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At least 541 records · Page 30

NCSU Black Carbon (SP2) Data

NCSU SP2 Data Data Level b1: QC checks applied to measurements Data Format: CSV Description: See "instrument description Site: Houston, TX; Tracking Aerosol Convection interactions ExpeRiment (HOU) Location: Houston, TX; AMF1 (main site for TRACER) Facility Code: M1 Category: Aerosol Properties Data Type: PI Data Source Instrument/Data: Single Particle Soot Photometer (SP2) Start Date: 2022-06-01 End Date: 2022-09-27 Contact PI: Markus Petters (mdpetter@ncsu.edu) Funding Source: DOE ASR award US Department of Energy, Office of Science, Biological and Environment Research (grant no. DE-SC 0021074) Instrument description The SP2 was located in the temperature-controlled trailer adjacent to the NCSU Flux Tower to observe refractory black carbon (rBC) number concentration and mixing states of black carbon. The sample line brought aerosol inside the trailer at 4.5 L min-1, where it was distributed between 3 CPCs (TSI 3776c, Dc ~ 2.5 nm, TSI 3771, Dc ~10nm, and TSI 3772, Dc ~40 nm) with different size cuts, a printed particle optical spectrometer (POPS), and SP2. Please contact mdpetter@ncsu.edu for further information.

54 ENVIRONMENTAL SCIENCES↗

Design Considerations for Controlling Silicon Nanoparticle Nucleation and Growth in a Nonthermal Plasma

Controlling the nucleation and growth of nanoparticles in low temperature plasma systems is imperative for controlling nanoparticle size distributions; and for some applications such as deposition and etching in microelectronic processing, preventing particle contamination. In this work, silicon nanoparticle (NP) production from silane is used as a model system to investigate the nucleation process. Although the mechanisms responsible for silicon NP nucleation and growth have been studied, it is unclear how controllable system parameters (e.g., pressure, system geometry, and gas composition) can be used to inhibit or promote NP formation. For example, the transport of reactive silane species is expected to significantly affect the feed fraction of silane required to nucleate silicon NP (the nucleation onset fraction) due to losses at the reactor walls. In this work, NP mass density was determined as a function of system pressure, gas composition, and reactor diameter for a tubular flow-through radiofrequency (RF) plasma using Ar/H2/He/SiH4 gas mixtures. A quartz crystal microbalance (QCM) impactor was developed to measure the total aerosol mass density downstream of the plasma and thereby identify the nucleation onset and its dependence on process parameters. Finally, a reaction mechanism was developed and incorporated into a global plasma chemistry model to better understand the nucleation onset and NP growth.

36 MATERIALS SCIENCE↗

Superlattices are Greener on the Other Side: How Light Transforms Self-Assembled Mixed Halide Perovskite Nanocrystals

Perovskite nanocrystal superlattices (NC SLs) are the nearest real-world approximations to monodisperse NC ensembles. NC SLs thus represent ideal model systems for evaluating the optical and structural stability of CsPb(I 1– x Br x ) 3 NCs at a macroscopic level. Here, photoinduced changes to CsPb(I 1– x Br x ) 3 NC SLs (0 < x < 1.0) are probed via in situ photoluminescence, X-ray diffraction, and electron microscopy. We find that prolonged (~10–20 h) ultraviolet–visible irradiation causes irreversible PL blueshifts, photobrightening, and crystal structure contractions. These changes stem from gradual photoinduced I 2 sublimation, which transforms CsPb(I 1– x Br x ) 3 into CsPbBr 3 . Despite eliminating half of the initial halides from individual CsPb(I 0.53 Br 0.47 ) 3 particles, NCs within SLs remarkably preserve their initial crystallinity, cuboidal shapes, edge lengths, and size distributions. This work illustrates compositional control toward generating precisely engineered perovskite NC SLs. It also highlights iodide photo-oxidation as a hurdle that must be overcome if mixed halide perovskite nanomaterials are to be applied beyond fundamental studies.

36 MATERIALS SCIENCE↗

Simulating Southern Ocean Aerosol and Ice Nucleating Particles in the Community Earth System Model Version 2

Southern Ocean (SO) low-level mixed phase clouds have been a long-standing challenge for Earth system models to accurately represent. While improvements to the Community Earth System Model version 2 (CESM2) resulted in increased supercooled liquid in SO clouds and improved model radiative biases, simulated SO clouds in CESM2 now contain too little ice. Previous observational studies have indicated that marine particles are major contributor to SO low-level cloud heterogeneous ice nucleation, a process that initiates a number of cloud processes that govern cloud radiative properties. In this study, we utilize detailed aerosol and ice nucleating particle (INP) measurements from two recent measurement campaigns to assess simulated aerosol abundance, number size distributions, and composition and INP parameterizations for use in CESM2. Our results indicate that CESM2 has a positive bias in simulated surface-level total aerosol surface area at latitudes north of 58°S. Measured INP populations were dominated by marine INPs and we present evidence of refractory INPs present over the SO assumed here to be mineral dust INPs. Results highlight a critical need to assess simulated mineral dust number and size distributions in CESM2 in order to adequately represent SO INP populations and their response to long-term changes in atmospheric transport patterns and land use change. Furthermore, we also discuss important cautions and limitations in applying a commonly used mineral dust INP parameterization to remote regions like the pristine SO.

58 GEOSCIENCES↗

High-Volume Precipitation Spectrometer (HVPS) Instrument Handbook

The high-volume precipitation spectrometer (HVPS) is a U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility instrument for measuring hydrometeors larger than 150 μm. It is an open-path instrument located on the outside of the aircraft, typically below the wing. A laser sheet throws a shadowgraph image of the hydrometeor (cloud droplets or ice crystals) in the sample volume on a photodiode array. As the hydrometeor moves through the sample volume, this optical array records the moving shape and a two-dimensional picture can be recorded. At an air speed of 100 m/s, the sample volume is 310 l/s. The recorded images can be analyzed for size distributions, number concentrations, and further cloud properties detailed below. Hydrometeors in the range of 0.3-19.2 mm can be fully recorded at a 150 μm resolution; larger particles can only be sized along the direction of flight.

54 ENVIRONMENTAL SCIENCES↗

Investigation of Nanoparticle Degradation in Hydrogen Fuel Cell Systems through Automated Electron Microscopy

Proton exchange membrane fuel cells (PEMFC) are promising devices for the deployment of hydrogen-powered heavy-duty vehicles, providing a higher efficiency for similar driving range and fueling time than the existing ones. However, PEMFCs still encounter durability challenges mainly due to catalyst degradation in the cathode. Mitigating these performance losses requires a better understanding of the degradation mechanisms under heavy-duty accelerated stress tests (ASTs) [1]. Scanning transmission electron microscopy (STEM) combined with energy dispersive X-ray spectroscopy (EDS) are key tools for the analysis of Pt and PtCo nanoparticle size, spatial distribution and composition [2]. Electron tomography is also used to determine the rate and type of degradation of catalyst nanoparticles as a function of their position on the carbon support. In this work, automated data acquisition software, paired with a custom Python code, have been used to study the effect of different accelerated stress tests (ASTs) on nanoparticle coarsening [2]. Figure 1 shows high-angle annular dark-field (HAADF)-STEM images and EDS maps comparing the cathodes of membrane electrode assemblies (MEAs) following an electrocatalyst AST performed under H2/N2 with that of the heavy-duty AST performed under H2/air. We will discuss how AST conditions affect considerably the spatial distribution of the nanoparticles across the electrode between the membrane and microporous layer. Although the median particle size increased more in the MEA aged under the heavy-duty AST, as determined using a high-throughput image analysis, the quantitative EDS measurements demonstrate that the electrocatalyst AST resulted in more Pt and Co dissolution from the cathode, which is another important indicator of electrocatalyst degradation. We will further present the impact of the relative humidity (% RH) on the degradation mechanisms demonstrated using the same approach. Electron tomography has been used to distinguish the Pt nanoparticles residing on the carbon support surface (exterior) from those within the pore structure (interior) in order to determine the relative stability of interior and exterior nanoparticles. As shown in Figure 2, we will compare the Pt catalyst particle size at the beginning of test (BOT) and end of test (EOT), and discuss the importance of automating the electron tomography workflow, i.e. acquisition, reconstruction, and visualization, to increase sampling and determine the standard deviation of these measurement. The outlook for utilizing low-dose cryo-tomography for limiting damage to the catalyst, support, and especially proton-conducting ionomer will also be discussed [3].

Amichi, Lynda↗

Understanding Aitken Mode Aerosol Variability over the Southern Ocean and Antarctica: Insights from Cloud Condensation Nuclei Data

Aitken mode aerosol particles play an important role influencing cloud properties and sustenance, acting as a reservoir of potential cloud condensation nuclei against precipitation scavenging. However, there is limited data on Aitken mode aerosols. In this study, we develop a method to estimate Aitken mode aerosol concentrations and size distribution using cloud condensation nuclei measurements (CCN) and κ-Köhler theory. The performance of this method is evaluated using scanning mobility particle sizer (SMPS) data from recent field campaigns to demonstrate its skills and applicability. The method reasonably estimates Aitken- and accumulation-mode aerosol concentrations, achieving correlations of 0.7–0.9 with only modest biases (mean fractional bias within ±23% for Aitken mode and ±34% for accumulation-mode). This method is further applied to measurements collected over the Southern Ocean and Antarctica in recent years from multiple platforms, including ground sites, aircraft, and ships, to derive Aitken and accumulation-mode aerosol concentrations. Using the derived data, we examine the seasonal cycle, latitudinal variations, and vertical distribution of aerosols. Aitken mode aerosol concentrations are elevated over the Southern Ocean and Antarctica during the austral summer similar to the accumulation mode. In the austral summer, the free troposphere has more Aitken mode aerosols and fewer accumulation mode aerosols than the boundary layer, and thus likely serves as an important source of cloud-forming aerosol while also diluting the accumulation mode.

Kang, Litai [University of Washington] (ORCID:0000↗

Shape Control of Colloidal Semiconductor Nanocrystals through Thermodynamically Driven Aggregative Growth

The optoelectronic properties of colloidal semiconductor nanocrystals (NCs) can be manipulated by changing their geometric shapes. The precise synthetic control over particle morphologies, however, has remained elusive. Conventional growth techniques rely on the kinetic assembly of atomic units, where supersaturation and precipitation processes can lead to a broad distribution of particle shapes. In this paper, we demonstrate that replacing atomic precursors with small-size nanocrystals as building blocks for larger colloids offers an easier, more predictive control over nanoparticle shape evolution. The reported growth strategy is illustrated via shape-selective syntheses of CdSe and CdS NC cubes, spheres, rods, as well as unprecedented “donut” and ring-like structures. Growth of desired particle morphologies was achieved by choosing an appropriate reaction solvent that minimizes the surface free energy through a unique shape formation. This so-called "aggregative growth mechanism" is explained using a thermodynamic model for interacting viscous colloids. We expect that this novel growth strategy will offer a viable platform for shape–selective synthesis of many inorganic colloids, providing pathways to optimizable optoelectronic materials.

36 MATERIALS SCIENCE↗

Surface Self-Diffusion Induced Sintering of Nanoparticles

Despite the critical role of sintering phenomena in constraining the long-term durability of nanosized particles, a clear understanding of nanoparticle sintering has remained elusive due to the challenges in atomically tracking the neck initiation and discerning different mechanisms. Through the integration of in situ transmission electron microscopy and atomistic modeling, this study uncovers the atomic dynamics governing the neck initiation of Pt–Fe nanoparticles via a surface self-diffusion process, allowing for coalescence without significant particle movement. Real-time imaging reveals that thermally activated surface morphology changes in individual nanoparticles induce significant surface self-diffusion. Further, the kinetic entrapment of self-diffusing atoms in the gaps between closely spaced nanoparticles leads to the nucleation and growth of atomic layers for neck formation. This surface self-diffusion-driven sintering process is activated at a relatively lower temperature compared to the classic Ostwald ripening and particle migration and coalescence processes. The fundamental insights have practical implications for manipulating the morphology, size distribution, and stability of nanostructures by leveraging surface self-diffusion processes.

36 MATERIALS SCIENCE↗

Detonation Soot: A New Class of Ice Nucleating Particle

Abstract Temperatures and pressures from high explosive detonations far exceed atmospheric conditions in typical combustion reactions, and consequently, detonation soot forms with physiochemical properties distinct from soot formed by combustion. In this study, samples of detonation soot from two high explosives, PBX 9502 and Composition B‐3, were analyzed. Ice nucleation experiments on soot collected after controlled detonations were conducted in the laboratory to probe immersion and contact mode freezing. Samples nucleated ice at temperatures warmer than commercially available nanodiamonds, which has a mean nucleation temperature of −20.7°C. Ice nucleation rate coefficients increase rapidly by two to three orders of magnitude below −20°C for every sample. Size‐selected 137 μm diameter particles produced during detonation in an ambient air atmosphere yield bimodal distributions of freezing temperature with primary and secondary nucleation modes centered at −20°C and −13°C, respectively. The presence of a secondary mode allows for enhanced ice nucleation rate coefficients (one to two orders of magnitude greater than samples without a secondary mode) at temperatures outside the influence of the primary mode (>−17°C). Given the observed onset nucleation temperatures of −9.2°C, our results imply that detonation soot of the type studied here would only need to reach an altitude of approximately 4 km to facilitate ice formation.

54 ENVIRONMENTAL SCIENCES↗

Planet-induced Vortices with Dust Coagulation in Protoplanetary Disks

In this work, we study how the dust coagulation/fragmentation will influence the evolution and observational appearances of vortices induced by a massive planet embedded in a low-viscosity disk by performing global 2D high-resolution hydrodynamical simulations. Within the vortex, due to its higher gas surface density and steeper pressure gradients, dust coagulation, fragmentation, and drift (to the vortex center) are all quite efficient, producing dust particles ranging from 1 μm to ~1.0 cm, as well as an overall high dust-to-gas ratio (above unity). In addition, the dust size distribution is quite nonuniform inside the vortex, with the mass-weighted average dust size at the vortex center (~4.0 mm) being a factor of ~10 larger than other vortex regions. Both large (~millimeter) and small (tens of microns) particles contribute strongly to affect the gas motion within the vortex. As such, we find that the inclusion of dust coagulation has a significant impact on the vortex lifetime and the typical vortex lifetime is about 1000 orbits. Furthermore, after the initial gaseous vortex is destroyed, the dust spreads into a ring with a few remaining smaller gaseous vortices with a high dust concentration and a large maximum size (~millimeter). At late time, the synthetic dust continuum images for the coagulation case show as a ring inlaid with several hot spots at the 1.33 mm band, while only distinct hot spots remain at 7.0 mm.

79 ASTRONOMY AND ASTROPHYSICS↗

Experimental Study of Transport Behavior of Swellable Microgel Particles in Superpermeable Channels for Conformance Control

Summary Gel treatment is an effective way to attack excessive water production during oil development. The transport behavior of gel materials in reservoirs is of crucial importance to the effectiveness of gel treatments. The aim of this paper is investigating the transport behavior of swellable micrometer-sized preformed particle gels (PPGs, or microgels) through superpermeable (super-K) channels. Sandpacks with permeabilities ranging from 27 to 221 darcies were used to mimic the super-K channels. Multiple pressure sensors were applied along the sandpack models to monitor the propagation behavior of the microgels. The tested microgel particles could transport through the super-K channels, and a higher driving pressure gradient was required when the particle/pore size ratio was larger. The pressure gradient distribution along the super-K channels was relatively uniform when the particle/pore ratio was low (less than 1.3). However, the inlet section would show increasingly higher pressure gradients as the particle/pore ratio was increased, indicating increased difficulty in propagation. The propagation of the gel particles was significantly slower compared with the carrying fluid. The delayed propagation behavior was more pronounced when the particle/pore ratio was higher. The injection pressure was much less sensitive to the injection flow rate compared with a Newtonian fluid. The gel dispersion exhibited an apparent shear thinning (pseudoplastic) behavior when transporting through the porous channels. Breakage of the gel particles was observed especially at high superficial velocities. The particle breakage was partially responsible for the apparent shear thinning behavior. The breakage phenomenon was in favor of deep placement of the gel particles. The channel permeabilities were significantly reduced by the microgels, bringing sufficient resistance to subsequent waterflooding (more than 99.5%). At given matching size conditions, softer gels were more likely to establish in-depth placement and uniform water blocking capacity in the channels. The microgel particles exhibited salinity-responsive behavior to the post-brine flush. The gel particles could shrink and reswell according to the salinity of the injected water. Possibilities were discussed to use this salinity-responsive behavior. Also, the microgels exhibited a particular disproportionate permeability reduction (DPR) effect. After gel injection, the channel permeability to water flow was reduced by more than 20 to 92 times of the permeability to oil flow. This work provides important support to understand the transport behavior of gel particles in super-K channels. The achievements are helpful for gel product selection and gel treatment design.

Engineering↗

Dynamic permeability in metastable droplet interfacial bilayers

Membrane pores are implicated in several critical functions, including cell fusion and the transport of signaling molecules for intercellular communication. However, these structural features are often difficult to probe directly. Droplet interfacial bilayers offer a synthetic platform to study such membrane properties. We develop a theory that links size-selective transport across a metastable membrane with its transient structural properties. The central quantity of our theory is a dynamic permeability that depends on the mechanism of pore growth, which controls the transient distribution of pore sizes in the membrane. We present a mechanical perspective to derive pore growth dynamics and the resulting size distribution for growth via Ostwald ripening and discuss how these dynamics compare to other growth mechanisms such as coalescence and growth through surfactant desorption. We find scaling relations between the transported particle size, the pore growth rate, and the time for a given fraction of particles to cross the membrane, from which one may deduce the dominant mechanism of pore growth, as well as material properties and structural features of the membrane. Finally, we suggest experiments using droplet interfacial bilayers to validate our theoretical predictions.

Sarma, Nivedina A↗

Ozone and aerosol size distribution measurements at the Oliktok Point, AK AMF3

Aerosol size distribution measurements at the Oliktok Point, AK AMF3 as measured by a TSI model 3082 scanning mobility particle sizer (SMPS), and ozone measurements at the Oliktok Point, AK AMF3 as measured by a 2B model 205 ozone monitor. 2B specifies a limit of detection (2&sigma;) of 2 ppb and these data were calibrated using a 2B model 306 ozone calibration source. Users of the data are asked to contact PI Pratt prior to use for consultation, discussion of co-authorship, and to ensure that the most up-to-date information is provided.

54 ENVIRONMENTAL SCIENCES↗

Characterization of a modified printed optical particle spectrometer for high-frequency and high-precision laboratory and field measurements

Abstract. The printed optical particle spectrometer (POPS) is a lightweight, low-cost instrument for measurements of aerosol number concentrations and size distributions. This work reports on modifications of the Handix Scientific commercial version of the POPS to facilitate its use in multi-instrument aerosol sampling systems. The flow system is modified by replacing the internal pump with a needle valve and a vacuum pump. The instrument is integrated into closed-flow systems by routing the sheath flow from filtered inlet air. A high-precision multichannel analyzer (MCA) card is added to sample the analog pulse signal. The MCA card is polled at 10 Hz frequency using an external data acquisition system and improves upon the count-rate limitation associated with the POPS internal data acquisition system. The times required to change the concentration between 90 % and 10 % and vice versa for a step change in concentration were measured to be 0.17 and 0.41 s at a flow rate of 5 cm3 s−1. This yields a sampling frequency of ∼ 1–2 Hz, below which the amplitude of measured fluctuations is captured with > 70 % efficiency. The modified POPS was integrated into the dual tandem differential mobility analyzer system to explore the coalescence of dimer particles. Results show that the pulse-height response increases upon dimer coalescence. The magnitude of the increase is broadly consistent with the change in light-scattering amplitude predicted by the T-matrix method. It is anticipated that this modified version of the POPS will extend the utilization of the technique for a range of field and laboratory applications.

54 ENVIRONMENTAL SCIENCES↗

Earthquake-triggered submarine canyon flushing transfers young terrestrial and marine organic carbon into the deep sea

Submarine canyons transfer substantial amounts of sediment and organic carbon (OC) into the deep ocean, nourishing deep-sea ecosystems and contributing to the global carbon cycle through OC burial and sequestration. Tracking lateral OC transport through submarine canyon systems is challenged by the deep-ocean setting, difficulties with constraining episodic depositional events, and the need to assess the composition and age of marine and terrestrial organic matter. We apply innovative parallel ramped pyrolysis oxidation accelerator mass spectrometry and pyrolysis-gas chromatography-mass spectrometry with isotope analyses to track OC age and sources in the 2016 Kaikoura earthquake-triggered, canyon-flushing event that deposited along >1300 km of a submarine canyon-channel system, offshore Aotearoa New Zealand. Specifically, these techniques allow us to determine the ages, sources, and partitioning of OC within the Kaikoura turbidite deposit and test hypotheses of how submarine canyon systems contribute to lateral OC flux and burial. Our results show that, despite considerable canyon floor erosion, substantial amounts of young OC were flushed into the deep sea, with relatively little (~2%) pre-Holocene OC contributions. Even without a direct connection between rivers and submarine canyons, most (~55%) of the OC in the Kaikoura event bed is from terrestrial sources. However, the deposit also contains substantial amounts (~22%) of marine-derived OC and ~23% of the material is of unassignable origin. Particle sorting imparts variability on the age and composition of OC within turbidite deposits and along the turbidity current flow path. Terrestrial-derived OC is preferentially older than marine-derived OC and concentrated in coarser particle sizes found more commonly at the deposit base and in proximal settings. Young, marine-derived OC is concentrated at the surface of the deposits and tends to be enriched in finer particle sizes. Such OC partitioning in turbidites supports the relevance of depositional models for predicting and quantifying distribution of OC in deep-sea deposits. Earthquake-triggered, canyon flushing events and resulting turbidites enhance OC burial efficiency and can sequester OC effectively, contributing an important carbon sink to the sedimentary carbon cycle.

54 ENVIRONMENTAL SCIENCES↗