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338 records · Page 18

Sodium-Ion Battery Cathode with Dominating Copper and Oxygen Redox Chemistry

Sodium-ion batteries offer low-cost energy storage solutions for the grid and electric vehicles, leveraging the established "rocking-chair" Li-ion design and the natural abundance of sodium. However, SIBs face challenges such as relatively lower voltage and capacity than lithium-ion batteries, as well as dependence on nickel resources. Here, in this work, a new nickel-free cathode material, Na 0.75 Li 0.08 Cu 0.25 Mn 0.66 O 2 , was designed and synthesized. This material has a capacity of ~125 mAh/g and an average discharge voltage of 3.5 V. Notably, more than one-third of the capacity arises from lithium substitution of Cu (~8 mol.%) and high voltage activation to 4.6 V. Multimodal synchrotron x-ray characterization combining spectroscopy, microscopy, and scattering reveal the capacity is primarily from the redox of copper and oxygen, with a minor contribution from the manganese redox. Lithium substitution alters the phase transition mechanism from a two-phase transition in P3-Na 2/3 Cu 1/3 Mn 2/3 O 2 to a solid-solution in Na 0.75 Li 0.08 Cu 0.25 Mn 0.66 O 2 , enhancing the reversibility of this material.

25 ENERGY STORAGE

Revealing key structures for reversible sulfur redox in amorphous polymeric sulfur

Amorphous polymeric sulfur cathodes, such as sulfurized polyacrylonitrile (SPAN), enable high-energy lithium-sulfur batteries without cobalt or nickel, leveraging abundant sulfur. However, the limited in situ understanding of their synthesis and electrochemistry has impeded targeted optimization. Here, in this study, we integrate operando high-energy total scattering with sulfur K-edge X-ray absorption spectroscopy to monitor SPAN's formation and cycling in real time. Our results show that S-C bond formation halts further fusion of cyclized polyacrylonitrile, fostering π-π stacking and a transition from long-chain to short-chain sulfur-critical for reversible sulfur redox. These features synergistically minimize polysulfide dissolution and charge-transfer resistance, enabling optimized SPAN to achieve high capacity retention over 1,000 cycles. Operando X-ray absorption spectroscopy reveals that residual protons drive thiol-thione tautomerism, with lithium replacement during the first discharge causing ~20% irreversible capacity loss. To enhance performance, minimizing -NH groups and expanding pyridine networks are key. These findings transform SPAN optimization from empirical tuning to mechanism‑guided engineering and point the way towards sulfur loadings and energy densities competitive with state‑of‑the‑art Li‑ion cathodes.

25 ENERGY STORAGE

SAVY-4000 Finite-Element Drop Test Analysis

PFE Auxiliary Systems conducted drop testing on SAVY-4000 containers to evaluate structural response under 12-foot drop conditions. In support of that effort, a finite-element modeling capability was developed to simulate drop response across multiple container sizes and impact orientations. The purpose of this work was to provide a consistent analysis framework that could support interpretation of testing, compare response trends across multiple configurations, and generate quantities of interest for later comparison with experimental data. More broadly, the analysis and testing were intended to assess whether the containers continued to perform their primary function after a 12-foot drop, namely maintaining structural integrity and containment of the contents. The modeling approach combined an implicit preload analysis with an explicit drop simulation so that each drop event began from a mechanically realistic assembled condition, including compression of the silicone O-ring. Separate models were developed for 2-quart, 5-quart, 12-quart, and 10-gallon containers. The results were evaluated in terms of strain-gauge response, collar-lid gap behavior, and accumulated plastic strain. In addition, parametric studies were performed on the 2-quart container to assess sensitivity to O-ring stiffness, friction, canister thickness, geometry tolerance, and mesh density. The simulations showed that predicted drop responses depended strongly on both container size and drop orientation. Gap metrics identified cases in which the predicted collar-lid opening exceeded the nominal O-ring cross-section threshold, while plastic strain metrics identified localized regions of elevated permanent deformation. Parametric studies showed that the predicted response was especially sensitive to the assumed O-ring stiffness and contact friction, while the geometry tolerance study produced smaller changes in the cases examined. The main value of this work was that it established a repeatable modeling and simulation workflow to support drop-test implementation, evaluate effects of future configuration changes, and understand modeling assumptions that most influenced predicted response. At the current stage, the results were viewed as preliminary model predictions rather than validated predictions. The next step would be to compare drop-test data to the model so that predictive values of the workflow could be refined and used with greater confidence to assess whether the containers maintained structural integrity and containment of the contents after a 12-foot drop.

42 ENGINEERING

Probing the role of local tunnel variations in early-stage lithiation of α-MnO₂ nanowires via in situ TEM

Understanding lithium-ion transport in tunnel-structured manganese oxides is essential for designing high-performance lithium-ion battery electrode materials. Here, we elucidate the early-stage lithiation mechanism of potassium-stabilized α-MnO 2 nanowires using in situ transmission electron microscopy (TEM) coupled with electron energy-loss spectroscopy (EELS), high-resolution TEM (HRTEM), and geometric phase analysis (GPA). Real-time TEM imaging reveals clear volume expansion at the reaction front, while EELS analysis uncovers lithium-ion diffusion far beyond this region, where no visible expansion is observed, indicating fast, defect-assisted transport. GPA and HRTEM analyses show that localized tensile and compressive strain fields, originating from pre-existing local tunnel structural variations, persist after lithiation. The tensile-strained regions enable lithium-ion insertion with minimal lattice distortion, offering additional free volume that facilitates rapid lithium-ion accommodation ahead of the structural transformation. Our results demonstrate a local tunnel variation-mediated fast diffusion pathway that precedes bulk reaction, underscoring the critical role of local strain in enabling early-stage lithium transport. Given the structural versatility of MnO 2 and its ability to accommodate diverse atomic arrangements beyond the well-known tunnel phases (β-, γ-, δ-, λ-, R-phases), our findings highlight the importance of understanding and engineering local structural environments. This work provides fundamental insights into the interplay between defects, strain, and ion dynamics, and presents defect engineering as a promising approach to enhance both rate performance and structural stability in manganese-based cathodes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND

Innovations Driven by Advanced Characterization to Strategize Critical Mineral Production and Beneficial Reuse from Fossil Energy Waste

Critical minerals (CM), such as rare earth elements (REE), cobalt, nickel, and lithium, have important uses in modern electronics and advanced manufacturing, yet are vulnerable to potential supply chain disruptions. Relatively abundant and readily available fossil energy (FE) wastes, such as coal combustion ash, acid mine drainage (AMD) and treatment solids (AMD solids), and Oil and Gas (O&G) drilling wastes (drill cuttings and produced waters) are under consideration as CM feedstocks. The National Energy Technology Laboratory (NETL) has studied CM resources for various FE wastes as part of the U.S. Department of Energy’s mission of bolstering the domestic CM supply, and makes the data available to the public on EDX at sites such as the NEWTS group. Advanced characterization utilizing synchrotron x-ray techniques coupled with laboratory extractions has been performed to identify CM hosting phases in these FE wastes to inform CM recoverability mechanisms. Novel methods to selectively recover CMs while co-producing other valuable byproducts have been developed. Successful examples discussed here include: (1) The identification of REE/Co/Ni/Sc binding and hosting phases in select FE waste (coal combustion ash and AMD solids), resulting in the development of a patented CM step-extraction process, (2) coupled production of functional sorbents from these extraction wastes and for CM recovery. A pilot-scale testing to evaluate the patent’s technical feasibility for extracting REE from coal ash on a barrel scale has been successfully performed. Additionally, (3) evaluation and measurements of brine geochemistry from U.S. O&G produced waters has informed a high Li recovery potential from Marcellus Shale produced water. NETL researchers have been developing tailored pre-treatment processes, an innovative and highly durable lithium sorbent, and geochemical model guided precipitation to accelerate Li production from the Marcellus Shale produced waters. These innovations driven by characterization are integral for maximizing and advancing the potential for CM recovery while offsetting the cost and environmental footprint for FE waste management.

critical mineral processing

Improving Ionic Conformality Across Polymer Electrolyte|Electrode Interfaces

Maintaining uniform ionic transport at electrode|electrolyte interfaces, i.e., ionic conformality, remains challenging in polymer electrolyte (PE)-based solid-state batteries. Morphological conformality does not necessarily imply ionic conformality. In PEs, which typically consist of a mechanically supporting component and distinct ionically conductive components, the rearrangement or depletion of mobile ion-conductive domains at interfaces can disrupt ionic transport pathways. Such localized ionic depletion contributes to interfacial instability and capacity degradation in high-voltage lithium-metal batteries. Herein, an electrolyte design approach aimed at minimizing interfacial heterogeneities is demonstrated through compositional adjustments, characterized by spatially resolved structural and chemical X-ray techniques and NMR diffusometry to elucidate ion transport dynamics. This approach improves ionic conformality at electrode interfaces, enhancing cycling stability in Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NMC811) coin and pouch cells cycled at high voltages. These results contribute to understanding interfacial behaviors in multiphase PEs and inform strategies for improving stability across solid-state battery interfaces.

36 MATERIALS SCIENCE

Direct comparison of gamma, electron beam and X-ray radiation effects on the polymers of a pulsed lavage device

Gamma radiation used for sterilization of medical devices is challenged by cobalt-60 supply and commercial capacity. To maintain a robust radiation sterilization marketplace for the rapidly growing single-use medical device industry, investigation of potential alternatives to gamma technology, such as electron beam (e-beam) and X-ray technology, is critical. In this work, we directly compare the effects of radiation source and absorbed dose level on the polymeric materials and function of a commercial pulsed lavage device used for wound care. Product functionality, polymer mechanical, and polymer optical properties were evaluated using standard methods and input from the device manufacturer. Test results show that functionality of the product was not inhibited by radiation although the battery in the device exposed to X-ray exhibited greater voltage loss compared to batteries in products exposed to gamma or e-beam. Statistically significant differences between gamma and e-beam exposure and between gamma and X-ray exposure were also observed for product appearance in terms of yellowness index of several of the polymers considered. Overall, the results of this study support the viability of e-beam and X-ray radiation technologies as alternatives to cobalt-60 gamma technology for sterilization of the single-use pulsed lavage medical device investigated.

Electron beam

Reduced fast-ion transport calculations of m = n = 1 fishbone-like instabilities in MAST-U

Fast-ion transport associated with an m = n = 1 fishbone-like burst in MAST-U discharge 47128 is investigated using a reduced guiding-center-based transport model (ORBIT-Kick) constrained by multi-diagnostic measurements. The two-dimensional beam-emission spectroscopy system provides measurements of the core poloidal mode structure and fluctuation amplitude, while EFIT++ reconstructions constrained by the motional Stark effect diagnostic indicate a flat q-profile with q 0 > 1⁠, indicating the absence of a resonant q = 1 surface and supporting a pressure-driven infernal-mode interpretation. Analytic m = n = 1 displacement profiles consistent with the measured core mode structure and equilibrium constraints are used as the mode structure inputs to ORBIT-Kick. The calculations show that the dominant resonances occur between the mode and co-passing fast ions, producing redistribution localized near the magnetic axis. Synthetic neutron camera signals from TRANSP-Kick recover up to 90% of the experimentally observed neutron deficit at the time of peak mode amplitude, indicating that the measured m = n = 1 mode is a dominant contributor to core fast-ion transport. However, the synthetic neutron signals recover rapidly, whereas the measured neutron emission continues to decrease after the peak amplitude. In conclusion, the remaining discrepancy may arise from contributions not included in the present single-harmonic model, including higher-m and higher-n harmonics, multi-harmonic interactions, and additional transport mechanisms, motivating future diagnostic development and modeling efforts to resolve and incorporate these additional contributions.

Wong, Henry H. [University of California, Los Ange

Understanding Discharge‐Driven Growth of Cathode Impedance in Ni‐Rich NMC Cathodes

Degradation of LiNi x Mn y Co 1-x-y O 2 (NMC)-based lithium-ion batteries depends strongly on cut-off voltage ranges. In addition to the high upper cut-off voltage, a high depth of discharge (i.e., lower cut-off voltage) significantly worsens cathode impedance growth and capacity fade during long-term cycling. However, there is currently no consensus on the mechanism behind the negative role of a deep discharge. Here, this phenomenon was investigated in graphite||NMC cells with single-crystal cathodes (LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NMC622) or LiNi 0.76 Co 0.14 Mn 0.10 O 2 (NMC76)) using targeted aging protocols (constant high-voltage holds vs. charge–discharge cycling), while monitoring transition-metal (TM) dissolution, cathode-electrolyte interface (CEI) impedance, and NMC surface composition. We demonstrate a correlation between discharge-driven CEI impedance growth and increased TM dissolution. Furthermore, this degradation pathway is more pronounced in lower-Ni NMC622 than in higher-Ni (NMC76) under comparable delithiation states at charge, with both compositions undergoing the H2→H3 phase transition. X-ray photoelectron spectroscopy (XPS) reveals NMC composition-dependent evolution of surface lattice oxygen and restructured surface layer composition between charged and discharged states. These findings add mechanistic depth to the role of discharge as an active driver of interfacial degradation and provide new insights into its composition dependence.

25 ENERGY STORAGE

PET waste- and bio-derived imine vitrimers for shape-memory, intrinsic flame-retardant, and recyclable carbon fiber composites

Developing circular multifunctional vitrimers and carbon fiber–reinforced polymers (CFRPs) that are simultaneously recyclable, mechanically robust, and intrinsically flame retardant remains a major challenge. Here, in this study, we report multifunctional vitrimers and their carbon fiber–reinforced vitrimer (CFRV) composites, where the vitrimer design integrates closed-loop recyclability, enhanced interfacial adhesion, and intrinsic flame retardancy within a single materials platform. The vitrimer matrix is synthesized from post-consumer polyethylene terephthalate (PET) waste and a vanillin-derived phosphorus-containing crosslinker, forming an imine-based network. The resulting vitrimer resin exhibits high tensile strength, thermal healability, repeated reprocessability, programmable shape memory, and rapid chemical depolymerization under mild conditions. Amine-functionalized carbon fibers significantly improve fiber–matrix interfacial bonding, yielding CFRVs with tensile strengths up to 789 MPa and complete recovery of structurally intact fibers after chemical recycling. The phosphorus-rich aromatic network further imparts intrinsic flame retardancy, enabling self-extinguishing behavior without external additives. This work advances a materials design paradigm for next-generation multifunctional, sustainable vitrimers and CFRVs, while simultaneously addressing the recycling challenges associated with both plastic and CFRP waste.

Bio-derived crosslinker

Identifying Strain Stacking Boundaries between Multiphase Domains in Atomically Thin Two-Dimensional Magnets

Stacking engineering of van der Waals materials is an important strategy to control the materials’ properties, such as electronic correlations, ferroelectricity, and layer-dependent two-dimensional magnetism. A timely testbed for the study of the latter is atomically thin chromium trihalides (CrX 3 , X = Cl, Br, I). Notably, by understanding the sliding mechanism between different stacking sequences, control of the stacking arrangement, and thus magnetic properties in CrX 3 , can be achieved. Such insight, however, is currently lacking. Here, in this study, advanced electron microscopy methods are used to identify multiple stacking sequences corresponding to different bulk phases in atomically thin CrX 3 (X = Cl and Br) down to bilayer thickness and with lateral domain sizes as small as tens of nanometers. Indications of nanometer scale transitions and interactions at the stacking boundaries are found, including a universally preferred sliding direction that is consistent with density functional theory calculations and the strain fields at lateral heterostructure boundaries. This study demonstrates the necessity to consider local stacking structures when interpreting averaged magnetic properties measured with macroscale probes. Additionally, the preferred sliding direction insight from this study provides a strategy to control stacking sequence in atomically thin CrX 3 samples during the exfoliation and sample fabrication process.

DFT calculations

Thermal Disorder‐Induced Strain and Carrier Localization Activate Reverse Halide Segregation

The reversal of halide ions is studied under various conditions. However, the underlying mechanism of heat-induced reversal remains unclear. This work finds that dynamic disorder-induced localization of self-trapped polarons and thermal disorder-induced strain (TDIS) can be co-acting drivers of reverse segregation. Localization of polarons results in an order of magnitude decrease in excess carrier density (polaron population), causing a reduced impact of the light-induced strain (LIS – responsible for segregation) on the perovskite framework. Meanwhile, exposing the lattice to TDIS exceeding the LIS can eliminate the photoexcitation-induced strain gradient, as thermal fluctuations of the lattice can mask the LIS strain. Under continuous 0.1 W cm -2 illumination (upon segregation), the strain disorder is estimated to be 0.14%, while at 80 °C under dark conditions, the strain is 0.23%. However, in situ heating of the segregated film to 80 °C under continuous illumination (upon reversal) increases the total strain disorder to 0.25%, where TDIS is likely to have a dominant contribution. Therefore, the contribution of entropy to the system's free energy is likely to dominate, respectively. Various temperature-dependent in situ measurements and simulations further support the results. These findings highlight the importance of strain homogenization for designing stable perovskites under real-world operating conditions.

36 MATERIALS SCIENCE

Modeling Radiolysis and Chemical Reactions during Dry Storage of Aluminum-clad Spent Nuclear Fuel

After aluminum-clad spent nuclear fuel (ASNF) is removed from the reactor, it is initially stored in spent fuel pools, which are specially designed water-filled basins that provide temporary cooling to reduce the temperature of the fuel assemblies and provide radiation shielding. ASNF continues to generate heat due to the radioactive decay of elements within the fuel, which persists for many years post-shutdown as the residual radioactive products decay into more stable elements. During the wet storage period, an oxyhydroxide layer composed of boehmite/bayerite forms on the surfaces of the aluminum cladding from exposure to water in the pools. Road-ready packaging for long-term disposition of the ASNF involves dry storage in helium backfilled DOE standard canisters (DSCs). When the ASNF is removed from water storage and dried, most of the water is removed, but some physisorbed and chemisorbed water remains in the oxyhydroxide layers. This residual water can produce hydrogen when exposed to radiation from the ASNF during dry storage. Predicting hydrogen accumulation over time in the DSCs is critical for long-term storage considerations. Previous modeling efforts have developed coupled computational fluid dynamics (CFD)-chemical models to simulate temperature, pressure, and gas phase concentrations within the DSCs. These models use the thermal field predicted by CFD as input to a radiolysis model for the gas phase and the surface oxyhydroxide layer chemistry. Given the long storage period of the DSCs and the impracticality of long-term experiments, a simulation-based approach is necessary to assess chemical evolution within the canisters. This study advances the development of a modeling framework designed to simulate the chemical evolution of spent fuel canisters. Both thermal and radiation-driven reactions are considered, with radiation kinetics quantified using G-values. Sensitivity analysis identifies key parameters influencing species composition. Reaction pathway diagrams offer insight into dominant species formation routes, enabling more effective comparisons between model predictions and experimental observations, particularly regarding the production of hydrogen. Results show that the model predicts significant hydrogen gas production with minimal oxygen generation, primarily due to hydrogen formation via boehmite pathways. These findings underscore the importance of accurately characterizing surface-bound species and radiolysis kinetics. A deeper understanding of these mechanisms is critical for evaluating the long-term safety of nuclear waste storage.

12 - MGMT OF RADIOACTIVE AND NON-RADIOACTIVE WASTE

Statistical Uncertainty of Inhalation Dose Coefficients: Impact of Particle Deposition in ICRP 66 Human Respiratory Tract Model

Inhaled radioactive materials can pose a long-term health concern, as the material can be incorporated into the body’s metabolic pathways and remain in organs and tissues for extended durations. During the retention period, the radioactive material may localize in a source organ and irradiate adjacent target organs and tissues. Distribution of these materials changes over time, requiring biokinetic modeling to evaluate their movement through various tissues and organs. The evolving distribution depends on multiple inputs characterizing the inhaled material, such as particle size and size distribution, particle density, aspect ratio, specific radionuclide, the chemical form, and solubility. In addition, biological parameters such as breathing rate, breathing type (nasal or nasal/oral), respiratory system morphometry, tidal volume, functional residual capacity, and anatomical dead space all influence material transport. These aerosol properties and physiological characteristics of the respiratory tract jointly define a range of initial conditions that influence the time-dependent distribution of radioactive material. To evaluate both uncertainty in the initial conditions of inhalation exposure and the final output (committed effective dose) from biokinetic models, a Python-based software tool, Radiological Exposure Dose Calculator (REDCAL), was developed to propagate uncertainty within the human respiratory tract model. Focusing on deposition fraction uncertainty, the primary objective was to characterize the initial activity distribution across respiratory regions as a function of anticipated particle sizes and distributions. The impact of the deposition fraction uncertainty was propagated to committed effective dose coefficients for selected radionuclides in a companion publication. For each particle size, a lognormal distribution, characterized by its geometric mean as defined within ICRP Publication 66, serves as the basis for introducing uncertainty into the physical processes governing deposition in various lung regions. Finally, this study addresses the deposition process and examines how uncertainty in deposition mechanisms affects activity distribution in the airways, ultimately presenting the expected range and standard deviation of deposited activity as a function of particle size.

International Commission on Radiological Protectio

Elimination of detrimental grain boundary segregation in garnets

Garnet Li 7 La 3 Zr 2 O 12 electrolyte is considered a key enabler of solid-state batteries with Li metal electrodes, but the grain boundaries impair its performance. To date, the understanding of grain boundary structures and its impact on performance remains elusive. Here, we show that element segregation at Li 7 La 3 Zr 2 O 12 grain boundaries critically governs Li transport and nucleation. During conventional sintering, Al, Ta, and La segregate at grain boundaries, locally depleting Li and creating space-charge layers that lower total ionic conductivity. Simultaneously, this segregation leads to higher electronic conductivity along grain boundaries, which promotes Li nucleation at grain boundary edges with increased risk of dendrite formation. The underlying mechanism of segregation is governed by both thermodynamic driving forces and diffusion kinetics. Building on this understanding, we develop a strategy to achieve segregation-free grain boundaries through a rapid sintering protocol that utilizes the onset of solid-state softening. This approach yields transparent, polycrystalline Li 7 La 3 Zr 2 O 12 with negligible grain boundary impedance and enhanced dendrite tolerance. By elucidating the structural origins and electrochemical consequences of grain boundary segregation, this work provides a guidance for the rational optimization of solid electrolytes.

Energy - Storage

High Pressure Synthesis of Ultrasmall Nanodiamonds with Nitrogen Vacancy Centers

C–H terminated nanometer scale diamonds ( d = 1 to 15 nm) are synthesized from 1-fluoroadamantane at high pressure (6–8 GPa) and high temperature (500–1500 °C) in a multianvil press. High resolution transmission electron microscopy, X-ray diffraction, Raman, diffuse reflectance Fourier transform infrared, and X-ray absorption spectroscopies demonstrate the excellent crystallinity and atomically flat C–H terminated surfaces of nanodiamonds with (111) and (110) facets. The importance of hydrogen to the synthesis of nanodiamond and its faceting is discussed. Following vacancy generation, annealing and oxidation of the nanodiamonds, optically detected magnetic resonance and electron spin resonance coherence times ( T 2 = 0.9 and 2.1 μs) of nitrogen vacancy (NV) centers are measured. Finally, the obtained T 2 values are equivalent to the shallow NV centers (depth <10 nm) in bulk diamond crystals and larger nanocrystals prepared by mechanical milling.

36 MATERIALS SCIENCE

Multi-modal dynamic radiography using short-pulse laser-generated probe beams

Radiography is an important tool for the interrogation of dynamic experiments in the fields of dynamic properties of materials, and in condensed matter, high explosive, and high-energy-density physics. Multi-modal radiography advances the hypothesis that combining the information delivered by multiple radiographic modalities can lead to more constrained (improved) “reconstruction” of the scene than can be obtained from a single probe. We identify four modalities: multi-probe, time sequence, multi-view, and multi-messenger. Multi-probe radiography is a promising candidate for a next-generation dynamic radiographic facility. High-energy X-rays are the most frequently used probe for dynamic radiography, although recent developments show the utility of proton (pRad), electron (eRad), and neutron probe beams. Because each probing species interacts with material in the radiographic scene through quantitatively different mechanisms, each returns independent information about the scene, which can add extra constraints to the reconstruction process. How to conduct detailed, quantitative “co-analysis” of multiple data streams remains an area of active research. Multi-beam, short-pulse, laser-generated probes offer sufficient dose, an appropriate spectrum, and appropriate spatio-temporal resolution to produce high-quality dynamic radiographs. This paper reports on technology development to advance the state of the art of multi-modal/multi-probe radiography and the pursuit of both deterministic and inferential (AI/ML assisted) co-analysis methodologies to produce more constrained reconstructions from multi-modal data.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY

Aerosol-deep convection interaction based on joint cell-thermal tracking in Large Eddy Simulations during the TRACER campaign

In cumulus clouds, aerosol concentrations control cloud droplet concentrations, modifying cloud radiative properties, precipitation processes, and cloud electrification. However, mechanisms of aerosol-deep convection interactions are not well understood due to complex cloud dynamics and microphysics. We investigate the interaction of aerosols with isolated deep convection using Large Eddy Simulations of two cases during the TRacking Aerosol Convection interactions ExpeRiment (TRACER) near Houston, Texas, using a joint cell-thermal tracking algorithm. Cumulus thermals are droplet generators, since supersaturation and droplet nucleation coincide with thermal centers, where the strongest updrafts occur. Primary ice crystal formation does not take place inside thermals, but at layers where previous thermals detrained moisture. As subsequent thermals containing supercooled droplets penetrate these layers, hail and graupel form at or near these thermals. Higher aerosol concentrations result in higher droplet concentrations that suppress drizzle, delay warm rain processes, and transport more moisture aloft. This increases snow and ice amount, as well as graupel and hail, leading to more lightning. Polluted thermals initiate at slightly higher altitudes, and are slightly larger and faster, suggesting a weak invigoration. We also find more thermals per cell, but fewer isolated cells, since convection is more aggregated and intense, especially near the end of the 24 h simulation. Non-linear mesoscale feedback likely triggered by temperature and moisture responses to aerosol-thermal interactions causes the aggregation. Time-lagged aerosol-reinitialization experiments show that the mesoscale response is the predominant forcing for the invigoration. These changes happen within one day, on a smaller scale than previously suggested.

54 ENVIRONMENTAL SCIENCES