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Rudich, Yinon

Publications and source records attributed to Rudich, Yinon.

Spectro-Microscopic Analysis of Soot Particle Composition and Source Attribution

Ambient soot particles significantly impact Earth’s radiative balance, human health, and atmospheric visibility. Their microstructural properties depend on formation and aging mechanisms, which vary by emission source and atmospheric processes. Hence, accurately identifying sources of soot enhances our understanding of their physicochemical properties and atmospheric implications. This study used a multi-modal approach to characterize and attribute sources of submicron soot particles collected in Israel during new particle formation events, biomass burning episodes, and background atmospheric conditions. Synchrotron-based X-ray microscopy was used to map soot (elemental carbon), organic carbon, and inorganic species. Implemented atomic force microscopy showed highly diverse phase states, with soot consistently exhibiting a solid-like phase. Automated µ-Raman analysis was subsequently performed on ~690 particles, identifying three soot classes based on spectral features corresponding to the "Defect" (D) and "Graphite" (G) bands of soot. We applied two-peak and five-peak fitting approaches to deconvolute the “Defect” peaks (D1, D2, D3, and D4) and G band from average Raman, revealing varying degrees of graphitic order. The degree of graphitic order was determined from metrics such as the D3 peak area, often observed when soot was internally mixed with organic material. Raman spectral features, along with temporal variations in particle classes contributions, suggest that Particle Type 1 corresponds to traffic related soot and Particle Type 2 to less graphitic soot from biomass burning, while Particle Type 3 is associated with more heterogeneous particulate representative of soot-OC mixtures emitted during new particle formation and biomass burning episodes.

Rivera-Adorno, Felipe (ORCID:0000000273557999)↗

Stochastic nucleation processes and substrate abundance explain time-dependent freezing in supercooled droplets

Atmospheric immersion freezing (IF), a heterogeneous ice nucleation process where an ice nucleating particle (INP) is immersed in supercooled water, is a dominant ice formation pathway impacting the hydrological cycle and climate. Implementation of IF derived from field and laboratory data in cloud and climate models is difficult due to the high variability in spatio-temporal scales, INP composition, and morphological complexity. We demonstrate that IF can be consistently described by a stochastic nucleation process accounting for uncertainties in the INP surface area. This approach accounts for time-dependent freezing, a wide range of surface areas and challenges phenomenological descriptions typically used to interpret IF. The results have an immediate impact on the current description, interpretation, and experiments of IF and its implementation in models. The findings are in accord with nucleation theory, and thus should hold for any supercooled liquid material that nucleates in contact with a substrate.

54 ENVIRONMENTAL SCIENCES↗

Variation in Global Chemical Composition of PM2.5: Emerging Results from SPARTAN

The Surface PARTiculate mAtter Network (SPARTAN) is a long-term project that includes characterization of chemical and physical attributes of aerosols from filter samples collected worldwide. This paper discusses the ongoing efforts of SPARTAN to define and quantify major ions and trace metals found in fine particulate matter (PM (sub 2.5). Our methods infer the spatial and temporal variability of PM (sub 2.5) in a cost-effective manner. Gravimetrically weighed filters represent multi-day averages of PM (sub 2.5), with a collocated nephelometer sampling air continuously. SPARTAN instruments are paired with AErosol RObotic NETwork (AERONET) sun photometers to better understand the relationship between ground-level PM (sub 2.5) and columnar aerosol optical depth (AOD). We have examined the chemical composition of PM (sub 2.5) at 12 globally dispersed, densely populated urban locations and a site at Mammoth Cave (US) National Park used as a background comparison. So far, each SPARTAN location has been active between the years 2013 and 2016 over periods of 2-26 months, with an average period of 12 months per site. These sites have collectively gathered over 10 years of quality aerosol data. The major PM (sub 2.5) constituents across all sites (relative contribution plus or minus Standard Deviation) are ammoniated sulfate (20 percent plus or minus 11 percent), crustal material (13.4 percent plus or minus 9.9 percent), equivalent black carbon (11.9 percent plus or minus 8.4 percent), ammonium nitrate (4.7 percent plus or minus 3.0 percent), sea salt (2.3 percent plus or minus 1.6 percent), trace element oxides (1.0 percent plus or minus 1.1 percent), water (7.2 percent plus or minus 3.3 percent) at 35 percent relative humidity, and residual matter (40 percent plus or minus 24 percent). Analysis of filter samples reveals that several PM (sub 2.5) chemical components varied by more than an order of magnitude between sites. Ammoniated sulfate ranges from 1.1 microns per cubic meter (Buenos Aires, Argentina) to 17 microns per cubic meter (Kanpur, India in the dry season). Ammonium nitrate ranged from 0.2 microns per cubic meter (Mammoth Cave, in summer) to 6.8 microns per cubic meter (Kanpur, dry season). Equivalent black carbon ranged from 0.7 microns per cubic meter (Mammoth Cave) to over 8 microns per cubic meter (Dhaka, Bangladesh and Kanpur, India). Comparison of SPARTAN vs. coincident measurements from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network at Mammoth Cave yielded a high degree of consistency for daily PM (sub 2.5) (r squared equals 0.76, slope equals 1.12), daily sulfate (r squared equals 0.86, slope equals 1.03), and mean fractions of all major PM (sub 2.5) components (within 6 percent). Major ions generally agree well with previous studies at the same urban locations (e.g. sulfate fractions agree within 4 percent for 8 out of 11 collocation comparisons). Enhanced anthropogenic dust fractions in large urban areas (e.g. Singapore, Kanpur, Hanoi, and Dhaka) are apparent from high Zn to Al ratios. The expected water contribution to aerosols is calculated via the hygroscopicity parameter kappa (sub v (volume)) for each filter. Mean aggregate values ranged from 0.15 (Ilorin) to 0.28 (Rehovot). The all-site parameter mean is 0.20 plus or minus 0.04. Chemical composition and water retention in each filter measurement allows inference of hourly PM (sub 2.5) at 35 percent relative humidity by merging with nephelometer measurements. These hourly PM (sub 2.5) estimates compare favourably with a beta attenuation monitor (MetOne) at the nearby US embassy in Beijing, with a coefficient of variation r squared equals 0.67 (number equals 3167), compared to r squared equals 0.62 when v (volume) was not considered. SPARTAN continues to provide an open-access database of PM (sub 2.5) compositional filter information and hourly mass collected from a global federation of instruments.

Snider, Graydon↗

Clouds Aerosols Internal Affaires: Increasing Cloud Fraction and Enhancing the Convection

Clouds developing in a polluted environment have more numerous, smaller cloud droplets that can increase the cloud lifetime and liquid water content. Such changes in the cloud droplet properties may suppress low precipitation allowing development of a stronger convection and higher freezing level. Delaying the washout of the cloud water (and aerosol), and the stronger convection will result in higher clouds with longer life time and larger anvils. We show these effects by using large statistics of the new, 1km resolution data from MODIS on the Terra satellite. We isolate the aerosol effects from meteorology by regression and showing that aerosol microphysical effects increases cloud fraction by average of 30 presents for all cloud types and increases convective cloud top pressure by average of 35mb. We analyze the aerosol cloud interaction separately for high pressure trade wind cloud systems and separately for deep convective cloud systems. The resultant aerosol radiative effect on climate for the high pressure cloud system is: -10 to -13 W/sq m at the top of the atmosphere (TOA) and -11 to -14 W/sq m at the surface. For deeper convective clouds the forcing is: -4 to -5 W/sq m at the TOA and -6 to -7 W/sq m at the surface.

Koren, Ilan↗