scholarly journals Sensitivity of aerosol radiative effects to different mixing assumptions in the AEROPT 1.0 submodel of the EMAC atmospheric-chemistry–climate model

2014 ◽  
Vol 7 (5) ◽  
pp. 2503-2516 ◽  
Author(s):  
K. Klingmüller ◽  
B. Steil ◽  
C. Brühl ◽  
H. Tost ◽  
J. Lelieveld

Abstract. The modelling of aerosol radiative forcing is a major cause of uncertainty in the assessment of global and regional atmospheric energy budgets and climate change. One reason is the strong dependence of the aerosol optical properties on the mixing state of aerosol components, such as absorbing black carbon and, predominantly scattering sulfates. Using a new column version of the aerosol optical properties and radiative-transfer code of the ECHAM/MESSy atmospheric-chemistry–climate model (EMAC), we study the radiative transfer applying various mixing states. The aerosol optics code builds on the AEROPT (AERosol OPTical properties) submodel, which assumes homogeneous internal mixing utilising the volume average refractive index mixing rule. We have extended the submodel to additionally account for external mixing, partial external mixing and multilayered particles. Furthermore, we have implemented the volume average dielectric constant and Maxwell Garnett mixing rule. We performed regional case studies considering columns over China, India and Africa, corroborating much stronger absorption by internal than external mixtures. Well-mixed aerosol is a good approximation for particles with a black-carbon core, whereas particles with black carbon at the surface absorb significantly less. Based on a model simulation for the year 2005, we calculate that the global aerosol direct radiative forcing for homogeneous internal mixing differs from that for external mixing by about 0.5 W m−2.

2014 ◽  
Vol 7 (3) ◽  
pp. 3367-3402
Author(s):  
K. Klingmüller ◽  
B. Steil ◽  
C. Brühl ◽  
H. Tost ◽  
J. Lelieveld

Abstract. The modelling of aerosol radiative forcing is a major cause of uncertainty in the assessment of global and regional atmospheric energy budgets and climate change. One reason is the strong dependence of the aerosol optical properties on the mixing state of aerosol components like black carbon and sulphates. Using a new column version of the aerosol optical properties and radiative transfer code of the atmospheric chemistry-climate model EMAC, we study the radiative transfer applying various mixing states. The aerosol optics code builds on the AEROPT submodel which assumes homogeneous internal mixing utilising the volume average refractive index mixing rule. We have extended the submodel to additionally account for external mixing, partial external mixing and multi-layered particles. Furthermore, we have implemented the volume average dielectric-constant and Maxwell Garnett Mixing rule. We performed regional case studies considering columns over China, India and Africa, corroborating much stronger absorption by internal than external mixtures. Well mixed aerosol is a good approximation for particles with a black carbon core, whereas particles with black carbon at the surface absorb significantly less. Based on a model simulation for the year 2005 we calculate that the global aerosol direct radiative-forcing for homogeneous internal mixing differs from that for external mixing by about 0.5 W m−2.


2016 ◽  
Author(s):  
Simone Dietmüller ◽  
Patrick Jöckel ◽  
Holger Tost ◽  
Markus Kunze ◽  
Cathrin Gellhorn ◽  
...  

Abstract. The Modular Earth Submodel System (MESSy) provides an interface to couple submodels to a basemodel via a highly flexible data management facility (Jöckel et al., 2010). In the present paper we present the four new radiation related submodels RAD, AEROPT, CLOUDOPT and ORBIT. The submodel RAD (with shortwave radiation scheme RAD_FUBRAD) simulates the radiative transfer, the submodel AEROPT calculates the aerosol optical properties, the submodel CLOUDOPT calculates the cloud optical properties, and the submodel ORBIT is responsible for Earth orbit calculations. These submodels are coupled via the standard MESSy infrastructure and are largely based on the original radiation scheme of the general circulation model ECHAM5, however, expanded with additional features. These features comprise, among others, user-friendly and flexibly controllable (by namelists) on-line radiative forcing calculations by multiple diagnostic calls of the radiation routines. With this, it is now possible to calculate radiative forcing (instantaneous as well as stratosphere adjusted) of various greenhouse gases simultaneously in only one simulation, as well as the radiative forcing of cloud perturbations. Examples of on-line radiative forcing calculations in the ECHAM/MESSy Atmospheric Chemistry (EMAC) model are presented.


2017 ◽  
Vol 10 (1) ◽  
pp. 433-452 ◽  
Author(s):  
Bjorn Stevens ◽  
Stephanie Fiedler ◽  
Stefan Kinne ◽  
Karsten Peters ◽  
Sebastian Rast ◽  
...  

Abstract. A simple plume implementation of the second version (v2) of the Max Planck Institute Aerosol Climatology, MACv2-SP, is described. MACv2-SP provides a prescription of anthropogenic aerosol optical properties and an associated Twomey effect. It was created to provide a harmonized description of post-1850 anthropogenic aerosol radiative forcing for climate modeling studies. MACv2-SP has been designed to be easy to implement, change and use, and thereby enable studies exploring the climatic effects of different patterns of aerosol radiative forcing, including a Twomey effect. MACv2-SP is formulated in terms of nine spatial plumes associated with different major anthropogenic source regions. The shape of the plumes is fit to the Max Planck Institute Aerosol Climatology, version 2, whose present-day (2005) distribution is anchored by surface-based observations. Two types of plumes are considered: one predominantly associated with biomass burning, the other with industrial emissions. These differ in the prescription of their annual cycle and in their optical properties, thereby implicitly accounting for different contributions of absorbing aerosol to the different plumes. A Twomey effect for each plume is prescribed as a change in the host model's background cloud-droplet population density using relationships derived from satellite data. Year-to-year variations in the amplitude of the plumes over the historical period (1850–2016) are derived by scaling the plumes with associated national emission sources of SO2 and NH3. Experiments using MACv2-SP are performed with the Max Planck Institute Earth System Model. The globally and annually averaged instantaneous and effective aerosol radiative forcings are estimated to be −0.6 and −0.5 W m−2, respectively. Forcing from aerosol–cloud interactions (the Twomey effect) offsets the reduction of clear-sky forcing by clouds, so that the net effect of clouds on the aerosol forcing is small; hence, the clear-sky forcing, which is more readily measurable, provides a good estimate of the total aerosol forcing.


2022 ◽  
Vol 22 (1) ◽  
pp. 561-575
Author(s):  
Jiaxing Sun ◽  
Zhe Wang ◽  
Wei Zhou ◽  
Conghui Xie ◽  
Cheng Wu ◽  
...  

Abstract. Atmospheric aerosols play an important role in the radiation balance of the earth–atmosphere system. However, our knowledge of the long-term changes in equivalent black carbon (eBC) and aerosol optical properties in China is very limited. Here we analyze the 9-year measurements of eBC and aerosol optical properties from 2012 to 2020 in Beijing, China. Our results showed large reductions in eBC by 71 % from 6.25 ± 5.73 µg m−3 in 2012 to 1.80 ± 1.54 µg m−3 in 2020 and 47 % decreases in the light extinction coefficient (bext, λ = 630 nm) of fine particles due to the Clean Air Action Plan that was implemented in 2013. The seasonal and diurnal variations of eBC illustrated the most significant reductions in the fall and at nighttime, respectively. ΔeBC / ΔCO also showed an annual decrease from ∼ 7 to 4 ng m−3 ppbv−1 and presented strong seasonal variations with high values in spring and fall, indicating that primary emissions in Beijing have changed significantly. As a response to the Clean Air Action Plan, single-scattering albedo (SSA) showed a considerable increase from 0.79 ± 0.11 to 0.88 ± 0.06, and mass extinction efficiency (MEE) increased from 3.2 to 3.8 m2 g−1. These results highlight the increasing importance of scattering aerosols in radiative forcing and a future challenge in visibility improvement due to enhanced MEE. Brown carbon (BrC) showed similar changes and seasonal variations to eBC during 2018–2020. However, we found a large increase of secondary BrC in the total BrC in most seasons, particularly in summer with the contribution up to 50 %, demonstrating an enhanced role of secondary formation in BrC in recent years. The long-term changes in eBC and BrC have also affected the radiative forcing effect. The direct radiative forcing (ΔFR) of BC decreased by 67 % from +3.36 W m−2 in 2012 to +1.09 W m−2 in 2020, and that of BrC decreased from +0.30 to +0.17 W m−2 during 2018–2020. Such changes might have important implications for affecting aerosol–boundary layer interactions and the improvement of future air quality.


2021 ◽  
Author(s):  
Yaowei Li ◽  
John Dykema ◽  
Frank Keutsch

<p>Model results suggest organic aerosol represents a significant fraction of total stratospheric aerosol radiative forcing, which in itself could represent as much as a quarter of global radiative forcing. Other model investigations suggest that the radiative influence of organic aerosols and dust must be included to obtain consistency with satellite measurements of stratospheric aerosols. <em>In situ</em> observations suggest that stratospheric aerosol composition is strongly vertically dependent and contains a significant organic component in the lower stratosphere. Laboratory studies suggest a range of possible values for the complex refractive index of organic aerosols in the stratosphere. The real part of the refractive index could vary over a range that brackets the value of the real refractive index for pure sulfuric acid/water aerosols. The imaginary part of the refractive index of the organic component is highly uncertain, suggesting aerosols that range from being purely refractive to significantly absorbing (eg, brown carbon). The mixing state of these mixed composition aerosols is also uncertain; depending on the complex refractive index of the organic component, morphological variation could have a significant influence on aerosol radiative properties. In this work we perform a sensitivity study of shortwave radiative forcing of stratospheric aerosols, examining the influence of different plausible values of complex refractive index and particle morphologies. <em>In situ</em> measurements of aerosol size and composition are used to represent the size distribution, vertical profile, and organic mass fraction for the computation of aerosol optical properties. These profiles of aerosol optical properties are used as inputs to a radiative transfer model to calculate profiles of shortwave fluxes and radiative heating rates for standard model atmospheres. The implications of the variations in aerosol optical depth and resulting radiative forcing are interpreted in terms of implications for satellite measurements of stratospheric radiative forcing. The various radiative forcing results and remote sensing implications for different scenarios of organic complex refractive index and morphology call for better understandings of the effects of chemical evolution and transport dynamics on the aerosol optical properties in the stratosphere.</p>


2016 ◽  
Vol 9 (5) ◽  
pp. 1803-1826 ◽  
Author(s):  
Emma Andersson ◽  
Michael Kahnert

Abstract. A new aerosol-optics model is implemented in which realistic morphologies and mixing states are assumed, especially for black carbon particles. The model includes both external and internal mixing of all chemical species, it treats externally mixed black carbon as fractal aggregates, and it accounts for inhomogeneous internal mixing of black carbon by use of a novel "core-grey-shell" model. Simulated results of aerosol optical properties, such as aerosol optical depth, backscattering coefficients and the Ångström exponent, as well as radiative fluxes are computed with the new optics model and compared with results from an older optics-model version that treats all particles as externally mixed homogeneous spheres. The results show that using a more detailed description of particle morphology and mixing state impacts the aerosol optical properties to a degree of the same order of magnitude as the effects of aerosol-microphysical processes. For instance, the aerosol optical depth computed for two cases in 2007 shows a relative difference between the two optics models that varies over the European region between −28 and 18 %, while the differences caused by the inclusion or omission of the aerosol-microphysical processes range from −50 to 37 %. This is an important finding, suggesting that a simple optics model coupled to a chemical transport model can introduce considerable errors affecting radiative fluxes in chemistry-climate models, compromising comparisons of model results with remote sensing observations of aerosols, and impeding the assimilation of satellite products for aerosols into chemical-transport models.


2021 ◽  
Author(s):  
Jiaxing Sun ◽  
Zhe Wang ◽  
Wei Zhou ◽  
Conghui Xie ◽  
Cheng Wu ◽  
...  

Abstract. Atmospheric aerosols play an important role in radiation balance of the earth-atmosphere system. However, our knowledge of the long-term changes in black carbon (BC) and aerosol optical properties in China are very limited. Here we analyze the nine-year measurements of BC and aerosol optical properties from 2012 to 2020 in Beijing, China. Our results showed large reductions in eBC by 67 % from 5.54 ± 5.25 µg m−3 in 2012 to 1.80 ± 1.54 µg m−3 in 2020, and 47 % decreases in light extinction coefficient (bext, λ = 630 nm) of fine particles due to clean air action plan since 2013. The seasonal and diurnal variations of eBC illustrated the most significant reductions in the fall and night time, respectively. ΔeBC/ΔCO also showed an annual decrease from ~6 to 4 ng m−3 ppbv−1 and presented strong seasonal variations with high values in spring and fall, indicating that primary emissions in Beijing have changed significantly. As a response to clean air action, single scattering albedo (SSA) showed a considerable increase from 0.79 ± 0.11 to 0.88 ± 0.06, and mass extinction efficiency (MEE) increased from 3.2 to 3.8 m2 g−1. These results highlight an increasing importance of scattering aerosols in radiative forcing, and a future challenge in visibility improvement due to enhanced MEE. Brown carbon (BrC) showed similar changes and seasonal variations to eBC during 2018–2020. However, we found a large increase of secondary BrC in the total BrC in most seasons, particularly in summer with the contribution up to 50 %, demonstrating an enhanced role of secondary formation in BrC in recent years. The long-term changes in eBC and BrC have also affected the radiative forcing effect. The direct radiative forcing (ΔFR) of BC decreased by 64 % from +3.00 W m−2 in 2012 to +1.09 W m−2 in 2020, and that of BrC decreased from +0.30 to +0.17 W m−2 during 2018–2020. Such changes might have important implications in affecting aerosol and boundary-layer interactions and the future air quality improvement.


2013 ◽  
Vol 13 (10) ◽  
pp. 5089-5101 ◽  
Author(s):  
B. V. Scarnato ◽  
S. Vahidinia ◽  
D. T. Richard ◽  
T. W. Kirchstetter

Abstract. According to recent studies, internal mixing of black carbon (BC) with other aerosol materials in the atmosphere alters its aggregate shape, absorption of solar radiation, and radiative forcing. These mixing state effects are not yet fully understood. In this study, we characterize the morphology and mixing state of bare BC and BC internally mixed with sodium chloride (NaCl) using electron microscopy and examine the sensitivity of optical properties to BC mixing state and aggregate morphology using a discrete dipole approximation model (DDSCAT). DDSCAT is flexible in simulating the geometry and refractive index of particle aggregates. DDSCAT predicts a higher mass absorption coefficient (MAC), lower single scattering albedo (SSA), and higher absorption Angstrom exponent (AAE) for bare BC aggregates that are lacy rather than compact. Predicted values of SSA at 550 nm range between 0.16 and 0.27 for lacy and compact aggregates, respectively, in agreement with reported experimental values of 0.25 ± 0.05. The variation in absorption with wavelength does not adhere precisely to a power law relationship over the 200 to 1000 nm range. Consequently, AAE values depend on the wavelength region over which they are computed. The MAC of BC (averaged over the 200–1000 nm range) is amplified when internally mixed with NaCl (100–300 nm in radius) by factors ranging from 1.0 for lacy BC aggregates partially immersed in NaCl to 2.2 for compact BC aggregates fully immersed in NaCl. The SSA of BC internally mixed with NaCl is higher than for bare BC and increases with the embedding in the NaCl. Internally mixed BC SSA values decrease in the 200–400 nm wavelength range, a feature also common to the optical properties of dust and organics. Linear polarization features are also predicted in DDSCAT and are dependent on particle size and morphology. This study shows that DDSCAT predicts complex morphology and mixing state dependent aerosol optical properties that have been reported previously and are relevant to radiative transfer, climate modeling, and interpretation of remote sensing measurements.


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