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At least 271 records · Page 15

Measurement report: The Fifth International Workshop on Ice Nucleation phase 1 (FIN-01): intercomparison of single-particle mass spectrometers

Knowledge of the chemical composition and mixing state of aerosols at a single-particle level is critical for gaining insights into atmospheric processes. One common tool to make these measurements is single-particle mass spectrometry. There remains a need to compare the performance of different single-particle mass spectrometers (SPMSs). An intercomparison of SPMSs was conducted at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) chamber at the Karlsruhe Institute of Technology (KIT) in November 2014, as part of the first phase of the Fifth International Workshop on Ice Nucleation (FIN-01). In this paper we compare size distributions and mass spectra of atmospherically relevant particle types measured by five SPMSs. These include different minerals, desert and soil dusts, soot, bioaerosol (Snomax; protein granule), secondary organic aerosol (SOA), and SOA-coated mineral particles. Most SPMSs reported similar vacuum aerodynamic diameter (d va ) within typical instrumental ranges from ~100–200 nm (lower limit) to ~2–3 µm (upper limit). In general, all SPMSs exhibited a wide dynamic range (up to ~10 3 ) and high signal-to-noise ratio (up to ~10 4 ) in mass spectra. Common spectral features with small diversities in mass spectra were found with high average Pearson's correlation coefficients, i.e., for average positive spectra r avg-pos =0.74 ± 0.12 and average negative spectra r avg-neg =0.67 ± 0.22. We found that instrument-specific detection efficiency (DE) was more dependent on particle size than particle type, and particle identification favored the use of bipolar, rather than monopolar, instruments. Particle classification from “blind experiments” showed that all instruments differentiated SOA, soot, and soil dust and detected subtle changes in the particle internal mixing but had difficulties differentiating among specific mineral types and dusts. This study helps to further understand the capabilities and limitations of the single-particle mass spectrometry technique in general and the specific performance of the instrument in characterizing atmospheric aerosol particles.

54 ENVIRONMENTAL SCIENCES↗

Nuclear structure and band mixing in Pt 194

We introduce a two-particle, two-hole mixed configuration scheme to fit E2 strengths for the 0 ↔ 2, 2 ↔ 4, and 4 ↔ 6 transitions in 194 Pt. The interaction includes two sets of pairing operators, {S ± (t), S 0 (t)} (t = s, d). Solutions within this framework are used to analyze energy spectra, E2 transitions, and band-mixing features of the model. The results confirm that mixing is small and similar for J = 2, 4, and 6, with the calculated energies and transition matrix elements in excellent agreement with experimental data.

190 ≤ A ≤ 219↗

MATRIX-VBS (v1.0): Implementing an Evolving Organic Aerosol Volatility in an Aerosol Microphysics Model

The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

volatility-basis set↗

Measurements of condensation nuclei in the Airborne Arctic Stratospheric Expedition - Observations of particle production in the polar vortex

The ER-2 Condensation Nucleus Counter (ER-2 CNC) was operated in the Airborne Arctic Stratospheric Expedition (AASE) in January and February 1989. The ER-2 CNC measures the mixing ratio of particles, CN, with diameters from approximately 0.02 to approximately 1 micron. The spatial distribution of CN in the Arctic polar vortex was found to resemble that measured in the Antarctic in the Spring of 1987. The vertical profile of CN in the vortex was lowered by subsidence. At altitudes above the minimum in the CN mixing ratio profile, CN mixing ratios correlated negatively with that of N2O, demonstrating new particle production. CN serve as nuclei in the formation of Polar Stratospheric Clouds (PSCs) and the concentration of CN can affect PSC properties.

Wilson, J. C.↗

Quantitative determination of mineral types and abundances from reflectance spectra using principal components analysis

A procedure was developed for analyzing remote reflectance spectra, including multispectral images, that quantifies parameters such as types of mineral mixtures, the abundances of mixed minerals, and particle sizes. Principal components analysis reduced the spectral dimensionality and allowed testing the uniqueness and validity of spectral mixing models. By analyzing variations in the overall spectral reflectance curves, the type of spectral mixture was identified, mineral abundances quantified and the effects of particle size identified. The results demonstrate an advantage in classification accuracy over classical forms of analysis that ignore effects of particle-size or mineral-mixture systematics on spectra. The approach is applicable to remote sensing data of planetary surfaces for quantitative determinations of mineral abundances.

Smith, M. O.↗

Steady-state mixing state of black carbon aerosols from a particle-resolved model

Abstract. Black carbon (BC) exerts a notable warming effect due to its strong light absorption, largely influenced by its “mixing state”. However, due to computational constraints, the mixing state is challenging to accurately represent in large-scale models. In this study, we employ a particle-resolved model to simulate the evolution of BC mixing state based on field observation. Our result shows that aerosol compositions, coating thickness (CT) distribution, and optical properties of BC aerosols all exhibit a tendency toward a steady state with a characteristic timescale of less than 1 d, considerably shorter than the BC atmospheric lifetime. The rapid attainment of a steady state suggests that it is reasonable to disregard this pre-steady-state period and instead concentrate on the average properties of BC across extensive spatial and temporal scales. The distribution of CT follows an exponential linear distribution and can be characterized by a single slope parameter k. This distribution is independent of the BC core's distribution. In the model simulation, the mean CT, equivalent to the 1/k, is 62 nm, which is consistent with the statistical results indicating a mean CT of 63 nm. Utilizing the slope parameter k, which effectively characterizes the CT distribution under the steady-state simplifying assumption, the BC absorption enhancement closely corresponds to the results obtained via the particle-resolved method. This study simplifies the BC mixing state description and yields a precise evaluation of the BC optical properties, which has the potential utility for modeling efforts in the refinement of the assessment of BC's radiative effects.

Zhang, Zhouyang↗

The influence of temperature history and flow mixing on the vapor-phase speciation of uranium oxide nanoparticles

The transport of radioactive material following a nuclear event depends heavily on fallout characteristics (e.g., composition, shape, and size), which in turn are controlled by the conditions under which the fallout forms. To this end, we use a novel plasma flow reactor (PFR) to explore how conditions including temperature history and gas mixing influence the chemical speciation and physical characteristics of uranium oxide nanoparticles. The PFR consists of a glass tube attached to an inductively coupled plasma (ICP) torch via an adaptor piece (ring flow injector) located downstream of the plasma-generating RF coil. We increase the gas flow rates from normal ICP operating conditions to higher values both upstream at the RF coil and downstream at the ring flow injector to create four distinct temperature profiles and two distinct gas flow mixing conditions (normal and higher Ar atomic ratios). Ex situ transmission electron microscopy (TEM) analysis is used to determine the crystal structure, morphology, and size distribution of the synthesized particles as a function of temperature and mixing. The particles display a striking dependence on these conditions in terms of the resulting speciation of uranium oxide: lower temperature (higher upstream) and slower cooling (normal downstream with normal Ar atomic ratio mixing) favor the formation of α-UO 3 particles, while faster cooling (higher downstream with higher Ar atomic ratio mixing) and higher temperature (normal upstream) favor the formation of UO 2 particles. The extent of gas mixing dictates particle aggregation: better mixing encourages the particles to aggregate more extensively. Here these results demonstrate the sensitivity of uranium to initial local conditions and can be used to improve our understanding of the kinetics that drive uranium speciation and ultimately inform fallout transport models.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Chemical imaging of individual stratospheric particles sampled over North America

The increasing size, severity, and frequency of wildfires have led to dramatic increases in particulate matter concentrations in the troposphere. Severe wildfires can generate intense convective systems capable of transporting large quantities of biomass burning organic aerosols (BBOA) to the upper troposphere and lower stratosphere (UTLS). Chemically complex organic matter and light-absorbing carbonaceous material is introduced into stratospheric regions that were historically isolated from direct surface emissions. In this study, stratospheric particles were sampled over North America during the Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) campaign, an aircraft-based research project designed to characterize convective perturbation in the UTLS. Particle samples collected from six research flights during summer 2022 were analyzed using Computer-Controlled Scanning Electron Microscopy and Scanning Transmission X-ray Microscopy to investigate particle size distributions, morphology, chemical composition, and mixing state of stratospheric particles along transects across the continental United States and adjacent Pacific Ocean airspace. Analysis revealed that all sampled particles contained detectable levels of carbon, with most exhibiting organic volume fractions of 0.37 ± 0.20. Notably, about 5% of the particles also contained soot inclusions, which indicates the presence of refractory black carbon transported to stratospheric altitudes and provides direct evidence of wildfire-derived black carbon reaching the UTLS. Typical particle morphology exhibits organic shells over soot and inorganic cores and suggests secondary processing and aging of BBOA during transport to and within the UTLS. These findings provide compelling evidence that wildfire emissions play a critical role in affecting the long-term composition and radiative properties of stratospheric particles.

Sharpe, Steven [Purdue Univ., West Lafayette, IN (↗

Erosion Experimentation in Solar Power Systems

An alternate and sustainable form of energy is concentrated solar power (CSP) systems, which capture and store the sun’s energy in the form of heat. To increase the efficiency and overall cost of the plant, particles were used as a heat transfer medium. As particles flow through this system, the movement of particles creates erosion, in the forms of abrasion and attrition. Experiments were tested at room temperature and 800 degrees Celsius for both abrasion wear and attrition erosion. In abrasion wear, specimens were placed inside a container, particles were added, and the specimen rotated in and out of the particles. In attrition erosion, a steel disk rotated amongst particles which resulted in particles rubbing against each other. Abrasion wear increased when temperature increased while attrition showed that the particles broke down as the amount of time increased. For attrition at 800 degrees Celsius, oxide was increased and mixed with the particles. Durability models will be created to predict attrition and abrasion based on the particle and specimen mechanical properties. This discovery shows that this method of utilizing particles for CSP plants would improve efficiency and decrease overall costs.

14 SOLAR ENERGY↗

Atmospheric Tar Balls: Particles from Biomass and Biofuel Burning

Tar balls are amorphous, carbonaceous spherules that occur in the tropospheric aerosol as a result of biomass and biofuel burning. They form a distinct group of particles with diameters typically between 30 and 500 nm and readily identifiable with electron microscopy. Their lack of a turbostratic microstructure distinguishes them from soot, and their morphology and composition (approximately 90 mol% carbon) renders them distinct from other carbonaceous particles. Tar balls are particularly abundant in slightly aged (minutes to hours old) biomass smoke, indicating that they likely form by gas-to-particle conversion within smoke plumes. The material of tar balls is initially hygroscopic; however, the particles become largely insoluble as a result of free radical polymerization of their organic molecules. Consequently, tar balls are primarily externally mixed with other particle types, and they do not appreciably increase in size during aging. When tar balls coagulate with water-bearing particles, their material may partly dissolve and no longer be recognizable as distinct particles. Tar balls may contain organic compounds that absorb sunlight. They are an important, previously unrecognized type of carbonaceous (organic) atmospheric particle.

Posfai, Mihaly↗

Preferrential Concentration of Particles in Protoplanetary Nebula Turbulence

Preferential concentration in turbulence is a process that causes inertial particles to cluster in regions of high strain (in-between high vorticity regions), with specifics depending on their stopping time or Stokes number. This process is thought to be of importance in various problems including cloud droplet formation and aerosol transport in the atmosphere, sprays, and also in the formation of asteroids and comets in protoplanetary nebulae. In protoplanetary nebulae, the initial accretion of primitive bodies from freely-floating particles remains a problematic subject. Traditional growth-by-sticking models encounter a formidable "meter-size barrier" [1] in turbulent nebulae. One scenario that can lead directly from independent nebula particulates to large objects, avoiding the problematic m-km size range, involves formation of dense clumps of aerodynamically selected, typically mm-size particles in protoplanetary turbulence. There is evidence that at least the ordinary chondrite parent bodies were initially composed entirely of a homogeneous mix of such particles generally known as "chondrules" [2]. Thus, while it is arcane, turbulent preferential concentration acting directly on chondrule size particles are worthy of deeper study. Here, we present the statistical determination of particle multiplier distributions from numerical simulations of particle-laden isotopic turbulence, and a cascade model for modeling turbulent concentration at lengthscales and Reynolds numbers not accessible by numerical simulations. We find that the multiplier distributions are scale dependent at the very largest scales but have scale-invariant properties under a particular variable normalization at smaller scales.

protoplanetary nebulae↗