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At least 163 records · Page 9

Bond breaking in epoxy systems: A combined QM/MM approach

A novel method to combine quantum mechanics (QM) and molecular mechanics has been developed to accurately and efficiently account for covalent bond breaking in polymer systems under high strain without the use of predetermined break locations. Use of this method will provide a better fundamental understanding of the mechano-chemical origins of fracture in thermosets. Since classical force fields cannot accurately account for bond breaking, and QM is too demanding to simulate large systems, a hybrid approach is required. In the method presented here, strain is applied to the system using a classical force field, and all bond lengths are monitored. When a bond is stretched past a threshold value, a zone surrounding the bond is used in a QM energy minimization to determine which, if any, bonds break. The QM results are then used to reconstitute the system to continue the classical simulation at progressively larger strain until another QM calculation is triggered. In this way, a QM calculation is only computed when and where needed, allowing for efficient simulations. A robust QM method for energy minimization has been determined, as well as appropriate values for the QM zone size and the threshold bond length. Compute times do not differ dramatically from classical molecular mechanical simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Fast b -tagging at the high-level trigger of the ATLAS experiment in LHC Run 3

The ATLAS experiment relies on real-time hadronic jet reconstruction and b-tagging to record fully hadronic events containing b-jets. These algorithms require track reconstruction, which is computationally expensive and could overwhelm the high-level-trigger farm, even at the reduced event rate that passes the ATLAS first stage hardware-based trigger. In LHC Run 3, ATLAS has mitigated these computational demands by introducing a fast neural-network-based b-tagger, which acts as a low-precision filter using input from hadronic jets and tracks. It runs after a hardware trigger and before the remaining high-level-trigger reconstruction. This design relies on the negligible cost of neural-network inference as compared to track reconstruction, and the cost reduction from limiting tracking to specific regions of the detector. In the case of Standard Model HH → bb̅bb̅, a key signature relying on b-jet triggers, the filter lowers the input rate to the remaining high-level trigger by a factor of five at the small cost of reducing the overall signal efficiency by roughly 2%.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Ballistic Ejection of Microdroplets from Overpacked Interfacial Assemblies

Spontaneous emulsification, resulting from the assembly and accumulation of surfactants at liquid–liquid interfaces, is an interfacial instability where microdroplets are generated and diffusively spread from the interface until complete emulsification. Here, it is shown that an external magnetic field can modulate the assembly of paramagnetic nanoparticle surfactants (NPSs) at liquid–liquid interfaces to trigger an oversaturation in the areal density of the NPSs at the interface, as evidenced by a marked reduction in the interfacial tension, γ, and corroborated with a magnetostatic continuum theory. Despite the significant reduction in γ, the presence of the magnetic field does not cause stable interfaces to become unstable. Upon rapid removal of the field, however, an explosive ejection of a plume of microdroplets from the surface occurs, a dynamical interfacial instability which is termed explosive emulsification. Further, this explosive event rapidly reduces the areal density of the NPSs to its pre-field level, stabilizing the interface. The ability to externally suppress or trigger the explosive emulsification and controlled generation of tens of thousands of microdroplets, uncovers an efficient energy storage and release process, that has potential applications for controlled and directed delivery of chemicals and remotely controlled soft microrobots, taking advantage of the ferromagnetic nature of the microdroplets.

36 MATERIALS SCIENCE↗

Molecular dynamics of laser-assisted decomposition of unstable molecules at the surface of carbon nanotubes: case study of CH 2 (NO 2 ) 2 on CNT(4,0)

In this study, photoreactions of the dinitromethane molecule noncovalently adsorbed on the (4, 0) carbon nanotube (CNT) have been investigated by time-dependent, excited-state molecular dynamics, which takes into account simultaneous evolution of electronic excitation and nuclear positions under periodic optical excitations. It is found that desorption of molecular adsorbate from CNT surface can be controlled by UV-vis photoexcitations. In addition, it is shown that the presence of CNT substrate facilitates photodecomposition of the adsorbate molecule, related to optically controlled explosion. This model demonstrates potential of photoinduced charge transfer between the adsorbate and substrate, which can affect efficiency of desorption and decomposition reactions. This process has a potential use as a remote trigger for larger scale detonations, or as a mechanism for ‘cleaning’ CNTs of unwanted functionalisation.

Disrud, Brendon↗

Probing Ultrafast Charge Transfer Dynamics in Heterostructured Nanomaterials

The increasing demand for renewable and low‐cost energy has triggered a vast amount of research aimed at developing, characterizing and optimizing materials that can efficiently convert sun light into useful chemical energy in the form of electricity or chemical fuels. So‐ called quantum dot sensitized solar cell (QDSC) materials have gained much attention in recent years based on the advantageous physicochemical properties of semiconducting quantum dots (QDs) as sensitizers, as well as their promising potential to increase the conversion efficiency beyond the Shockley‐Queisser limit of ∼33% by making use of hot‐electron transfer (HET) routes and multiple exciton generation (MEG). By finely tuning the size of the QDs, the band gap can be carefully aligned to the metal oxide (MO) conduction band such that charge transfer from the photoexcited QD is thermodynamically favorable.

14 SOLAR ENERGY↗

The Trigger System of ICARUS-T600 Detector at Fermilab

The ICARUS-T600 liquid argon (LAr) time projection chamber (TPC) detector is currently deployed as a far detector of the Short Baseline Neutrino (SBN) program at Fermilab (USA) to search for a possible LSND-like sterile neutrino signal at $\Deltam^2 \approx 1eV^2$ with the Booster (BNB) and Main Injector (NuMI) Neutrino Beams. A global physical event rate of $\approx 0.6$ Hz, including the genuine neutrino interactions in LAr, beam halos and cosmic interactions inside the proton pulse time windows, is expected, roughly corresponding to $\approx 4$ PB of data for the total 6.6 $10^{20}$ pot exposure if the full ICARUS-T600 detector is readout ($\approx 200$ MB event size). The designed trigger system described here will collect the genuine neutrino interactions with a $\approx 95$\% expected efficiency.

Copello, S. [INFN, Pavia]↗

Rapid Inference of Logic Gate Neural Networks for Anomaly Detection in High Energy Physics

The increasing data rates and complexity of detectors at the Large Hadron Collider (LHC) necessitate fast and efficient machine learning models, particularly for rapid selection of what data to store, known as triggering. Building on recent work in differentiable logic gates, we present a public implementation of a Convolutional Differentiable Logic Gate Neural Network (CLGN). We apply this to detecting anomalies at the Level-1 Trigger at CMS using public data from the CICADA project. We demonstrate that the CLGN achieves physics performance on par with or superior to conventional quantized neural networks. We also synthesize an LGN for a Field-Programmable Gate Array (FPGA) and show highly promising FPGA characteristics, notably zero Digital Signal Processor (DSP) resource usage. This work highlights the potential of logic gate networks for high-speed, on-detector inference in High Energy Physics and beyond.

FOS: Physical sciences↗

GMC Collisions as Triggers of Star Formation. III. Density and Magnetically Regulated Star Formation

We study giant molecular cloud (GMC) collisions and their ability to trigger star cluster formation. We further develop our three-dimensional magnetized, turbulent, colliding GMC simulations by implementing star formation subgrid models. Two such models are explored: (1) “Density-Regulated,” i.e., fixed efficiency per free-fall time above a set density threshold and (2) “Magnetically Regulated,” i.e., fixed efficiency per free-fall time in regions that are magnetically supercritical. Variations of parameters associated with these models are also explored. In the non-colliding simulations, the overall level of star formation is sensitive to model parameter choices that relate to effective density thresholds. In the GMC collision simulations, the final star formation rates and efficiencies are relatively independent of these parameters. Between the non-colliding and colliding cases, we compare the morphologies of the resulting star clusters, properties of star-forming gas, time evolution of the star formation rate (SFR), spatial clustering of the stars, and resulting kinematics of the stars in comparison to the natal gas. We find that typical collisions, by creating larger amounts of dense gas, trigger earlier and enhanced star formation, resulting in 10 times higher SFRs and efficiencies. The star clusters formed from GMC collisions show greater spatial substructure and more disturbed kinematics.

79 ASTRONOMY AND ASTROPHYSICS↗

SPLENDAQ: A Detector-Agnostic Data Acquisition System for Small-Scale Physics Experiments

Many scientific applications from rare-event searches to condensed matter system characterization to high-rate nuclear experiments require time-domain triggering on a raw stream of data, where the triggering is generally threshold-based or randomly acquired. When carrying out detector R &D, there is a need for a general data acquisition (DAQ) system to quickly and efficiently process such data. In the SPLENDOR collaboration, we are developing the Python-based SPLENDAQ package for this exact purpose—it offers two main features for offline analysis of continuous data: a threshold triggering algorithm based on the time-domain optimal filter formalism and an algorithm for randomly choosing nonoverlapping segments for noise measurements. Further, combined with the commercially available Moku platform, developed by Liquid Instruments, we have a full pipeline of event building off raw data with minimal setup. Here, we review the underlying principles of this detector-agnostic DAQ package and give concrete examples of its utility in various applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Trigger Detection for the sPHENIX Experiment via Bipartite Graph Networks with Set Transformer

Trigger (interesting events) detection is crucial to high-energy and nuclear physics experiments because it improves data acquisition efficiency. It also plays a vital role in facilitating the downstream offline data analysis process. The sPHENIX detector, located at the Relativistic Heavy Ion Collider in Brookhaven National Laboratory, is one of the largest nuclear physics experiments on a world scale and is optimized to detect physics processes involving charm and beauty quarks. Furthermore, these particles are produced in collisions involving two proton beams, two gold nuclei beams, or a combination of the two and give critical insights into the formation of the early universe. This paper presents a model architecture for trigger detection with geometric information from two fast silicon detectors. Transverse momentum is introduced as an intermediate feature from physics heuristics. We also prove its importance through our training experiments. Each event consists of tracks and can be viewed as a graph. A bipartite graph neural network is integrated with the attention mechanism to design a binary classification model. Compared with the state-of-the-art algorithm for trigger detection, our model is parsimonious and increases the accuracy and the AUC score by more than 15%.

97 MATHEMATICS AND COMPUTING↗

Efficient Oxidative Decomposition of Jet-Fuel exo -Tetrahydrodicyclopentadiene (JP-10) by Aluminum Nanoparticles in a Catalytic Microreactor: An Online Vacuum Ultraviolet Photoionization Study

The oxidation of gas-phase exo-tetrahydrodicyclopentadiene (JP-10, C 10 H 16 ) over aluminum nanoparticles (AlNP) has been explored between a temperature range of 300 and 1250 K with a novel chemical microreactor. The results are compared with those obtained from chemical microreactor studies of helium-seeded JP-10 and of helium–oxygen-seeded JP-10 without AlNP to gauge the effects of molecular oxygen and AlNP, respectively. Vacuum ultraviolet (VUV) photoionization mass spectrometry reveals that oxidative decomposition of JP-10 in the presence of AlNP is lowered by 350 and 200 K with and without AlNP, respectively, in comparison with pyrolysis of the fuel. Overall, 63 nascent gas-phase products are identified through photoionization efficiency (PIE) curves; these can be categorized as oxygenated molecules and their radicals as well as closed-shell hydrocarbons along with hydrocarbon radicals. Quantitative branching ratios of the products reveal diminishing yields of oxidized species and enhanced branching ratios of hydrocarbon species with the increase in temperature. While in the low-temperature regime (300–1000 K), AlNP solely acts as an efficient heat transfer medium, in the higher-temperature regime (1000–1250 K), chemical reactivity is triggered, facilitating the primary decomposition of the parent JP-10 molecule. Furthermore, this enhanced reactivity of AlNP could plausibly be linked to the exposed reactive surface of the aluminum (Al) core generated upon the rupture of the alumina shell material above the melting point of the metal (Al).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Quantum Associative Memory in Hep Track Pattern Recognition

We have entered the Noisy Intermediate-Scale Quantum Era. A plethora of quantum processor prototypes allow evaluation of potential of the Quantum Computing paradigm in applications to pressing computational problems of the future. Growing data input rates and detector resolution foreseen in High-Energy LHC (2030s) experiments expose the often high time and/or space complexity of classical algorithms. Quantum algorithms can potentially become the lower-complexity alternatives in such cases. In this work we discuss the potential of Quantum Associative Memory (QuAM) in the context of LHC data triggering. We examine the practical limits of storage capacity, as well as store and recall errorless efficiency, from the viewpoints of the state-of-the-art IBM quantum processors and LHC real-time charged track pattern recognition requirements. We present a software prototype implementation of the QuAM protocols and analyze the topological limitations for porting the simplest QuAM instances to the public IBM 5Q and 14Q cloud-based superconducting chips.

97 MATHEMATICS AND COMPUTING↗

Free-standing membrane incorporating single-atom catalysts for ultrafast electroreduction of low-concentration nitrate

The release of wastewaters containing relatively low levels of nitrate (NO 3 ⁻) results in sufficient contamination to induce harmful algal blooms and to elevate drinking water NO 3 ⁻ concentrations to potentially hazardous levels. In particular, the facile triggering of algal blooms by ultra-low concentrations of NO 3 ⁻ necessitates the development of efficient methods for NO 3 ⁻ destruction. However, promising electrochemical methods suffer from weak mass transport under low reactant concentrations, resulting in long treatment times (on the order of hours) for complete NO 3 ⁻ destruction. In this study, we present flow-through electrofiltration via an electrified membrane incorporating nonprecious metal single-atom catalysts for NO 3 ⁻ reduction activity enhancement and selectivity modification, achieving near-complete removal of ultra-low concentration NO 3 ⁻ (10 mg-N L -1 ) with a residence time of only a few seconds (10 s). By anchoring Cu single atoms supported on N-doped carbon in a carbon nanotube interwoven framework, we fabricate a free-standing carbonaceous membrane featuring high conductivity, permeability, and flexibility. The membrane achieves over 97% NO 3 ⁻ removal with high N 2 selectivity of 86% in a single-pass electrofiltration, which is a significant improvement over flow-by operation (30% NO 3 ⁻ removal with 7% N 2 selectivity). This high NO 3 ⁻ reduction performance is attributed to the greater adsorption and transport of nitric oxide under high molecular collision frequency coupled with a balanced supply of atomic hydrogen through H 2 dissociation during electrofiltration. Overall, our findings provide a paradigm of applying a flow-through electrified membrane incorporating single-atom catalysts to improve the rate and selectivity of NO 3 ⁻ reduction for efficient water purification.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Developing new analysis tools for near surface radio-based neutrino detectors

The ARIANNA experiment is an Askaryan radio detector designed to measure high-energy neutrino induced cascades within the Antarctic ice. Ultra-high-energy neutrinos above 10 16 eV have an extremely low flux, so experimental data captured at trigger level need to be classified correctly to retain as much neutrino signal as possible. We first describe two new physics-based neutrino selection methods, or "cuts", (the updown and dipole cut) that extend the previously published analysis to a specialized ARIANNA station with 8 antenna channels, which is double the number used in the prior analysis. For a standard trigger with a threshold signal to noise ratio at 4.4, the new cuts produce a neutrino efficiency of > 95% per station-year of operation, while rejecting 99.93% of the background (corresponding to 53 remaining experimental background events). When the new cuts are combined with a previously developed cut using neutrino waveform templates, all background is removed at no change of efficiency. In addition, the neutrino efficiency is extrapolated to 1,000 station-years of operation, obtaining 91%. This work then introduces a new selection method (the deep learning cut) to augment the identification of neutrino events by using deep learning methods and compares the efficiency to the physics-based analysis. The deep learning cut gives 99% signal efficiency per station-year of operation while rejecting 99.997% of the background (corresponding to 2 remaining experimental background events), which are subsequently removed by the waveform template cut at no significant change in efficiency. Here the results of the deep learning cut were verified using measured cosmic rays which shows that the simulations do not introduce artifacts with respect to experimental data. The paper demonstrates that the background rejection and signal efficiency of near surface antennas meets the requirements of a large scale future array, as considered in baseline design of the radio component of IceCube-Gen2.

97 MATHEMATICS AND COMPUTING↗

Unraveling the Luminescence Quenching Mechanism in Strong and Weak Quantum-Confined CsPbBr 3 Triggered by Triarylamine-Based Hole Transport Layers

Luminescence quenching by hole transport layers (HTLs) is one of the major issues in developing efficient perovskite light-emitting diodes (PeLEDs), particularly prominent in blue-emitting devices. While a variety of material systems have been used as interfacial layers, the origin of such quenching and the type of interactions between perovskites and HTLs are still ambiguous. Here, we present a systematic investigation of the luminescence quenching of CsPbBr 3 by a commonly employed hole transport polymer, Poly(9,9-dioctylfluorene-alt-N-(4-sec-butylphenyl)-diphenylamine) (TFB) in LEDs. Strong and weakly quantum-confined CsPbBr 3 (nanoplatelets (NPLs)/nanocrystals (NCs)) are rationally selected to study the quenching mechanism by considering the differences in their morphology, energy level alignments, and quantum confinement. The steady-state and time-resolved Stern-Volmer plots unravel the dominance of dynamic and static quenching at lower and higher concentrations of TFB, respectively, with maximum quenching efficiency of 98%. The quenching rate in NCs is faster than in NPLs owing to their longer PL lifetimes and weak quantum confinement. The ultrafast transient absorption results support these dynamics and rule out the involvement of Forster or Dexter energy transfer. Finally, the 1D 1 H and 2D NOESY NMR study confirms the exchange of native ligands at the NCs surface with TFB, leading to dark CsPbBr 3 -TFB ensemble formation accountable for luminescence quenching. This highlights the critical role of the triarylamine functional group on TFB (also the backbone of many HTLs) in the quenching process. These results shed light on the underlying reasons for the luminescence quenching in PeLEDs and will help to choose the interfacial layers rationally for developing efficient LEDs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Catalytic Reaction Triggered by Magnetic Induction Heating Mechanistically Distinguishes Itself from the Standard Thermal Reaction

As a recent advancement in chemical engineering, magnetic induction heating (MIH) is utilized to initiate the intended reactions by enabling the self-heating of the ferromagnetic catalyst particles. While MIH can be energy-efficient and industrially scalable, its full potential has been underappreciated in catalysis because of the perception that MIH is merely an alternative heating approach. Unexpectedly, we show that the MIH-triggered reaction could go beyond standard thermal catalysis. Specifically, by probing the representative Pt/Fe 3 O 4 catalysts with CO oxidation in both thermal and MIH modes with consistent temperature profiles and catalyst structures, we found that the MIH mode boosts the reactivity more than 25 times by modifying Pt-FeO x interfacial synergies and promoting facile oxidation of the adsorbed carbonyl species by atomic oxygen. Further, as we preliminarily observed, this beneficial MIH-catalysis can be translational to other thermal reactions, potentially paving the way to launch MIH-catalysis as a distinct reaction category.

CO oxidation↗

Rational Regulation of Layer‐by‐Layer Processed Active Layer via Trimer‐Induced Pre‐Swelling Strategy for Efficient and Robust Thick‐Film Organic Solar Cells

Thick-film (>300 nm) organic solar cells (OSCs) have garnered intensifying attention due to their compatibility with commercial roll-to-roll printing technology for the large-scale continuous fabrication process. However, due to the uncontrollable donor/acceptor (D/A) arrangement in thick-film condition, the restricted exciton splitting and severe carrier traps significantly impede the photovoltaic performance and operability. For this work, combined with layer-by-layer deposition technology, a twisted 3D star-shaped trimer (BTT-Out) is synthesized to develop a trimer-induced pre-swelling (TIP) strategy, where the BTT-Out is incorporated into the buried D18 donor layer to enable the fabrication of thick-film OSCs. The integrated approach characterizations reveal that the exceptional configuration and spontaneous self-organization behavior of BTT-Out trimer could pre-swell the D18 network to facilitate the acceptor's infiltration and accelerate the formation of D/A interfaces. This enhancement triggers the elevated polarons formation with amplified hole-transfer kinetics, which is essential for the augmented exciton splitting efficiency. Furthermore, the regulated swelling process can initiate the favorable self-assembly of L8-BO acceptors, which would ameliorate carrier transport channels and mitigate carrier traps. As a result, the TIP-modified thin-film OSC devices achieve the champion performance of 20.3% (thin-film) and 18.8% (thick-film) with upgraded stability, among one of the highest performances reported of thick-film OSCs.

36 MATERIALS SCIENCE↗

Precisely modulate interfacial Bi-O bridge bond in Co-TCPP/Bi 3 O 4 Br to trigger long-lasting charge separation for boosting CO 2 photoreduction

Insufficient charge separation and feeble CO 2 activation limit the CO 2 photoreduction efficiency. It is highly desirable to consciously construct organic–inorganic hybrid composites to simultaneously accelerate charge separation and provide favorable active sites. Herein, a defect-induced interfacial Bi-O bridge bond is constructed by grafting terminal O of cobalt porphyrin (Co-TCPP) with Bi 3 O4Br. Systematic investigations reveal that the Bi-O bridge bond as the charge migration bridge accelerates the extraction and transfer of electron from the external [Bi 3 O 4 ] layers to Co-TCPP, and the millisecond separation lifetime of electrons on Co-TCPP can be achieved. Co atoms as the active sites optimized the CO 2 adsorption and activation, thus promoting the formation of COOH*. As a result, the CO 2 photoreduction rate of 0.5% Co-TCPP/Bi 3 O4Br reaches 71.3 μmol g -1 h -1 in pure water, 2.53-fold of that on the pristine Bi 3 O4Br. This work provides atomistic insights and strategies for the construction of new organic–inorganic hybrid materials for artificial photosynthesis and CO 2 photoreduction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗