Biomass burning aerosol heating rates from the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) 2016 and 2017 experiments

Aerosol heating due to shortwave absorption has implications for local atmospheric stability and regional dynamics. The derivation of heating rate profiles from space-based observations is challenging because it requires the vertical profile of relevant properties such as the aerosol extinction coefficient and single-scattering albedo (SSA). In the southeastern Atlantic, this challenge is amplified by the presence of stratocumulus clouds below the biomass burning plume advected from Africa, since the cloud properties affect the magnitude of the aerosol heating aloft, which may in turn lead to changes in the cloud properties and life cycle. The combination of spaceborne lidar data with passive imagers shows promise for future derivations of heating rate profiles and curtains, but new algorithms require careful testing with data from aircraft experiments where measurements of radiation, aerosol, and cloud parameters are better colocated and readily available. In this study, we derive heating rate profiles and vertical cross sections (curtains) from aircraft measurements during the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) project in the southeastern Atlantic. Spectrally resolved irradiance measurements and the derived column absorption allow for the separation of total heating rates into aerosol and gas (primarily water vapor) absorption. The nine cases we analyzed capture some of the co-variability of heating rate profiles and their primary drivers, leading to the development of a new concept: the heating rate efficiency (HRE; the heating rate per unit aerosol extinction). HRE, which accounts for the overall aerosol loading as well as vertical distribution of the aerosol layer, varies little with altitude as opposed to the standard heating rate. The large case-to-case variability for ORACLES is significantly reduced after converting from heating rate to HRE, allowing us to quantify its dependence on SSA, cloud albedo, and solar zenith angle.

Non-reversible aging can increase solar absorption in African biomass burning aerosol plumes of intermediate age

Recent studies highlight that biomass-burning aerosol over the remote southeast Atlantic is some of the most sunlight-absorbing aerosol on the planet. In-situ measurements of single-scattering albedo at the 530 nm wavelength (SSA530nm) range from 0.83 to 0.89 within six flights (five in September, 2016 and one in late August, 2017) of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) aircraft campaign, increasing with the organic aerosol to black carbon (OA : BC) mass ratio. OA : BC mass ratios of 10 to 14 are lower than some model values and consistent with BC-enriched source emissions, based on indirect inferences of fuel type (savannah grasslands) and dry, flame-efficient combustion conditions. These primarily explain the low single-scattering albedos. We investigate whether continued chemical aging of aerosol plumes of intermediate age (4–7 days after emission, as determined from model tracers) within the free troposphere can further lower the SSA530nm. A mean OA to organic carbon mass ratio of 2.2 indicates highly oxygenated aerosol with the chemical marker f44 indicating the free-tropospheric aerosol continues to oxidize after advecting offshore of continental Africa. Two flights, for which BC to carbon monoxide (CO) ratios remain constant with increasing chemical age, are analyzed further. In both flights, the OA : BC mass ratio decreases over the same time span, indicating continuing net aerosol loss. One flight sampled younger (∼ 4 days) aerosol within the strong zonal outflow of the 4–6 km altitude African Easterly Jet-South. This possessed the highest OA : BC mass ratio of the 2016 campaign and overlaid slightly older aerosol with proportionately less OA, although the age difference of one day is not enough to attribute to a large-scale recirculation and subsidence pattern. The other flight sampled aerosol constrained closer to the coast by a mid-latitude disturbance and found older aerosol aloft overlying younger aerosol. Its vertical increase in OA : BC and nitrate to BC was less pronounced than when younger aerosol overlaid older aerosol, consistent with compensation between a net aerosol loss through aging and a thermodynamical partitioning. Organic nitrate provided 68 % on average of the total nitrate for the 6 flights, in contrast to measurements made at Ascension Island that only found inorganic nitrate. Some evidence for the thermodynamical partitioning to the particle phase at higher altitudes with higher relative humidities for nitrate is still found. The 470–660 nm absorption Angstrom exponent is slightly higher near the African coast than further offshore (approximately 1.2 versus 1.0–1.1), indicating some brown carbon may be present near the coast. The data support the following parameterization: SSA530nm = 0.80+0056*(OA : BC). This indicates a 20 % decrease in SSA can be attributed to chemical aging, or the net 25 % reduction in OA : BC documented for constant BC : CO ratios.

A Satellite Data Based Detailed Study of the Aerosol Emitted from Open Biomass Burning in Northeast China

Due to its unique natural conditions and agricultural tradition, northeast China (NEC) has formed a distinctive open biomass burning habit with local-specific biomass burning aerosol features. In this research, with the help of a newly optimized biomass burning aerosol identification method, which combines satellite aerosol and fire observational products with the HYSPLIT model forward trajectories, a systematic and quantitative analysis of aerosol emitted from open biomass burning in the NEC region are conducted to determine in detail its local-specific features, such as influence region, aging characteristics, and seasonal variation. During the 72-h aging process after biomass burning emission, aerosol particle size growth found with the Angstrom exponent declines from 1.6 to 1.54. Additionally, the volume fraction of black carbon decreases from 4.5% to 3.1%, leading to the Single Scattering Albedo (SSA) increasing from the fresh state of 0.84 to the aged state of 0.89. The cooling effect at TOA, due to the existence of aerosol, is enhanced by more than 70%, indicating its severe and dynamic influence on climate change. The average AOD in spring is 0.63, which is higher than autumn’s value of 0.52, indicating that biomass burning is more intensive in spring. Compared to autumn, aerosols emitted from spring biomass burning in the NEC region have lower sphere fraction, smaller particle size, higher volume fraction of black carbon, higher absorbability, and weaker cooling effect at TOA, which can be partly explained by the drier ambient environment and lower water content of the burned crop straw in spring.

Functionality-Based Formation of Secondary Organic Aerosol from m-Xylene Photooxidation

Photooxidation of volatile organic compounds (VOCs) produces condensable oxidized organics (COOs) to yield secondary organic aerosol (SOA), but the fundamental chemical mechanism for gas-to-particle conversion remains uncertain. Here we elucidate the production of COOs and their roles in SOA and brown carbon (BrC) formation from m-xylene oxidation by simultaneous monitoring the evolutions of gas-phase products and aerosol properties in an environmental chamber. Four COO types with the distinct functionalities of dicarbonyls, carboxylic acids, polyhydroxy aromatics/quinones, and nitrophenols are identified from early-generation oxidation, with the yields of 25 %, 37 %, 5 %, and 3 %, respectively. SOA formation occurs via several heterogeneous processes, including interfacial interaction, ionic dissociation/acid-base reaction, and oligomerization, with the yields of (20 ± 4) % and (32 ± 7) % at 10 % and 70 % relative humidity (RH), respectively. Chemical speciation shows the dominant presence of oligomers, nitrogen-containing organics, and carboxylates at RH and carboxylates at low RH. The identified BrC includes N-heterocycles/N-heterochains and nitrophenols, as evident from reduced single scattering albedo. The measured uptake coefficient (γ) for COOs is dependent on the functionality, ranging from 3.7 × 10−4 to 1.3 × 10−2. A kinetic framework is developed to predict SOA production from the concentrations and uptake coefficients for COOs. This functionality-based approach well reproduces SOA formation from m-xylene oxidation and is broadly applicable to VOC oxidation for other species. Our results reveal that photochemical oxidation of m-xylene represents a major source for SOA and BrC formation under urban environments, because of its large abundance, high reactivity with OH, and high yields for COOs.

Comparative analysis of the error of the single scattering approximation when solving one inverse problem in two-dimensional and three- dimensional cases

The inverse problem for the nonstationary radiative transfer equation is considered, which consists in finding the scattering coefficient for a given time-angular distribution of the solution to the equation at a certain point. To solve this problem, the single scattering approximation in the pulsed sounding mode is used. A comparative analysis of the error in solving the inverse problem in the single scattering approximation for two-dimensional and three-dimensional models describing the process of high-frequency acoustic sounding in a fluctuating ocean is carried out. It is shown that in the two-dimensional case the error of the approximate solution significantly exceeds the error in the three-dimensional model.

A survey on rendering homogeneous participating media

Participating media are frequent in real-world scenes, whether they contain milk, fruit juice, oil, or muddy water in a river or the ocean. Incoming light interacts with these participating media in complex ways: refraction at boundaries and scattering and absorption inside volumes. The radiative transfer equation is the key to solving this problem. There are several categories of rendering methods which are all based on this equation, but using different solutions. In this paper, we introduce these groups, which include volume density estimation based approaches, virtual point/ray/beam lights, point based approaches, Monte Carlo based approaches, acceleration techniques, accurate single scattering methods, neural network based methods, and spatially-correlated participating media related methods. As well as discussing these methods, we consider the challenges and open problems in this research area.

NUMERICAL-ANALYTICAL MODEL OF THE LUMINANCE FACTOR OF AN ARBITRARY SURFACE

Road safety is determined by the distribution of luminance created by asphalt concrete surfaces. On the one hand, experimental determination of the bidirectional reflectance distribution function is laborious, on the other hand, for some angles this task is difficult. The authors propose to use both analytical and statistical models of the luminance factor, which allow determining the luminance factors or coefficients for arbitrary angles of incidence and sighting. The models are based on the idea of a plane-parallel layer, in the volume of which radiation scattering occurs. With correctly selected optical properties of the layer (the optical thickness of the medium, the albedo of single scattering, the phase function of the particles included in the composition), the models allow obtaining reliable results, which was confirmed when compared with the measurement results. The models can also be applicable not only for asphalt concrete pavements, but also for any other surfaces.