (4) ◽  
pp. 4823-4877 ◽  
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 ◽  
Southeastern Us ◽  
Fertilizer Application Rate

Abstract. Bi-directional air–surface exchange of ammonia (NH3) has been neglected in many air quality models. In this study, we implement the bi-directional 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 US, 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 bi-directional exchange model largely extends the NH3 lifetime in the atmosphere. Including bi-directional 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. Bi-directional exchange does not largely impact NH4+ wet deposition overall. While bi-directional 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 US. The adjoint of bi-directional 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 uni-directional NH3 emissions.

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 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 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.

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 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.

The Carbon:²³⁴Thorium ratios of sinking particles in the California Current Ecosystem 2: Examination of a thorium sorption, desorption, and particle transport model

2019 ◽  
Author(s):  
Michael Stukel ◽  
Thomas Kelly
Keyword(s):  
Organic Carbon ◽  
Water Column ◽  
Particulate Organic Carbon ◽  
Transport Model ◽  
California Current ◽  
In Situ Measurements ◽  
Power Law Distribution ◽  
Sinking Particles ◽  
Organic Carbon Concentration

Thorium-234 (234Th) is a powerful tracer of particle dynamics and the biological pump in the surface ocean; however, variability in carbon:thorium ratios of sinking particles adds substantial uncertainty to estimates of organic carbon export. We coupled a mechanistic thorium sorption and desorption model to a one-dimensional particle sinking model that uses realistic particle settling velocity spectra. The model generates estimates of 238U-234Th disequilibrium, particulate organic carbon concentration, and the C:234Th ratio of sinking particles, which are then compared to in situ measurements from quasi-Lagrangian studies conducted on six cruises in the California Current Ecosystem. Broad patterns observed in in situ measurements, including decreasing C:234Th ratios with depth and a strong correlation between sinking C:234Th and the ratio of vertically-integrated particulate organic carbon (POC) to vertically-integrated total water column 234Th, were accurately recovered by models assuming either a power law distribution of sinking speeds or a double log normal distribution of sinking speeds. Simulations suggested that the observed decrease in C:234Th with depth may be driven by preferential remineralization of carbon by particle-attached microbes. However, an alternate model structure featuring complete consumption and/or disaggregation of particles by mesozooplankton (e.g. no preferential remineralization of carbon) was also able to simulate decreasing C:234Th with depth (although the decrease was weaker), driven by 234Th adsorption onto slowly sinking particles. Model results also suggest that during bloom decays C:234Th ratios of sinking particles should be higher than expected (based on contemporaneous water column POC), because high settling velocities minimize carbon remineralization during sinking.

scholarly journals Simulating Secondary Inorganic Aerosols using the chemistry transport model MOCAGE version R2.15.0

2015 ◽  
Vol 8 (4) ◽  
pp. 3593-3651 ◽  
Author(s):  
J. Guth ◽  
B. Josse ◽  
V. Marécal ◽  
M. Joly
Keyword(s):  
North America ◽  
Transport Model ◽  
Regional Scale ◽  
In Situ Measurements ◽  
Aerosol Composition ◽  
Chemistry Transport Model ◽  
Inorganic Aerosols ◽  
Modis Aod ◽  
Inorganic Aerosol

Abstract. In this study we develop a Secondary Inorganic Aerosol (SIA) module for the chemistry transport model MOCAGE developed at CNRM. Based on the thermodynamic equilibrium module ISORROPIA II, the new version of the model is evaluated both at the global scale and at the regional scale. The results show high concentrations of secondary inorganic aerosols in the most polluted regions being Europe, Asia and the eastern part of North America. Asia shows higher sulfate concentrations than other regions thanks to emissions reduction in Europe and North America. Using two simulations, one with and the other without secondary inorganic aerosol formation, the model global outputs are compared to previous studies, to MODIS AOD retrievals, and also to in situ measurements from the HTAP database. The model shows a better agreement in all geographical regions with MODIS AOD retrievals when introducing SIA. It also provides a good statistical agreement with in situ measurements of secondary inorganic aerosol composition: sulfate, nitrate and ammonium. In addition, the simulation with SIA gives generally a better agreement for secondary inorganic aerosols precursors (nitric acid, sulfur dioxide, ammonia) in particular with a reduction of the Modified Normalised Mean Bias (MNMB). At the regional scale, over Europe, the model simulation with SIA are compared to the in situ measurements from the EMEP database and shows a good agreement with secondary inorganic aerosol composition. The results at the regional scale are consistent with those obtained with the global simulations. The AIRBASE database was used to compare the model to regulated air quality pollutants being particulate matter, ozone and nitrogen dioxide concentrations. The introduction of the SIA in MOCAGE provides a reduction of the PM2.5 MNMB of 0.44 on a yearly basis and even 0.52 on a three spring months period (March, April, May) when SIA are maximum.

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.

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