Erratum to “Heterogeneous chemistry of individual mineral dust particles from different dust source regions: the importance of particle mineralogy”

2005 ◽  
Vol 39 (2) ◽  
pp. 395 ◽  
Author(s):  
B.J. Krueger ◽  
V.H. Grassian ◽  
J.P. Cowin ◽  
A. Laskin
2008 ◽  
Vol 8 (6) ◽  
pp. 18765-18802
Author(s):  
Y. H. Lee ◽  
K. Chen ◽  
P. J. Adams

Abstract. A mineral dust module is developed and implemented into the global aerosol microphysics model, GISS-TOMAS. The model is evaluated against long-term measurements of dust surface mass concentrations and deposition fluxes. Predicted mass concentrations and deposition fluxes are in error on average by a factor of 3 and 5, respectively. The comparison shows that the model performs better near the dust source regions but underestimates surface concentrations and deposition fluxes in more remote regions. For example, including only sites with measured dust concentrations of at least 0.5 μg m−3, the model prediction agrees with observations to within a factor of 2. It was hypothesized that the lifetime of dust, 2.6 days in our base case, is too short and causes the underestimation in remote areas. However, a sensitivity simulation with smaller dust particles and increased lifetime, 3.7 days, does not significantly improve the comparison. We conclude that the underestimation of mineral dust in remote areas results from local factors and sources not well described by the dust source function and/or the GCM meteorology. The effect of dust aerosols on CCN(0.2%) concentrations is negligible in most regions of the globe; however, CCN(0.2%) concentrations decrease by 10–20% in dusty regions as a result of coagulational scavenging of CCN particles by dust and a decrease in H2SO4 condensation to CCN particles due to the additional surface area of dust.


2009 ◽  
Vol 9 (7) ◽  
pp. 2441-2458 ◽  
Author(s):  
Y. H. Lee ◽  
K. Chen ◽  
P. J. Adams

Abstract. A mineral dust module is developed and implemented into the global aerosol microphysics model, GISS-TOMAS. The model is evaluated against long-term measurements of dust surface mass concentrations and deposition fluxes. Predicted mass concentrations and deposition fluxes are in error on average by a factor of 3 and 5, respectively. The comparison shows that the model performs better near the dust source regions but underestimates surface concentrations and deposition fluxes in more remote regions. Including only sites with measured dust concentrations of at least 0.5 μg m−3, the model prediction agrees with observations to within a factor of 2. It was hypothesized that the lifetime of dust, 2.6 days in our base case, is too short and causes the underestimation in remote areas. However, a sensitivity simulation with smaller dust particles and increased lifetime, 3.7 days, does not significantly improve the comparison. These results suggest that the underestimation of mineral dust in remote areas may result from local factors/sources not well described by the global dust source function used here or the GCM meteorology. The effect of dust aerosols on CCN(0.2%) concentrations is negligible in most regions of the globe; however, CCN(0.2%) concentrations change decrease by 10–20% in dusty regions the impact of dust on CCN(0.2%) concentrations in dusty regions is very sensitive to the assumed size distribution of emissions. If emissions are predominantly in the coarse mode, CCN(0.2%) decreases in dusty regions up to 10–20% because dust competes for condensable H2SO4, reducing the condensational growth of ultrafine mode particles to CCN sizes. With significant fine mode emissions, however, CCN(0.2%) doubles in Saharan source regions because the direct emission of dust particles outweighs any microphysical feedbacks. The impact of dust on CCN concentrations active at various water supersaturations is also investigated. Below 0.1%, CCN concentrations increase significantly in dusty regions due to the presence of coarse dust particles. Above 0.2%, CCN concentrations show a similar behavior as CCN(0.2%).


2018 ◽  
Vol 18 (19) ◽  
pp. 14609-14622 ◽  
Author(s):  
Zechen Yu ◽  
Myoseon Jang

Abstract. To improve the simulation of the heterogeneous oxidation of SO2 and NOx in the presence of authentic mineral dust particles under ambient environmental conditions, the explicit kinetic mechanisms were constructed in the Atmospheric Mineral Aerosol Reaction (AMAR) model. The formation of sulfate and nitrate was divided into three phases: the gas phase, the non-dust aqueous phase, and the dust phase. In particular, AMAR established the mechanistic role of dust chemical characteristics (e.g., photoactivation, hygroscopicity, and buffering capacity) in heterogeneous chemistry. The photoactivation kinetic process of different dust particles was built into the model by measuring the photodegradation rate constant of an impregnated surrogate (malachite green dye) on a dust filter sample (e.g., Arizona test dust – ATD – and Gobi Desert dust – GDD) using an online reflective UV–visible spectrometer. The photoactivation parameters were integrated with the heterogeneous chemistry to predict the formation of reactive oxygen species on dust surfaces. A mathematical equation for the hygroscopicity of dust particles was also included in the AMAR model to process the multiphase partitioning of trace gases and in-particle chemistry. The buffering capacity of dust, which is related to the neutralization of dust alkaline carbonates with inorganic acids, was included in the model to dynamically predict the hygroscopicity of aged dust. The AMAR model simulated the formation of sulfate and nitrate using experimental data obtained in the presence of authentic mineral dust under ambient sunlight using a large outdoor smog chamber (University of Florida Atmospheric Photochemical Outdoor Reactor, UF-APHOR). Overall, the influence of GDD on the heterogeneous chemistry was much greater than that of ATD. Based on the model analysis, GDD enhanced the sulfate formation mainly via its high photoactivation capability. In the case of NO2 oxidation, dust-phase nitrate formation is mainly regulated by the buffering capacity of dust. The measured buffering capacity of GDD was 2 times greater than that of ATD, and consequently, the maximum nitrate concentration with GDD was nearly 2 times higher than that with ATD. The model also highlights that in urban areas with high NOx concentrations, hygroscopic nitrate salts quickly form via titration of the carbonates in the dust particles, but in the presence of SO2, the nitrate salts are gradually depleted by the formation of sulfate.


2013 ◽  
Vol 13 (14) ◽  
pp. 7097-7114 ◽  
Author(s):  
L. Zhang ◽  
Q. B. Li ◽  
Y. Gu ◽  
K. N. Liou ◽  
B. Meland

Abstract. Atmospheric mineral dust particles exert significant direct radiative forcings and are important drivers of climate and climate change. We used the GEOS-Chem global three-dimensional chemical transport model (CTM) coupled with the Fu-Liou-Gu (FLG) radiative transfer model (RTM) to investigate the dust radiative forcing and heating rate based on different vertical profiles for April 2006. We attempt to actually quantify the sensitivities of radiative forcing to dust vertical profiles, especially the discrepancies between using realistic and climatological vertical profiles. In these calculations, dust emissions were constrained by observations of aerosol optical depth (AOD). The coupled calculations utilizing a more realistic dust vertical profile simulated by GEOS-Chem minimize the physical inconsistencies between 3-D CTM aerosol fields and the RTM. The use of GEOS-Chem simulated vertical profile of dust extinction, as opposed to the FLG prescribed vertical profile, leads to greater and more spatially heterogeneous changes in the estimated radiative forcing and heating rate produced by dust. Both changes can be attributed to a different vertical structure between dust and non-dust source regions. Values of the dust vertically resolved AOD per grid level (VRAOD) are much larger in the middle troposphere, though smaller at the surface when the GEOS-Chem simulated vertical profile is used, which leads to a much stronger heating rate in the middle troposphere. Compared to the FLG vertical profile, the use of GEOS-Chem vertical profile reduces the solar radiative forcing at the top of atmosphere (TOA) by approximately 0.2–0.25 W m−2 over the African and Asian dust source regions. While the Infrared (IR) radiative forcing decreases 0.2 W m−2 over African dust belt, it increases 0.06 W m−2 over the Asian dust belt when the GEOS-Chem vertical profile is used. Differences in the solar radiative forcing at the surface between the use of the GEOS-Chem and FLG vertical profiles are most significant over the Gobi desert with a value of about 1.1 W m−2. The radiative forcing effect of dust particles is more pronounced at the surface over the Sahara and Gobi deserts by using FLG vertical profile, while it is less significant over the downwind area of Eastern Asia.


2013 ◽  
Vol 13 (1) ◽  
pp. 2415-2456 ◽  
Author(s):  
L. Zhang ◽  
Q. B. Li ◽  
Y. Gu ◽  
K. N. Liou ◽  
B. Meland

Abstract. Atmospheric mineral dust particles exert significant direct radiative forcings and are critical drivers of climate change. Here, we use the GEOS-Chem global three-dimensional chemical transport model (3-D CTM) coupled online with the Fu-Liou-Gu (FLG) radiative transfer model (RTM) to investigate the dust radiative forcing and heating rates based on different dust vertical profiles. The coupled calculations using a realistic dust vertical profile simulated by GEOS-Chem minimize the physical inconsistencies between 3-D CTM aerosol fields and the RTM. The use of GEOS-Chem simulated aerosol optical depth (AOD) vertical profiles as opposed to the FLG prescribed AOD vertical profiles leads to greater and more spatially heterogeneous changes in estimated radiative forcing and heating rate produced by dust. Both changes can be attributed to a different vertical structure between dust and non-dust source regions. Values of the dust AOD are much larger in the middle troposphere, though smaller at the surface when the GEOS-Chem simulated AOD vertical profile is used, which leads to a much stronger heating rate in the middle troposphere. Compared to FLG vertical profile, the use of GEOS-Chem vertical profile reduces the solar radiative forcing effect by about 0.2–0.25 W m−2 and the Infrared (IR) radiative forcing over the African and Asia dust source regions by about 0.1–0.2 W m−2. Differences in the solar radiative forcing at the surface between using the GEOS-Chem vertical profile and the FLG vertical profile are most significant over the Gobi desert with a value of about 1.1 W m−2. The radiative forcing effect of dust particles is more pronounced at the surface over the Sahara and Gobi deserts by using FLG vertical profile, while it is less significant over the downwind area of Eastern Asia.


2019 ◽  
Vol 11 (6) ◽  
pp. 701 ◽  
Author(s):  
Di Liu ◽  
Tianliang Zhao ◽  
Richard Boiyo ◽  
Siyu Chen ◽  
Zhengqi Lu ◽  
...  

The spatiotemporal and especially the vertical distributions of dust aerosols play crucial roles in the climatic effect of dust aerosol. In the present study, the spatial-temporal distribution of dust aerosols over East Asia was investigated using Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) retrievals (01/2007–12/2011) from the perspective of the frequency of dust occurrence (FDO), dust top layer height (TH) and profile of aerosol subtypes. The results showed that a typical dust belt was generated from the dust source regions (the Taklimakan and Gobi Deserts), in the latitude range of 25°N~45°N and reaching eastern China, Japan and Korea and, eventually, the Pacific Ocean. High dust frequencies were found over the dust source regions, with a seasonal sequence from high to low as follows: spring, summer, autumn and winter. Vertically, FDOs peaked at about 2 km over the dust source regions. In contrast, FDOs decreased with altitude over the downwind regions. On the dust belt from dust source regions to downwind regions, the dust top height (TH) was getting higher and higher. The dust TH varied in the range of 1.9–3.1 km above surface elevation (a.s.e.), with high values over the dust source regions and low values in the downwind areas, and a seasonally descending sequence of summer, spring, autumn and winter in accord with the seasonal variation of the boundary layer height. The annual AOD (Aerosol Optical Depth) was generally characterized by two high and two low AOD centers over East Asia. The percent contribution of the Dust Aerosol Optical Depth to the total AOD showed a seasonal variation from high to low as follows: spring, winter, autumn and summer. The vertical profile of the extinction coefficient revealed the predominance of pure dust particles in the dust source regions and a mixture of dust particles and pollutants in the downwind regions. The dust extinction coefficients over the Taklimakan Desert had a seasonal pattern from high to low as follows: spring, winter, summer and autumn. The results of the present study offered an understanding of the horizontal and vertical structures of dust aerosols over East Asia and can be used to evaluate the performance aerosol transport models.


2018 ◽  
Vol 18 (3) ◽  
pp. 2119-2138 ◽  
Author(s):  
Xin Wang ◽  
Hui Wen ◽  
Jinsen Shi ◽  
Jianrong Bi ◽  
Zhongwei Huang ◽  
...  

Abstract. Mineral dust aerosols (MDs) not only influence the climate by scattering and absorbing solar radiation but also modify cloud properties and change the ecosystem. From 3 April to 16 May 2014, a ground-based mobile laboratory was deployed to measure the optical and microphysical properties of MDs near dust source regions in Wuwei, Zhangye, and Dunhuang (in chronological order) along the Hexi Corridor over northwestern China. Throughout this dust campaign, the hourly averaged (±standard deviation) aerosol scattering coefficients (σsp, 550 nm) of the particulates with aerodynamic diameters less than 2.5 µm (PM2.5) at these three sites were sequentially 101.5 ± 36.8, 182.2 ± 433.1, and 54.0 ± 32.0 Mm−1. Correspondingly, the absorption coefficients (σap, 637 nm) were 9.7 ± 6.1, 6.0 ± 4.6, and 2.3 ± 0.9 Mm−1; single-scattering albedos (ω, 637 nm) were 0.902 ± 0.025, 0.931 ± 0.037, and 0.949 ± 0.020; and scattering Ångström exponents (Åsp, 450–700 nm) of PM2.5 were 1.28 ± 0.27, 0.77 ± 0.51, and 0.52 ± 0.31. During a severe dust storm in Zhangye (i.e., from 23 to 25 April), the highest values of σsp2.5 (∼ 5074 Mm−1), backscattering coefficient (σbsp2.5, ∼ 522 Mm−1), and ω637 (∼ 0.993) and the lowest values of backscattering fraction (b2.5, ∼ 0.101) at 550 nm and Åsp2.5 (∼ −0.046) at 450–700 nm, with peak values of aerosol number size distribution (appearing at the particle diameter range of 1–3 µm), exhibited that the atmospheric aerosols were dominated by coarse-mode dust aerosols. It is hypothesized that the relatively higher values of mass scattering efficiency during floating dust episodes in Wuwei and Zhangye are attributed to the anthropogenic soil dust produced by agricultural cultivations.


2018 ◽  
Author(s):  
Zechen Yu ◽  
Myoseon Jang

Abstract. To improve the simulation of the heterogeneous oxidation of SO2 and NOx in the presence of authentic mineral dust particles under ambient environmental conditions, the explicit kinetic mechanism was constructed in Atmospheric Mineral Aerosol Reaction (AMAR) model. The formation of sulfate and nitrate was divided into three phases: gas phase, non-dust aqueous phase and dust phase. Specially, AMAR established the mechanistic role of dust chemical characteristics (e.g., photoactivation, hygroscopicity, and buffering capacity) on heterogeneous chemistry. The photo-activation kinetic process of different dust particles was built into the model by measuring the photodegradation rate constant of an impregnated surrogate (malachite green dye) on a dust filter sample (e.g., Arizona Test dust (ATD) and Gobi Desert dust (GDD)) using an online reflective UV-visible spectrometer. The photoactivation parameters were integrated with the heterogeneous chemistry to predict OH radical formation on dust surfaces. A mathematical equation for the hygroscopicity of dust particles was also included in the AMAR model to process the multiphase partitioning of tracers and in-particle chemistry. The buffering capacity of dust, which is related to the neutralization of dust alkaline carbonates with inorganic acids, was included in the model to dynamically predict the hygroscopicity of aged dust. The AMAR model simulated the formation of sulfate and nitrate using experimental data obtained in the presence of authentic mineral dust under ambient sunlight using a large outdoor smog chamber (UF-APHOR). Overall, both GDD and ATD significantly enhanced the formation of sulfate and nitrate, compared to that in the system without dust particles. However, the influence of GDD on the heterogeneous chemistry was much greater than that of ATD. Based on the model analysis, GDD enhanced the sulfate formation mainly via its high photoactivation capability. In the case of NO2 oxidation, dust-phase nitrate formation is mainly regulated by the buffering capacity of dust. The measured buffering capacity of GDD was two times greater than that of ATD, and consequently, the maximum nitrate concentration with GDD was nearly two times higher than that with ATD. The model also highlights that in urban areas with high NOx concentrations, hygroscopic nitrate salts quickly form via titration of the carbonates in the dust phase, but in the presence of SO2, the nitrate salts are gradually depleted by sulfate.


2018 ◽  
Author(s):  
Stelios Myriokefalitakis ◽  
Akinori Ito ◽  
Maria Kanakidou ◽  
Athanasios Nenes ◽  
Maarten C. Krol ◽  
...  

Abstract. This work reports on the current status of global modelling of iron (Fe) deposition fluxes and atmospheric concentrations and analyses of the differences between models, as well as between models and observations. A total of four global 3-D chemistry-transport (CTMs) and general circulation (GCMs) models have participated in this intercomparison, in the framework of the United Nations Joint Group of Experts on the Scientific Aspects of Marine Environmental Protection (GESAMP) Working Group 38, The Atmospheric Input of Chemicals to the Ocean. The global total Fe (TFe) emissions strength in the models is equal to ~ 72 Tg-Fe yr−1 (38–134 Tg-Fe yr−1) from mineral dust sources and around 2.1 Tg-Fe yr−1 (1.8–2.7 Tg-Fe yr−1) from combustion processes (sum of anthropogenic combustion/biomass burning and wildfires). The mean global labile Fe (LFe) source strength in the models, considering both the primary emissions and the atmospheric processing, is calculated to be 0.7 (±0.3) Tg-Fe yr−1, accounting for mineral dust and combustion aerosols together. The multi model ensemble global TFe and LFe deposition fluxes into the global ocean are calculated to be ~ 15 Tg-Fe yr−1 and ~ 0.3 Tg-Fe yr−1, respectively. The model intercomparison analysis indicates that the representation of the atmospheric Fe cycle varies among models, in terms of both the magnitude of natural and combustion Fe emissions as well as the complexity of atmospheric processing parametrizations of Fe-containing aerosols. The model comparison with aerosol Fe observations over oceanic regions indicate that most models overestimate surface level TFe mass concentrations near the dust source regions and tend to underestimate the low concentrations observed in remote ocean regions. All models are able to simulate the tendency of higher Fe loading near and downwind from the dust source regions, with the mean normalized bias for the Northern Hemisphere (~ 14), larger than the Southern Hemisphere (~ 2.4) for the ensemble model mean. This model intercomparison and model–observation comparison study reveals two critical issues in LFe simulations that require further exploration: 1) the Fe-containing aerosol size distribution and 2) the relative contribution of dust and combustion sources of Fe to labile Fe in atmospheric aerosols over the remote oceanic regions.


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