scholarly journals Key factors affecting single scattering albedo calculation: Implications for aerosol climate forcing

2017 ◽  
Author(s):  
Duseong S. Jo ◽  
Rokjin J. Park ◽  
Jaein I. Jeong ◽  
Gabriele Curci ◽  
Hyung-Min Lee ◽  
...  
Keyword(s):  
Particulate Matter ◽  
Radiative Forcing ◽  
Transport Model ◽  
Geometric Mean ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Geometric Standard Deviation ◽  
Physical Parameters ◽  
Chemical Transport Model ◽  
Aerosol Mass

Abstract. Single Scattering Albedo (SSA), the ratio of scattering efficiency to total extinction efficiency, is an essential parameter used to estimate the Direct Radiative Forcing (DRF) of aerosols. However, SSA is one of the large contributors to the uncertainty of DRF estimations. In this study, we examined the sensitivity of SSA calculations to the physical properties of absorbing aerosols, in particular, Black Carbon (BC), Brown Carbon (BrC), and dust. We used GEOS-Chem 3-D global chemical transport model (CTM) simulations and a post-processing tool for the aerosol optical properties (FlexAOD). The model and input parameters were evaluated by comparison against the observed aerosol mass concentrations and the Aerosol Optical Depth (AOD) values obtained from global surface observation networks such as the global Aerosol Mass Spectrometer (AMS) dataset, the Surface Particulate Matter Network (SPARTAN), and the Aerosol Robotic Network (AERONET). The model was generally successful in reproducing the observed variability of both the Particulate Matter 2.5 μm (PM2.5) and AOD (R ~ 0.76) values, although it underestimated the magnitudes by approximately 20 %. Our sensitivity tests of the SSA calculation revealed that the aerosol physical parameters, which have generally received less attention than the aerosol mass loadings, can cause large uncertainties in the resulting DRF estimation. For example, large variations in the calculated BC absorption may result from slight changes of the geometric mean radius, geometric standard deviation, real and imaginary refractive indices, and density. The inclusion of BrC and observationally-constrained dust size distributions also significantly affected the SSA, and resulted in a remarkable improvement for the simulated SSA at 440 nm (bias was reduced by 44–49 %) compared with the AERONET observations. Based on the simulations performed during this study, we found that the global aerosol direct radiative effect was increased by 10 % after the SSA bias was reduced.

scholarly journals Interpretation of measured aerosol mass scattering efficiency over North America using a chemical transport model

2019 ◽  
Vol 19 (4) ◽  
pp. 2635-2653 ◽  
Author(s):  
Robyn N. C. Latimer ◽  
Randall V. Martin
Keyword(s):  
North America ◽  
Transport Model ◽  
Geometric Mean ◽  
Chemical Transport ◽  
Hygroscopic Growth ◽  
Chemical Transport Model ◽  
Scattering Efficiency ◽  
Alternative Representation ◽  
Aerosol Mass ◽  
Dry Conditions

Abstract. Aerosol mass scattering efficiency affects climate forcing calculations, atmospheric visibility, and the interpretation of satellite observations of aerosol optical depth. We evaluated the representation of aerosol mass scattering efficiency (αsp) in the GEOS-Chem chemical transport model over North America using collocated measurements of aerosol scatter and mass from IMPROVE network sites between 2000 and 2010. We found a positive bias in mass scattering efficiency given current assumptions of aerosol size distributions and particle hygroscopicity in the model. We found that overestimation of mass scattering efficiency was most significant in dry (RH <35 %) and midrange humidity (35 % < RH <65 %) conditions, with biases of 82 % and 40 %, respectively. To address these biases, we investigated assumptions surrounding the two largest contributors to fine aerosol mass, organic (OA) and secondary inorganic aerosols (SIA). Inhibiting hygroscopic growth of SIA below 35 % RH and decreasing the dry geometric mean radius, from 0.069 µm for SIA and 0.073 µm for OA to 0.058 µm for both aerosol types, significantly decreased the overall bias observed at IMPROVE sites in dry conditions from 82 % to 9 %. Implementation of a widely used alternative representation of hygroscopic growth following κ-Kohler theory for secondary inorganic (hygroscopicity parameter κ=0.61) and organic (κ=0.10) aerosols eliminated the remaining overall bias in αsp. Incorporating these changes in aerosol size and hygroscopicity into the GEOS-Chem model resulted in an increase of 16 % in simulated annual average αsp over North America, with larger increases of 25 % to 45 % in northern regions with high RH and hygroscopic aerosol fractions, and decreases in αsp up to 15 % in the southwestern U.S. where RH is low.

scholarly journals Characterization of a large biogenic secondary organic aerosol event from eastern Canadian forests

2009 ◽  
Vol 9 (5) ◽  
pp. 18113-18158 ◽  
Author(s):  
J. G. Slowik ◽  
C. Stroud ◽  
J. W. Bottenheim ◽  
P. C. Brickell ◽  
R. Y.-W. Chang ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Secondary Organic Aerosol ◽  
Transport Model ◽  
Cloud Condensation Nuclei ◽  
Coniferous Forest ◽  
Organic Aerosol ◽  
Early Summer ◽  
Chemical Mechanism ◽  
Chemical Transport Model ◽  
Aerosol Mass

Abstract. Biogenic secondary organic aerosol levels many times larger than past observations have been measured 70 km north of Toronto during a period of increasing temperatures and outflow from Northern Ontario and Quebec forests in early summer. A regional chemical transport model approximately predicts the event timing and accurately predicts the aerosol loading, identifying the precursors as monoterpene emissions from the coniferous forest. The agreement between the measured and modeled biogenic aerosol concentrations contrasts with model underpredictions for polluted regions. Correlations of the oxygenated organic aerosol mass with tracers such as CO support a secondary aerosol source and distinguish biogenic, pollution, and biomass burning periods during the field campaign. Using the Master Chemical Mechanism, it is shown that the levels of CO observed during the biogenic event are consistent with a photochemical source arising from monoterpene oxidation. The biogenic aerosol mass correlates with satellite measurements of regional aerosol optical depth, indicating that the event extends across the eastern Canadian forest. This regional event correlates with increased temperatures, indicating that temperature-dependent forest emissions can significantly affect climate through enhanced direct radiative forcing and higher cloud condensation nuclei numbers.

scholarly journals Physical-chemical characterization of the particulate matter inside two road tunnels in the São Paulo Metropolitan Area

2013 ◽  
Vol 13 (8) ◽  
pp. 20839-20883 ◽  
Author(s):  
J. Brito ◽  
L. V. Rizzo ◽  
P. Herckes ◽  
P. C. Vasconcellos ◽  
S. E. S. Caumo ◽  
...  
Keyword(s):  
Trace Elements ◽  
Particulate Matter ◽  
Real Time ◽  
Metropolitan Area ◽  
Single Scattering ◽  
Sao Paulo ◽  
Single Scattering Albedo ◽  
Fuel Composition ◽  
São Paulo ◽  
Road Tunnels

Abstract. The notable increase in biofuel usage by the road transportation sector in Brazil during recent years has significantly altered the vehicular fuel composition. Consequently, many uncertainties are currently found in particulate matter vehicular emission profiles. In an effort to better characterize the emitted particulate matter, measurements of aerosol physical and chemical properties were undertaken inside two tunnels located in the São Paulo Metropolitan Area (SPMA). The tunnels show very distinct fleet profiles: in the Jânio Quadros (JQ) tunnel, the vast majority of the circulating fleet are Light Duty Vehicles (LDVs), fuelled on average with the same amount of ethanol as gasoline. In the Rodoanel (RA) tunnel, the particulate emission is dominated by Heavy Duty Vehicles (HDVs) fuelled with diesel (5% biodiesel). In the JQ tunnel, PM2.5 concentration was on average 52 μg m−3, with the largest contribution of Organic Mass (OM, 42%), followed by Elemental Carbon (EC, 17%) and Crustal elements (13%). Sulphate accounted for 7% of PM2.5 and the sum of other trace elements was 10%. In the RA tunnel, PM2.5 was on average 233 μg m−3, mostly composed of EC (52%) and OM (39%). Sulphate, crustal and the trace elements showed a minor contribution with 5%, 1% and 1%, respectively. The average OC:EC ratio in the JQ tunnel was 1.59 ± 0.09, indicating an important contribution of EC despite the high ethanol fraction in the fuel composition. In the RA tunnel, the OC:EC ratio was 0.49 ± 0.12, consistent with previous measurements of diesel fuelled HDVs. Besides bulk carbonaceous aerosol measurement, Polycyclic Aromatic Hydrocarbons (PAHs) were quantified. The sum of the PAHs concentration was 56 ± 5 ng m−3 and 45 ± 9 ng m−3 in the RA and JQ tunnel, respectively. In the JQ tunnel, Benzo(a)pyrene (BaP) ranged from 0.9 to 6.7 ng m−3 (0.02–0.1‰ of PM2.5) in the JQ tunnel whereas in the RA tunnel BaP ranged from 0.9 to 4.9 ng m−3 (0.004–0.02‰ of PM2.5), indicating an important relative contribution of LDVs emission to atmospheric BaP. Real-time measurements performed in both tunnels provided aerosol size distributions and optical properties. The average particle count yielded 73 000 cm−3 in the JQ tunnel and 366 000 cm−3 in the RA tunnel, with an average diameter of 48 nm in the former and 39 nm in the latter. Aerosol single scattering albedo, calculated from scattering and absorption observations in the JQ tunnel, showed a minimum value of 0.4 at the peak of the morning rush hour, reached 0.6 around noon and stabilized at 0.5 in the afternoon and evening. Such single scattering albedo range is close to other tunnel studies results, despite significant biofuel usage. Given the exceedingly high Black Carbon loadings in the RA tunnel, real time light absorption measurements were possible only in the JQ tunnel. Nevertheless, using EC measured from the filters a single scattering albedo of 0.32 for the RA tunnel has been estimated. The results presented here characterize particulate matter emitted from nearly 1 million vehicles fuelled with a considerable amount of biofuel, providing an unique experimental site worldwide.

Aerosol radiative forcing deduced from observations and models over an urban location and sensitivity to single scattering albedo

2011 ◽  
Vol 45 (34) ◽  
pp. 6163-6171 ◽  
Author(s):  
Rohit Srivastava ◽  
S. Ramachandran ◽  
T.A. Rajesh ◽  
Sumita Kedia
Keyword(s):  
Radiative Forcing ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Aerosol Radiative Forcing ◽  
Urban Location ◽  
Aerosol Radiative

scholarly journals Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

2015 ◽  
Vol 15 (20) ◽  
pp. 11807-11833 ◽  
Author(s):  
W. W. Hu ◽  
P. Campuzano-Jost ◽  
B. B. Palm ◽  
D. A. Day ◽  
A. M. Ortega ◽  
...  
Keyword(s):  
Mass Spectrometer ◽  
Secondary Organic Aerosol ◽  
Transport Model ◽  
Organic Aerosol ◽  
Oxidation Products ◽  
Chemical Transport Model ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
Multiple Field

Abstract. Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene oxidation pathways, was quantified by applying positive matrix factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of organic aerosol (OA) in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the Southern Oxidant and Aerosol Study (SOAS), 78 % of PMF-resolved IEPOX-SOA is accounted by the measured IEPOX-SOA molecular tracers (2-methyltetrols, C5-Triols, and IEPOX-derived organosulfate and its dimers), making it the highest level of molecular identification of an ambient SOA component to our knowledge. An enhanced signal at C5H6O+ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine fC5H6O (fC5H6O= C5H6O+/OA) across multiple field, chamber, and source data sets. A background of ~ 1.7 ± 0.1 ‰ (‰ = parts per thousand) is observed in studies strongly influenced by urban, biomass-burning, and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.6 ‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0 ‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7 ‰), which leaves some room to separate both contributions to OA. Locations strongly influenced by isoprene emissions under low-NO levels had higher fC5H6O (~ 6.5 ± 2.2 ‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. fC5H6O in IEPOX-SOA is always elevated (12–40 ‰) but varies substantially between locations, which is shown to reflect large variations in its detailed molecular composition. The low fC5H6O (< 3 ‰) reported in non-IEPOX-derived isoprene-SOA from chamber studies indicates that this tracer ion is specifically enhanced from IEPOX-SOA, and is not a tracer for all SOA from isoprene. We introduce a graphical diagnostic to study the presence and aging of IEPOX-SOA as a triangle plot of fCO2 vs. fC5H6O. Finally, we develop a simplified method to estimate ambient IEPOX-SOA mass concentrations, which is shown to perform well compared to the full PMF method. The uncertainty of the tracer method is up to a factor of ~ 2, if the fC5H6O of the local IEPOX-SOA is not available. When only unit mass-resolution data are available, as with the aerosol chemical speciation monitor (ACSM), all methods may perform less well because of increased interferences from other ions at m/z 82. This study clarifies the strengths and limitations of the different AMS methods for detection of IEPOX-SOA and will enable improved characterization of this OA component.

scholarly journals Concentrations and source regions of light absorbing impurities in snow/ice in northern Pakistan and their impact on snow albedo

2017 ◽  
Author(s):  
Chaman Gul ◽  
Siva Praveen Puppala ◽  
Shichang Kang ◽  
Bhupesh Adhikary ◽  
Yulan Zhang ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Transport Model ◽  
Chemical Transport ◽  
Small Contribution ◽  
Northern Pakistan ◽  
Chemical Transport Model ◽  
Transport Modelling ◽  
Snow Albedo ◽  
Source Regions ◽  
Snow And Ice

Abstract. Black carbon (BC), water-insoluble organic carbon (OC), and mineral dust are important particulate impurities in snow and ice, which significantly reduce albedo and accelerate melting. Surface snow and ice samples were collected from the Karakoram–Himalayan region of northern Pakistan during 2015 and 2016 in summer (six glaciers), autumn (two glaciers), and winter (six mountain valleys). The average BC concentration overall was 2130 ± 1560 ngg−1 in summer samples, 2883 ± 3439 ngg−1 in autumn samples, and 992 ± 883 ngg−1 in winter samples. The average water insoluble OC concentration overall was 1839 ± 1108 ngg−1 in summer samples, 1423 ± 208 ngg−1 in autumn samples, and 1342 ± 672 ngg−1 in winter samples. The overall concentration of BC, OC, and dust in aged snow samples collected during the summer campaign was higher than the concentration in ice samples. The values are relatively high compared to reports by others for the Himalayas and Tibetan Plateau. This is probably the result of taking more representative samples at lower elevation where deposition is higher and the effects of ageing and enrichment more marked. A reduction in snow albedo of 0.1–8.3 % for fresh snow and 0.9–32.5 % for aged snow was calculated for selected solar zenith angles during day time using the Snow, Ice, and Aerosol Radiation (SNICAR) model. Daily mean albedo was reduced by 0.07–12.0 %. The calculated radiative forcing ranged from 0.16 to 43.45 Wm−2 depending on snow type, solar zenith angle, and location. The potential source regions of the deposited pollutants were identified using spatial variance in wind vector maps, emission inventories coupled with backward air trajectories, and simple region tagged chemical transport modelling. Central, South, and West Asia were the major sources of pollutants during the sampling months, with only a small contribution from East Asia. Analysis based on the Weather Research and Forecasting (WRF-STEM) chemical transport model identified a significant contribution (more than 70 %) from South Asia at selected sites. Research into the presence and effect of pollutants in the glaciated areas of Pakistan is economically significant because the surface water resources in the country mainly depend on the rivers (the Indus and its tributaries) that flow from this glaciated area.

scholarly journals Direct Aerosol Radiative Forcing Uncertainty Based on a Radiative Perturbation Analysis

2010 ◽  
Vol 23 (19) ◽  
pp. 5288-5293 ◽  
Author(s):  
Norman G. Loeb ◽  
Wenying Su
Keyword(s):  
Radiative Forcing ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Aerosol Radiative Forcing ◽  
Clear Sky ◽  
Radiative Perturbation ◽  
Sky Conditions ◽  
Global Mean ◽  
Aerosol Properties ◽  
Aerosol Radiative

Abstract To provide a lower bound for the uncertainty in measurement-based clear- and all-sky direct aerosol radiative forcing (DARF), a radiative perturbation analysis is performed for the ideal case in which the perturbations in global mean aerosol properties are given by published values of systematic uncertainty in Aerosol Robotic Network (AERONET) aerosol measurements. DARF calculations for base-state climatological cloud and aerosol properties over ocean and land are performed, and then repeated after perturbing individual aerosol optical properties (aerosol optical depth, single-scattering albedo, asymmetry parameter, scale height, and anthropogenic fraction) from their base values, keeping all other parameters fixed. The total DARF uncertainty from all aerosol parameters combined is 0.5–1.0 W m−2, a factor of 2–4 greater than the value cited in the Intergovernmental Panel on Climate Change’s (IPCC’s) Fourth Assessment Report. Most of the total DARF uncertainty in this analysis is associated with single-scattering albedo uncertainty. Owing to the greater sensitivity to single-scattering albedo in cloudy columns, DARF uncertainty in all-sky conditions is greater than in clear-sky conditions, even though the global mean clear-sky DARF is more than twice as large as the all-sky DARF.

scholarly journals Intercomparison of biomass burning aerosol optical properties from in situ and remote-sensing instruments in ORACLES-2016

2019 ◽  
Vol 19 (14) ◽  
pp. 9181-9208 ◽  
Author(s):  
Kristina Pistone ◽  
Jens Redemann ◽  
Sarah Doherty ◽  
Paquita Zuidema ◽  
Sharon Burton ◽  
...  
Keyword(s):  
Optical Properties ◽  
Case Studies ◽  
Biomass Burning ◽  
Radiative Forcing ◽  
Measurement Techniques ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Aerosol Optical Properties ◽  
Biomass Burning Aerosol

Abstract. The total effect of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in anthropogenic radiative forcing on the climate. Correct characterization of intensive aerosol optical properties, particularly in conditions where absorbing aerosol is present, is a crucial factor in quantifying these effects. The southeast Atlantic Ocean (SEA), with seasonal biomass burning smoke plumes overlying and mixing with a persistent stratocumulus cloud deck, offers an excellent natural laboratory to make the observations necessary to understand the complexities of aerosol–cloud–radiation interactions. The first field deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in September of 2016 out of Walvis Bay, Namibia. Data collected during ORACLES-2016 are used to derive aerosol properties from an unprecedented number of simultaneous measurement techniques over this region. Here, we present results from six of the eight independent instruments or instrument combinations, all applied to measure or retrieve aerosol absorption and single-scattering albedo. Most but not all of the biomass burning aerosol was located in the free troposphere, in relative humidities typically ranging up to 60 %. We present the single-scattering albedo (SSA), absorbing and total aerosol optical depth (AAOD and AOD), and absorption, scattering, and extinction Ångström exponents (AAE, SAE, and EAE, respectively) for specific case studies looking at near-coincident and near-colocated measurements from multiple instruments, and SSAs for the broader campaign average over the month-long deployment. For the case studies, we find that SSA agrees within the measurement uncertainties between multiple instruments, though, over all cases, there is no strong correlation between values reported by one instrument and another. We also find that agreement between the instruments is more robust at higher aerosol loading (AOD400>0.4). The campaign-wide average and range shows differences in the values measured by each instrument. We find the ORACLES-2016 campaign-average SSA at 500 nm (SSA500) to be between 0.85 and 0.88, depending on the instrument considered (4STAR, AirMSPI, or in situ measurements), with the interquartile ranges for all instruments between 0.83 and 0.89. This is consistent with previous September values reported over the region (between 0.84 and 0.90 for SSA at 550nm). The results suggest that the differences observed in the campaign-average values may be dominated by instrument-specific spatial sampling differences and the natural physical variability in aerosol conditions over the SEA, rather than fundamental methodological differences.

Source apportionment of fine particulate matter in China in 2013 using a source-oriented chemical transport model

2017 ◽  
Vol 601-602 ◽  
pp. 1476-1487 ◽  
Author(s):  
Zhihao Shi ◽  
Jingyi Li ◽  
Lin Huang ◽  
Peng Wang ◽  
Li Wu ◽  
...  
Keyword(s):  
Particulate Matter ◽  
Source Apportionment ◽  
Transport Model ◽  
Fine Particulate Matter ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Fine Particulate

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.

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