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At least 235 records · Page 13

Autotuning of Double-Dot Devices In Situ with Machine Learning

The current practice of manually tuning quantum dots (QDs) for qubit operation is a relatively time-consuming procedure that is inherently impractical for scaling up and applications. In this work, we report on the in situ implementation of a recently proposed autotuning protocol that combines machine learning (ML) with an optimization routine to navigate the parameter space. In particular, we show that a ML algorithm trained using exclusively simulated data to quantitatively classify the state of a double-QD device can be used to replace human heuristics in the tuning of gate voltages in real devices. Here, we demonstrate active feedback of a functional double-dot device operated at millikelvin temperatures and discuss success rates as a function of the initial conditions and the device performance. Modifications to the training network, fitness function, and optimizer are discussed as a path toward further improvement in the success rate when starting both near and far detuned from the target double-dot range.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Antiferromagnetic order in Co-doped Fe 5 GeTe 2 probed by resonant magnetic x-ray scattering

The quasi-two-dimensional van der Waals magnet Fe 5-δ GeTe 2 has emerged as a promising platform for electronic and spintronic functionalities at room temperature, owing to its large ferromagnetic ordering temperature T C ≈ 315 K. Interestingly, by cobalt (Co) substitution of iron in F5GT, i.e., (Fe 1-x Co x ) 5-δ GeTe 2 (Co-F5GT), not only can its magnetic transition temperature be further enhanced, but the magnetic and structural ground states can also be tuned. Specifically, an antiferromagnetic (AFM) order is induced beyond the Co doping level x ≥ 0.4. Here, in this work, we investigate the magnetic properties of a Co-F5GT single crystal at x = 0.45(1), by utilizing the element-specific, resonant magnetic x-ray scattering technique. Our study reveals an A-type, Ising-like AFM ground state, with a transition temperature T N ≈ 340 K. In addition, our work unveils an important contribution from Co magnetic moments to the magnetic order. The application of the in-plane magnetic fields gradually polarizes the spin moments along the field direction, but without inducing incommensurate spin texture(s).

36 MATERIALS SCIENCE↗

Beyond Conventional Sensing: Hybrid Plasmonic Metasurfaces and Bound States in the Continuum

Fano resonances result from the strong coupling and interference between a broad background state and a narrow, almost discrete state, leading to the emergence of asymmetric scattering spectral profiles. Under certain conditions, Fano resonances can experience a collapse of their width due to the destructive interference of strongly coupled modes, resulting in the formation of bound states in the continuum (BIC). In such cases, the modes are simultaneously localized in the nanostructure and coexist with radiating waves, leading to an increase in the quality factor, which is virtually unlimited. In this work, we report on the design of a layered hybrid plasmonic-dielectric metasurface that facilitates strong mode coupling and the formation of BIC, resulting in resonances with a high quality factor. We demonstrate the possibility of controlling Fano resonances and tuning Rabi splitting using the nanoantenna dimensions. We also experimentally demonstrate the generalized Kerker effect in a binary arrangement of silicon nanodisks, which allows for the tuning of the collective modes and creates new photonic functionalities and improved sensing capabilities. Our findings have promising implications for developing plasmonic sensors that leverage strong light-matter interactions in hybrid metasurfaces.

36 MATERIALS SCIENCE↗

Evidence for Interfacial Octahedral Coupling as a Route to Enhance Magnetoresistance in Perovskite Oxide Superlattices

Engineering octahedral rotations in oxide heterostructures is a promising route for controlling magnetic properties in perovskites, with recent work focusing on magnetic-ordering temperatures and magnetic anisotropies. Here the effects of interfacial octahedral coupling on magnetoresistance are demonstrated in a series of (La 0.7 Sr 0.3 MnO 3 ) n /(LaFeO 3 ) 10 superlattices grown on (001)- and (111)-oriented SrTiO 3 substrates. The different crystallographic orientations allow for the interfacial octahedral connectivity to be tuned, with weaker interfacial coupling present at the (001)-oriented than the (111)-oriented structures as revealed by density functional theory calculations. In n = 14 superlattices, the effect of orientation on the physical properties is minimal with both (001)- and (111)-oriented samples exhibiting similar magnetoresistance. As the fraction of interfacial volume within the LSMO layers is increased by decreasing n, the magnetoresistive behavior of the samples diverges with significantly larger magnetoresistance magnitudes present in the (111)-oriented superlattices. Furthermore, the results are consistent with octahedral coupling playing a greater role in the functional properties at (111)-heterointerfaces and demonstrate a structure-driven approach to tuning interfacial magnetoresistance in complex-oxide heterostructures.

36 MATERIALS SCIENCE↗

Density dependence of the excitation gaps in an undoped Si/SiGe double-quantum-well heterostructure

In this work, we report low-temperature magneto-transport measurements of an undoped Si/SiGe asymmetric double quantum well heterostructure. The density in both layers is tuned independently utilizing top and bottom gates, allowing the investigation of quantum wells at both imbalanced and matched densities. Integer quantum Hall states at total filling factor v T =1 and v T =2 are observed in both density regimes, and the evolution of their excitation gaps is reported as a function of the density. The v T =1 gap evolution departs from the behavior generally observed for valley splitting in the single layer regime. Furthermore, by comparing the v T =2 gap to the single particle tunneling energy, Δ SAS , obtained from Schrödinger–Poisson (SP) simulations, evidence for the onset of spontaneous interlayer coherence is observed for a relative filling fraction imbalance smaller than ~50%.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Single-hole physics in GaAs/AlGaAs double quantum dot system with strong spin–orbit interaction

There is rapidly expanding interest in exploiting the spin of valence-band holes rather than conduction-band electrons for spin qubit semiconductor circuits composed of coupled quantum dots. The hole platform offers stronger spin–orbit interaction (SOI), large difference between in-dot-plane and out-of-dot-plane g-factors, i.e. g-factor anisotropy, and a significantly reduced hyperfine coupling to nuclei in the host material. These attributes collectively can deliver fast all-electric coherent spin manipulation, efficient spin-flip inter-dot tunneling channels, a voltage tunable effective g-factor, a g-factor adjustable to nearly zero in an appropriately oriented external magnetic field, and long spin relaxation and coherence times. In this work, we review our recent work on the physics of heavy holes confined in a planar GaAs/AlGaAs double quantum dot system with strong SOI. For a single-hole, we have performed resonant tunneling magneto-spectroscopy to extract spin-flip and spin-conserving tunneling strengths, implemented spin-flip Landau–Zener–Stückelberg–Majorana (LZSM) interferometry, determined the spin relaxation time T 1 as a function of magnetic field using a fast single-shot latched charge technique, electrically tuned the effective g-factor revealed by electric dipole spin resonance, and found signatures of the hyperfine interaction and dynamic nuclear polarization with holes. For two-holes, we have measured the energy spectrum in the presence of strong SOI (and so not limited by Pauli spin blockade), quantified the heavy-hole (HH) g-factor anisotropy on tilting the magnetic field, described a scheme to employ HHs whose g-factor is tunable to nearly zero for an in-plane magnetic field for a coherent photon-to-spin interface, and observed a well-defined LZSM interference pattern at small magnetic fields on pulsing through the singlet-triplet anti-crossing.

74 ATOMIC AND MOLECULAR PHYSICS↗

Implementation and Synthesis of Math Library Functions

Achieving speed and accuracy for math library functions like exp, sin, and log is difficult. This is because low-level implementation languages like C do not help math library developers catch mathematical errors, build implementations incrementally, or separate high-level and low-level decision making. This ultimately puts development of such functions out of reach for all but the most experienced experts. To address this, we introduce MegaLibm, a domain-specific language for implementing, testing, and tuning math library implementations. MegaLibm is safe, modular, and tunable. Implementations in MegaLibm can automatically detect mathematical mistakes like sign flips via semantic wellformedness checks, and components like range reductions can be implemented in a modular, composable way, simplifying implementations. Once the high-level algorithm is done, tuning parameters like working precisions and evaluation schemes can be adjusted through orthogonal tuning parameters to achieve the desired speed and accuracy. MegaLibm also enables math library developers to work interactively, compiling, testing, and tuning their implementations and invoking tools like Sollya and type-directed synthesis to complete components and synthesize entire implementations. MegaLibm can express 8 state-of-the-art math library implementations with comparable speed and accuracy to the original C code, and can synthesize 5 variations and 3 from-scratch implementations with minimal guidance.

97 MATHEMATICS AND COMPUTING↗

Operational Parameters, Considerations, and Design Decisions for Resource-Constrained Ion Trap Mass Spectrometers

Mass spectrometers are increasingly finding applications in new and unique areas, often in situations where key operational resources (i.e. power, weight and size) are limited. One such example is the Mars Organic Molecule Analyzer (MOMA). This instrument is a joint venture between NASA and the European Space Agency (ESA) to develop an ion trap mass spectrometer for chemical analysis on Mars. The constraints on such an instrument are significant as are the performance requirements. While the ideal operating parameters for an ion trap are generally well characterized, methods to maintain analytical performance with limited power and system weight need to be investigated and tested. Methods Experiments have been performed on two custom ion trap mass spectrometers developed as prototypes for the MOMA instrument. This hardware consists of quadrupole ion trap electrodes that are 70% the size of common commercial instrumentation. The trapping RF voltage is created with a custom tank circuit that can be tuned over a range of RF frequencies and is driven using laboratory supplies and amplifiers. The entire instrument is controlled with custom Lab VIEW software that allows a high degree of flexibility in the definition of the scan function defining the ion trap experiment. Ions are typically generated via an internal electron ionization source, however, a laser desorption source is also in development for analysis of larger intact molecules. Preliminary Data The main goals in this work have been to reduce the power required to generate the radio frequency trapping field used in an ion trap mass spectrometer. Generally minimizing the power will also reduce the volume and mass of the electronics to support the instrument. In order to achieve optimum performance, commercial instruments typically utilize RF frequencies in the 1 MHz range. Without much concern for power usage, they simply generate the voltage required to access the mass range of interest. In order to reduce the required RF voltage (and power), operation of the ion trap at lower RF frequencies has been investigated. Surprisingly, the performance of the instrument has only been slightly degraded at RF frequencies all the way down to 500 kHz. Mass resolution is relatively stable to this point and depending on the resonant ejection point used, the peak intensity is also quite stable. To date only masses up to m/z 200 have been fully investigated, however, additional studies are planned to verify the performance with higher mass ions. The lower frequency and voltage should reduce the pseudo potential well depth, eventually affecting the trapping efficiency of the instrument -- effect that could manifest itself in significantly limiting the mass range of trapped ions. Other methods to reduce the RF power while maintaining analytical performance are also under investigation. This includes ion ejection at lower q(sub z) values to access a given mass with a lower RF voltage. The loss of mass resolution at lower q(sub eject) points has been measured and current work is underway to leverage scan speed and the use of non-linear resonances in order to counter this trend. The overall trap performance under this range of operating conditions will be presented with a goal of identifying what trade-offs are acceptable.

Danell, Ryan M.↗

Transferring a Molecular Foundation Model for Polymer Property Predictions

Transformer-based large language models have remarkable potential to accelerate design optimization for applications such as drug development and material discovery. Self-supervised pretraining of transformer models requires large-scale data sets, which are often sparsely populated in topical areas such as polymer science. Further, state-of-the-art approaches for polymers conduct data augmentation to generate additional samples but unavoidably incur extra computational costs. In contrast, large-scale open-source data sets are available for small molecules and provide a potential solution to data scarcity through transfer learning. In this work, we show that using transformers pretrained on small molecules and fine-tuned on polymer properties achieves comparable accuracy to those trained on augmented polymer data sets for a series of benchmark prediction tasks.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

In situ multimodal imaging for nanoscale visualization of tribofilm formation

A third of the energy from fuel combustion in passenger car gasoline engines is lost due to friction. Carefully designed engine lubricants can recover some of these losses by reducing friction and wear by forming a nanometer-scale chemico-physico tribofilm between surfaces. Accordingly, attention has focused on developing oil formulations that form low-friction tribofilms. However, analyses of resultant tribofilms are typically conducted after tribo-tests with conventional characterization tools and do not offer insights into tribofilm formation and evolution, precluding information critical to tuning tribofilm properties. In this work, we developed a unique multimodal methodology based on Atomic Force Microscopy (AFM) with local probe heating for in situ tribological studies that activates friction modifiers and simultaneously captures the evolution of friction and surface roughness, with nanometer resolution. As a platform to demonstrate the ability of this methodology to visualize dynamics of tribofilm formation in situ, we apply it to molybdenum-based friction modifiers to distinguish key factors in their functionality and correlate nanoscale AFM and Friction Force Microscopy data to bench tribo-tests used in the industry. To decode the formation mechanisms observed in situ and underlying chemistry of tribofilms, we performed ab initio Molecular Dynamics (AIMD) simulations at comparable conditions. AIMD simulations confirmed both nanoscale and bench tribo-test results and showed deviations in molecular organization in tribofilms that are formed from different molybdenum-based friction modifiers that corroborates with surface functionality. With this innovative methodology, we demonstrate proof-of-principle in situ formation of molybdenum-based tribofilms directly on steel surfaces that could be applied generally to studying tribofilm formation.

36 MATERIALS SCIENCE↗

Measurement of the muon neutrino charged-current mesonless cross section in the NOvA near detector

NOvA is a long-baseline accelerator neutrino experiment at Fermilab. Its physics goals include precision neutrino oscillation measurements, neutrino interaction cross-section measurements and beyond Standard Model explorations. We present a measurement of muon neutrino charged-current cross section with zero mesons in the final state at the NOvA near detector. This measurement is performed as a function of the kinematics of the final state muon. Our chosen interaction channel is especially sensitive to quasielastic and meson exchange current interactions and it provides handles for constraining the cross section systematic uncertainties in oscillation analyses in present and future experiments. For particle identification, we use a convolutional neural network (CNN) trained on individual particles simulated in the NOvA Near detector. This allows us to select the desired signal while reducing the potential bias from neutrino interaction modeling. We study strategies for constraining the remaining charged-pion background via Michel electron information in a template fitting approach. The main experimental result is a two-dimensional differential cross section as a function of final-state muon kinetic energy and polar angle. The parameters of this measurement, including binning and unfolding, were optimized to reduce the expected systematic uncertainty in the total cross section. The final result shows good agreement with the main GENIE-based simulation framework that was independently fine-tuned in NOvA. We finally propose improvements and subsequent steps that build on this analysis and further dissect the final states of neutrino interactions. This work has been supported by US DOE grant DE-SC0015684.

Sánchez Falero, Sebastián Jesús [Iowa State U.]↗

Tuning Molecular Interactions between Peptoids and Substrates to Achieve Surface-Agnostic Coating

Achieving programmable and robust coatings that maintain functionality while adhering to various surface types with molecular-level tunability and programmable features remains challenging. In this study, we develop adaptable and stable surface-agnostic coatings (SACs) based on crystalline peptoid membranes by tuning interpeptoid and peptoid-substrate interactions. We utilize two complementary methods: (1) surfaceinduced assembly, where peptoid membranes form directly on substrates, and (2) depositing preformed peptoid crystalline membranes via an aqueous layer-by-layer (LbL) assembly technique. These strategies are applied to substrates with diverse surface chemistries and topographies, including mica, highly ordered pyrolytic graphite (HOPG), MoS 2 , sapphire, and porous membranes like porous alumina and polysulfide. Atomic force microscopy confirms the formation of peptoid coatings and reveals differences in assembly behavior across surfaces. Moisture vapor transport measurements serve as a proof-of-concept test for membrane continuity and tunable permeance. Together, these findings demonstrate the adaptability and programmability of peptoid-based SACs, enabling rational coating design on surfaces with diverse chemical and topographical features. Furthermore, this work opens pathways for using peptoid membranes as programmable surface modifiers in functional interfaces, protective coatings, and membrane platforms.

biomimetic polymers↗

Pressure dependent magnetic properties on bulk CrBr 3 single crystals

The van der Waals class of materials offer an approach to two-dimensional magnetism as their spin fluctuations can be tuned upon exfoliation of layers. Moreover, it has recently been shown that spin-lattice coupling and long-range magnetic ordering can be modified with pressure in van der Waals materials. In this work, the magnetic properties of quasi two-dimensional CrBr 3 are reported applying hydrostatic pressure. The application of pressure up to 0.844 GPa shows a 1.77% decrease in saturation magnetization with a decrease in the Curie temperature from 33.05 to 30.41 K. Density functional theory calculations with pressure up to 1 GPa show a reduction in volume and interplanar distance as pressure increases. To further understand the magnetic properties with applied pressure, the magnetocrystalline anisotropy energy (MAE) and exchange coupling parameter (J) are calculated. There is small decrease in MAE and the first nearest neighbor interaction (J 1 ) (U = 2.7 eV and J = 0.7 eV) is increasing with respect to increasing pressure. Overall, CrBr 3 displays ferromagnetic interlayer coupling and the calculated exchange coupling and MAE parameters match well with the observations from the experimental work.

36 MATERIALS SCIENCE↗

Design of Graphene/Ionic Liquid Composites for Carbon Capture

Pore size is a crucial factor impacting gas separation in porous separation materials, but how to control the pore size to optimize the separation performance remains a challenge. Here, we propose a design of graphene/ionic liquid composites with tunable slit pore sizes, where cations and anions of ionic liquids are intercalated between graphene layers. By varying the sizes of the ions, we show from first-principles density functional theory calculations that the accessible pore size can be tuned from 3.4 to 6.0 Å. Grand canonical Monte Carlo simulations of gas sorption find that the composite materials possess high CO 2 uptake at room temperature and 1 bar (up to ~8.5 mmol/g). Further simulations of the sorption of gas mixtures reveal that high CO 2 /N 2 and CO 2 /CH 4 adsorption selectivities can be obtained when the accessible pore size is <5 Å. This work suggests a new strategy to achieve tunable pore sizes via the graphene/IL composites for highly selective CO 2 /N 2 and CO 2 /CH 4 adsorption.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Molecular Insight into the Effects of Clustering on the Dynamics of Ionomers in Solutions

Ionizable groups tethered to polymers enable their many current and potential applications. However, these functionalities drive the formation of physical networks through clustering of the ionic groups, resulting in constrained dynamics of the macromolecules. Understanding the molecular origin of this hindrance remains a critical fundamental question, whose solution will directly impact the processing of ionizable polymers from molecules to viable materials. Here, in this work, using quasielastic neutron scattering accompanied by molecular dynamics simulations, segmental dynamics of slightly sulfonated polystyrene is studied in solutions as the cohesion of the ionic assemblies is tuned. We find that in cyclohexane the ionic assemblies act as centers of confinement, affecting dynamics both on macroscopic lengths and in the vicinity of the ionic assemblies. Addition of a small amount of ethanol affects the packing of the ionizable groups within the assemblies, which in turn enhances the chain dynamics.

36 MATERIALS SCIENCE↗

Facile Generation of Active Sites in Nodes of Ni-MFU-4l Metal–Organic Framework for Hydrogenation Reaction

Metal–organic frameworks (MOFs) represent a well-defined class of materials capable of incorporating catalytically active sites for gas-phase catalysis. However, the reducing conditions of hydrogenation catalysis can lead to nanoparticle formation in MOFs, which can significantly diminish the catalytic activity of single-site metals and reduce the longevity of MOF-based hydrogen solutions. In this work, we present a straightforward approach to accessing catalytically active single metal sites in a robust Ni-MFU-4l MOF for gas-phase hydrogenation without the formation of Ni nanoparticles. By carefully tuning the local node chemistry through postsynthetic exchange of the terminal ligand coordinated to the Ni(II) centers in the MOF, from −Cl to −OH or −HCOO, we can readily generate Ni–H active species. We further demonstrate, using in situ pair-distribution function analysis, that these Ni–H sites are the sole catalytically active sites in the terminal ligand-exchanged counterparts, whereas nanoparticles readily form in the parent Ni-MFU-4l-Cl under otherwise identical catalytic conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Monolayer CrCl 3 as an Ideal Test Bed for the Universality Classes of 2D Magnetism

The monolayer halides CrX 3 (X=Cl, Br, I) attract significant attention for realizing 2D magnets with genuine long-range order (LRO), challenging the Mermin-Wagner theorem. In this work, we show that monolayer CrCl 3 has the unique benefit of exhibiting tunable magnetic anisotropy upon applying a compressive strain. This opens the possibility to use CrCl 3 for producing and studying both ferromagnetic and antiferromagnetic 2D Ising-type LRO as well as the Berezinskii-Kosterlitz-Thouless (BKT) regime of 2D magnetism with quasi-LRO. Using state-of-the-art density functional theory, we explain how realistic compressive strain could be used to tune the monolayer's magnetic properties so that it could exhibit any of these phases. Building on large-scale quantum Monte Carlo simulations, we compute the phase diagram of strained CrCl 3 , as well as the magnon spectrum with spin-wave theory. Our results highlight the eminent suitability of monolayer CrCl 3 to achieve very high BKT transition temperatures, around 50 K, due to their singular dependence on the weak easy-plane anisotropy of the material.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Carbon-Assisted, Continuous Syngas Production in a Chemical Looping Scheme

In the current energy and environment scenario, it is imperative to develop energy efficient routes for chemical manufacturing that also pave the way for mitigation of greenhouse gas emissions. This work presents an efficient pathway for continuous syngas production via a chemical looping conversion of the two most potent greenhouse gases—CH 4 , and CO 2 . The well-known dry-reforming process of converting CH 4 , and CO 2 to syngas is energy-intensive and suffers from catalyst deactivation. The chemical looping approach, on the other hand, provides avenues for mitigating catalyst deactivation and enabling improved energy efficiency. The key to such process enhancements lies in the intricate structure–function relationships of the catalyst and its correlation to the process variables. We present the reduction and oxidation characteristics of 5 wt.% Ni/Ce 1-x Zr x O 2 -based catalysts (x = 0, 0.4, and 0.625). We demonstrate low temperature CH4 activation over Ni-promoted samples as opposed to pure Ce 1-x Zr x O 2 . Moreover, our results depict an optimum regeneration of these catalysts when oxidized by CO 2 , and H 2 O, which allows for chemical looping operation of steam reforming of methane as well. Process variables were tuned to optimize the CH 4 conversion (over 80%), and H 2 /CO ratio at 650 °C. The critical surface reactions—carbon accumulation and gasification, and thermocatalytic CO 2 splitting were investigated to elucidate the dynamic nature of the catalyst surface. In conclusion, the impact of this work lies in showcasing the opportunities to design chemical looping reactors for energy efficient syngas production from waste greenhouse gases.

25 ENERGY STORAGE↗