scholarly journals A new data set of soil mineralogy for dust-cycle modeling

2014 ◽  
Vol 14 (8) ◽  
pp. 3801-3816 ◽  
Author(s):  
E. Journet ◽  
Y. Balkanski ◽  
S. P. Harrison

Abstract. The mineralogy of airborne dust affects the impact of dust particles on direct and indirect radiative forcing, on atmospheric chemistry and on biogeochemical cycling. It is determined partly by the mineralogy of the dust-source regions and partly by size-dependent fractionation during erosion and transport. Here we present a data set that characterizes the clay and silt-sized fractions of global soil units in terms of the abundance of 12 minerals that are important for dust–climate interactions: quartz, feldspars, illite, smectite, kaolinite, chlorite, vermiculite, mica, calcite, gypsum, hematite and goethite. The basic mineralogical information is derived from the literature, and is then expanded following explicit rules, in order to characterize as many soil units as possible. We present three alternative realizations of the mineralogical maps, taking the uncertainties in the mineralogical data into account. We examine the implications of the new database for calculations of the single scattering albedo of airborne dust and thus for dust radiative forcing.

2013 ◽  
Vol 13 (9) ◽  
pp. 23943-23993 ◽  
Author(s):  
E. Journet ◽  
Y. Balkanski ◽  
S. P. Harrison

Abstract. The mineralogy of airborne dust affects the impact of dust particles on direct and indirect radiative forcing, on atmospheric chemistry and on biogeochemical cycling. It is determined partly by the mineralogy of the dust-source regions and partly by size-dependent fractionation during erosion and transport. Here we present a data set that characterizes the clay and silt sized fractions of global soil units in terms of the abundance of 12 minerals that are important for dust-climate interactions: quartz, feldspars, illite, smectite, kaolinite, chlorite, vermiculite, mica, calcite, gypsum, hematite and goethite. The basic mineralogical information is derived from the literature, and is then expanded following explicit rules, in order to characterize as many soil units as possible. We present three alternative realisations of the mineralogical maps that account for the uncertainties in the mineralogical data. We examine the implications of the new database for calculations of the single scattering albedo of airborne dust and thus for dust radiative forcing.


2021 ◽  
Author(s):  
María Gonçalves Ageitos ◽  
Matt Dawson ◽  
Vincenzo Obiso ◽  
Martina Klose ◽  
Ron Miller ◽  
...  

<p>Dust aerosols consist on a variety of minerals with different physic and chemical properties. As such, they interact with short and long wave radiation, potentially form clouds, act as nutrients modulating biogeochemical cycles, or influence atmospheric chemistry, differently. Most current state-of-the-art Earth System Models (ESMs) neglect the complexity in dust composition, mainly due to computational constraints, but also to the existing uncertainties in the size resolved composition of parent soils, the resulting distribution of minerals in airborne dust, and the scarcity of observations to constrain them.</p><p>Within this work, we assess the variability of global dust composition due to uncertainties in the characterization of the parent soil mineralogy. To that end, we consider two available global soil mineralogy atlases, developed by Claquin et al. (1999) –C1999- and Journet et al. (2014) –J2014-, which represent respectively 8 and 12 relevant minerals for climate (namely: illite, smectite/montmorillonite, kaolinite, calcite, gypsum, hematite, quartz, and feldspars in C1999, and those plus chlorite, vermiculite, goethite, and mica in J2014). Thanks to a recently developed feature of the MONARCH atmospheric-chemistry model, we are able to explicitly resolve the minerals’ atmospheric cycle. Therefore, we define two global experiments to assess changes on airborne dust composition attributed to the soil mineralogy assumptions and provide a measure of their variability. We also perform a preliminary evaluation of the global mineralogy results against available observations of mineral fractions in surface dust concentration.</p><p>Our results will inform the climate modelling community about the potential variability in dust composition, an aspect that will gain relevance as ESMs continue growing in complexity and new processes to better characterize aerosols’ forcing or biogeochemical cycles are added. Further observational constraints, such as those that will derive from the EMIT NASA mission on soil composition or the FRAGMENT experimental campaigns on airborne dust characterization, will be key in the near future to improve our understanding of the impact of dust mineralogy on fundamental climate features.</p>


Atmosphere ◽  
2019 ◽  
Vol 10 (12) ◽  
pp. 728 ◽  
Author(s):  
Meihua Wang ◽  
Jing Su ◽  
Xugang Li ◽  
Chen Wang ◽  
Jinming Ge

In this study, we present parameterization schemes of dust single-scattering properties (SSPs) in order to establish a fast and accurate way to obtain the SSPs for dust shortwave radiative flux calculation. Based on the assumption that dust particles are spheroids, we represent a single nonspherical particle with a collection of monodisperse spheres that contain the same total surface area and volume as the original particle to convert the spheroid to a sphere. The SSPs of dust particles were parameterized in terms of the effective radius ( R e ) and imaginary part of the refractive index ( M i ). The averaged relative errors of the parameterized to the “exact” single-scattering properties, which refer to the results from the Mie theory program, are below 1.5%. To further quantify the impact of parametrization on the radiative flux simulation, we computed the radiative fluxes at both the top of the atmosphere (TOA) and the surface by using SSPs from the parameterization and the “exact”, respectively. The maximum relative errors were below 1% at both the TOA and the surface, proving that the SSPs of dust calculated by our parameterization schemes are well suited for radiative flux calculations. This parameterization differs from previous works by being formulated not only with R e but also with M i . We also investigated the sensitivity of dust-aerosol forcing to R e , M i , optical depth (τ), and solar zenith angle (SZA). The results show that the value of shortwave (SW) radiative forcing (RF) at the TOA changes from negative to positive as the M i is increasing, which means that, as the absorption of dust particles becomes stronger, more energy is kept in the atmosphere to heat the earth–atmosphere system. The SW RF gradually becomes less negative at the TOA and more negative at the surface with increasing R e , due to the decreases of reflection and transmission along with the single-scattering albedo decreasing. As the optical depth increases, the values of the SW RF decrease because of the strong attenuation for heavy loading. When SZA increases, the SW RF becomes more negative at both the TOA and the surface due to the long optical path at a large SZA. The errors induced from the parameterized SSPs of dust in the SW RF calculation are very small, which are less than 2.1%, demonstrating the accuracy of the parameterization and its reliability for climate model applications.


2019 ◽  
Vol 12 (3) ◽  
pp. 1209-1225 ◽  
Author(s):  
Christoph A. Keller ◽  
Mat J. Evans

Abstract. Atmospheric chemistry models are a central tool to study the impact of chemical constituents on the environment, vegetation and human health. These models are numerically intense, and previous attempts to reduce the numerical cost of chemistry solvers have not delivered transformative change. We show here the potential of a machine learning (in this case random forest regression) replacement for the gas-phase chemistry in atmospheric chemistry transport models. Our training data consist of 1 month (July 2013) of output of chemical conditions together with the model physical state, produced from the GEOS-Chem chemistry model v10. From this data set we train random forest regression models to predict the concentration of each transported species after the integrator, based on the physical and chemical conditions before the integrator. The choice of prediction type has a strong impact on the skill of the regression model. We find best results from predicting the change in concentration for long-lived species and the absolute concentration for short-lived species. We also find improvements from a simple implementation of chemical families (NOx = NO + NO2). We then implement the trained random forest predictors back into GEOS-Chem to replace the numerical integrator. The machine-learning-driven GEOS-Chem model compares well to the standard simulation. For ozone (O3), errors from using the random forests (compared to the reference simulation) grow slowly and after 5 days the normalized mean bias (NMB), root mean square error (RMSE) and R2 are 4.2 %, 35 % and 0.9, respectively; after 30 days the errors increase to 13 %, 67 % and 0.75, respectively. The biases become largest in remote areas such as the tropical Pacific where errors in the chemistry can accumulate with little balancing influence from emissions or deposition. Over polluted regions the model error is less than 10 % and has significant fidelity in following the time series of the full model. Modelled NOx shows similar features, with the most significant errors occurring in remote locations far from recent emissions. For other species such as inorganic bromine species and short-lived nitrogen species, errors become large, with NMB, RMSE and R2 reaching >2100 % >400 % and <0.1, respectively. This proof-of-concept implementation takes 1.8 times more time than the direct integration of the differential equations, but optimization and software engineering should allow substantial increases in speed. We discuss potential improvements in the implementation, some of its advantages from both a software and hardware perspective, its limitations, and its applicability to operational air quality activities.


2017 ◽  
Author(s):  
Ben Newsome ◽  
Mat Evans

Abstract. Chemical rate constants determine the composition of the atmosphere and how this composition has changed over time. They are central to our understanding of climate change and air quality degradation. Atmospheric chemistry models, whether online or offline, box, regional or global use these rate constants. Expert panels synthesise laboratory measurements, making recommendations for the rate constants that should be used. This results in very similar or identical rate constants being used by all models. The inherent uncertainties in these recommendations are, in general, therefore ignored. We explore the impact of these uncertainties on the composition of the troposphere using the GEOS-Chem chemistry transport model. Based on the JPL and IUPAC evaluations we assess 50 mainly inorganic rate constants and 10 photolysis rates, through simulations where we increase the rate of the reactions to the 1σ upper value recommended by the expert panels. We assess the impact on 4 standard metrics: annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime. Uncertainty in the rate constants for NO2 + OH    M →  HNO3, OH + CH4 → CH3O2 + H2O and O3 + NO → NO2 + O2 are the three largest source of uncertainty in these metrics. We investigate two methods of assessing these uncertainties, addition in quadrature and a Monte Carlo approach, and conclude they give similar outcomes. Combining the uncertainties across the 60 reactions, gives overall uncertainties on the annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime of 11, 12, 17 and 17 % respectively. These are larger than the spread between models in recent model inter-comparisons. Remote regions such as the tropics, poles, and upper troposphere are most uncertain. This chemical uncertainty is sufficiently large to suggest that rate constant uncertainty should be considered when model results disagree with measurement. Calculations for the pre-industrial allow a tropospheric ozone radiative forcing to be calculated of 0.412 ± 0.062 Wm−2. This uncertainty (15 %) is comparable to the inter-model spread in ozone radiative forcing found in previous model-model inter-comparison studies where the rate constants used in the models are all identical or very similar. Thus the uncertainty of tropospheric ozone radiative forcing should expanded to include this additional source of uncertainty. These rate constant uncertainties are significant and suggest that refinement of supposedly well known chemical rate constants should be considered alongside other improvements to enhance our understanding of atmospheric processes.


2017 ◽  
Author(s):  
Jianrong Bi ◽  
Jianping Huang ◽  
Jinsen Shi ◽  
Zhiyuan Hu ◽  
Tian Zhou ◽  
...  

Abstract. We conducted a comprehensive field campaign on exploring the optical characteristics of mineral dust in Dunhuang farmland nearby the Gobi deserts of northwest China during spring of 2012. The day-to-day and diurnal variations of dust aerosol showed prominent features throughout the experiment, primarily attributable to frequent dust events and local anthropogenic emissions. The overall average mass concentration of the particulate matter with an aerodynamic diameter less than 10 μm (PM10), light scattering coefficient (σsp,670), absorption coefficient (σap,670), and single-scattering albedo (SSA670) were 113±169 μgm-3, 53.3 ± 74.8 Mm-1,  3.2± 2.4 Mm-1, and 0.913 ± 0.05, which were comparable to the background levels in southern United States, but smaller than that in the eastern and other northwestern China. The anthropogenic dust produced by agricultural cultivations (e.g., land planning, plowing, and disking) exerted a significant superimposed effect on high dust concentrations in Dunhuang farmland prior to the growing season (i.e., from 1 April to 10 May). Strong south valley wind and vertical mixing in daytime scavenged the pollution and weak northeast mountain wind and stable inversion layer at night favorably accumulated the air pollutants near the surface. In the afternoon (13:00–18:00 LT), mean SSA670 was 0.945 ± 0.04 that was predominant by dust particles, whereas finer particles and lower SSA670 values (~ 0.90–0.92) were measured at night, suggesting the potential influence by the mixed dust-pollutants. During a typical biomass burning event on 4 April 2012, σap,670 changed from ~ 2.0 Mm-1 to 4.75 Mm-1 and SSA670 changed from ~ 0.90 to ~ 0.83, implying remarkable modification of aerosol absorptive properties induced by human activities. The findings of this study would help to advance an in-depth understanding of the interaction among dust aerosol, atmospheric chemistry, and climate change in desert source region.


2015 ◽  
Vol 8 (7) ◽  
pp. 2901-2907 ◽  
Author(s):  
Z. Wang ◽  
D. Liu ◽  
Y. Wang ◽  
Z. Wang ◽  
G. Shi

Abstract. A strong diurnal variation of aerosol has been observed in many heavily polluted regions in China. This variation could affect the direct aerosol radiative forcing (DARF) evaluation if the daily averaged value is used as normal rather than the time-resolved values. To quantify the effect of using the daily averaged DARF, 196 days of high temporal resolution ground-based data collected in SKYNET Hefei site during the period from 2007 to 2013 is used to perform an assessment. We demonstrate that strong diurnal changes of heavy aerosol loading have an impact on the 24-h averaged DARF when daily averaged optical properties are used to retrieve this quantity. The DARF errors varying from −7.6 to 15.6 W m−2 absolutely and from 0.1 to 28.5 % relatively were found between the calculations using daily average aerosol properties, and those using time-resolved aerosol observations. These errors increase with increasing daily aerosol optical depth (AOD) and decreasing daily single-scattering albedo (SSA), indicating that the high temporal resolution DARF data set should be used in the model instead of the normal daily-averaged one, especially under heavy aerosol loading conditions for regional campaign studies. We also found that statistical errors (0.3 W m−2 absolutely and 11.8 % relatively) will be less, which means that the effect of using the daily averaged DARF can be weakened by using a long-term observational data set.


2020 ◽  
Author(s):  
Franziska Winterstein ◽  
Patrick Jöckel ◽  
Martin Dameris ◽  
Michael Ponater ◽  
Fabian Tanalski ◽  
...  

&lt;p&gt;Methane (CH&lt;sub&gt;4&lt;/sub&gt;) is the second most important greenhouse gas, which atmospheric concentration is influenced by human activities and currently on a sharp rise. We present a study with numerical simulations using a Chemistry-Climate-Model (CCM), which are performed to assess possible consequences of strongly enhanced CH&lt;sub&gt;4&lt;/sub&gt; concentrations in the Earth's atmosphere for the climate.&lt;/p&gt;&lt;p&gt;Our analysis includes experiments with 2xCH&lt;sub&gt;4&lt;/sub&gt; and 5xCH&lt;sub&gt;4&lt;/sub&gt; present day (2010) lower boundary mixing ratios using the CCM EMAC. The simulations are conducted with prescribed oceanic conditions, mimicking present day tropospheric temperatures as its changes are largely suppressed. By doing so we are able to investigate the quasi-instantaneous chemical impact on the atmosphere. We find that the massive increase in CH&lt;sub&gt;4&lt;/sub&gt; strongly influences the tropospheric chemistry by reducing the OH abundance and thereby extending the tropospheric CH&lt;sub&gt;4&lt;/sub&gt; lifetime as well as the residence time of other chemical pollutants. The region above the tropopause is impacted by a substantial rise in stratospheric water vapor (SWV). The stratospheric ozone (O&lt;sub&gt;3&lt;/sub&gt;) column increases overall, but SWV induced stratospheric cooling also leads to enhanced ozone depletion in the Antarctic lower stratosphere. Regional&amp;#160; patterns of ozone change are affected by modification of stratospheric dynamics, i.e. increased tropical up-welling and stronger meridional transport&amp;#160; towards the polar regions. We calculate the net radiative impact (RI) of the 2xCH&lt;sub&gt;4&lt;/sub&gt; experiment to be 0.69 W m&lt;sup&gt;-2&lt;/sup&gt; and for the 5xCH&lt;sub&gt;4&lt;/sub&gt; experiment to be 1.79 W m&lt;sup&gt;-2&lt;/sup&gt;. A substantial part of the RI is contributed by chemically induced O&lt;sub&gt;3&lt;/sub&gt; and SWV changes, in line with previous radiative forcing estimates and is for the first time splitted and spatially asigned to its chemical contributors.&lt;/p&gt;&lt;p&gt;This numerical study using a CCM with prescibed oceanic conditions shows the rapid responses to significantly enhanced CH&lt;sub&gt;4&lt;/sub&gt; mixing ratios, which is the first step towards investigating the impact of possible strong future CH&lt;sub&gt;4&lt;/sub&gt; emissions on atmospheric chemistry and its feedback on climate.&lt;/p&gt;


2014 ◽  
Vol 14 (1) ◽  
pp. 267-282 ◽  
Author(s):  
A. T. Brown ◽  
M. P. Chipperfield ◽  
N. A. D. Richards ◽  
C. Boone ◽  
P. F. Bernath

Abstract. Fluorine-containing species can be extremely effective atmospheric greenhouse gases. We present fluorine budgets using organic and inorganic species retrieved by the ACE-FTS satellite instrument supplemented with output from the SLIMCAT 3-D chemical transport model. The budgets are calculated between 2004 and 2009 for a number of latitude bands: 70–30° N, 30–00° N, 00° N–30° S, and 30–70° S. At lower altitudes total fluorine profiles are dominated by the contribution from CFC-12, up to an altitude of 20 km in the extra-tropics and 29 km in the tropics; above these altitudes the profiles are dominated by hydrogen fluoride (HF). Our data show that total fluorine profiles at all locations have a negative slope with altitude, providing evidence that overall fluorine emissions (measured by their F content) have been increasing with time. Total stratospheric fluorine is increasing at a similar rate in the tropics: 32.5 ± 4.9 ppt yr−1 (1.31 ± 0.20% per year) in the Northern Hemisphere (NH) and 29.8 ± 5.3 ppt yr−1 (1.21 ± 0.22% per year) in the Southern Hemisphere (SH). Extra-tropical total stratospheric fluorine is also increasing at a similar rate in both the NH and SH: 28.3 ± 2.7 ppt per year (1.12 ± 0.11% per year) in the NH and 24.3 ± 3.1 ppt per year (0.96 ± 0.12% per year) in the SH. The calculation of radiative efficiency-weighted total fluorine allows the changes in radiative forcing between 2004 and 2009 to be calculated. These results show an increase in radiative forcing of between 0.23 ± 0.11% per year and 0.45 ± 0.11% per year, due to the increase in fluorine-containing species during this time. The decreasing trends in the mixing ratios of halons and chlorofluorocarbons (CFCs), due to their prohibition under the Montreal Protocol, have suppressed an increase in total fluorine caused by increasing mixing ratios of hydrofluorocarbons (HFCs). This has reduced the impact of fluorine-containing species on global warming.


2009 ◽  
Vol 9 (1) ◽  
pp. 1977-2020
Author(s):  
F. Khosrawi ◽  
R. Müller ◽  
M. H. Proffitt ◽  
R. Ruhnke ◽  
O. Kirner ◽  
...  

Abstract. 1-year data sets of monthly averaged nitrous oxide (N2O) and ozone (O3) derived from satellite measurements were used as a tool for the evaluation of atmospheric photochemical models. Two 1-year data sets, one derived from the Improved Limb Atmospheric Spectrometer (ILAS and ILAS-II) and one from the Odin Sub-Millimetre Radiometer (Odin/SMR) were employed. Here, these data sets are used for the evaluation of two Chemical Transport Models (CTMs), the Karlsruhe Simulation Model of the Middle Atmosphere (KASIMA) and the Chemical Lagrangian Model of the Stratosphere (CLaMS) as well as for one Chemistry-Climate Model (CCM), the atmospheric chemistry general circulation model ECHAM5/MESSy1 (E5M1) in the lower stratosphere with focus on the Northern Hemisphere. Since the Odin/SMR measurements cover the entire hemisphere, the evaluation is performed for the entire hemisphere as well as for the low latitudes, midlatitudes and high latitudes using the Odin/SMR 1-year data set as reference. To assess the impact of using different data sets for such an evaluation study we repeat the evaluation for the polar lower stratosphere using the ILAS/ILAS-II data set. Only small differences were found using ILAS/ILAS-II instead of Odin/SMR as a reference, thus, showing that the results are not influenced by the particular satellite data set used for the evaluation. The evaluation of CLaMS, KASIMA and E5M1 shows that all models are in good agreement with Odin/SMR and ILAS/ILAS-II. Differences are generally in the range of ±20%. Larger differences (up to −40%) are found in all models at 500±25 K for N2O mixing ratios greater than 200 ppb. Generally, the largest differences were found for the tropics and the lowest for the polar regions. However, an underestimation of polar winter ozone loss was found both in KASIMA and E5M1 both in the Northern and Southern Hemisphere.


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