scholarly journals Interpreting the Ultraviolet Aerosol Index observed with the OMI satellite instrument to understand absorption by organic aerosols: implications for atmospheric oxidation and direct radiative effects

2015 ◽  
Vol 15 (19) ◽  
pp. 27405-27447
Author(s):  
M. S. Hammer ◽  
R. V. Martin ◽  
A. van Donkelaar ◽  
V. Buchard ◽  
O. Torres ◽  
...  
Keyword(s):  
Radiative Transfer ◽  
South America ◽  
Biomass Burning ◽  
Southern Africa ◽  
Radiative Forcing ◽  
Transport Model ◽  
Organic Aerosol ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Aerosol Index

Abstract. Satellite observations of the Ultraviolet Aerosol Index (UVAI) are sensitive to absorption of solar radiation by aerosols; this absorption affects photolysis frequencies and radiative forcing. We develop a global simulation of the UVAI using the 3-D chemical transport model GEOS-Chem coupled with the Vector Linearized Discrete Ordinate Radiative Transfer model (VLIDORT). The simulation is applied to interpret UVAI observations from the Ozone Monitoring Instrument (OMI) for the year 2007. Simulated and observed values are highly consistent in regions where mineral dust dominates the UVAI, but a large negative bias (−0.32 to −0.97) exists between simulated and observed values in biomass burning regions. We determine effective optical properties for absorbing organic aerosol, known as brown carbon (BrC), and implement them into GEOS-Chem to better represent observed UVAI values over biomass burning regions. The addition of absorbing BrC decreases the mean bias between simulated and OMI UVAI values from −0.57 to −0.09 over West Africa in January, from −0.32 to +0.0002 over South Asia in April, from −0.97 to −0.22 over southern Africa in July, and from −0.50 to +0.33 over South America in September. The spectral dependence of absorption after adding BrC to the model is broadly consistent with reported observations for biomass burning aerosol, with Absorbing Angstrom Exponent (AAE) values ranging from 2.9 in the ultraviolet (UV) to 1.3 across the UV-Near IR spectrum. We assess the effect of the additional UV absorption by BrC on atmospheric photochemistry by examining tropospheric hydroxyl radical (OH) concentrations in GEOS-Chem. The inclusion of BrC decreases OH by up to 35 % over South America in September, up to 25 % over southern Africa in July, and up to 20 % over other biomass burning regions. Global annual mean OH concentrations in GEOS-Chem decrease due to the presence of absorbing BrC, increasing the methyl chloroform lifetime from 5.62 to 5.68 years, thus reducing the bias against observed values. We calculate the direct radiative effect (DRE) of BrC using GEOS-Chem coupled with the radiative transfer model RRTMG (GC-RT). Treating organic aerosol as containing absorbing BrC rather than as primarily scattering changes global annual mean all-sky top of atmosphere (TOA) DRE by +0.05 W m-2 and all-sky surface DRE by −0.06 W m-2. Regional changes of up to +0.5 W m-2 at TOA and down to −1 W m-2 at the surface are found over major biomass burning regions.

scholarly journals Interpreting the ultraviolet aerosol index observed with the OMI satellite instrument to understand absorption by organic aerosols: implications for atmospheric oxidation and direct radiative effects

2016 ◽  
Vol 16 (4) ◽  
pp. 2507-2523 ◽  
Author(s):  
Melanie S. Hammer ◽  
Randall V. Martin ◽  
Aaron van Donkelaar ◽  
Virginie Buchard ◽  
Omar Torres ◽  
...  
Keyword(s):  
Radiative Transfer ◽  
South America ◽  
Biomass Burning ◽  
Southern Africa ◽  
Radiative Forcing ◽  
Transport Model ◽  
Organic Aerosol ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Aerosol Index

Abstract. Satellite observations of the ultraviolet aerosol index (UVAI) are sensitive to absorption of solar radiation by aerosols; this absorption affects photolysis frequencies and radiative forcing. We develop a global simulation of the UVAI using the 3-D chemical transport model GEOS-Chem coupled with the Vector Linearized Discrete Ordinate Radiative Transfer model (VLIDORT). The simulation is applied to interpret UVAI observations from the Ozone Monitoring Instrument (OMI) for the year 2007. Simulated and observed values are highly consistent in regions where mineral dust dominates the UVAI, but a large negative bias (−0.32 to −0.97) exists between simulated and observed values in biomass burning regions. We determine effective optical properties for absorbing organic aerosol, known as brown carbon (BrC), and implement them into GEOS-Chem to better represent observed UVAI values over biomass burning regions. The inclusion of absorbing BrC decreases the mean bias between simulated and OMI UVAI values from −0.57 to −0.09 over West Africa in January, from −0.32 to +0.0002 over South Asia in April, from −0.97 to −0.22 over southern Africa in July, and from −0.50 to +0.33 over South America in September. The spectral dependence of absorption after including BrC in the model is broadly consistent with reported observations for biomass burning aerosol, with absorbing Ångström exponent (AAE) values ranging from 2.9 in the ultraviolet (UV) to 1.3 across the UV–Near IR spectrum. We assess the effect of the additional UV absorption by BrC on atmospheric photochemistry by examining tropospheric hydroxyl radical (OH) concentrations in GEOS-Chem. The inclusion of BrC decreases OH by up to 30 % over South America in September, up to 20 % over southern Africa in July, and up to 15 % over other biomass burning regions. Global annual mean OH concentrations in GEOS-Chem decrease due to the presence of absorbing BrC, increasing the methyl chloroform lifetime from 5.62 to 5.68 years, thus reducing the bias against observed values. We calculate the direct radiative effect (DRE) of BrC using GEOS-Chem coupled with the radiative transfer model RRTMG (GC-RT). Treating organic aerosol as containing more strongly absorbing BrC changes the global annual mean all-sky top of atmosphere (TOA) DRE by +0.03 W m−2 and all-sky surface DRE by −0.08 W m−2. Regional changes of up to +0.3 W m−2 at TOA and down to −1.5 W m−2 at the surface are found over major biomass burning regions.

Estimation of Surface and Top-of-Atmosphere Shortwave Irradiance in Biomass-Burning Regions during SCAR-B

2000 ◽  
Vol 39 (10) ◽  
pp. 1742-1753 ◽  
Author(s):  
Sundar A. Christopher ◽  
Xiang Li ◽  
Ronald M. Welch ◽  
Jeffrey S. Reid ◽  
Peter V. Hobbs ◽  
...  
Keyword(s):  
Radiative Transfer ◽  
Biomass Burning ◽  
Optical Thickness ◽  
Radiative Forcing ◽  
Wavelength Dependence ◽  
Single Scattering ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Aerosol Radiative Forcing ◽  
Mean Square Errors

Abstract Using in situ measurements of aerosol optical properties and ground-based measurements of aerosol optical thickness (τs) during the Smoke, Clouds and Radiation—Brazil (SCAR-B) experiment, a four-stream broadband radiative transfer model is used to estimate the downward shortwave irradiance (DSWI) and top-of-atmosphere (TOA) shortwave aerosol radiative forcing (SWARF) in cloud-free regions dominated by smoke from biomass burning in Brazil. The calculated DSWI values are compared with broadband pyranometer measurements made at the surface. The results show that, for two days when near-coincident measurements of single-scattering albedo ω0 and τs are available, the root-mean-square errors between the measured and calculated DSWI for daytime data are within 30 W m−2. For five days during SCAR-B, however, when assumptions about ω0 have to be made and also when τs was significantly higher, the differences can be as large as 100 W m−2. At TOA, the SWARF per unit optical thickness ranges from −20 to −60 W m−2 over four major ecosystems in South America. The results show that τs and ω0 are the two most important parameters that affect DSWI calculations. For SWARF values, surface albedos also play an important role. It is shown that ω0 must be known within 0.05 and τs at 0.55 μm must be known to within 0.1 to estimate DSWI to within 20 W m−2. The methodology described in this paper could serve as a potential strategy for determining DSWI values in the presence of aerosols. The wavelength dependence of τs and ω0 over the entire shortwave spectrum is needed to improve radiative transfer calculations. If global retrievals of DSWI and SWARF from satellite measurements are to be performed in the presence of biomass-burning aerosols on a routine basis, a concerted effort should be made to develop methodologies for estimating ω0 and τs from satellite and ground-based measurements.

Radiative forcing over the Arctic of aerosols from the August 2017 Canadian and Greenlandic wildfires

2021 ◽  
Author(s):  
Filippo Calì Quaglia ◽  
Daniela Meloni ◽  
Alcide Giorgio di Sarra ◽  
Tatiana Di Iorio ◽  
Virginia Ciardini ◽  
...  
Keyword(s):  
Radiative Transfer ◽  
Radiative Forcing ◽  
Solar Zenith Angle ◽  
Surface Albedo ◽  
High Arctic ◽  
The Arctic ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Aerosol Layer ◽  
Radiative Effect

<p>Extended and intense wildfires occurred in Northern Canada and, unexpectedly, on the Greenlandic West coast during summer 2017. The thick smoke plume emitted into the atmosphere was transported to the high Arctic, producing one of the largest impacts ever observed in the region. Evidence of Canadian and Greenlandic wildfires was recorded at the Thule High Arctic Atmospheric Observatory (THAAO, 76.5°N, 68.8°W, www.thuleatmos-it.it) by a suite of instruments managed by ENEA, INGV, Univ. of Florence, and NCAR. Ground-based observations of the radiation budget have allowed quantification of the surface radiative forcing at THAAO. </p><p>Excess biomass burning chemical tracers such as CO, HCN, H2CO, C2H6, and NH3 were  measured in the air column above Thule starting from August 19 until August 23. The aerosol optical depth (AOD) reached a peak value of about 0.9 on August 21, while an enhancement of wildfire compounds was  detected in PM10. The measured shortwave radiative forcing was -36.7 W/m2 at 78° solar zenith angle (SZA) for AOD=0.626.</p><p>MODTRAN6.0 radiative transfer model (Berk et al., 2014) was used to estimate the aerosol radiative effect and the heating rate profiles at 78° SZA. Measured temperature profiles, integrated water vapour, surface albedo, spectral AOD and aerosol extinction profiles from CALIOP onboard CALIPSO were used as model input. The peak  aerosol heating rate (+0.5 K/day) was  reached within the aerosol layer between 8 and 12 km, while the maximum radiative effect (-45.4 W/m2) is found at 3 km, below the largest aerosol layer.</p><p>The regional impact of the event that occurred on August 21 was investigated using a combination of atmospheric radiative transfer modelling with measurements of AOD and ground surface albedo from MODIS. The aerosol properties used in the radiative transfer model were constrained by in situ measurements from THAAO. Albedo data over the ocean have been obtained from Jin et al. (2004). Backward trajectories produced through HYSPLIT simulations (Stein et al., 2015) were also employed to trace biomass burning plumes.</p><p>The radiative forcing efficiency (RFE) over land and ocean was derived, finding values spanning from -3 W/m2 to -132 W/m2, depending on surface albedo and solar zenith angle. The fire plume covered a vast portion of the Arctic, with large values of the daily shortwave RF (< -50 W/m2) lasting for a few days. This large amount of aerosol is expected to influence cloud properties in the Arctic, producing significant indirect radiative effects.</p>

scholarly journals Contrasting the direct radiative effect and direct radiative forcing of aerosols

2014 ◽  
Vol 14 (11) ◽  
pp. 5513-5527 ◽  
Author(s):  
C. L. Heald ◽  
D. A. Ridley ◽  
J. H. Kroll ◽  
S. R. H. Barrett ◽  
K. E. Cady-Pereira ◽  
...  
Keyword(s):  
Energy Balance ◽  
Radiative Forcing ◽  
Transport Model ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Radiative Effect ◽  
Chemical Transport Model ◽  
Anthropogenic Aerosols ◽  
Anthropogenic Aerosol ◽  
Direct Radiative Forcing

Abstract. The direct radiative effect (DRE) of aerosols, which is the instantaneous radiative impact of all atmospheric particles on the Earth's energy balance, is sometimes confused with the direct radiative forcing (DRF), which is the change in DRE from pre-industrial to present-day (not including climate feedbacks). In this study we couple a global chemical transport model (GEOS-Chem) with a radiative transfer model (RRTMG) to contrast these concepts. We estimate a global mean all-sky aerosol DRF of −0.36 Wm−2 and a DRE of −1.83 Wm−2 for 2010. Therefore, natural sources of aerosol (here including fire) affect the global energy balance over four times more than do present-day anthropogenic aerosols. If global anthropogenic emissions of aerosols and their precursors continue to decline as projected in recent scenarios due to effective pollution emission controls, the DRF will shrink (−0.22 Wm−2 for 2100). Secondary metrics, like DRE, that quantify temporal changes in both natural and anthropogenic aerosol burdens are therefore needed to quantify the total effect of aerosols on climate.

Greenhouse effects of aircraft emissions as calculated by a radiative transfer model

1995 ◽  
Vol 13 (4) ◽  
pp. 413-418 ◽  
Author(s):  
J. P. F. Fortuin ◽  
R. van Dorland ◽  
W. M. F. Wauben ◽  
H. Kelder
Keyword(s):  
Water Vapor ◽  
Radiative Transfer ◽  
Indirect Effect ◽  
Radiative Forcing ◽  
Combustion Products ◽  
Ozone Production ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Aircraft Emissions ◽  
The North

Abstract. With a radiative transfer model, assessments are made of the radiative forcing in northern mid-latitudes due to aircraft emissions up to 1990. Considered are the direct climate effects from the major combustion products carbon dioxide, nitrogen dioxide, water vapor and sulphur dioxide, as well as the indirect effect of ozone production from NOx emissions. Our study indicates a local radiative forcing at the tropopause which should be negative in summer (–0.5 to 0.0 W/m2) and either negative or positive in winter (–0.3 to 0.2 W/m2). To these values the indirect effect of contrails has to be added, which for the North Atlantic Flight Corridor covers the range –0.2 to 0.3 W/m2 in summer and 0.0 to 0.3 W/m2 in winter. Apart from optically dense non-aged contrails during summer, negative forcings are due to solar screening by sulphate aerosols. The major positive contributions come from contrails, stratospheric water vapor in winter and ozone in summer. The direct effect of NO2 is negligible and the contribution of CO2 is relatively small.

scholarly journals Improved estimate of global dust radiative forcing using a coupled chemical transport-radiative transfer model

2013 ◽  
Vol 13 (1) ◽  
pp. 2415-2456 ◽  
Author(s):  
L. Zhang ◽  
Q. B. Li ◽  
Y. Gu ◽  
K. N. Liou ◽  
B. Meland
Keyword(s):  
Radiative Transfer ◽  
Vertical Profile ◽  
Radiative Forcing ◽  
Chemical Transport ◽  
Dust Particles ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Vertical Profiles ◽  
Dust Source ◽  
Source Regions

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.

scholarly journals Exploring the observational constraints on the simulation of brown carbon

2017 ◽  
Author(s):  
Xuan Wang ◽  
Colette L. Heald ◽  
Jiumeng Liu ◽  
Rodney J. Weber ◽  
Pedro Campuzano-Jost ◽  
...  
Keyword(s):  
Optical Properties ◽  
Biomass Burning ◽  
Transport Model ◽  
Model Simulation ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Observational Constraints ◽  
Radiative Effect ◽  
Brown Carbon ◽  
Direct Measurements

Abstract. Organic aerosols (OA) that strongly absorbs solar radiation in the near-UV are referred to as brown carbon (BrC). However the sources, evolution, and optical properties of BrC remain highly uncertain, and contribute significantly to uncertainty in the estimate of the global direct radiative effect (DRE) of aerosols. Previous modeling studies of BrC optical properties and DRE have been unable to fully evaluate model performance due to the lack of direct measurements of BrC absorption. In this study, we develop a global model simulation (GEOS-Chem) of BrC and test it against BrC absorption measurements from two aircraft campaigns in the continental U.S. (SEAC4RS and DC3). To our knowledge, this is the first study to compare simulated BrC absorption with direct ambient measurements. We show that the BrC absorption properties from biomass burning estimated based on previous laboratory measurements overestimate the aircraft measurements of ambient BrC absorption. In addition, applying a photochemical scheme to simulate bleaching/degradation of BrC improves model skill. The airborne observations are consistent with a mass absorption coefficient (MAC) of freshly emitted biomass burning OA of 0.57 m2 g−1 at 365 nm with an absorption Ångström exponents (AAE) = 3.1 for 300 & 600 wavelengths pair, coupled with a 1 day whitening e-folding time. Using the GEOS-Chem chemical transport model integrated with the RRTMG radiative transfer model, we estimate that the top-of-atmosphere all-sky direct radiative effect (DRE) of OA is −0.350 Wm−2, 10 % higher than that without consideration of BrC absorption. Therefore, our best estimate of the absorption DRE of BrC is +0.042 Wm−2. We suggest that the DRE of BrC has been overestimated previously due to the lack of observational constraints from direct measurements and omission of the effects of photochemical whitening.

scholarly journals Brown carbon aerosol in the North American continental troposphere: sources, abundance, and radiative forcing

2015 ◽  
Vol 15 (14) ◽  
pp. 7841-7858 ◽  
Author(s):  
J. Liu ◽  
E. Scheuer ◽  
J. Dibb ◽  
G. S. Diskin ◽  
L. D. Ziemba ◽  
...  
Keyword(s):  
Biomass Burning ◽  
North American ◽  
Radiative Forcing ◽  
Single Scattering ◽  
Measurement Range ◽  
Radiative Transfer Model ◽  
Chemical Components ◽  
Transfer Model ◽  
Brown Carbon ◽  
The North

Abstract. Chemical components of organic aerosol (OA) selectively absorb light at short wavelengths. In this study, the prevalence, sources, and optical importance of this so-called brown carbon (BrC) aerosol component are investigated throughout the North American continental tropospheric column during a summer of extensive biomass burning. Spectrophotometric absorption measurements on extracts of bulk aerosol samples collected from an aircraft over the central USA were analyzed to directly quantify BrC abundance. BrC was found to be prevalent throughout the 1 to 12 km altitude measurement range, with dramatic enhancements in biomass-burning plumes. BrC to black carbon (BC) ratios, under background tropospheric conditions, increased with altitude, consistent with a corresponding increase in the absorption Ångström exponent (AAE) determined from a three-wavelength particle soot absorption photometer (PSAP). The sum of inferred BC absorption and measured BrC absorption at 365 nm was within 3 % of the measured PSAP absorption for background conditions and 22 % for biomass burning. A radiative transfer model showed that BrC absorption reduced top-of-atmosphere (TOA) aerosol forcing by ~ 20 % in the background troposphere. Extensive radiative model simulations applying this study background tropospheric conditions provided a look-up chart for determining radiative forcing efficiencies of BrC as a function of a surface-measured BrC : BC ratio and single scattering albedo (SSA). The chart is a first attempt to provide a tool for better assessment of brown carbon's forcing effect when one is limited to only surface data. These results indicate that BrC is an important contributor to direct aerosol radiative forcing.

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