scholarly journals Optical closure experiments for biomass smoke aerosols

2010 ◽  
Vol 10 (3) ◽  
pp. 7469-7494 ◽  
Author(s):  
L. E. Mack ◽  
E. J. T. Levin ◽  
S. M. Kreidenweis ◽  
D. Obrist ◽  
H. Moosmüller ◽  
...  
Keyword(s):  
Optical Properties ◽  
Complex Refractive Index ◽  
Single Scattering ◽  
Size Distributions ◽  
Laboratory Studies ◽  
Biomass Smoke ◽  
Scattering Coefficients ◽  
Aerosol Absorption ◽  
Southeastern Us ◽  
Highly Sensitive

Abstract. The FLAME experiments were a series of laboratory studies of the chemical, physical, and optical properties of fresh smokes from the combustion of wildland fuels that are burned annually in the western and southeastern US. The burns were conducted in the combustion chamber of the USFS Fire Sciences Laboratory in Missoula, Montana. Here we discuss the retrieval of optical properties for a variety of fuels burned in FLAME 2, using nephelometer-measured scattering coefficients, photoacoustically-measured aerosol absorption coefficients, and size distribution measurements. Uncertainties are estimated from the various instrument characteristics and from instrument calibration studies. Our estimates of single scattering albedo for different dry smokes varied from 0.43–0.99, indicative of the wide variations in smoke aerosol chemical composition that were observed. In selected case studies, we retrieved the complex refractive index from the measurements, but show that these are highly sensitive to the uncertainties in measured size distributions.

scholarly journals Optical closure experiments for biomass smoke aerosols

2010 ◽  
Vol 10 (18) ◽  
pp. 9017-9026 ◽  
Author(s):  
L. A. Mack ◽  
E. J. T. Levin ◽  
S. M. Kreidenweis ◽  
D. Obrist ◽  
H. Moosmüller ◽  
...  
Keyword(s):  
Optical Properties ◽  
Complex Refractive Index ◽  
Single Scattering ◽  
Biomass Smoke ◽  
Scattering Coefficients ◽  
Aerosol Absorption ◽  
Southeastern Us ◽  
Highly Sensitive ◽  
The Us ◽  
Us Forest Service

Abstract. A series of laboratory experiments at the Fire Laboratory at Missoula (FLAME) investigated chemical, physical, and optical properties of fresh smoke samples from combustion of wildland fuels that are burned annually in the western and southeastern US The burns were conducted in the combustion chamber of the US Forest Service Fire Sciences Laboratory in Missoula, Montana. Here we discuss retrieval of optical properties for a variety of fuels burned in FLAME 2, using nephelometer-measured scattering coefficients, photoacoustically-measured aerosol absorption coefficients, and size distribution measurements. Uncertainties are estimated from various instrument characteristics and instrument calibration studies. Our estimates of single scattering albedo for different dry smoke samples varied from 0.428 to 0.990, indicative of observed wide variations in smoke aerosol chemical composition. In selected case studies, we retrieved the complex refractive index from measurements but show that these are highly sensitive to uncertainties in measured size distributions.

scholarly journals Physical and optical properties of aged biomass burning aerosol from wildfires in Siberia and the Western USA at the Mt. Bachelor Observatory

2016 ◽  
Vol 16 (23) ◽  
pp. 15185-15197 ◽  
Author(s):  
James R. Laing ◽  
Daniel A. Jaffe ◽  
Jonathan R. Hee
Keyword(s):  
Optical Properties ◽  
Pacific Northwest ◽  
Biomass Burning ◽  
Geometric Mean ◽  
Fine Particulate Matter ◽  
Single Scattering ◽  
Absorption Efficiency ◽  
Size Distributions ◽  
Scanning Mobility Particle Sizer ◽  
Scattering Coefficients

Abstract. The summer of 2015 was an extreme forest fire year in the Pacific Northwest. Our sample site at the Mt. Bachelor Observatory (MBO, 2.7 km a.s.l.) in central Oregon observed biomass burning (BB) events more than 50 % of the time during August. In this paper we characterize the aerosol physical and optical properties of 19 aged BB events during August 2015. Six of the 19 events were influenced by Siberian fires originating near Lake Baikal that were transported to MBO over 4–10 days. The remainder of the events resulted from wildfires in Northern California and Southwestern Oregon with transport times to MBO ranging from 3 to 35 h. Fine particulate matter (PM1), carbon monoxide (CO), aerosol light scattering coefficients (σscat), aerosol light absorption coefficients (σabs), and aerosol number size distributions were measured throughout the campaign. We found that the Siberian events had a significantly higher Δσabs∕ΔCO enhancement ratio, higher mass absorption efficiency (MAE; Δσabs∕ΔPM1), lower single scattering albedo (ω), and lower absorption Ångström exponent (AAE) when compared with the regional events. We suggest that the observed Siberian events represent that portion of the plume that has hotter flaming fire conditions and thus enabled strong pyroconvective lofting and long-range transport to MBO. The Siberian events observed at MBO therefore represent a selected portion of the original plume that would then have preferentially higher black carbon emissions and thus an enhancement in absorption. The lower AAE values in the Siberian events compared to regional events indicate a lack of brown carbon (BrC) production by the Siberian fires or a loss of BrC during transport. We found that mass scattering efficiencies (MSE) for the BB events ranged from 2.50 to 4.76 m2 g−1. We measured aerosol size distributions with a scanning mobility particle sizer (SMPS). Number size distributions ranged from unimodal to bimodal and had geometric mean diameters (Dpm) ranging from 138 to 229 nm and geometric standard deviations (σg) ranging from 1.53 to 1.89. We found MSEs for BB events to be positively correlated with the geometric mean of the aerosol size distributions (R2 = 0.73), which agrees with Mie theory. We did not find any dependence on event size distribution to transport time or fire source location.

scholarly journals Heterogeneous OH oxidation of secondary brown carbon aerosol

2018 ◽  
Author(s):  
Elijah G. Schnitzler ◽  
Jonathan P. D. Abbatt
Keyword(s):  
Optical Properties ◽  
Single Scattering ◽  
Trace Gas ◽  
Absorption Enhancement ◽  
Brown Carbon ◽  
Scattering Coefficients ◽  
Aerosol Absorption ◽  
In Series ◽  
First Time ◽  
Slow Absorption

Abstract. Light-absorbing organic aerosol, or brown carbon (BrC), has significant but poorly-constrained effects on climate; for example, oxidation in the atmosphere may alter its optical properties, leading to absorption enhancement or bleaching. Here, we investigate for the first time the effects of heterogeneous OH oxidation on the optical properties of a laboratory surrogate of secondary BrC in a series of photo-oxidation chamber experiments. The BrC surrogate was generated from aqueous resorcinol, or 1,3-dihydroxybenzene, and H2O2 exposed to > 300 nm radiation, atomized, passed through trace gas denuders, and injected into the chamber, which was conditioned to either 15 or 60 % relative humidity (RH). Aerosol absorption and scattering coefficients and single scattering albedo (SSA) at 405 nm were measured using a photo-acoustic spectrometer. At 60 % RH, upon OH exposure, absorption first increased, and the SSA decreased sharply. Subsequently, absorption decreased faster than scattering, and SSA increased gradually. Comparisons to the modelled trend in SSA, based on Mie theory calculations, confirm that the observed trend is due to chemical evolution, rather than slight changes in particle size. The initial absorption enhancement is likely due to molecular functionalization and/or oligomerization, and the bleaching to fragmentation. By contrast, at 15 % RH, slow absorption enhancement was observed, without appreciable bleaching. A multi-layer kinetics model, consisting of two surface reactions in series, was constructed to provide further insights regarding the RH-dependence of the optical evolution. Candidate parameters suggest that the oxidation is efficient, with uptake coefficients on the order of unity, and the aerosol is very viscous, even at 60 % RH. At 15 % RH, the aerosol will be viscous enough to confine products of fragmentation, leading to their recombination, such that little bleaching is observed on the experimental timescale. These results further the current understanding of the complex processing of BrC that may occur in the atmosphere.

scholarly journals Heterogeneous OH oxidation of secondary brown carbon aerosol

2018 ◽  
Vol 18 (19) ◽  
pp. 14539-14553 ◽  
Author(s):  
Elijah G. Schnitzler ◽  
Jonathan P. D. Abbatt
Keyword(s):  
Optical Properties ◽  
Single Scattering ◽  
Trace Gas ◽  
Absorption Enhancement ◽  
Brown Carbon ◽  
Scattering Coefficients ◽  
Aerosol Absorption ◽  
Photoacoustic Spectrometer ◽  
In Series ◽  
First Time

Abstract. Light-absorbing organic aerosol, or brown carbon (BrC), has significant but poorly constrained effects on climate; for example, oxidation in the atmosphere may alter its optical properties, leading to absorption enhancement or bleaching. Here, we investigate for the first time the effects of heterogeneous OH oxidation on the optical properties of a laboratory surrogate of aqueous, secondary BrC in a series of photo-oxidation chamber experiments. The BrC surrogate was generated from aqueous resorcinol, or 1,3-dihydroxybenzene, and H2O2 exposed to >300 nm radiation that is atomized, passed through trace gas denuders, and injected into the chamber, which was conditioned to either 15 % or 60 % relative humidity (RH). Aerosol absorption and scattering coefficients and single scattering albedo (SSA) at 405 nm were measured using a photoacoustic spectrometer. At 60 % RH, upon OH exposure, absorption first increased, and the SSA decreased sharply. Subsequently, absorption decreased faster than scattering, and SSA increased gradually. Comparisons to the modelled trend in SSA, based on Mie theory calculations, confirm that the observed trend is due to chemical evolution, rather than slight changes in particle size. The initial absorption enhancement is likely due to molecular functionalization and/or oligomerization and the bleaching to fragmentation. By contrast, at 15 % RH, slow absorption enhancement was observed without appreciable bleaching. A multi-layer kinetics model, consisting of two surface reactions in series, was constructed to provide further insights regarding the RH dependence of the optical evolution. Candidate parameters suggest that the oxidation is efficient, with uptake coefficients on the order of unity. The parameters also suggest that, as RH decreases, reactivity decreases and aerosol viscosity increases, such that particles are well-mixed at 60 % RH but not at 15 % RH. These results further the current understanding of the complex processing of BrC that may occur in the atmosphere.

scholarly journals South African EUCAARI measurements: seasonal variation of trace gases and aerosol optical properties

2012 ◽  
Vol 12 (4) ◽  
pp. 1847-1864 ◽  
Author(s):  
L. Laakso ◽  
V. Vakkari ◽  
A. Virkkula ◽  
H. Laakso ◽  
J. Backman ◽  
...  
Keyword(s):  
Optical Properties ◽  
Seasonal Variation ◽  
Atmospheric Aerosols ◽  
Single Scattering ◽  
Observation System ◽  
Global Context ◽  
Scattering Coefficients ◽  
Aerosol Absorption ◽  
The Mean ◽  
Winter Time

Abstract. In this paper we introduce new in situ observations of atmospheric aerosols, especially chemical composition, physical and optical properties, on the eastern brink of the heavily polluted Highveld area in South Africa. During the observation period between 11 February 2009 and 31 January 2011, the mean particle number concentration (size range 10–840 nm) was 6310 cm3 and the estimated volume of sub-10 μm particles 9.3 μm3 m−3. The aerosol absorption and scattering coefficients at 637 nm were 8.3 Mm−1 and 49.5 Mm−1, respectively. The mean single-scattering albedo at 637 nm was 0.84 and the Ångström exponent of scattering was 1.5 over the wavelength range 450–635 nm. The mean O3, SO2, NOx and H2S-concentrations were 37.1, 11.5, 15.1 and 3.2 ppb, respectively. The observed range of concentrations was large and attributed to the seasonal variation of sources and regional meteorological effects, especially the anticyclonic re-circulation and strong winter-time inversions. In a global context, the levels of gases and particulates were typical for continental sites with strong anthropogenic influence, but clearly lower than the most polluted areas of south-eastern Asia. Of all pollutants observed at the site, ozone is the most likely to have adverse environmental effects, as the concentrations were high also during the growing season. The measurements presented here will help to close existing gaps in the ground-based global atmosphere observation system, since very little long-term data of this nature is available for southern Africa.

scholarly journals Improved Lorenz-Mie Look-Up Table for Lidar and Polarimeter Retrievals

2021 ◽  
Vol 2 ◽  
Author(s):  
Eduard Chemyakin ◽  
Snorre Stamnes ◽  
Sharon P. Burton ◽  
Xu Liu ◽  
Chris Hostetler ◽  
...  
Keyword(s):  
Refractive Index ◽  
Atmospheric Aerosols ◽  
Complex Refractive Index ◽  
Scattering Matrix ◽  
Single Scattering ◽  
Scattering Coefficients ◽  
Aerosol Absorption ◽  
Look Up Table ◽  
Speed Up ◽  
The Look

Lidar and polarimeter aerosol microphysical retrievals require calculating single-scattering properties that are computationally expensive. One of the easiest ways to speed up these calculations is to use a look-up table. Two important currently available look-up tables were created about 15 years ago. Advancements in modern computational hardware allows us to create a new look-up table with improved precision over a larger range of aerosol properties. In this new and improved Lorenz-Mie look-up table we tabulate the light scattering by an ensemble of homogeneous isotropic spheres at arbitrary wavelengths starting from 0.355 μm. The improved look-up table covers spherical atmospheric aerosols with radii in the range of 0.001–100 μm, with real parts of the complex refractive index in the range of 1.29–1.65, and with imaginary parts of the complex refractive index in the range of 0–0.05. We test twelve wavelengths from 0.355 to 2.264 μm and find that the elements of the normalized scattering matrix as well as the asymmetry parameter, the aerosol absorption, backscatter, extinction, and scattering coefficients are precise to within 1% for 99.99% of cases. The look-up table together with C++, Fortran, Matlab, and Python codes are freely available online.

scholarly journals A new approach for retrieving the UV–vis optical properties of ambient aerosols

2016 ◽  
Vol 9 (8) ◽  
pp. 3477-3490 ◽  
Author(s):  
Nir Bluvshtein ◽  
J. Michel Flores ◽  
Lior Segev ◽  
Yinon Rudich
Keyword(s):  
Optical Properties ◽  
Atmospheric Aerosols ◽  
Radiative Forcing ◽  
Complex Refractive Index ◽  
Single Scattering ◽  
Aerosol Size Distribution ◽  
Distribution Data ◽  
Ambient Aerosols ◽  
New Approach ◽  
Effective Radiative Forcing

Abstract. Atmospheric aerosols play an important part in the Earth's energy budget by scattering and absorbing incoming solar and outgoing terrestrial radiation. To quantify the effective radiative forcing due to aerosol–radiation interactions, researchers must obtain a detailed understanding of the spectrally dependent intensive and extensive optical properties of different aerosol types. Our new approach retrieves the optical coefficients and the single-scattering albedo of the total aerosol population over 300 to 650 nm wavelength, using extinction measurements from a broadband cavity-enhanced spectrometer at 315 to 345 nm and 390 to 420 nm, extinction and absorption measurements at 404 nm from a photoacoustic cell coupled to a cavity ring-down spectrometer, and scattering measurements from a three-wavelength integrating nephelometer. By combining these measurements with aerosol size distribution data, we retrieved the time- and wavelength-dependent effective complex refractive index of the aerosols. Retrieval simulations and laboratory measurements of brown carbon proxies showed low absolute errors and good agreement with expected and reported values. Finally, we implemented this new broadband method to achieve continuous spectral- and time-dependent monitoring of ambient aerosol population, including, for the first time, extinction measurements using cavity-enhanced spectrometry in the 315 to 345 nm UV range, in which significant light absorption may occur.

scholarly journals Atmospheric radiative effects of an in-situ measured Saharan dust plume and the role of large particles

2007 ◽  
Vol 7 (3) ◽  
pp. 7767-7817 ◽  
Author(s):  
S. Otto ◽  
M. de Reus ◽  
T. Trautmann ◽  
A. Thomas ◽  
M. Wendisch ◽  
...  
Keyword(s):  
Complex Refractive Index ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Saharan Dust ◽  
Dust Particles ◽  
Modal Parameters ◽  
Size Distributions ◽  
Radiative Effects ◽  
Enhanced Absorption ◽  
Large Particles

Abstract. This work will present aerosol size distributions measured in a Saharan dust plume between 0.9 and 12 km altitude during the ACE-2 campaign 1997. The distributions contain a significant fraction of large particles of diameters from 4 to 30 μm. Radiative transfer calculations have been performed using these data as input. Shortwave, longwave as well as total atmospheric radiative effects (AREs) of the dust plume are investigated over ocean and desert within the scope of sensitivity studies considering varied input parameters like solar zenith angle, scaled total dust optical depth, tropospheric standard aerosol profiles and particle complex refractive index. The results indicate that the large particle fraction has a predominant impact on the optical properties of the dust. A single scattering albedo of ωo=0.75–0.96 at 550 nm was simulated in the entire dust column as well as 0.76 within the Saharan dust layer at ~4 km altitude indicating enhanced absorption. The measured dust leads to cooling over the ocean but warming over the desert due to differences in their spectral surface albedo and surface temperature. The large particles absorb strongly and they contribute at least 20% to the ARE in the dusty atmosphere. From the measured size distributions modal parameters of a bimodal lognormal column volume size distribution were deduced, resulting in a coarse median diameter of ~9 μm and a column single scattering albedo of 0.78 at 550 nm. A sensitivity study demonstrates that variabilities in the modal parameters can cause completely different AREs and emphasises the warming effect of the large mineral dust particles.

scholarly journals Optical properties of atmospheric fine particles near Beijing during the HOPE-J<sup>3</sup>A Campaign

2015 ◽  
Vol 15 (22) ◽  
pp. 33675-33730
Author(s):  
X. Xu ◽  
W. Zhao ◽  
Q. Zhang ◽  
S. Wang ◽  
B. Fang ◽  
...  
Keyword(s):  
Refractive Index ◽  
Optical Properties ◽  
Fine Particles ◽  
Complex Refractive Index ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Organic Mass ◽  
Absorption Coefficients ◽  
Aerosol Composition ◽  
Inorganic Species

Abstract. The optical properties and chemical composition of PM1.0 (particulate with an aerodynamic diameter of less than 1.0 μm) particles in a suburban environment (Huairou) near the mega-city Beijing were measured during the HOPE-J3A (Haze Observation Project Especially for Jing-Jin-Ji Area) field campaign. The campaign covered the period November 2014 to January 2015 during the winter coal heating season. The average and standard deviations for the extinction, scattering, absorption coefficients, and the aerosol single scattering albedo (SSA) at λ = 470 nm during the measurement period were 201 ± 240, 164 ± 202, 37 ± 43 Mm-1, and 0.80 ± 0.08, respectively. The mean mass scattering (MSE) and absorption (MAE) efficiencies were 4.77 ± 0.01 and 0.87 ± 0.03 m2g-1, respectively. Highly time-resolved air pollution episodes clearly show the dramatic evolution of the PM1.0 size distribution, extensive optical properties (extinction, scattering, and absorption coefficients) and intensive optical properties (single scattering albedo and complex refractive index) during haze formation, development and decline. Time periods were classified into three different pollution levels (clear, slightly polluted, and polluted) for further analysis. It was found that: (1) The diurnal patterns of the aerosol extinction, scattering, absorption coefficients, and SSA differed for the three pollution classes. (2) The real and imaginary part of complex refractive index (CRI) increased, while the SSA decreased from clear to polluted days. (3) The relative contributions of organic and inorganic species to observed aerosol composition changed significantly from clear to polluted days: the organic mass fraction decreased (50 to 43 %) while the proportion of sulfates, nitrates, and ammonium increased strongly (34 to 44 %). (4) The fractional contribution of chemical components to extinction coefficients was calculated by using the modified IMPROVE algorithm. Organic mass was the largest contributor (58 %) to the total extinction of PM1.0. When the air quality deteriorated, the change of the relative contribution of sulfate aerosol to the total extinction was small, but the contribution of nitrate aerosol increased significantly (from 17 % on clear days to 23 % on polluted days). (5) The observed mass scattering efficiencies increased consistently with the pollution extent, however, the observed mass absorption efficiencies increased consistently with increasing mass concentration in slightly pollution conditions, but decreased under polluted conditions.

scholarly journals A shape model of internally mixed soot particles derived from artificial surface tension

2019 ◽  
Vol 12 (1) ◽  
pp. 107-118 ◽  
Author(s):  
Hiroshi Ishimoto ◽  
Rei Kudo ◽  
Kouji Adachi
Keyword(s):  
Surface Tension ◽  
Optical Properties ◽  
Single Scattering ◽  
Dipole Approximation ◽  
Water Soluble ◽  
Shape Model ◽  
Biomass Smoke ◽  
Soot Particles ◽  
Artificial Surface ◽  
Aggregate Shape

Abstract. To retrieve the physical properties of aerosols from multi-channel ground-based and satellite measurements, we developed a shape model of coated soot particles and created a dataset of their optical properties. Bare soot particles were assumed to have an aggregate shape, and two types of aggregates with different size–shape dependences were modeled using a polyhedral Voronoi structure. To simulate the detailed shape properties of mixtures of soot aggregates and adhered water-soluble substances, we propose a simple model of surface tension derived from the artificial surface potential. The light-scattering properties of the modeled particles with different volume fractions of water-soluble material were calculated using the finite-difference time-domain method and discrete-dipole approximation. The results of the single-scattering albedo and asymmetry factors were compared to those of conventional internally mixed spheres (i.e., effective medium spheres based on the Maxwell-Garnett approximation and simple core-shell spheres). In addition, the lidar backscattering properties (i.e., lidar ratios and linear depolarization ratios) of the modeled soot particles were investigated. For internally mixed soot particles, the lidar backscattering properties were sensitive to the shape of the soot particles and the volume mixing ratio of the assumed water-soluble components. However, the average optical properties of biomass smoke, which have been reported from in situ field and laboratory measurements, were difficult to explain based on the individually modeled particle. Nonetheless, our shape model and its calculated optical properties are expected to be useful as an alternative model for biomass smoke particles in advanced remote sensing via multi-channel radiometer and lidar measurements.

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