Monitoring automotive particulate matter emissions with LiDAR: A review

Automotive particulate matter (PM) causes deleterious effects on health and visibility. Physical and chemical properties of PM also influence climate change. Roadside remote sensing of automotive emissions is a valuable option for assessing the contribution of individual vehicles to the total PM burden. LiDAR represents a unique approach that allows measuring PM emissions from in-use vehicles with high sensitivity. This publication reviews vehicle emission remote sensing measurements using ultraviolet LiDAR and transmissometer systems. The paper discusses the measurement theory and documents examples of how these techniques provide a unique perspective for exhaust emissions of individual and groups of vehicles

Trapping and aerogelation of nanoparticles in negative gravity hydrocarbon flames

We report the experimental realization of continuous carbon aerogel production using a flame aerosol reactor by operating it in negative gravity (−g; up-side-down configuration). Buoyancy opposes the fuel and air flow forces in −g, which eliminates convectional outflow of nanoparticles from the flame and traps them in a distinctive non-tipping, flicker-free, cylindrical flame body, where they grow to millimeter-size aerogel particles and gravitationally fall out. Computational fluid dynamics simulations show that a closed-loop recirculation zone is set up in −g flames, which reduces the time to gel for nanoparticles by ≈10[superscript 6] s, compared to positive gravity (upward rising) flames. Our results open up new possibilities of one-step gas-phase synthesis of a wide variety of aerogels on an industrial scale

Charcoal analysis for temperature reconstruction with infrared spectroscopy

The duration and maximum combustion temperature of vegetation fires are important fire properties with implications for ecology, hydrology, hazard potential, and many other processes. Directly measuring maximum combustion temperature during vegetation fires is difficult. However, chemical transformations associated with temperature are reflected in the chemical properties of charcoals (a by-product of fire). Therefore, charcoal could be used indirectly to determine the maximum combustion temperature of vegetation fires with application to palaeoecological charcoal records. To evaluate the reliability of charcoal chemistry as an indicator of maximum combustion temperature, we studied the chemical properties of charcoal formed through two laboratory methods at measured temperatures. Using a muffle furnace, we generated charcoal from the woody material of ten different tree and shrub species at seven distinct peak temperatures (from 200°C to 800°C in 100°C increments). Additionally, we simulated more natural combustion conditions by burning woody material and leaves of four tree species in a combustion facility instrumented with thermocouples, including thermocouples inside and outside of tree branches. Charcoal samples generated in these controlled settings were analyzed using Fourier Transform Infrared (FTIR) spectroscopy to characterize their chemical properties. The Modern Analogue Technique (MAT) was employed on FTIR spectra of muffle furnace charcoal to assess the accuracy of inferring maximum pyrolysis temperature. The MAT model temperature matching accuracy improved from 46% for all analogues to 81% when including ±100°C. Furthermore, we used MAT to compare charcoal created in the combustion facility with muffle furnace charcoal. Our findings indicate that the spectra of charcoals generated in a combustion facility can be accurately matched with muffle furnace-created charcoals of similar temperatures using MAT, and the accuracy improved when comparing the maximum pyrolysis temperature from muffle furnace charcoal with the maximum inner temperature of the combustion facility charcoal. This suggests that charcoal produced in a muffle furnace may be representative of the inner maximum temperatures for vegetation fire-produced charcoals

Extensive soot compaction by cloud processing from laboratory and field observations

Soot particles form during combustion of carbonaceous materials and impact climate and air quality. When freshly emitted, they are typically fractal-like aggregates. After atmospheric aging, they can act as cloud condensation nuclei, and water condensation or evaporation restructure them to more compact aggregates, affecting their optical, aerodynamic, and surface properties. Here we survey the morphology of ambient soot particles from various locations and different environmental and aging conditions. We used electron microscopy and show extensive soot compaction after cloud processing. We further performed laboratory experiments to simulate atmospheric cloud processing under controlled conditions. We find that soot particles sampled after evaporating the cloud droplets, are significantly more compact than freshly emitted and interstitial soot, confirming that cloud processing, not just exposure to high humidity, compacts soot. Our findings have implications for how the radiative, surface, and aerodynamic properties, and the fate of soot particles are represented in numerical models

Extensive Soot Compaction by Cloud Processing from Laboratory and Field Observations

Soot particles form during combustion of carbonaceous materials and impact climate and air quality. When freshly emitted, they are typically fractal-like aggregates. After atmospheric aging, they can act as cloud condensation nuclei, and water condensation or evaporation restructure them to more compact aggregates, affecting their optical, aerodynamic, and surface properties. Here we survey the morphology of ambient soot particles from various locations and different environmental and aging conditions. We used electron microscopy and show extensive soot compaction after cloud processing. We further performed laboratory experiments to simulate atmospheric cloud processing under controlled conditions. We find that soot particles sampled after evaporating the cloud droplets, are significantly more compact than freshly emitted and interstitial soot, confirming that cloud processing, not just exposure to high humidity, compacts soot. Our findings have implications for how the radiative, surface, and aerodynamic properties, and the fate of soot particles are represented in numerical models.Peer reviewe

Parameterization of the Aerosol Upscatter Fraction as Function of the Backscatter Fraction and Their Relationships to the Asymmetry Parameter for Radiative Transfer Calculations

Simple analytical approximations for aerosol radiative forcing generally contain the aerosol upscatter fraction (the fraction of scattered light that is scattered into the upper hemisphere), while ambient measurements generally yield the backscatter fraction, and theoretical calculations of scattering phase functions often yield the asymmetry parameter. Therefore, simple analytical relationships and parameterizations relating these three parameters are very valuable for radiative transfer calculations. Here, we review published parameterizations, mostly based on the Henyey-Greenstein phase function, and evaluate their goodness and range of validity. In addition, we give new parameterizations that are valid over the full range of backscatter fractions that are possibly encountered in the ambient atmosphere (i.e., 0 to 0.5)

Parameterization of the Aerosol Upscatter Fraction as Function of the Backscatter Fraction and Their Relationships to the Asymmetry Parameter for Radiative Transfer Calculations

Simple analytical approximations for aerosol radiative forcing generally contain the aerosol upscatter fraction (the fraction of scattered light that is scattered into the upper hemisphere), while ambient measurements generally yield the backscatter fraction, and theoretical calculations of scattering phase functions often yield the asymmetry parameter. Therefore, simple analytical relationships and parameterizations relating these three parameters are very valuable for radiative transfer calculations. Here, we review published parameterizations, mostly based on the Henyey-Greenstein phase function, and evaluate their goodness and range of validity. In addition, we give new parameterizations that are valid over the full range of backscatter fractions that are possibly encountered in the ambient atmosphere (i.e., 0 to 0.5)

Monitoring Automotive Particulate Matter Emissions with LiDAR: A Review

Automotive particulate matter (PM) causes deleterious effects on health and visibility. Physical and chemical properties of PM also influence climate change. Roadside remote sensing of automotive emissions is a valuable option for assessing the contribution of individual vehicles to the total PM burden. LiDAR represents a unique approach that allows measuring PM emissions from in-use vehicles with high sensitivity. This publication reviews vehicle emission remote sensing measurements using ultraviolet LiDAR and transmissometer systems. The paper discusses the measurement theory and documents examples of how these techniques provide a unique perspective for exhaust emissions of individual and groups of vehicles

Characterizing Particulate Matter Emissions by Wildland Fires Relevant to Visibility Impairment and PM Non-Attainment

Carbonaceous aerosols, which include contributions from industrial and mobile source emissions and biomass combustion, exert a significant impact on regional air quality. Some preliminary semi-quantitative analyses suggest that smoke from fire-related activity may contribute significantly to observed organic mass concentrations. Further, these emissions have resulted in increased conflicts with the need to attain air quality standards, especially for particulate matter (PM) and visibility, as mandated by the Clean Air Act. However, federal land managers and policy makers currently lack several important tools needed for air quality assessments: composition profiles and analytical techniques necessary to differentiate carbonaceous aerosols originating from industrial and mobile source activity and those from fire emissions; measurement-based PM mass emissions rates for relevant fuels and combustion conditions; and reasonable optical properties and optical property emission rates to attach to fire emissions. In this project, we addressed these needs via a comprehensive, multi-investigator approach that included both laboratory studies and validation of findings via field measurements. Specific elements included: (1) development and validation of promising new, inexpensive methods suitable for quantitative measurement of smoke marker (levoglucosan and K+) concentrations from aerosol filter samples, such as those routinely collected by the IMPROVE or EPA STN networks; (2) laboratory measurements of smoke emission composition profiles for several important fuel types burned under a variety of conditions to provide urgently-needed source profiles for classes of fires believed to severely impact air quality in the western and southeastern U.S.; (3) concurrent with smoke emission profile measurements, measurement of key physical and optical properties and emission rates in the laboratory; and (4) field measurements of fresh smoke plumes to validate whether laboratory smoke studies, conducted under well controlled conditions, can simulate PM2.5 mass, composition, and optical property emissions characteristics of more complex, actual prescribed and wild fires. Further, the field study was to be complemented by lidar measurements to demonstrate the feasibility of using remote sensing methods for continuous monitoring of smoke-polluted atmospheres adjacent to severe wildfires, providing diurnal and spatial variation of aerosol properties, plume heights and dynamics, and direction and rate of smoke plume movement in near real-time. Our project resulted in the generation of a large database of emissions data, and numerous refereed publications describing the methods, findings and implications. Together, the results and methods developed during this study “support the needs of wildland fire managers and policy makers in determining the contribution of biomass burning to PM2.5 and visibility on a regional basis,” as requested in the Call for Proposals, with our work specifically focusing on the western and southeastern U.S. regions