A revised mineral dust emission scheme in GEOS-Chem: improvements in dust simulations over China

Mineral dust plays a significant role in climate change and air quality, but large uncertainties remain in terms of dust emission prediction. In this study, we improved the treatments of dust emission process in a Global 3-D Chemical Transport model (GEOS-Chem) v12.6.0, by incorporating the geographical variation of aerodynamic roughness length (Z0), smooth roughness length (Z0s), soil texture, introducing Owen effect and Lu and Shao (1999) formulation of sandblasting efficiency &#945;. To investigate the impact of the modifications incorporated in the model, several sensitivity simulations were performed for a severe dust storm during March 27, 2015 to April 2, 2015 over northern China. Results show that simulated threshold friction velocity is very sensitive to the updated Z0 and Z0s field, with the relative difference ranging from 10% to 60% compared to the original model with uniform value. An inclusion of Owen effect leads to an increase in surface friction velocity, which mainly occurs in the arid and semi-arid regions of northwest China. The substitution of fixed value of &#945; assumed in original scheme with one varying with friction velocity and soil texture based on observations reduces &#945; by 50% on average, especially over regions with sand texture. Comparisons of sensitivity simulations and measurements show that the revised scheme with the implement of updates provides more realistic threshold friction velocities and PM10 mass concentrations. The performance of the improved model has been evaluated against surface PM10 observations as well as MODIS aerosol optical depth (AOD) values, showing that the spatial and temporal variation of mineral dust are better captured by the revised scheme. Due to the inclusion of the improvement, average PM10 concentrations at observational sites are more comparable to the observations, and the average mean bias (MB) and normalized mean bias (NMB) values are reduced from -196.29&#956;g m-3 and -52.79% to -47.72&#956;g m-3 and -22.46% respectively. Our study suggests that the erodibility factor, sandblasting efficiency and soil-related properties which are simply assumed in the empirical scheme may lack physical mechanism and spatial-temporal representative. Further study and measurements should be conducted to obtain more realistic and detailed map of these parameters in order to improve dust representation in the model.&#160;

A revised mineral dust emission scheme in GEOS-Chem: improvements in dust simulations over China

10.5194/acp-2020-984 ◽

2020 ◽

Author(s):

Rong Tian ◽

Xiaoyan Ma ◽

Jianqi Zhao

Keyword(s):

Soil Texture ◽

Friction Velocity ◽

Roughness Length ◽

Transport Model ◽

Mineral Dust ◽

Dust Emission ◽

Northern China ◽

Spatial And Temporal Variation ◽

Abstract. Mineral dust plays a significant role in climate change and air quality, but large uncertainties remain in terms of dust emission prediction. In this study, we improved the treatments of dust emission process in a Global 3-D Chemical Transport model (GEOS-Chem) v12.6.0, by incorporating the geographical variation of aerodynamic roughness length (Z0), smooth roughness length (Z0s), soil texture, introducing Owen effect and Lu and Shao (1999) formulation of sandblasting efficiency α. To investigate the impact of the modifications incorporated in the model, several sensitivity simulations were performed for a severe dust storm during March 27, 2015 to April 2, 2015 over northern China. Results show that simulated threshold friction velocity is very sensitive to the updated Z0 and Z0s field, with the relative difference ranging from 10 % to 60 % compared to the original model with uniform value. An inclusion of Owen effect leads to an increase in surface friction velocity, which mainly occurs in the arid and semi-arid regions of northwest China. The substitution of fixed value of α assumed in original scheme with one varying with friction velocity and soil texture based on observations reduces α by 50 % on average, especially over regions with sand texture. Comparisons of sensitivity simulations and measurements show that the revised scheme with the implement of updates provides more realistic threshold friction velocities and PM10 mass concentrations. The performance of the improved model has been evaluated against surface PM10 observations as well as MODIS aerosol optical depth (AOD) values, showing that the spatial and temporal variation of mineral dust are better captured by the revised scheme. Due to the inclusion of the improvement, average PM10 concentrations at observational sites are more comparable to the observations, and the average mean bias (MB) and normalized mean bias (NMB) values are reduced from −196.29 μg m−3 and −52.79 % to −47.72 μg −3 and −22.46 % respectively. Our study suggests that the erodibility factor, sandblasting efficiency and soil-related properties which are simply assumed in the empirical scheme may lack physical mechanism and spatial-temporal representative. Further study and measurements should be conducted to obtain more realistic and detailed map of these parameters in order to improve dust representation in the model.

A revised mineral dust emission scheme in GEOS-Chem: improvements in dust simulations over China

Atmospheric Chemistry and Physics ◽

10.5194/acp-21-4319-2021 ◽

2021 ◽

Vol 21 (6) ◽

pp. 4319-4337

Author(s):

Rong Tian ◽

Xiaoyan Ma ◽

Jianqi Zhao

Keyword(s):

Soil Texture ◽

Friction Velocity ◽

Roughness Length ◽

Transport Model ◽

Mineral Dust ◽

Dust Emission ◽

Northern China ◽

Spatial And Temporal Variation ◽

Abstract. Mineral dust plays a significant role in climate change and air quality, but large uncertainties remain in terms of dust emission prediction. In this study, we improved treatment of the dust emission process in a global 3-D chemical transport model (GEOS-Chem v12.6.0), by incorporating the geographical variation of aerodynamic roughness length (Z0), smooth roughness length (Z0s) and soil texture and by introducing the Owen effect and the formulation of the sandblasting efficiency α by Lu and Shao (1999). To investigate the impact of the modifications incorporated in the model, several sensitivity simulations were performed for a severe dust storm during 27 March to 2 April 2015 over northern China. Results show that simulated threshold friction velocity is very sensitive to the updated Z0 and Z0s field, with the relative difference ranging from 10 % to 60 % compared to the original model with a uniform value. The inclusion of the Owen effect leads to an increase in surface friction velocity, which mainly occurs in the arid and semi-arid regions of northwest China. The substitution of a fixed value of α assumed in the original scheme with one varying with friction velocity and soil texture based on observations reduces α by 50 % on average, especially over regions with sand texture. Comparisons of sensitivity simulations and measurements show that the revised scheme with the implementation of updates provides more realistic threshold friction velocities and PM10 mass concentrations. The performance of the improved model has been evaluated against surface PM10 observations as well as MODIS aerosol optical depth (AOD) values, showing that the spatial and temporal variation of mineral dust are better captured by the revised scheme. Due to the inclusion of the improvement, average PM10 concentrations at observational sites are more comparable to the observations, and the average mean bias (MB) and normalized mean bias (NMB) values are reduced from −196.29 µg m−3 and −52.79 % to −47.72 µg m−3 and −22.46 % respectively. Our study suggests that the erodibility factor, sandblasting efficiency and soil-related properties which are simply assumed in the empirical scheme may lack a physical mechanism and spatial–temporal representativeness. Further study and measurements should be conducted to obtain a more realistic and detailed map of these parameters in order to improve dust representation in the model.

N2O5 uptake onto saline mineral dust: a potential missing source of tropospheric ClNO2 in inland China

10.5194/acp-2021-541 ◽

2021 ◽

Author(s):

Haichao Wang ◽

Chao Peng ◽

Xuan Wang ◽

Shengrong Lou ◽

Keding Lu ◽

...

Keyword(s):

Laboratory Experiments ◽

Transport Model ◽

Mineral Dust ◽

Heterogeneous Reaction ◽

Mixing Ratios ◽

Nitryl Chloride ◽

Mass Fractions ◽

The Impact ◽

Cl Atoms

Abstract. Nitryl chloride (ClNO2), an important precursor of Cl atoms, significantly affects atmospheric oxidation capacity and O3 formation. However, sources of ClNO2 in inland China have not been fully elucidated. In this work, laboratory experiments were conducted to investigate heterogeneous reaction of N2O5 with eight saline mineral dust samples collected from different regions in China, and substantial formation of ClNO2 was observed. ClNO2 yields, φ(ClNO2), showed large variations (ranging from < 0.05 to ~0.77) for different saline mineral dust samples, largely depending on mass fractions of particulate chloride. In addition, for different saline mineral dust samples, φ(ClNO2) could increase, decrease or show insignificant change as RH increased from 18 % to 75 %. We further found that current parameterizations significantly overestimated φ(ClNO2) for heterogeneous uptake of N2O5 onto saline mineral dust. Assuming a uniform φ(ClNO2) value of 0.10 for N2O5 uptake onto mineral dust, we used a 3-D chemical transport model to assess the impact of this reaction on tropospheric ClNO2 in China, and found that weekly mean nighttime maximum ClNO2 mixing ratios could be increased by up to 85 pptv during a severe dust event in May 2017. Overall, our work showed that heterogeneous reaction of N2O5 with saline mineral dust could be an important source of tropospheric ClNO2 in inland China.

Extending methane profiles from aircraft into the stratosphere for satellite total column validation using the ECMWF C-IFS and TOMCAT/SLIMCAT 3-D model

Atmospheric Chemistry and Physics ◽

10.5194/acp-17-6663-2017 ◽

2017 ◽

Vol 17 (11) ◽

pp. 6663-6678 ◽

Cited By ~ 2

Author(s):

Shreeya Verma ◽

Julia Marshall ◽

Mark Parrington ◽

Anna Agustí-Panareda ◽

Sebastien Massart ◽

...

Keyword(s):

Greenhouse Gases ◽

Transport Model ◽

A Priori ◽

Atmospheric Composition ◽

Random Errors ◽

Spatial Coverage ◽

Forecasting System ◽

The Impact ◽

Total Column

Abstract. Airborne observations of greenhouse gases are a very useful reference for validation of satellite-based column-averaged dry air mole fraction data. However, since the aircraft data are available only up to about 9–13 km altitude, these profiles do not fully represent the depth of the atmosphere observed by satellites and therefore need to be extended synthetically into the stratosphere. In the near future, observations of CO2 and CH4 made from passenger aircraft are expected to be available through the In-Service Aircraft for a Global Observing System (IAGOS) project. In this study, we analyse three different data sources that are available for the stratospheric extension of aircraft profiles by comparing the error introduced by each of them into the total column and provide recommendations regarding the best approach. First, we analyse CH4 fields from two different models of atmospheric composition – the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecasting System for Composition (C-IFS) and the TOMCAT/SLIMCAT 3-D chemical transport model. Secondly, we consider scenarios that simulate the effect of using CH4 climatologies such as those based on balloons or satellite limb soundings. Thirdly, we assess the impact of using a priori profiles used in the satellite retrievals for the stratospheric part of the total column. We find that the models considered in this study have a better estimation of the stratospheric CH4 as compared to the climatology-based data and the satellite a priori profiles. Both the C-IFS and TOMCAT models have a bias of about −9 ppb at the locations where tropospheric vertical profiles will be measured by IAGOS. The C-IFS model, however, has a lower random error (6.5 ppb) than TOMCAT (12.8 ppb). These values are well within the minimum desired accuracy and precision of satellite total column XCH4 retrievals (10 and 34 ppb, respectively). In comparison, the a priori profile from the University of Leicester Greenhouse Gases Observing Satellite (GOSAT) Proxy XCH4 retrieval and climatology-based data introduce larger random errors in the total column, being limited in spatial coverage and temporal variability. Furthermore, we find that the bias in the models varies with latitude and season. Therefore, applying appropriate bias correction to the model fields before using them for profile extension is expected to further decrease the error contributed by the stratospheric part of the profile to the total column.

Model sensitivity studies of the decrease in atmospheric carbon tetrachloride

Atmospheric Chemistry and Physics ◽

10.5194/acp-16-15741-2016 ◽

2016 ◽

Vol 16 (24) ◽

pp. 15741-15754 ◽

Cited By ~ 4

Author(s):

Martyn P. Chipperfield ◽

Qing Liang ◽

Matthew Rigby ◽

Ryan Hossaini ◽

Stephen A. Montzka ◽

...

Keyword(s):

Carbon Tetrachloride ◽

Transport Model ◽

Three Dimensional ◽

Montreal Protocol ◽

Uncertainty Range ◽

The Past ◽

Systematic Biases ◽

Lifetime Uncertainty ◽

Abstract. Carbon tetrachloride (CCl4) is an ozone-depleting substance, which is controlled by the Montreal Protocol and for which the atmospheric abundance is decreasing. However, the current observed rate of this decrease is known to be slower than expected based on reported CCl4 emissions and its estimated overall atmospheric lifetime. Here we use a three-dimensional (3-D) chemical transport model to investigate the impact on its predicted decay of uncertainties in the rates at which CCl4 is removed from the atmosphere by photolysis, by ocean uptake and by degradation in soils. The largest sink is atmospheric photolysis (74 % of total), but a reported 10 % uncertainty in its combined photolysis cross section and quantum yield has only a modest impact on the modelled rate of CCl4 decay. This is partly due to the limiting effect of the rate of transport of CCl4 from the main tropospheric reservoir to the stratosphere, where photolytic loss occurs. The model suggests large interannual variability in the magnitude of this stratospheric photolysis sink caused by variations in transport. The impact of uncertainty in the minor soil sink (9 % of total) is also relatively small. In contrast, the model shows that uncertainty in ocean loss (17 % of total) has the largest impact on modelled CCl4 decay due to its sizeable contribution to CCl4 loss and large lifetime uncertainty range (147 to 241 years). With an assumed CCl4 emission rate of 39 Gg year−1, the reference simulation with the best estimate of loss processes still underestimates the observed CCl4 (overestimates the decay) over the past 2 decades but to a smaller extent than previous studies. Changes to the rate of CCl4 loss processes, in line with known uncertainties, could bring the model into agreement with in situ surface and remote-sensing measurements, as could an increase in emissions to around 47 Gg year−1. Further progress in constraining the CCl4 budget is partly limited by systematic biases between observational datasets. For example, surface observations from the National Oceanic and Atmospheric Administration (NOAA) network are larger than from the Advanced Global Atmospheric Gases Experiment (AGAGE) network but have shown a steeper decreasing trend over the past 2 decades. These differences imply a difference in emissions which is significant relative to uncertainties in the magnitudes of the CCl4 sinks.

Global simulations of monoterpene-derived peroxy radical fates and the distributions of highly oxygenated organic molecules (HOM) and accretion products

10.5194/acp-2021-901 ◽

2021 ◽

Author(s):

Ruochong Xu ◽

Joel A. Thornton ◽

Ben H. Lee ◽

Yanxu Zhang ◽

Lyatt Jaeglé ◽

...

Keyword(s):

Rate Constants ◽

First Generation ◽

Transport Model ◽

Peroxy Radical ◽

Organic Aerosol ◽

Laboratory Studies ◽

Cross Reactions ◽

Formation Kinetics ◽

Abstract. We evaluate monoterpene-derived peroxy radical (MT-RO2) unimolecular autoxidation and self and cross reactions with other RO2 in the GEOS-Chem global chemical transport model. Formation of associated highly oxygenated organic molecule (HOM) and accretion products are tracked in competition with other bimolecular reactions. Autoxidation is the dominant fate up to 6–8 km for first-generation MT-RO2 which can undergo unimolecular H-shifts. Reaction with NO can be a more common fate for H-shift rate constants < 0.1 s−1 or at altitudes higher than 8 km due to the imposed Arrhenius temperature dependence of unimolecular H-shifts. For MT-derived HOM-RO2, generated by multi-step autoxidation of first-generation MT-RO2, reaction with other RO2 is predicted to be the major fate throughout most of the boreal and tropical forested regions, while reaction with NO dominates in temperate and subtropical forests of the Northern Hemisphere. The newly added reactions result in ~4 % global average decrease of HO2 and RO2 mainly due to faster self-/cross-reactions of MT-RO2, but the impact upon HO2/OH/NOx abundances is only important in the planetary boundary layer (PBL) over portions of tropical forests. Within the bounds of formation kinetics and HOM photochemical lifetime constraints from laboratory studies, predicted HOM concentrations in MT-rich regions and seasons reach 10 % or even exceed total organic aerosol as predicted by the standard GEOS-Chem model. Comparisons to observations reveal large uncertainties remain for key reaction parameters and processes, especially the photochemical lifetime of HOM and associated accretion products. Using the highest reported yields and H-shift rate constants of MT-RO2 that undergo autoxidation, HOM concentrations tend to exceed the limited set of observations. Similarly, we infer that RO2 cross reactions rate constants near the gas-kinetic limit with accretion product branching greater than ~0.25 are inconsistent with total organic aerosol unless there is rapid decomposition of accretion products, the accretion products have saturation vapor concentrations > > 1 μg m−3, or modeled MT emission rates are overestimated. This work suggests further observations and laboratory studies related to MT-RO2 derived HOM and gas-phase accretion product formation kinetics, and especially their atmospheric fate, such as gas-particle partitioning, multi-phase chemistry, and net SOA formation, are needed.

Aerosol concentrations variability over China: two distinct leading modes

10.5194/acp-2019-1194 ◽

2020 ◽

Author(s):

Juan Feng ◽

Jianlei Zhu ◽

Jianping Li ◽

Hong Liao

Keyword(s):

Transport Model ◽

Eastern China ◽

Practical Importance ◽

Negative Temperature ◽

Northern China ◽

Dipole Mode ◽

Boundary Layer Height ◽

The North ◽

The North Atlantic Oscillation

Abstract. Understanding the variability in aerosol concentrations (AC) over China is a scientific challenge and is of practical importance. The present study explored the month-to-month variability in AC over China based on simulations of an atmospheric chemical transport model with a fixed emissions level. The month-to-month variability in AC over China is dominated by two principal modes: the first leading mono-pole mode and the second meridional dipole mode. The mono-pole mode mainly indicates enhanced AC over eastern China, and the dipole mode displays a south–north out-of-phase pattern. The two leading modes are associated with different climatic systems. The mono-pole mode relates to the 3-month leading El Niño–South Oscillation (ENSO), while the dipole mode connects with the simultaneous variation in the North Atlantic Oscillation (NAO) or the Northern Hemisphere Annular Mode (NAM). The associated anomalous dynamic and thermal impacts of the two climatic variabilities are examined to explain their contributions to the formation of the two modes. For the mono-pole mode, the preceding ENSO is associated with anomalous convergence, decreased planetary boundary layer height (PBLH), and negative temperature anomalies, which are unfavorable for emissions. For the dipole mode, the positive NAO is accompanied by opposite anomalies in the convergence, PBLH, and temperature over southern and northern China, paralleling the spatial formation of the mode. This result suggests that the variations originating from the tropical Pacific and extratropical atmospheric systems contribute to the dominant variabilities of AC over China.

Influences of hydroxyl radicals (OH) on top-down estimates of the global and regional methane budgets

10.5194/acp-2019-1208 ◽

2020 ◽

Cited By ~ 1

Author(s):

Yuanhong Zhao ◽

Marielle Saunois ◽

Philippe Bousquet ◽

Xin Lin ◽

Antoine Berchet ◽

...

Keyword(s):

Spatial Distribution ◽

Climate Models ◽

Transport Model ◽

Atmospheric Transport ◽

Temporal Variations ◽

Oh Radicals ◽

Top Down ◽

Ch4 Emissions ◽

Abstract. The hydroxyl radical (OH), which is the dominant sink of methane (CH4), plays a key role to close the global methane budget. Previous research that assessed the impact of OH changes on the CH4 budget mostly relied on box modeling inversions with a very simplified atmospheric transport and no representation of the heterogeneous spatial distribution of OH radicals. Here using a variational Bayesian inversion framework and a 3D chemical transport model, LMDz, combined with 10 different OH fields derived from chemistry-climate models (CCMI experiment), we evaluate the influence of OH burden, spatial distribution, and temporal variations on the global CH4 budget. The global tropospheric mean CH4-reaction-weighted [OH] ([OH]GM-CH4) ranges 10.3–16.3 × 105 molec cm−3 across 10 OH fields during the early 2000s, resulting in inversion-based global CH4 emissions between 518 and 757 Tg yr−1. The uncertainties in CH4 inversions induced by the different OH fields are comparable to, or even larger than the uncertainty typically given by bottom-up and top-down estimates. Based on the LMDz inversions, we estimate that a 1 %-increase in OH burden leads to an increase of 4 Tg yr−1 in the estimate of global methane emissions, which is about 25 % smaller than what is estimated by box-models. The uncertainties in emissions induced by OH are largest over South America, corresponding to large inter-model differences of [OH] in this region. From the early to the late 2000s, the optimized CH4 emissions increased by 21.9 ± 5.7 Tg yr−1 (16.6–30.0 Tg yr−1), of which ~ 25 % (on average) is contributed by −0.5 to +1.8 % increase in OH burden. If the CCMI models represent the OH trend properly over the 2000s, our results show that a higher increasing trend of CH4 emissions is needed to match the CH4 observations compared to the CH4 emission trend derived using constant OH. This study strengthens the importance to reach a better representation of OH burden and of OH spatial and temporal distributions to reduce the uncertainties on the global CH4 budget.

Heterogeneous reaction of HO2 with airborne TiO2 particles and its implication for climate change mitigation strategies

10.5194/acp-2017-439 ◽

2017 ◽

Cited By ~ 1

Author(s):

Daniel R. Moon ◽

Giorgio S. Taverna ◽

Clara Anduix-Canto ◽

Trevor Ingham ◽

Martyn P. Chipperfield ◽

...

Keyword(s):

Transport Model ◽

Heterogeneous Reaction ◽

Three Dimensional ◽

Mitigation Strategies ◽

Heterogeneous Reactions ◽

Flow Tube ◽

Tio2 Particles ◽

The Impact ◽

Change Mitigation

Abstract. One geoengineering mitigation strategy for global temperature rises resulting from the increased concentrations of greenhouse gases is to inject particles into the stratosphere to scatter solar radiation back to space, with TiO2 particles emerging as a possible candidate. Uptake coefficients of HO2, γ(HO2), onto sub-micrometre TiO2 particles were measured at room temperature and different relative humidities (RH) using an atmospheric pressure aerosol flow tube coupled to a sensitive HO2 detector. Values of γ(HO2) increased from 0.021 ± 0.001 to 0.036 ± 0.007 as the RH was increased from 11 % to 66 %, and the increase in γ(HO2) correlated with the number of monolayers of water surrounding the TiO2 particles. The impact of the uptake of HO2 onto TiO2 particles on stratospheric concentrations of HO2 and O3 was simulated using the TOMCAT three-dimensional chemical transport model. The model showed that by injecting the amount of TiO2 required to achieve the same cooling effect as the Mt. Pinatubo eruption, heterogeneous reactions between HO2 and TiO2 would have a negligible effect on stratospheric concentrations of HO2 and O3.

Impacts of Current and Projected Oil Palm Plantation Expansion on Air Quality Over Southeast Asia

10.5194/acp-2016-158 ◽

2016 ◽

Author(s):

Sam J. Silva ◽

Colette L. Heald ◽

Jeffrey A. Geddes ◽

Kemen G. Austin ◽

Prasad S. Kasibhatla ◽

...

Keyword(s):

Air Quality ◽

Southeast Asia ◽

Oil Palm ◽

Urban Areas ◽

Transport Model ◽

Oil Palm Plantation ◽

Deposition Velocities ◽

Current Constellation ◽

Abstract. Over recent decades oil palm plantations have rapidly expanded across Southeast Asia (SEA). According to the United Nations, oil palm production in SEA increased by a factor of 3 from 1995 to 2010. We investigate the impacts of current (2010) and future (2020) oil palm expansion in SEA on surface-atmosphere exchange and the resulting air quality in the region. For this purpose, we use satellite data, high-resolution land maps, and the chemical transport model GEOS-Chem. Relative to a no oil palm plantation scenario (~ 1990), overall simulated isoprene emissions in the region increase by 13 % due to oil palm plantations in 2010 and a further 11 % by 2020. In addition, the expansion of palm plantations leads to local increases in ozone deposition velocities of up to 20 %. The net result of these changes is that oil palm expansion in SEA increases surface O3 by up to 3.5 ppbv over dense urban regions, and could rise more than 4.5 ppbv above baseline levels by 2020. Biogenic secondary organic aerosol loadings also increase by up to 1 μg m−3 due to oil palm expansion, and could increase a further 2.5 μg m−3 by 2020. Our analysis indicates that while the impact of recent oil palm expansion on air quality in the region has been significant, the retrieval error and sensitivity of the current constellation of satellite measurements limit our ability to observe these impacts from space. Oil palm expansion is likely to continue to degrade air quality in the region in the coming decade and hinder efforts to achieve air quality regulations in major urban areas such as Kuala Lumpur and Singapore.