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At least 37 records · Page 2

Impulse-driven release of gas-encapsulated drops

Gas-encapsulated drops, much like antibubbles, are drops enclosed in a bubble within a liquid. They show potential as payload carriers in fluid transport and mixing techniques where sound waves can be leveraged to induce the collapse of the gas core and the subsequent release of the drop. Here, the interaction of millimetre-sized gas-encapsulated drops with impulsive laser-induced shock waves is investigated to gain fundamental insights into the release process. Experimental synchrotron X-ray phase contrast imaging, which allows the drop dynamics to be visualised inside the encapsulating bubble, is complemented by numerical simulations to study the intricate physics at play. Three drop dynamical release regimes are discovered, namely the drop impact , partial deposition and jet impact regimes. The regime type is mainly dependent on the shape of the bubble interface impacting the drop and the associated Weber and Reynolds numbers. The drop dynamics of the drop impact and partial deposition regimes show similarities with the canonical configuration of drops impacting flat liquid surfaces, whereas the jet impact regime resembles binary drop collisions, which allows existing scaling laws to be applied to describe the underlying processes. The release of the drop is investigated numerically. The time evolution of the drop dissemination within the surrounding liquid discloses enhanced mixing for dynamics involving high Weber and Reynolds numbers such as the drop impact and jet impact regimes.

42 ENGINEERING

In Vitro Encapsulation of Functionally Active Abiotic Photosensitizers Inside a Bacterial Microcompartment Shell

Bacterial microcompartments (BMCs) are self-assembling, selectively permeable protein shells that encapsulate enzymes to enhance catalytic efficiency of segments of metabolic pathways through means of confinement. The modular nature of BMC shells' structure and assembly enables programming of shell permeability and underscores their promise in biotechnology engineering efforts for applications in industry, medicine, and clean energy. Realizing this potential requires methods for encapsulation of abiotic molecules, which have been developed here for the first time. We report in vitro cargo loading of BMC shells with ruthenium photosensitizers (RuPS) by two approaches-one involving site-specific covalent labeling and the other driven by diffusion, requiring no specific interactions between cargo molecules and shell proteins. The highly stable shells retain encapsulated cargo over 1 week without egress and preserve RuPS photophysical activity. Finally, this study is an important foundation for further work that will converge biological BMC architecture with synthetic chemistry to facilitate biohybrid photocatalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Developing the Science Basis for Understanding Polymer Encapsulant Degradation Mechanisms: DuraMAT 2.0 Final Project Report

Polymeric encapsulants are essential materials in photovoltaic modules, protecting sensitive electronics from the environment while providing mechanical integrity to the multilayered assembly. However, these polymeric materials are susceptible to degradation processes driven by the ingress of environmental species, ultraviolet radiation, thermal stresses, and mechanical loading. In this study, we employ a combined atomistic simulation and accelerated aging experimental approach to study the molecular-scale mechanisms of encapsulant degradation. Classical molecular dynamics simulations quantify the diffusion of environmental and degradation species through the polymer matrix, producing composition-specific diffusion coefficients. Reactive simulations characterize activation energy barriers and reaction rate constants for key chemical pathways. In parallel, thermal-desorption analyses coupled with mass spectrometry monitor the emergence and concentration profiles of degradation products under controlled stressor conditions. By integrating simulation and experiment, we establish quantitative correlations between polymer composition, species diffusivity, and chemical reactivity. We anticipate that these relations and quantitative values could serve as high-fidelity inputs to reaction-diffusion models, enabling physics-informed lifetime predictions and guiding the design of more durable encapsulant materials for solar energy applications.

36 MATERIALS SCIENCE

Preventing native oxide formation in niobium thin films through platinum encapsulation

Superconducting transmon qubits are a key technology in quantum computing, with niobium (Nb) widely used due to its favorable superconducting properties and compatibility with scalable fabrication. However, the performance of Nb-based qubits is hindered by two-level systems (TLS), which arise predominantly from native oxide layers at surfaces and interfaces. These oxides and suboxides form rapidly in air and contribute significantly to decoherence by introducing dielectric losses. While various mitigation strategies, including thermal-annealing, chemical-etching, and nitrogen plasma treatment, have been explored, many are challenging to integrate into large-scale manufacturing due to complexity and instability in ambient conditions. In this study, we investigate the structural, chemical, and superconducting properties of room-temperature sputtered Nb thin films grown on sapphire substrates. We focus on a surface protection strategy using noble metal encapsulation with platinum (Pt) to suppress oxides and reduce TLS-related losses. Structural and chemical characterization were performed using X-ray diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy. Superconducting properties were measured using a physical property measurement system. Results demonstrate that Pt encapsulation effectively suppresses surface oxidation and mitigates its detrimental impact on superconducting performance. In conclusion, this approach offers a promising path toward enhancing the coherence of Nb-based qubits while remaining compatible with scalable-fabrication processes.

36 MATERIALS SCIENCE

Encapsulation Enhances the Quantum Coherence of a Solid‐State Molecular Spin Qubit

Spins within molecules benefit from the atomistic control of synthetic chemistry for the realization of qubits. One advantage is that the quantum superpositions of the spin states encoding the qubit can be coherently manipulated using electromagnetic radiation. The main challenge is the fragility of these superpositions when qubits are to partake of solid-state devices. We address this issue with a supramolecular approach for protecting molecular spin qubits against decoherence. The molecular qubit [Cr(ox)3]3- has been encapsulated inside the diamagnetic triple-stranded helicate [Zn2L3]4+ (L is a bis-pyrazolylpyridine ligand). The quantum coherence of the protected qubit is then analyzed with pulsed EPR spectroscopy and compared with the unprotected qubit, both in solution and in the solid state. Crucially, the spin-spin relaxation in the solid state has been examined within diamagnetic crystal lattices of the isostructural ([Al(ox)3]@[Zn2L3])+ or [Al(ox)3]3- assemblies, respectively, doped with the Cr3+ qubit in two different (<10%) concentrations. The study unveils a surprising increase of the phase memory time of the qubit upon encapsulation only in the solid. Spin-lattice relaxation times also exhibit a significant enhancement, as established from inversion recovery pulse sequences and from slow relaxation of the magnetization of the protected qubit, not featured by the free qubit.

Swain, Abinash

Thermal and mechanical performance of gypsum composites containing fly ash cenosphere encapsulated phase change materials

Utilizing phase change materials (PCMs) within construction materials improves the thermal energy storage capabilities in the built environment. Notably, integrating PCMs into drywalls presents a promising avenue to reduce building energy use. However, incorporating PCMs into drywalls poses challenges, particularly reduced mechanical properties and workability limitations as it can adversely affect the hardening and cohesiveness of gypsum composites. To address these challenges, this study explores a novel strategy to incorporate PCMs into gypsum composites through fly ash cenosphere-encapsulated PCM, namely CenoPCM, aiming to enhance the mechanical properties and thermal conductivity over existing commercial counterparts. An experimental program was conducted to study the impact of the inclusion of CenoPCM on the mechanical and thermal performance of gypsum composites, and the results were compared to those of commercially available polymerencapsulated PCM benchmark (Micronal). The findings highlighted that PCM-charged samples exhibited up to 95.90 J/g (CenoPCM) of latent heat with 70 % CenoPCM loading. The results of mechanical tests also showed that CenoPCM outperformed its polymer-encapsulated counterpart, achieving 55 % higher mechanical strength on average. Here, this improvement is attributed to the rigid shell of fly ash cenosphere (FAC) serving as a PCM carrier, providing a skeleton-like structure to gypsum composites for higher load-bearing capacity. Additionally, hotbox tests demonstrated that the CenoPCM-charged wall panels yielded a 20 % higher thermal conductivity and a 22 % increased time lag compared to Micronal PCM-charged panels, indicating its potential to shift the peak load in buildings.

Ceno PCM

Oxide-Encapsulated Ruthenium Oxide Catalysts for Selective Oxygen Evolution in Unbuffered pH-Neutral Seawater

Direct seawater electrolysis is a promising approach to producing green hydrogen in water-scarce environments using renewable energy. However, the undesirable chlorine evolution reaction and hypochlorite evolution reaction compete with the desired oxygen evolution reaction (OER) at the anode electrocatalyst. This issue is most pronounced in unbuffered pH-neutral solutions due to local acidification resulting from the OER. To overcome this challenge, this study provides a comprehensive evaluation of the use of silicon oxide (SiO x ) and titanium oxide (TiO x ) nanoscale overlayers coated on metallic ruthenium (Ru) and ruthenium oxide (RuO x ) thin film electrodes and their ability to block chloride ions from reaching active sites during operation in an unbuffered 0.6 M NaCl electrolyte. Using a combination of (electro)analytical techniques, encapsulated RuO x anodes are shown to effectively suppress Cl - transport to buried catalyst active sites while allowing for the desired OER to occur, leading to increases in OER faradaic efficiency at moderate overpotentials. Evidence for the ability of SiO x overlayers to block Cl - ions from reaching the active buried interface was obtained by monitoring the ν(O-H) stretching mode of OH adsorbates using in situ Raman spectroscopy. Here, this study also reports trade-offs between the activity, selectivity, and stability of bare and encapsulated Ru and RuO x electrocatalysts, finding that the magnitude of these trade-offs strongly depends on the complex interplay between electrode architecture, material properties, and catalytic performance, especially in unbuffered pH-neutral seawater.

58 GEOSCIENCES

Mitigating electrochemical degradation in CsPbBr{sub 3} gamma detectors by organic and inorganic encapsulation.

CsPbBr3 perovskite semiconductors have emerged as a leading candidate for nextgeneration radiation detectors because of their exceptional charge transport properties, defect tolerance, and record-breaking sensitivity and energy resolution. Their long-term stability, however, is hindered by electrode-driven electrochemical decomposition, which is accelerated by moisture- and oxygen-assisted ion migration during operation. Here, we investigated organic and inorganic encapsulation strategies as both environmental barriers and means to suppress interfacial degradation pathways. Atomic layer deposition (ALD) of Al2O3 provided a conformal passivation layer that blocked environmental ingress, suppressed ionic diffusion, reduced leakage current, enhanced energy resolution and expanded the operational electric-field window beyond 5 kV∙cm1 . By contrast, organic encapsulants such as paraffin wax and polystyrene slowed moisture diffusion but did not suppress interfacial reactions, with wax extending stability to over 90 days. These results show that ALD-Al2O3 suppresses dominant interfacial degradation pathways, enabling stable, high-field operation and advancing the practical deployment of CsPbBr3 γ-ray detectors.

Unal, Mustafa

Unveiling the Stability of Encapsulated Pt Catalysts Using Nanocrystals and Atomic Layer Deposition

Platinum exhibits desirable catalytic properties, but it is scarce and expensive. Optimizing its use in key applications such as emission control catalysis is important to reduce our reliance on such a rare element. Supported Pt nanoparticles (NPs) used in emission control systems deactivate over time because of particle growth in sintering processes. Here, in this work, we shed light on the stability against sintering of Pt NPs supported on and encapsulated in Al 2 O 3 using a combination of nanocrystal catalysts and atomic layer deposition (ALD) techniques. We find that small amounts of alumina overlayers created by ALD on preformed Pt NPs can stabilize supported Pt catalysts, significantly reducing deactivation caused by sintering, as previously observed by others. Combining theoretical and experimental insights, we correlate this behavior to the decreased propensity of oxidized Pt species to undergo Ostwald ripening phenomena because of the physical barrier imposed by the alumina overlayers. Furthermore, we find that highly stable catalysts can present an abundance of under-coordinated Pt sites after restructuring of both Pt particles and alumina overlayers at a high temperature (800 °C) in C 3 H 6 oxidation conditions. The enhanced stability significantly improves the Pt utilization efficiency after accelerated aging treatments, with encapsulated Pt catalysts reaching reaction rates more than two times greater than those of a control supported Pt catalyst.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Enabling ambient stability and quantum integration of organometallic magnonic ferrimagnets via atomic layer encapsulation

Magnons, the quanta of spin waves in magnetic materials, are promising for hybrid quantum systems by bridging electromagnetic and spin degrees of freedom. The organometallic ferrimagnet vanadium tetracyanoethylene (V[TCNE] x , x ≈ 2) is especially well-suited for quantum magnonics due to its low Gilbert damping and substrate versatility. However, its rapid chemical degradation in ambient conditions hinders practical applications. Incumbent encapsulation methods provide some protection, but are bulky, obscure intrinsic properties of V[TCNE] x , introduce thermal stress at cryogenic temperatures, and complicate microwave device integration. Here, we demonstrate that ultrathin alumina films deposited via low-temperature atomic layer deposition effectively protect V[TCNE] x by preserving its magnetic and magnonic properties following ambient exposure. The sub-100 nm transparent films also enable advanced spectroscopy, magnetometry, and cavity magnonic measurements that reveal the intrinsic properties of V[TCNE] x . This encapsulation strategy advances molecule-based quantum information science by providing a robust route toward scalable, monolithic integration in hybrid quantum technologies.

magnetic materials

Eliminating Surface Oxides of Superconducting Circuits with Noble Metal Encapsulation

The lifetime of superconducting qubits is limited by dielectric loss, and a major source of dielectric loss is the native oxide present at the surface of the superconducting metal. Specifically, tantalum-based superconducting qubits have been demonstrated with record lifetimes, but a major source of loss is the presence of two-level systems in the surface tantalum oxide. Here, we demonstrate a strategy for avoiding oxide formation by encapsulating the tantalum with noble metals that do not form native oxide. By depositing a few nanometers of Au or AuPd alloy before breaking vacuum, we completely suppress tantalum oxide formation. Microwave loss measurements of superconducting resonators reveal that the noble metal is proximitized, with a superconducting gap over 80% of the bare tantalum at thicknesses where the oxide is fully suppressed. Further, our findings suggest that losses in resonators fabricated by subtractive etching are dominated by oxides on the sidewalls, pointing to total surface encapsulation by additive fabrication as a promising strategy for eliminating surface oxide two-level system loss in superconducting qubits.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND

Förster Resonance Energy Transfer and Enhanced Emission in Cs 4 PbBr 6 Nanocrystals Encapsulated in Silicon Nano-Sheets for Perovskite Light Emitting Diode Applications

Encapsulating Cs 4 PbBr 6 quantum dots in silicon nano-sheets not only stabilizes the halide perovskite, but also takes advantage of the nano-sheet for a compatible integration with the traditional silicon semiconductor. Here, we report the preparation of un-passivated Cs 4 PbBr 6 ellipsoidal nanocrystals and pseudo-spherical quantum dots in silicon nano-sheets and their enhanced photoluminescence (PL). For a sample with low concentrations of quantum dots in silicon nano-sheets, the emission from Cs 4 PbBr 6 pseudo-spherical quantum dots is quenched and is dominated with Pb 2+ ion/silicene emission, which is very stable during the whole measurement period. For a high concentration of Cs 4 PbBr 6 ellipsoidal nanocrystals in silicon nano-sheets, we have observed Förster resonance energy transfer with up to 87% efficiency through the oscillation of two PL peaks when UV excitation switches between on and off, using recorded video and PL lifetime measurements. In an area of a non-uniform sample containing both ellipsoidal nanocrystals and pseudo-spherical quantum dots, where Pb 2+ ion/silicene emissions, broadband emissions from quantum dots, and bandgap edge emissions (515 nm) appear, the 515 nm peak intensity increases five times over 30 min of UV excitation, probably due to a photon recycling effect. This irradiated sample has been stable for one year of ambient storage. Cs 4 PbBr 6 quantum dots encapsulated in silicon nano-sheets can lead to applications of halide perovskite light emitting diodes (PeLEDs) and integration with traditional semiconductor materials.

36 MATERIALS SCIENCE

FTIR analysis of unaged encapsulants

Fourier transform infrared spectroscopy (FITR) analysis (in ATR mode) of unaged encapsulants (EVA, POE, EPE) from a commercial source.

characterization

Oxygen Distribution and Segregation at Grain Boundaries in Nb and Ta-Encapsulated Nb Thin Films for Superconducting Qubits

We report on atomic-scale analyses of oxygen distribution and segregation at grain boundaries (GBs) of Nb and Ta-encapsulated Nb (Ta/Nb) thin films for superconducting qubits using atom probe tomography (APT) and transmission electron microscopy (TEM). We observe oxygen segregation at grain boundaries (GBs) relative to the oxygen concentration within the grains for both Nb and Ta-capped Nb thin films and find that a higher oxygen concentration in the interior of Nb grains leads to greater oxygen segregation levels at GBs. This finding reveals that the formation of a local equilibrium of oxygen concentration between GBs and grain interiors of Nb is the primary driving force of the oxygen segregation behaviors in Nb and Ta-capped Nb. The enrichment factors (CGB/Cgrain) for oxygen segregation at GBs in Nb and Ta-capped Nb range from 2.4 ± 0.3 to 2.7 ± 0.4. The current results also highlight that controlling oxygen impurities in Nb during film deposition and fabrication processing is important to concomitantly reducing the level of oxygen segregation at GBs in Nb. Finally, we find that increases in the oxygen concentration in both Nb grains and GBs correlate with a suppression in the critical temperature for superconductivity (Tc). Together, our comparative chemical and charge transport property analyses provide atomic-scale insights into a potential mechanism, contributing to the decoherence in superconducting qubits.

Lee, Jaeyel [Fermilab] (ORCID:0000000185429612)