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At least 289 records · Page 16

Molecular Specificity and Proton Transfer Mechanisms in Aerosol Prenucleation Clusters Relevant to New Particle Formation

Atmospheric aerosol particles influence Earth’s radiative energy balance and cloud properties either directly through interacting with the solar radiation or indirectly through acting as cloud condensation nuclei (CCN), thus impacting Earth’s climate change, air quality, and human health. Regarding both the important scientific and overarching practical implications of aerosols, the past two decades have seen an extensive research effort, with emphasis on the chemical compositions and underlying mechanisms of aerosol formation. New particle formation (NPF) has been recognized as an important pathway, contributing up to 50% of atmospheric aerosols. Nowadays, the general consensus in NPF is that it proceeds via two distinct stages—the nucleation from gaseous precursors to form critical nuclei of sub-1–2 nanometer size, and the subsequent growth into large particles. However, a fundamental understanding of both the NPF process and the molecular-level characterization of the critical size aerosol clusters is still largely missing, hampering the development of reliable and predictive aerosol nucleation and climate models.

Hou, Gao-Lei↗

Active Compensation of Radiation Effects on Optical Fibers for Sensing Applications

Neutron and gamma irradiation is known to compact silica, resulting in macroscopic changes in refractive index (RI) and geometric structure. The change in RI and linear compaction in a radiation environment is caused by three well-known mechanisms: (i) radiation-induced attenuation (RIA), (ii) radiation-induced compaction (RIC), and (iii) radiation-induced emission (RIE). These macroscopic changes induce errors in monitoring physical parameters such as temperature, pressure, and strain in optical fiber-based sensors, which limit their application in radiation environments. We present a cascaded Fabry–Perot interferometer (FPI) technique to measure macroscopic properties, such as radiation-induced change in RI and length compaction in real time to actively account for sensor drift. The proposed cascaded FPI consists of two cavities: the first cavity is an air cavity, and the second is a silica cavity. The length compaction from the air cavity is used to deduce the RI change within the silica cavity. We utilize fast Fourier transform (FFT) algorithm and two bandpass filters for the signal extraction of each cavity. Inclusion of such a simple cascaded FPI structure will enable accurate determination of physical parameters under the test.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Quantifying the structural uncertainty of the aerosol mixing state representation in a modal model

Abstract. Aerosol mixing state is an important emergent property that affects aerosol radiative forcing and aerosol–cloud interactions, but it has not been easy to constrain this property globally. This study aims to verify the global distribution of aerosol mixing state represented by modal models. To quantify the aerosol mixing state, we used the aerosol mixing state indices for submicron aerosol based on the mixing of optically absorbing and non-absorbing species (χo), the mixing of primary carbonaceous and non-primary carbonaceous species (χc), and the mixing of hygroscopic and non-hygroscopic species (χh). To achieve a spatiotemporal comparison, we calculated the mixing state indices using output from the Community Earth System Model with the four-mode version of the Modal Aerosol Module (MAM4) and compared the results with the mixing state indices from a benchmark machine-learned model trained on high-detail particle-resolved simulations from the particle-resolved stochastic aerosol model PartMC-MOSAIC. The two methods yielded very different spatial patterns of the mixing state indices. In some regions, the yearly averaged χ value computed by the MAM4 model differed by up to 70 percentage points from the benchmark values. These errors tended to be zonally structured, with the MAM4 model predicting a more internally mixed aerosol at low latitudes and a more externally mixed aerosol at high latitudes compared to the benchmark. Our study quantifies potential model bias in simulating mixing state in different regions and provides insights into potential improvements to model process representation for a more realistic simulation of aerosols towards better quantification of radiative forcing and aerosol–cloud interactions.

54 ENVIRONMENTAL SCIENCES↗

Entrainment and aerosol effects on marine boundary-layer clouds: An investigation using ACE-ENA data from HOLODEC, G1, Pico and ACTOS (Final Report on Project Activities)

Marine boundary-layer clouds cover large regions of the globe and are known to strongly influence radiative balances. The microphysical properties and persistence of these clouds are tightly coupled with cloud-top entrainment and aerosol properties within both the boundary layer and the overlying free troposphere. This work addressed the microphysical response to entrainment and aerosol properties in marine stratocumulus clouds, using data from the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) project. Specifically, emphasis was placed on 1. extensive in situ measurements taken with the Atmospheric Radiation Measurement (ARM) G1 aircraft using the Holographic Detector for Clouds (Holodec) instrument; 2. airborne measurements obtained with the helicopter-borne Airborne Cloud Turbulence Observation System (ACTOS) operated by the Leibniz Institute for Tropospheric Research (TROPOS) during the first phase of ACE-ENA; and 3. above-boundary-layer, mountain-top measurements taken at the Pico Mountain Observatory (OMP) by the research group of the co-investigator and scientists from TROPOS during the first phase of ACE-ENA. The work is aligned with the topic “Warm Boundary-Layer Atmospheric Processes.” Key results include the following. Data from the Holographic Detector for Clouds (Holodec) were reprocessed, refined, and validated through a careful instrument intercomparison, resulting in a high-quality dataset available on the ARM archive for ACE-ENA. High-resolution ACTOS measurements of thermodynamics, microphysical, and turbulence properties were analyzed to explore the behavior of the entrainment velocity at cloud top. Analysis of the vertical variability of cloud droplet size distribution shape suggests that mixing is more inhomogeneous near cloud top, and more homogeneous deeper into the cloud. Analysis of aerosol measurements from OMP explored the mixing state and cloud condensation nucleus properties, as well as the implications for radiative forcing. Finally, a machine learning algorithm was developed for identifying characteristic cloud droplet size distributions, and was employed to explore microphysical regimes in stratocumulus clouds observed during ACE-ENA. The characteristic size distributions are narrow, and only when spatially averaged do they produce the broad “gamma” distributions typically assumed in models. This implies that precipitation development should account for variability and correlations in the distribution shape as well as the number concentration of cloud droplets.

54 ENVIRONMENTAL SCIENCES↗

Synthesis of CdZnTeSe single crystals for room temperature radiation detector fabrication: mitigation of hole trapping effects using a convolutional neural network

In this article, we report the growth of Cd 0.9 Zn 0.1 Te 0.97 Se 0.03 (CZTS) wide bandgap semiconductor single crystals for room temperature gamma-ray detection using a modified vertical Bridgman method. Charge transport properties measured in the radiation detectors, fabricated from the grown CZTS crystals, indicated signs of hole trapping. Hole traps inhibit high-resolution radiation detection especially for energetic gamma rays. Machine learning (ML) applications are gaining tremendous mpetus in improving device and sensor performance by compensating for limi tations arising from such intrinsic material properties. In this article, we describe a deep convolutional neural network (CNN) that has demonstrated remarkable efficiency in identifying the energy of a gamma photon detected by a CZTS detector. The CNN has been trained using simulated data that resemble output pulses from actual CZTS detectors when exposed to 662-keV gamma photons. The device properties required for the simulation have been derived from radiation detection measurements on a real Cd 0.9 Zn 0.1 Te 0.97 Se 0.03 detector fabricated in our laboratory. The CNN has been trained with detector pulses arising through photoelectric (PE) and Compton scattering (CS) separately. The percentage error in predicting the detected energies, within an extremely small duration of 0.28 ms, was found to be lower than 0.1% for gamma energies above 50 keV and for training datasets con taining PE and CS events separately. The CNN was also validated for a mixed PE and CS dataset to obtain a prediction error of 1%. Additionally, the effect of detector resolution on the efficiency of the CNN was also explored.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Undulator radiation of single electrons: coherence length and quantum-optical properties

The aims of the CLARA experiment at the Fermilab Integrable Optics Test Accelerator (IOTA) were to directly measure the coherence length of undulator radiation emitted by a single electron and to test whether the radiation is in a pure classical Glauber coherent state or in a quantum mixture of coherent and Fock states. We used a Mach-Zehnder interferometer (MZI) to study visible radiation generated by 150-MeV electrons circulating in the ring. The relative delay between the two arms of the MZI was adjusted by varying the length of one of them with a resolution of 10 nm. The intensity of the circulating beam spanned several orders of magnitude, down to single electrons. A pair of single-photon avalanche diodes (SPADs) was placed at the output of the MZI arms to detect photocounts with high efficiency and timing resolution. We describe the observed interference patterns and photocount rates as a function of interferometer delay and discuss their implications.

43 PARTICLE ACCELERATORS↗

Undulator Radiation of Single Electrons: Coherence Length and Quantum-Optical Properties

The aims of the CLARA experiment at the Fermilab Integrable Optics Test Accelerator (IOTA) were to directly measure the coherence length of undulator radiation emitted by a single electron and to test whether the radiation is in a pure classical Glauber coherent state or in a quantum mixture of coherent and Fock states. We used a Mach-Zehnder interferometer (MZI) to study visible radiation generated by 150-MeV electrons circulating in the ring. The relative delay between the two arms of the MZI was adjusted by varying the length of one of them with a resolution of 10 nm. The intensity of the circulating beam spanned several orders of magnitude, down to single electrons. A pair of single-photon avalanche diodes (SPADs) was placed at the output of the MZI arms to detect photocounts with high efficiency and timing resolution. We describe the observed interference patterns and photocount rates as a function of interferometer delay and discuss their implications.

43 PARTICLE ACCELERATORS↗

Characterization of carbonaceous aerosols during TRACER-CAT

Absorbing aerosols (AA) have an important impact on the global radiation budget and cloud properties. The composition and properties of AA can vary substantially throughout the atmosphere, depending on the particle source and the influence of chemical aging. Uncertainties associated with the radiative effects of AA remain substantial. A key contributor to this uncertainty is understanding the extent to which coatings in general, and water uptake especially, alters absorption by AA particles and how this depends on particle composition. We deployed new and existing experimental tools during the Tracking Aerosol Convection Interactions Experiment (TRACER) campaign in Houston, TX as part of the Carbonaceous Aerosols Thrust (CAT) to provide detailed characterization of aerosol optical, chemical, and physical properties. Our TRACER-CAT measurements complemented and expanded on the planned TRACER instrumentation, allowing for more detailed characterization of aerosol properties of relevance to cloud development (a core focus of TRACER), such as the composition of particles that can act as cloud condensation nuclei, than would otherwise be available. Our measurements have allowed for assessment of the relationship(s) between AA optical properties (with a focus on absorption) and the chemical and physical characteristics (including the mixing state of black carbon (BC) containing particles). These field observations occurred in collaboration with Los Alamos National Laboratory in summer 2022 during the TRACER intensive operating period. The instrumentation we co-deployed provided for measurement of (i) multi-wavelength dry aerosol absorption, scattering, and extinction, (ii) the size-dependent composition and abundance of sub-micron aerosol, differentiating between those particles that do and do not contain BC, (iii) BC-specific concentrations and size distributions, (iv) particle size, and (v) the first field measurements at an ARM site of the influence of RH on multi-wavelength absorption by ambient AA. We have leveraged the natural variability of the atmosphere and of aerosol sources in the Houston region to (i) specifically disentangle contributions to light absorption from BC, absorbing organic carbon (brown carbon), and coatings on BC, (ii) characterize the mixing state of BC and assess the factors that give rise to compositional differences between BC-containing and BC-free aerosol, and (iii) establish how water uptake influences absorption and how any such effect depends on particle composition and BC mixing state. Overall, our study contributed to the mission of the Atmospheric System Research program in multiple ways. Through the deployment of complementary, advanced instrumentation for characterization of a wide range of aerosol properties our work helped to maximize the scientific impact of the TRACER campaign. Our work also allowed for development of new insights into the relationship(s) between aerosol composition, hygroscopicity, and the mixing state of BC with aerosol optical properties. Through this, our work has provided knowledge that can improve understanding and model representation of aerosol processes as they affect the Earth’s radiation budget.

54 ENVIRONMENTAL SCIENCES↗

Measurement of Spontaneous Undulator Radiation Statistics Generated by a Single Electron (URSSE)

As previously stated in the experiment proposal [1], the goal of the URSSE experiment was to study statistical properties of the undulator radiation generated by a single electron, circulating inthe IOTA storage ring. Namely, the idea was to study the distribution of the number of photons detected in a certain time window, and the distribution of the inter-arrival times of the photons. We wanted to see if the photostatistics was exactly Poissonian, as predicted or if there was some deviation towards Sub-Poissonian light, similar to what was observed in another study.

43 PARTICLE ACCELERATORS↗

Impact of Radiation on the Electronic Structure of MoS 2

Electrons in a semiconductor occupy states within certain energy ranges, called energy bands. The position of the Fermi level with respect to these energy bands determines the charge carrier type of the semiconductor. Molybdenum disulfide (MoS 2 ) is a two-dimensional, n-type semiconductor with potential applications in flexible electronics, transparent electronics, and optoelectronics. Electronic devices containing MoS 2 could be used in environments where radiation affects device performance. Thus, it is important to determine the impact of radiation on MoS 2 . A one-molecule-thick layer of MoS 2 (monolayer) and a two-molecule-thick layer of MoS 2 (bilayer) were placed onto different areas of a gold (Au) substrate containing 1.2-µm-deep holes. The MoS 2 was suspended over these holes but supported by the Au elsewhere on the substrate. This sample configuration was used to determine the effect of He + radiation on the electronic properties of the suspended MoS 2 and the Au-supported MoS 2 . The MoS 2 was irradiated by He+ ions in two stages. The energy bands of the MoS 2 were measured with respect to the Fermi level via photoelectron emission microscopy before irradiation and after each irradiation stage. From each measurement, the charge carrier type of the MoS 2 after the corresponding irradiation stage was determined. The Fermi levels of the suspended monolayer and bilayer decreased by ≈0.15 eV with respect to the bands during the first irradiation stage During the second irradiation stage, however, the Fermi levels didn’t change significantly. This lack of change supports the existence of a radiation threshold, above which the electronic properties of suspended MoS 2 remain the same. The Fermi levels of the supported monolayer and bilayer increased over the cumulative irradiation and didn’t show evidence of a threshold. Thus, suspended MoS 2 becomes less n-type as it is irradiated. Supported MoS 2 , however, becomes more n-type as it is irradiated. These results could inform the development of radiation tolerance standards for MoS 2 , and thus, radiation-tolerant MoS 2 -based electronics.

36 MATERIALS SCIENCE↗

Aerosol-Cloud Interactions From Aviation Soot Emissions

Current models estimate global aviation contributes approximately 5% to the total anthropogenic climate forcing, with aerosol-cloud interactions having the greatest effect. However, radiative forcing estimates from aviation aerosol-cloud interactions remain undetermined. There is an expected significant increase in aircraft emissions with aviation demand expected to rise by over 4% per year. Soot may play an important role in the ice nucleation of aircraft-induced cirrus formation due to a high emission rate, but the ice nucleating properties are poorly constrained. Understanding the microphysical processes leading to atmospheric ice crystal formation is crucial for the reliable parameterization of aerosol-cloud interactions in climate models due to their impact on precipitation and cloud radiative properties. Ice nucleation of aircraft-emitted soot is potentially affected by particle morphology with condensation of supercooled water occurring in pores followed by ice nucleation. However, soot has heterogeneous properties and undergoes atmospheric aging and oxidation that could change surface properties and contribute to complex ice nucleation processes. Further, this review synthesizes current knowledge of ice nucleation catalyzed by aviation in the cirrus regime and its effects on global radiative forcing. Further research is required to determine the ice nucleation and microphysical processes of cirrus cloud formation from aviation emissions in both controlled laboratory and field investigations to inform models for more accurate climate predictions and to provide efficient mitigation strategies.

54 ENVIRONMENTAL SCIENCES↗

Development of a Random-Forest Cloud-Regime Classification Model Based on Surface Radiation and Cloud Products

Various methods have been developed to characterize cloud type, otherwise referred to as cloud regime. These include manual sky observations, combining radiative and cloud vertical properties observed from satellite, surface-based remote sensing, and digital processing of sky imagers. While each method has inherent advantages and disadvantages, none of these cloud-typing methods actually includes measurements of surface shortwave or longwave radiative fluxes. Here, a method that relies upon detailed, surface-based radiation and cloud measurements and derived data products to train a random-forest machine-learning cloud classification model is introduced. Measurements from five years of data from the ARM Southern Great Plains site were compiled to train and independently evaluate the model classification performance. A cloud-type accuracy of approximately 80% using the random-forest classifier reveals that the model is well suited to predict climatological cloud properties. Furthermore, an analysis of the cloud-type misclassifications is performed. While physical cloud types may be misreported, the shortwave radiative signatures are similar between misclassified cloud types. From this, we assert that the cloud-regime model has the capacity to successfully differentiate clouds with comparable cloud–radiative interactions. Therefore, we conclude that the model can provide useful cloud-property information for fundamental cloud studies, inform renewable energy studies, and be a tool for numerical model evaluation and parameterization improvement, among many other applications.

54 ENVIRONMENTAL SCIENCES↗

Photoluminescence Induced in Mineral Oil by Ionizing Radiation

We have studied photoluminescence (PL) properties of vacuum pump mineral oil as a function of the type and intensity of ionizing radiation exposure. The mineral oil has a simple aliphatic structure, which possesses no chromophore in the traditional sense. Unexpected PL in the mineral oil has characteristic features such as variation of the emission peak wavelength depending on the excitation wavelength and intensity dramatically increasing with radiation dose. The observed behavior can be understood in the framework of a previously suggested model introducing aggregation-induced PL and the formation of conjugated clusters comprising nontraditional chromophores. Our findings can be used for the development of optical sensors for real-time monitoring of oil utilized in vacuum pumps in nuclear fusion reactors.

Bliznyuk, Valery N.↗

Ultra-rapid, physics-based development pathway for reactor-relevant RF antenna materials

This paper presents a rapid, atomistically-informed, experimental development pathway for fusion reactor-relevant radio frequency (RF) antenna materials in the Cu-Cr-(Nb,Al,Zr) composition system, with the goal of improving upon GRCop-84. RF antennas in a tokamak fusion reactor will face a unique set of challenges as both structural and functional materials. The desired material must simultaneously achieve and maintain high electrical conductivity, high strength, high thermal conductivity, resist high temperatures, possess low nuclear activation, and incur low damage due to neutron bombardment. The GRCop-84 alloy serves as a starting point for iterative improvement, with the desire to reduce or eliminate Nb from the material to minimize nuclear activation. The rapid development pathway makes use of a multi-target combinatorial thick film sputtering process to produce full ternary phase diagrams on a Si wafer substrate. Transient grating spectroscopy (TGS), a laser-ultrasonic method, will determine spatially-varying thermo-elastic properties, while four terminal electrical conductivity measurements will map out the best per- forming regions of the sample for in-depth study at larger length scales. High energy proton and self-ion irradiation emulates the effects of neutron damage on the thermal/electric properties. With rapid turnaround time (∼days) in terms of mapping radiation damage-induced material property changes in the full ternary system, these techniques allow rapid iteration towards an optimal material, testing hundreds of nearby compositions in the time it took to test one. Focused testing of larger, single composition samples (produced in an arc furnace or by laser sintering) provides data on structural and high power RF properties, and validates our thick-film based workflow.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Engineered optical fibers and uses thereof

A system comprises an electromagnetic radiation source, a polarizing element, a mode converter, an optical fiber, and a measurement device. The polarizing element receives electromagnetic radiation produced by the electromagnetic radiation source and outputs linearly-polarized electromagnetic radiation having a linear polarization angle θ1. The mode converter converts the linearly-polarized electromagnetic radiation to an orbital angular momentum (OAM) mode of linearly-polarized electromagnetic radiation with topological charge Li. The OAM mode of linearly-polarized electromagnetic radiation is a superposition of first and second OAM modes with topological charges Li and opposite circular polarizations. The optical fiber supports propagation of the first and second OAM modes with an absolute effective index difference Δneff greater than or equal to 5×10−5, such that linearly-polarized electromagnetic radiation with linear polarization angle θ2 is emitted by the optical fiber. The measurement device is configured to determine a property of the electromagnetic radiation based on the polarization angle θ2.

Ramachandran, Siddharth↗

Deposition-controlled phase separation in CuNb metallic alloys

Vapor co-deposited metal nanocomposites with immiscible components have shown to have several superior properties including mechanical performance, radiation tolerance, and enhanced functionalities. The morphology and structural design of these nanocomposites are important in determining the expression of these properties. The conditions used to deposit thin film nanocomposites are the governing factors in determining the final nanostructure. In this work, we link the effects of process gas pressure, substrate temperature, and sputtering target power on resultant Cu/Nb thin film nanostructures. Here, we find that for films with equiatomic phase fractions of Cu and Nb, inhomogeneous precipitate segregation dominated the structure at lower substrate temperature depositions while higher temperatures distributed the Cu and Nb phases more uniformly. Increasing process gas pressure during deposition lead to a spatially homogeneous, nanocrystalline structure of Cu/Nb. In situ annealing of this sample shows that the phase separated morphology of the two immiscible materials depends on the initial composition. Finally, compositions of Cu and Nb that were highly disparate lead to interface segregation of the minority phase. The morphological evolution observed in the Cu/Nb system is compatible with modified structural zone models for immiscible thin film systems.

36 MATERIALS SCIENCE↗

Edge fluctuation measurements in EDA H-mode and QCE plasmas in ASDEX Upgrade using the correlation electron cyclotron emission diagnostic

The requirement of a plasma solution without large edge-localized modes (ELMs) for future fusion devices motivates the study of plasmas without Type I ELMs. The enhanced D–α (EDA) and quasi-continuous exhaust (QCE) scenarios are two such Type I ELM free plasmas, but their underlying physics principles are not fully understood. A database of EDA and QCE plasmas from ASDEX Upgrade was compiled and analyzed using the correlation electron cyclotron emission diagnostic in order to study differences between properties of the quasi-coherent mode (QCM) between these two regimes. Investigations into measured spectral properties of the QCM, radiated temperature fluctuations δT rad /T rad , and radial correlation lengths L c showed no differences between the two regimes. Spectral properties using the cross-power spectral density, G xy were similar between regimes, with the values measured to be a central frequency, $f$ $QCM$ ≈ 20 - 50 kHz; spectral width, Δ $f$ ≈ 5 - 40 kHz; δT rad /T rad ≈ 4-6%; and L c ≈ 1-2 cm. Investigations into a quantity representing the relative bandwidth Δ$f$/$f$ $QCM$ revealed differences between EDA and QCE plasmas when plotted radially, suggesting some type of interaction between the QCM in QCE plasmas with the surrounding broadband turbulence that is not present in EDA phases. Additionally, investigations into various drive terms for hypothesized instability drivers for the QCM are performed showing no difference in the parameter spaces of collisionality and the ion temperature, electron temperature, or electron pressure scale lengths between each regime indicating that there is no observable difference between the drive behind the QCM in each regime.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗