scholarly journals Large hemispheric difference in nucleation mode aerosol concentrations in the lowermost stratosphere at mid- and high latitudes

2021 ◽  
Vol 21 (11) ◽  
pp. 9065-9088
Author(s):  
Christina J. Williamson ◽  
Agnieszka Kupc ◽  
Andrew Rollins ◽  
Jan Kazil ◽  
Karl D. Froyd ◽  
...  

Abstract. The details of aerosol processes and size distributions in the stratosphere are important for both heterogeneous chemistry and aerosol–radiation interactions. Using in situ, global-scale measurements of the size distribution of particles with diameters > 3 nm from the NASA Atmospheric Tomography Mission (ATom), we identify a mode of aerosol smaller than 12 nm in the lowermost stratosphere (LMS) at mid- and high latitudes. This mode is substantial only in the Northern Hemisphere (NH) and was observed in all four seasons. We also observe elevated SO2, an important precursor for new particle formation (NPF) and growth, in the NH LMS. We use box modelling and thermodynamic calculations to show that NPF can occur in the LMS conditions observed on ATom. Aircraft emissions are shown as likely sources of this SO2, as well as a potential source of nucleation mode particles directly emitted by or formed in the plume of the engines. These nucleation mode particles have the potential to grow to larger sizes and to coagulate with larger aerosol, affecting heterogeneous chemistry and aerosol–radiation interactions. Understanding all sources and characteristics of stratospheric aerosols is important in the context of anthropogenic climate change as well as proposals for climate intervention via stratospheric sulfur injection. This analysis not only adds to the, currently sparse, observations of the global impact of aviation, but also introduces another aspect of climate influence, namely a size distribution shift of the background aerosol distribution in the LMS.

2021 ◽  
Author(s):  
Christina J. Williamson ◽  
Agnieszka Kupc ◽  
Andrew Rollins ◽  
Jan Kazil ◽  
Karl D. Froyd ◽  
...  

Abstract. The details of aerosol processes and size distributions in the stratosphere are important for both heterogeneous chemistry and aerosol-radiation interactions. Using in-situ, global-scale measurements of the size distribution of particles with diameters > 3 nm from the NASA Atmospheric Tomography Mission (ATom), we identify a mode of ultrafine aerosol in the lowermost stratosphere (LMS) at mid and high latitudes. This mode is substantial only in the northern hemisphere (NH), and was observed in all four seasons. We also observe elevated SO2, an important precursor for new particle formation (NPF) and growth, in the NH LMS. We use box modelling and thermodynamic calculations to show that NPF can occur in the LMS conditions observed on ATom. Aircraft emissions are shown as likely sources of this SO2, as well as a potential source of ultrafine particles directly emitted by, or formed in the plume of the engines. These ultra-fine particles have the potential to grow to larger sizes, and to coagulate with larger aerosol, affecting heterogeneous chemistry and aerosol-radiation interactions. Understanding all sources and characteristics of stratospheric aerosol is important in the context of anthropogenic climate change as well as proposals for climate intervention via stratospheric sulphur injection. This analysis not only adds to the, currently sparse, observations of the global impact of aviation, but also introduces another aspect of climate influence, namely a size distribution shift of the background aerosol distribution in the LMS.


2017 ◽  
Vol 17 (3) ◽  
pp. 1901-1929 ◽  
Author(s):  
Claudia Di Biagio ◽  
Paola Formenti ◽  
Yves Balkanski ◽  
Lorenzo Caponi ◽  
Mathieu Cazaunau ◽  
...  

Abstract. Modeling the interaction of dust with long-wave (LW) radiation is still a challenge because of the scarcity of information on the complex refractive index of dust from different source regions. In particular, little is known about the variability of the refractive index as a function of the dust mineralogical composition, which depends on the specific emission source, and its size distribution, which is modified during transport. As a consequence, to date, climate models and remote sensing retrievals generally use a spatially invariant and time-constant value for the dust LW refractive index. In this paper, the variability of the mineral dust LW refractive index as a function of its mineralogical composition and size distribution is explored by in situ measurements in a large smog chamber. Mineral dust aerosols were generated from 19 natural soils from 8 regions: northern Africa, the Sahel, eastern Africa and the Middle East, eastern Asia, North and South America, southern Africa, and Australia. Soil samples were selected from a total of 137 available samples in order to represent the diversity of sources from arid and semi-arid areas worldwide and to account for the heterogeneity of the soil composition at the global scale. Aerosol samples generated from soils were re-suspended in the chamber, where their LW extinction spectra (3–15 µm), size distribution, and mineralogical composition were measured. The generated aerosol exhibits a realistic size distribution and mineralogy, including both the sub- and super-micron fractions, and represents in typical atmospheric proportions the main LW-active minerals, such as clays, quartz, and calcite. The complex refractive index of the aerosol is obtained by an optical inversion based upon the measured extinction spectrum and size distribution. Results from the present study show that the imaginary LW refractive index (k) of dust varies greatly both in magnitude and spectral shape from sample to sample, reflecting the differences in particle composition. In the 3–15 µm spectral range, k is between ∼ 0.001 and 0.92. The strength of the dust absorption at ∼ 7 and 11.4 µm depends on the amount of calcite within the samples, while the absorption between 8 and 14 µm is determined by the relative abundance of quartz and clays. The imaginary part (k) is observed to vary both from region to region and for varying sources within the same region. Conversely, for the real part (n), which is in the range 0.84–1.94, values are observed to agree for all dust samples across most of the spectrum within the error bars. This implies that while a constant n can be probably assumed for dust from different sources, a varying k should be used both at the global and the regional scale. A linear relationship between the magnitude of the imaginary refractive index at 7.0, 9.2, and 11.4 µm and the mass concentration of calcite and quartz absorbing at these wavelengths was found. We suggest that this may lead to predictive rules to estimate the LW refractive index of dust in specific bands based on an assumed or predicted mineralogical composition, or conversely, to estimate the dust composition from measurements of the LW extinction at specific wavebands. Based on the results of the present study, we recommend that climate models and remote sensing instruments operating at infrared wavelengths, such as IASI (infrared atmospheric sounder interferometer), use regionally dependent refractive indices rather than generic values. Our observations also suggest that the refractive index of dust in the LW does not change as a result of the loss of coarse particles by gravitational settling, so that constant values of n and k could be assumed close to sources and following transport. The whole dataset of the dust complex refractive indices presented in this paper is made available to the scientific community in the Supplement.


2021 ◽  
Author(s):  
Christina J Williamson ◽  
Agnieszka Kupc ◽  
Andrew Rollins ◽  
Jan Kazil ◽  
Karl D Froyd ◽  
...  

<p>On the NASA Atmospheric Tomography Mission (ATom), we observed a sharp hemispheric contrast in the concentration of ultrafine aerosols (3-12 nm diameter) in the lowermost stratosphere that persisted through all four seasons. Exploring possible causes, we show that this is likely caused by aircraft, which emit both ultrafine aerosol and precursor gases for new particle formation (NPF) in quantities that agree well with our observations. While aircraft may emit a range of NPF precursors, we focus here on sulphur dioxide (a major source of atmospheric sulphuric acid), of which we have observations from the same mission.  We observe the same hemispheric contrast in sulphur dioxide as ultrafine aerosol, and find that the observed concentrations are in alignment with inventoried aircraft emissions. We present box modeling and thermodynamic calculations that support the plausibility of NPF under the conditions and sulphur dioxide concentrations observed on ATom.</p><p>While the direct climate impact of ultrafine aerosol in the lowermost stratosphere (LMS) may currently be small, our observations show a definitive size distribution shift of the background aerosol distribution in the northern hemisphere. This is important for assessing aviation impacts, and the expected impacts of increased air-traffic. Furthermore, climate intervention via injection of sulphate or aerosols into the stratosphere is a current subject of research. Our study shows that NPF is possible and likely already happening in the LMS, which must be accounted for in models for stratospheric modification, and points out that we must consider that any intentional stratospheric modification will be applied to two very different hemispheres: a largely pristine southern hemisphere; and an already anthropogenically modified northern hemisphere.</p>


2016 ◽  
Author(s):  
Claudia Di Biagio ◽  
Paola Formenti ◽  
Yves Balkanski ◽  
Lorenzo Caponi ◽  
Mathieu Cazaunau ◽  
...  

Abstract. Modelling the interaction of dust with longwave (LW) radiation is still a challenge due to the scarcity of information on the complex refractive index of dust from different source regions. In particular, little is known on the variability of the refractive index as a function of the dust mineralogical composition, depending on the source region of emission, and the dust size distribution, which is modified during transport. As a consequence, to date, climate models and remote sensing retrievals generally use a spatially-invariant and time-constant value for the dust LW refractive index. In this paper the variability of the mineral dust LW refractive index as a function of its mineralogical composition and size distribution is explored by in situ measurements in a large smog chamber. Mineral dust aerosols were generated from nineteen natural soils from Northern Africa, Sahel, Middle East, Eastern Asia, North and South America, Southern Africa, and Australia. Soil samples were selected from a total of 137 samples available in order to represent the diversity of sources from arid and semi-arid areas worldwide and to account for the heterogeneity of the soil composition at the global scale. Aerosol samples generated from soils were re-suspended in the chamber, where their LW extinction spectra (2–16 µm), size distribution, and mineralogical composition were measured. The generated aerosol exhibits a realistic size distribution and mineralogy, including both the sub- and super-micron fractions, and represents in typical atmospheric proportions the main LW-active minerals, such as clays, quartz, and calcite. The complex refractive index of the aerosol is obtained by an optical inversion based upon the measured extinction spectrum and size distribution. Results from the present study show that the LW refractive index of dust varies greatly both in magnitude and spectral shape from sample to sample, following the changes in the measured particle composition. The real part (n) of the refractive index is between 0.84 and 1.94, while the imaginary part (k) is ~ 0.001 and 0.92. For instance, the strength of the absorption at ~ 7 and 11.4 µm depends on the amount of calcite within the samples, while the absorption between 8 and 14 µm is determined by the relative abundance of quartz and clays. A linear relationship between the magnitude of the refractive index at 7.0, 9.2, and 11.4 µm and the mass concentration of calcite and quartz absorbing at these wavelengths was found. We suggest that this may lead to predictive rules to estimate the LW refractive index of dust in specific bands based on an assumed or predicted mineralogical composition, or conversely, to estimate the dust composition from measurements of the LW extinction at specific wavebands. Based on the results of the present study, we recommend using refractive indices specific for the different source regions, rather than generic values, in climate models and remote sensing applications. Our observations also suggest that the refractive index of dust in the LW does not change due to the loss of coarse particles by gravitational settling, so that a constant value could be assumed close to sources and during transport. The results of the present study also clearly suggest that the LW refractive index of dust varies at the regional scale. This regional variability has to be characterized further in order to better assess the influence of dust on regional climate, as well as to increase the accuracy of satellite retrievals over regions affected by dust. We make the whole dataset of the dust complex refractive indices obtained here available to the scientific community by publishing it in the supplementary material to this paper.


2020 ◽  
Vol 20 (21) ◽  
pp. 12955-12982
Author(s):  
Debbie O'Sullivan ◽  
Franco Marenco ◽  
Claire L. Ryder ◽  
Yaswant Pradhan ◽  
Zak Kipling ◽  
...  

Abstract. We investigate the dust forecasts from two operational global atmospheric models in comparison with in situ and remote sensing measurements obtained during the AERosol properties – Dust (AER-D) field campaign. Airborne elastic backscatter lidar measurements were performed on board the Facility for Airborne Atmospheric Measurements during August 2015 over the eastern Atlantic, and they permitted us to characterise the dust vertical distribution in detail, offering insights on transport from the Sahara. They were complemented with airborne in situ measurements of dust size distribution and optical properties, as well as datasets from the Cloud–Aerosol Transport System (CATS) spaceborne lidar and the Moderate Resolution Imaging Spectroradiometer (MODIS). We compare the airborne and spaceborne datasets to operational predictions obtained from the Met Office Unified Model (MetUM) and the Copernicus Atmosphere Monitoring Service (CAMS). The dust aerosol optical depth predictions from the models are generally in agreement with the observations but display a low bias. However, the predicted vertical distribution places the dust lower in the atmosphere than highlighted in our observations. This is particularly noticeable for the MetUM, which does not transport coarse dust high enough in the atmosphere or far enough away from the source. We also found that both model forecasts underpredict coarse-mode dust and at times overpredict fine-mode dust, but as they are fine-tuned to represent the observed optical depth, the fine mode is set to compensate for the underestimation of the coarse mode. As aerosol–cloud interactions are dependent on particle numbers rather than on the optical properties, this behaviour is likely to affect their correct representation. This leads us to propose an augmentation of the set of aerosol observations available on a global scale for constraining models, with a better focus on the vertical distribution and on the particle size distribution. Mineral dust is a major component of the climate system; therefore, it is important to work towards improving how models reproduce its properties and transport mechanisms.


2016 ◽  
Vol 16 (14) ◽  
pp. 9435-9455 ◽  
Author(s):  
Matthew J. Alvarado ◽  
Chantelle R. Lonsdale ◽  
Helen L. Macintyre ◽  
Huisheng Bian ◽  
Mian Chin ◽  
...  

Abstract. Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10–23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction throughout the aerosol size distribution. Using a core-shell mixing rule in ASP overestimates aerosol absorption, especially for the fresh biomass burning aerosol measured in ARCTAS-B, suggesting the need for modeling the time-varying mixing states of aerosols in future versions of ASP.


2021 ◽  
Vol 13 (11) ◽  
pp. 2081
Author(s):  
Elisa Adirosi ◽  
Mario Montopoli ◽  
Alessandro Bracci ◽  
Federico Porcù ◽  
Vincenzo Capozzi ◽  
...  

The high relevance of satellites for collecting information regarding precipitation at global scale implies the need of a continuous validation of satellite products to ensure good data quality over time and to provide feedback for updating and improving retrieval algorithms. However, validating satellite products using measurements collected by sensors at ground is still a challenging task. To date, the Dual-frequency Precipitation Radar (DPR) aboard the Core Satellite of the Global Precipitation Measurement (GPM) mission is the only active sensor able to provide, at global scale, vertical profiles of rainfall rate, radar reflectivity, and Drop Size Distribution (DSD) parameters from space. In this study, we compare near surface GPM retrievals with long time series of measurements collected by seven laser disdrometers in Italy since the launch of the GPM mission. The comparison shows limited differences in the performances of the different GPM algorithms, be they dual- or single-frequency, although in most cases, the dual-frequency algorithms present the better performances. Furthermore, the agreement between satellite and ground-based estimates depends on the considered precipitation variable. The agreement is very promising for rain rate, reflectivity factor, and the mass-weighted mean diameter (Dm), while the satellite retrievals need to be improved for the normalized gamma DSD intercept parameter (Nw).


2014 ◽  
Vol 67 (4) ◽  
pp. 405-412
Author(s):  
Christiane Ribeiro da Silva ◽  
Vládia C. G. de Souza ◽  
Jair C. Koppe

A methodology to determine the size distribution curve of the ROM was developed in a Brazilian iron ore mine. The size of the larger fragments was determined taking photographs and setting the scale of the images to analyze their dimensions (length of their edges and areas). This was implemented according to a specific protocol of sampling that involves split and homogenization stages in situ of a considerable quantity of ore (about 259 metric tonnes). During the sampling process, larger fragments were separated and smaller size material was screened. The methodology was developed initially in order to preview the performance of a primary gyratory crusher that is fed directly from trucks. Operational conditions of the equipment such as closed and open-side settings could be adjusted previously, obtaining different product size distributions. Variability of size of the fragments affects subsequent stages of crushing and can increase circulating load in the circuit. This leads to a decrease of productivity or recovery of the ore dressing. The results showed insignificant errors of accuracy and reproducibility of the sampling protocol when applied to friable itabirite rocks.


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