scholarly journals Sensitivity of aerosol extinction to new mixing rules in the AEROPT submodel of the ECHAM5/MESSy1.9 atmospheric chemistry (EMAC) model

2014 ◽  
Vol 7 (3) ◽  
pp. 3367-3402
Author(s):  
K. Klingmüller ◽  
B. Steil ◽  
C. Brühl ◽  
H. Tost ◽  
J. Lelieveld
Keyword(s):  
Optical Properties ◽  
Radiative Transfer ◽  
Black Carbon ◽  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Strong Dependence ◽  
Mixing Rule ◽  
Aerosol Optical Properties ◽  
Volume Average ◽  
Internal Mixing

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.

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
Keyword(s):  
Optical Properties ◽  
Radiative Transfer ◽  
Black Carbon ◽  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Climate Model ◽  
Mixing Rule ◽  
Aerosol Optical Properties ◽  
Internal Mixing ◽  
Aerosol Radiative

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.

scholarly journals A new radiation infrastructure for the Modular Earth Submodel System (MESSy, based on version 2.51)

2016 ◽  
Author(s):  
Simone Dietmüller ◽  
Patrick Jöckel ◽  
Holger Tost ◽  
Markus Kunze ◽  
Cathrin Gellhorn ◽  
...  
Keyword(s):  
Optical Properties ◽  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
General Circulation ◽  
Circulation Model ◽  
Shortwave Radiation ◽  
Aerosol Optical Properties ◽  
On Line ◽  
User Friendly ◽  
Radiation Scheme

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.

scholarly journals Measurement report: Long-term changes in black carbon and aerosol optical properties from 2012 to 2020 in Beijing, China

2022 ◽  
Vol 22 (1) ◽  
pp. 561-575
Author(s):  
Jiaxing Sun ◽  
Zhe Wang ◽  
Wei Zhou ◽  
Conghui Xie ◽  
Cheng Wu ◽  
...  
Keyword(s):  
Optical Properties ◽  
Black Carbon ◽  
Seasonal Variations ◽  
Radiative Forcing ◽  
Action Plan ◽  
Aerosol Optical Properties ◽  
Long Term Changes ◽  
Clean Air ◽  
Beijing China

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.

scholarly journals Coupling aerosol optics to the MATCH (v5.5.0) chemical transport model and the SALSA (v1) aerosol microphysics module

2016 ◽  
Vol 9 (5) ◽  
pp. 1803-1826 ◽  
Author(s):  
Emma Andersson ◽  
Michael Kahnert
Keyword(s):  
Optical Properties ◽  
Black Carbon ◽  
Aerosol Optical Depth ◽  
Transport Model ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Aerosol Optical Properties ◽  
Radiative Fluxes ◽  
Internal Mixing ◽  
Microphysical Processes

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.

scholarly journals Measurement report: Long-term changes in black carbon and aerosol optical properties from 2012 to 2020 in Beijing, China

2021 ◽  
Author(s):  
Jiaxing Sun ◽  
Zhe Wang ◽  
Wei Zhou ◽  
Conghui Xie ◽  
Cheng Wu ◽  
...  
Keyword(s):  
Optical Properties ◽  
Black Carbon ◽  
Seasonal Variations ◽  
Radiative Forcing ◽  
Aerosol Optical Properties ◽  
Seasonal And Diurnal Variations ◽  
Long Term Changes ◽  
Clean Air ◽  
Beijing China

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.

scholarly journals Effects of internal mixing and aggregate morphology on optical properties of black carbon using a discrete dipole approximation model

2013 ◽  
Vol 13 (10) ◽  
pp. 5089-5101 ◽  
Author(s):  
B. V. Scarnato ◽  
S. Vahidinia ◽  
D. T. Richard ◽  
T. W. Kirchstetter
Keyword(s):  
Optical Properties ◽  
Black Carbon ◽  
Radiative Forcing ◽  
Dipole Approximation ◽  
Discrete Dipole Approximation ◽  
Approximation Model ◽  
Mixing State ◽  
Internal Mixing ◽  
Aggregate Morphology ◽  
Nm Range

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.

scholarly journals A new radiation infrastructure for the Modular Earth Submodel System (MESSy, based on version 2.51)

2016 ◽  
Vol 9 (6) ◽  
pp. 2209-2222 ◽  
Author(s):  
Simone Dietmüller ◽  
Patrick Jöckel ◽  
Holger Tost ◽  
Markus Kunze ◽  
Catrin Gellhorn ◽  
...  
Keyword(s):  
Optical Properties ◽  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
General Circulation ◽  
Circulation Model ◽  
Shortwave Radiation ◽  
Earth Orbit ◽  
Aerosol Optical Properties ◽  
User Friendly ◽  
Radiation Scheme

Abstract. The Modular Earth Submodel System (MESSy) provides an interface to couple submodels to a base model 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 (including the 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) online 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 online radiative forcing calculations in the ECHAM/MESSy Atmospheric Chemistry (EMAC) model are presented.

scholarly journals Modelling black carbon absorption of solar radiation: combining external and internal mixing assumptions

2019 ◽  
Vol 19 (1) ◽  
pp. 181-204 ◽  
Author(s):  
Gabriele Curci ◽  
Ummugulsum Alyuz ◽  
Rocio Barò ◽  
Roberto Bianconi ◽  
Johannes Bieser ◽  
...  
Keyword(s):  
Optical Properties ◽  
Black Carbon ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Absorption Enhancement ◽  
Core Shell ◽  
Mixing State ◽  
Aerosol Optical Properties ◽  
Internal Mixing ◽  
Carbon Absorption

Abstract. An accurate simulation of the absorption properties is key for assessing the radiative effects of aerosol on meteorology and climate. The representation of how chemical species are mixed inside the particles (the mixing state) is one of the major uncertainty factors in the assessment of these effects. Here we compare aerosol optical properties simulations over Europe and North America, coordinated in the framework of the third phase of the Air Quality Model Evaluation International Initiative (AQMEII), to 1 year of AERONET sunphotometer retrievals, in an attempt to identify a mixing state representation that better reproduces the observed single scattering albedo and its spectral variation. We use a single post-processing tool (FlexAOD) to derive aerosol optical properties from simulated aerosol speciation profiles, and focus on the absorption enhancement of black carbon when it is internally mixed with more scattering material, discarding from the analysis scenes dominated by dust. We found that the single scattering albedo at 440 nm (ω0,440) is on average overestimated (underestimated) by 3–5 % when external (core-shell internal) mixing of particles is assumed, a bias comparable in magnitude with the typical variability of the quantity. The (unphysical) homogeneous internal mixing assumption underestimates ω0,440 by ∼14 %. The combination of external and core-shell configurations (partial internal mixing), parameterized using a simplified function of air mass aging, reduces the ω0,440 bias to -1/-3 %. The black carbon absorption enhancement (Eabs) in core-shell with respect to the externally mixed state is in the range 1.8–2.5, which is above the currently most accepted upper limit of ∼1.5. The partial internal mixing reduces Eabs to values more consistent with this limit. However, the spectral dependence of the absorption is not well reproduced, and the absorption Ångström exponent AAE675440 is overestimated by 70–120 %. Further testing against more comprehensive campaign data, including a full characterization of the aerosol profile in terms of chemical speciation, mixing state, and related optical properties, would help in putting a better constraint on these calculations.

scholarly journals Influence of light absorbing particles on snow spectral irradiance profiles

2019 ◽  
Author(s):  
François Tuzet ◽  
Marie Dumont ◽  
Laurent Arnaud ◽  
Didier Voisin ◽  
Maxim Lamare ◽  
...  
Keyword(s):  
Optical Properties ◽  
Radiative Transfer ◽  
Black Carbon ◽  
Mineral Dust ◽  
Strong Dependence ◽  
Surface Energy Budget ◽  
Spectral Irradiance ◽  
Light Extinction ◽  
Chemical Measurements ◽  
Radiative Impact

Abstract. Light Absorbing Particles (LAP) such as black carbon or mineral dust are some of the main drivers of snow radiative transfer. Small amounts of LAP significantly increase snowpack absorption in the visible wavelengths where ice absorption is particularly weak, impacting the surface energy budget of snow-covered areas. However, linking measurements of LAP concentration in snow to their actual radiative impact is a challenging issue which is not fully resolved. In the present paper, we point out a new method based on Spectral Irradiance Profile (SIP) measurements which makes it possible to identify the radiative impact of LAP on visible light extinction in homogeneous layers of the snowpack. From this impact on light extinction it is possible to infer LAP concentrations present in each layer using radiative transfer theory. This study relies on a unique dataset composed of 26 spectral irradiance profile measurements in the wavelength range 350–950 nm with concomitant profile measurements of snow physical properties and LAP concentrations, collected in the Alps over two snow seasons in winter and spring conditions. For 55 homogeneous snow layers identified in our dataset, the concentrations retrieved from SIP measurements are compared to chemical measurements of LAP concentrations. A good correlation is observed for measured concentrations higher than 5 ng g−1 (r2 = 0.74) despite a clear positive bias. The potential causes of this bias are discussed, underlining a strong dependence of our method to LAP optical properties and to the relationship between snow microstructure and snow optical properties used in the theory. Additional uncertainties such as artefacts in the measurement technique for SIP and chemical contents along with LAP absorption efficiency, may explain part of this bias. In addition, spectral information on LAP absorption can be retrieved from SIP measurements. We show that for layers containing a unique absorber, this absorber can be identified in some cases (e.g: mineral dust vs black carbon). We also observe an enhancement of light absorption between 350 and 650 nm in presence of liquid water in the snowpack which is discussed but not fully elucidated. A single SIP acquisition lasts approximately one minute and is hence much faster than collecting a profile of chemical measurements. With the recent advances in modelling LAP-snow interactions, our method could become an attractive alternative to estimate vertical profiles of LAP concentrations in snow.

scholarly journals Modelling black carbon absorption of solar radiation: combining external and internal mixing assumptions

2018 ◽  
Author(s):  
Gabriele Curci ◽  
Ummugulsum Alyuz ◽  
Rocio Barò ◽  
Roberto Bianconi ◽  
Johannes Bieser ◽  
...  
Keyword(s):  
Optical Properties ◽  
Black Carbon ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Absorption Enhancement ◽  
Core Shell ◽  
Mixing State ◽  
Aerosol Optical Properties ◽  
Internal Mixing ◽  
Carbon Absorption

Abstract. An accurate simulation of the absorption properties is key for assessing the radiative effects of aerosol on meteorology and climate. The representation of how chemical species are mixed inside the particles (the mixing state) is one of the major uncertainty factors in the assessment of these effects. Here we compare aerosol optical properties simulations over Europe and North America, coordinated in the framework of the third phase of the Air Quality Model Evaluation International Initiative (AQMEII), to one year of AERONET sunphotometer retrievals, in an attempt to identify a mixing state representation that better reproduces the observed single scattering albedo and its spectral variation. We use a single post-processing tool (FlexAOD) to derive aerosol optical properties from simulated aerosol speciation profiles, and focus on the absorption enhancement of black carbon when it is internally mixed with more scattering material, discarding from the analysis scenes dominated by dust. We found that the single scattering albedo at 440 nm (ω0,440) is on average overestimated (underestimated) by 3–5 % when external (core-shell internal) mixing of particles is assumed, a bias comparable in magnitude with the typical variability of the quantity. The (unphysical) homogeneous internal mixing assumption underestimates ω0,440 by ~ 14 %. The combination of external and core-shell configurations (partial internal mixing), parameterized using a simplified function of air mass aging, reduces the ω0,440 bias to −1/−3 %. The black carbon absorption enhancement (Eabs) in core-shell with respect to the externally mixed state is in the range 1.8–2.5, which is above the currently most accepted upper limit of ~ 1.5. The partial internal mixing reduces Eabs to values more consistent with this limit. However, the spectral dependence of the absorption is not well reproduced, and the absorption Angostrom exponent AAE440675 is overestimated by 70–120 %. Further testing against more comprehensive campaign data, including a full characterization of the aerosol profile in terms of chemical speciation, mixing state, and related optical properties, would help in putting a better constraint on these calculations.

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