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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 217 records · Page 12

Factors Influencing Gas Evolution from High‐Nickel Layered Oxide Cathodes in Lithium‐Based Batteries

Abstract Gas evolution from high‐nickel layered oxide cathodes (>90% Ni) remains a major issue for their practical application. Gaseous species, such as CO 2 , O 2 , and CO, that are evolved at high states of charge (SOC) worsen the overall safety of batteries, as pressure build‐up within the cell may lead to cell rupture. Since these gasses are produced during cathode degradation, tracking the formation of gasses is also important in diagnosing cathode failure. Online electrochemical mass spectrometry (OEMS) is a powerful in situ technique to study gas evolution from the cathode during high‐voltage charge. However, the differences in the OEMS experimental setups between different groups make it challenging to compare results between groups. In this perspective, the various factors that influence gas evolution based on the OEMS results collected in this group are presented. The focus is on the conditions that lead to gas release, with a particular emphasis on reactive oxygen formation and subsequent chemical reactions with the electrolyte. Promising strategies, such as electrolytes, compositional tuning, and surface coatings that are effective at suppressing gas evolution from the cathode are highlighted. Critical insights into mitigating cathode degradation and gas evolution are provided to guide the development of safer, high‐energy batteries.

Chemistry↗

The theoretical and experimental investigations on multiple pure tone noise.

An investigation on multiple pure tone (MPT) noise is described. The model fan is operated, in Freon 12, in a closed loop acoustical facility. It has been found experimentally that the rotor relative Mach number and incidence angle are parameters important to the evolution of the MPT sound and the inlet duct length has a significant influence on the MPT sound emission. The experimental results are compared with a previous analysis. From the known blade nonuniformities of the model fan, the MPT distributions are computed. The analysis correctly predicts the frequency of the dominant multiple pure tone and sound pressures of the blade passing frequency noise and the dominant MPT that are in the same range as the experimental values.

Kantola, R. A.↗

Experimental Evaluation of Silica as a Thermal Protection System for Planetary Entry Probes

The evolution and pursuit of the reflecting heat-shield concept has resulted in a refined and sophisticated high-performance material: ultra-pure, slip-cast, fused silica (SCFS). Silica is "tailored" to the intense planetary entry environments through a combination of its good ablative qualities and outstanding reflective properties in the correct spectral region. Extensive development of SCFS has produced a series of candidate materials which are experimentally evaluated and compared in a simulated entry environment. The detailed response of silica to combined heating is discussed, and the relative merits of SCFS and carbon phenolic are indicated.

David L Peterson↗

The electrospray: Fundamentals and combustion applications

Liquid fuel dispersion in practical systems is typically achieved by spraying the fuel into a polydisperse distribution of droplets evaporating and burning in a turbulent gaseous environment. In view of the nearly unsurmountable difficulties of this two-phase flow, it would be useful to use an experimental arrangement that allow a systematic study of spray evolution and burning in configurations of gradually increasing levels of complexity, starting from laminar sprays to fully turbulent ones. An Electrostatic Spray (ES) of charged droplets lends itself to this type of combustion experiments under well-defined conditions and can be used to synthesize gradually more complex spray environments. In its simplest configuration, a liquid is fed into a small metal tube maintained at several kilovolts relative to a ground electrode few centimeters away. Under the action of the electric field, the liquid meniscus at the outlet of the capillary takes a conical shape, with a thin jet emerging from the cone tip. This jet breaks up farther downstream into a fine spray of charged droplets. Several advantages distinguish the electrospray from alternative atomization techniques: the self-dispersion property of the spray due to coulombic repulsion; the absence of droplet coalescence; the potential control of the trajectories of charged droplets by suitable disposition of electrostatic fields; and the decoupling of atomization, which is strictly electrostatic, from gas flow processes. Furthermore, as recently shown in our laboratory, the electrospray can produce quasi-monodisperse droplets over a very broad size range (1-100 microns). The ultimate objective of this research project is to study the formation and burning of electrosprays of liquid fuels first in laminar regimes and then in turbulent ones. Combustion will eventually be investigated in conditions of three-dimensional droplet-droplet interaction, for which experimental studies have been limited to either qualitative observations in sprays or more quantitative observations on simplified systems consisting of a small number of droplets or droplet arrays. The compactness and potential controllability of this spray generaiton system makes it appealing for studies to be undertaken in the next two years on electrospray combustion in reduced-gravity environments such as those achievable at NASA microgravity test facilities.

Gomez, Alessandro↗

Dynamic control of quantum phases in two-dimensional materials via Floquet engineering

The dynamical engineering of quantum states through periodic optical driving, known as Floquet engineering, has emerged as a powerful frontier in condensed matter physics, offering a pathway to realize material properties inaccessible in static equilibrium. This review provides a comprehensive overview of recent theoretical and experimental advances in the optical manipulation of two-dimensional (2D) quantum materials. We begin by systematically reviewing the evolution of the field from its pioneering applications in graphene and twisted moiré superlattices, highlighting the experimental realization of the light-induced anomalous Hall effect (AHE) to the complex spin-valley physics in transition metal dichalcogenides (TMDs). Furthermore, we briefly examine recent advances in 2D magnetic materials, demonstrating how optical driving can actively compete with intrinsic magnetism to dynamically switch magnetic orders and topological invariants. Moreover, we discuss the emerging frontiers of multi-frequency driving, quantum optimal control theory (QOCT), and ultrafast lightwave electronics. We highlight how tailored waveforms, such as bicircular light fields, and sub-cycle attosecond control can selectively break spatial symmetries to generate novel nonlinear photocurrents, mitigate dissipation, and extend the boundaries of quantum control well beyond the perturbative steady-state regime. Finally, we summarize the key experimental challenges for Floquet engineering, including effects such as heating and scattering, which limit coherent quantum control.

Wang, Wenpeng [Northeastern University, Shenyang, ↗

Phase-field modeling and experiments of dynamic fracture in single crystal quartz

Predicting the onset and characteristics of brittle fracture is important for a wide range of engineering and geological material applications. In this paper, we study important aspects of brittle fracture in α-quartz by phase-field modeling and experiments using a top-down approach. In the modeling framework, the work term in the Griffith energy balance is replaced with internal energy contributions that represent surface energy, thermal energy, and elastic strain energy stored in defects. This allows parametrization of individual energy contributions in terms of internal state variables and keeps track of energy partitioning after the onset of fracture. The path and history dependence of fracture is included in evolution laws for internal state variables, e.g., entropy evolution, while the energy remains a true potential. In the experimental part, dynamic compression experiments coupled with X-ray phase contrast imaging are performed on cube-like samples with a hole. In the top-down analysis, dynamic compression and three point bending experiments from the literature are simulated with the developed phase-field damage model. In conclusion, the fitted model highlights the strain rate, size, and stress state dependence of damage nucleation and evolution in single crystal α-quartz.

36 MATERIALS SCIENCE↗

Focused Ion Beam Tomography of Alloy 617 Corroded in Molten Chloride Salt

Materials qualification of reactor structural materials is a critical step in rapid implementation of advanced nuclear reactor technologies, particularly to assess the corrosion performance in these designs. Accelerated qualification of reactor structural materials requires incorporating powerful computational toolsets, such as phase field modelling in the Multiphysics Object-Oriented Simulation Environment (MOOSE) framework, to predict the evolution of structural materials due to corrosion. Accordingly, computational toolsets will require experimental data generated at appropriate length scales to validate accuracy. Focused ion beam (FIB) provides a high degree of control over manipulation of materials for analytical purposes, including capturing data on the evolution in the microstructure and elemental composition of materials at the mesoscale, an appropriate length scale for phase field modelling of intergranular diffusion phenomena using the MOOSE framework. For instance, the FEI Helios G4 UX dual beam plasma FIB microscope at the Irradiated Materials Characterization Laboratory (IMCL) is capable of backscatter diffraction (EBSD) and energy-dispersive x-ray spectroscopy (EDS) documenting the evolution in the microstructure and elemental composition, respectively. The Helios can perform EDS and EBSD three-dimensionally (3D) using tomography, which is then combined using different software packages to visualize 3D volumes correlating elemental composition to microstructural data. The purpose of this investigation was to develop a streamlined characterization and data processing workflow for 3D tomography studies on the FEI Helios G4 plasma FIB. The investigation is segmented into three parts: 1) Optimizing the data collection workflow, 2) identifying appropriate data processing and visualization software (i.e. DREAM.3D, MIPAR, and VGStudioMax), and 3) establishing an infrastructure for public release. The optimization of the data collection workflow is in collaboration with members of the U220 department to setup formal training on the tomography operation of the G4, through ThermoFisher Scientific, and exploring DREAM.3D, MIPAR, and VGStudioMax data processing/visualization software packages. VGStudioMax currently demonstrates the most promise for future use. Optimization of the data collection and processing workflow is still ongoing. A collaboration with INL High Performance Computing (HPC) established an open-source license for expediting the public release of FIB tomography datasets through HPC. FIB tomography data generated by the G4 will provide comprehensive data for validating 3D phase field mesoscale modelling tools within the MOOSE framework for accelerated qualification of reactor structural materials.

Copeland-Johnson, Trishelle↗

Computational Role of Tunneling in a Programmable Quantum Annealer

Quantum tunneling is a phenomenon in which a quantum state tunnels through energy barriers above the energy of the state itself. Tunneling has been hypothesized as an advantageous physical resource for optimization. Here we present the first experimental evidence of a computational role of multiqubit quantum tunneling in the evolution of a programmable quantum annealer. We developed a theoretical model based on a NIBA Quantum Master Equation to describe the multi-qubit dissipative cotunneling effects under the complex noise characteristics of such quantum devices.We start by considering a computational primitive, the simplest non-convex optimization problem consisting of just one global and one local minimum. The quantum evolutions enable tunneling to the global minimum while the corresponding classical paths are trapped in a false minimum. In our study the non-convex potentials are realized by frustrated networks of qubit clusters with strong intra-cluster coupling. We show that the collective effect of the quantum environment is suppressed in the critical phase during the evolution where quantum tunneling decides the right path to solution. In a later stage dissipation facilitates the multiqubit cotunneling leading to the solution state. The predictions of the model accurately describe the experimental data from the D-WaveII quantum annealer at NASA Ames. In our computational primitive the temperature dependence of the probability of success in the quantum model is opposite to that of the classical paths with thermal hopping. Specially, we provide an analysis of an optimization problem with sixteen qubits,demonstrating eight qubit cotunneling that increases success probabilities. Furthermore, we report results for larger problems with up to 200 qubits that contain the primitive as subproblems.

hard problems↗

CFD Predictions of Boiling Regime Transitions during Line Chilldown validated against a 1G LN2 Experiment

Introduction Before filling a propellant tank on the ground or in Space, the transfer line between the donor and receiver tanks must be cooled down preferably by sacrificing a minimum amount of the cryogenic fluid. The cryogenic line chill-down process involves a transition between different flow boiling regimes, namely, film boiling, transition film boiling, and nucleate boiling which are complex and may be quite gravity-dependent. Capturing these boiling phenomena and predicting the transition between them in a CFD framework is new and challenging both for 1g and microgravity applications. Materials & Methods The present work addresses this challenge by employing a two-phase Eulerian approach in the context of a homogeneous fluid mixture together with the Lee phase change model to capture the film boiling regime of the chill-down process using ANSYS Fluent®. The nucleate boiling regime is predicted by incorporating an in-house developed sub-grid model that accounts for bubble nucleation, bubble growth, bubble departure diameter, and their shedding frequency. The sub-grid model is encoded and implemented into Fluent via a user-defined function for the wall-fluid heat flux calculations. The mathematical formulation and numerical implementation of the CFD model are described in detail. The coupled CFD-Subgrid model is validated against published experimental data for liquid nitrogen chill-down of a heated stainless-steel pipe in 1g. Results Numerical simulation results show good agreements between the CFD predictions of the wall temperature evolution, rewetting temperature, and transition between film and nucleate boiling, with the experimental measurements published by Darr et al [2] for several different LN2 flowrates in the vertical pipe orientation. The CFD predictions for the wall temperature distribution indicate a rapid quenching of the wall at two upstream and downstream temperature sensing locations as compared to the experimental measurement. The only tuning parameter in the CFD model is the Lee mass transfer coefficient. The CFD Model predicts the Liedenfrost rewetting temperature in close agreement with the experiment. This marks a transition between stable and transitionary flow boiling regimes. The CFD-predicted boiling curve for the downstream sensor location is also compared against its experimental counterpart and indicates that the model is able to predict all the key temperature and heat flux parameters during the transitions from stable to transitionary film boiling to nucleate boiling in close agreement with the experiment. A sequence of predicted volume fraction, and temperature contours depicting these transitions will be presented.

Evaporation Condensation↗

Effect of Zn Addition on Phase Evolution in AlCrFeCoNiZn High–Entropy Alloy

The addition of Zn to AlCrFeCoNi high-entropy alloy (HEA) poses intriguing questions as to how it would affect phase evolution. Herein, the phase evolution in AlCrFeCoNiZn is studied using a combination of experimental techniques (X-ray diffraction, scanning electron microscopy, energy-dispersive spectroscopy, and differential scanning calorimetry) and computational (density-functional theory [DFT], calculation of phase diagrams, and machine-learning) methods. Mechanically alloyed and spark-plasma-sintered AlCrFeCoNiZn assumes a metastable single-phase, body-centered-cubic (BCC) structure that undergoes diffusion-controlled phase separation upon subsequent heat treatment to form separate (Al, Cr)-rich, (Fe, Co)-rich, and (Zn, Ni)-rich phases. The formation of (Al, Cr)-rich phase, not reported previously in AlCrFeCoNi-based HEAs, is attributed to strong clustering tendency of Cr–Zn and Cr–Ni pairs, combined with the strong ordering of Zn–Ni pair, driving out Cr that in turn combines with Al to form a (Al, Cr)-rich phase. In the DFT results, the formation of thermodynamically stable L1 2 phase is shown wherein Cr–Fe–Zn [Al–Ni-Co] preferably occupy1a (000) [3c (0 ½ ½)] positions. Furthermore, the sluggish diffusional transformation to L1 2 phase from BCC precursors is attributed to the small stacking-fault energy of AlCrFeCoNiZn. The equilibrated HEA exhibits a high microhardness of 8.24 GPa with an elastic modulus of 184 GPa.

36 MATERIALS SCIENCE↗

Computational simulation of transition to turbulence through inverse modeling

The present investigation has focused on a computational methodology for the fundamental case of transition in channel flow, in which recently published experimental data are utilized both as a stimulus and as a measure of merit of the method. The research has proceeded along three avenues in parallel. The first task has consisted of the development and verification of a computer code which calculates the mean evolution of flow in a channel similar to the one employed experimentally by Blair and Anderson. An analytical test case was created for the dual purposes of code verification and of highlighting the interactions between the Reynolds stress and the mean velocity profile. This test case generated a Reynolds stress by the residue in the momentum equation which is produced by a typical analytical velocity profile. By a substitution of this Reynolds stress into the appropriate code module, the correctness of the code may be verified, along with the accuracy of the computational method. The second task pursued has involved the development of a triple layer model for the Reynolds stress profile, which was suggested and derived from experimental velocity profiles. It is demonstrated that the innermost length scale is based on the local friction velocity, the intermediate layer corresponds to the usual logarithmic law of the wall region in which the normalized Reynolds stress is approximately unity, and the outermost layer is represented by a closed mathematical form depending explicitly on the velocity profile in the wake region. The third task was comprised of scrutiny of the excellent databases developed by Blair and others, and the planning of its incorporation into the transition analysis. These extensive measurements indicate that turbulent statistics in the transition regime may be considered to alternate between laminar and fully turbulent types, the proportions of which are quantified by a measured intermittency function.

Sepri, Paavo↗

A Computational and Experimental Investigation of Shear Coaxial Jet Atomization

The instability and subsequent atomization of a viscous liquid jet emanated into a high-pressure gaseous surrounding is studied both computationally and experimentally. Liquid water issued into nitrogen gas at elevated pressures is used to simulate the flow conditions in a coaxial shear injector element relevant to liquid propellant rocket engines. The theoretical analysis is based on a simplified mathematical formulation of the continuity and momentum equations in their conservative form. Numerical solutions of the governing equations subject to appropriate initial and boundary conditions are obtained via a robust finite difference scheme. The computations yield real-time evolution and subsequent breakup characteristics of the liquid jet. The experimental investigation utilizes a digital imaging technique to measure resultant drop sizes. Data were collected for liquid Reynolds number between 2,500 and 25,000, aerodynamic Weber number range of 50-500 and ambient gas pressures from 150 to 1200 psia. Comparison of the model predictions and experimental data for drop sizes at gas pressures of 150 and 300 psia reveal satisfactory agreement particularly for lower values of investigated Weber number. The present model is intended as a component of a practical tool to facilitate design and optimization of coaxial shear atomizers.

Ibrahim, Essam A.↗

An Integrated High-Speed Microstructural Characterization Method Using Simultaneous XRD, Stereo-DIC, and PCI

High-speed characterization of the deformation mechanisms in polycrystalline metals requires the quantification of full strain fields and local microstructural evolutions simultaneously. In this paper, we present a novel experimental method to integrate phase-contrast imaging (PCI), stereographic digital image correlation (stereo-DIC), and full-ring X-ray diffraction (XRD) to allow for the simultaneous characterization of polycrystalline metals at 1MHz or higher. A Kolsky bar was integrated into the synchrotron X-ray source in Sector 32 ID-B at the Advance Photon Source (APS) at Argonne National Laboratory. When the sample is dynamically loaded, the diagnostic methods of full-ring XRD, PCI, and stereo-DIC are properly synchronized to record the deformation behavior at both continuum and microstructural scales as a function of the loading history. An advanced high-strength steel (AHSS) is used as a model material to demonstrate the capabilities of this new experimental method.

36 MATERIALS SCIENCE↗

The development and applications of multidimensional biomolecular spectroscopy illustrated by photosynthetic light harvesting

The parallel and synergistic developments of atomic resolution structural information, new spectroscopic methods, their underpinning formalism, and the application of sophisticated theoretical methods have led to a step function change in our understanding of photosynthetic light harvesting, the process by which photosynthetic organisms collect solar energy and supply it to their reaction centers to initiate the chemistry of photosynthesis. The new spectroscopic methods, in particular multidimensional spectroscopies, have enabled a transition from recording rates of processes to focusing on mechanism. We discuss two ultrafast spectroscopies – two-dimensional electronic spectroscopy and two-dimensional electronic-vibrational spectroscopy – and illustrate their development through the lens of photosynthetic light harvesting. Both spectroscopies provide enhanced spectral resolution and, in different ways, reveal pathways of energy flow and coherent oscillations which relate to the quantum mechanical mixing of, for example, electronic excitations (excitons) and nuclear motions. The new types of information present in these spectra provoked the application of sophisticated quantum dynamical theories to describe the temporal evolution of the spectra and provide new questions for experimental investigation. While multidimensional spectroscopies have applications in many other areas of science, we feel that the investigation of photosynthetic light harvesting has had the largest influence on the development of spectroscopic and theoretical methods for the study of quantum dynamics in biology, hence the focus of this review. We conclude with key questions for the next decade of this review.

59 BASIC BIOLOGICAL SCIENCES↗

Kinetic Monte Carlo Framework for Coupled Degradation and Dehydration of Anion Exchange Membranes

Kinetic Monte Carlo (kMC) simulations, augmented with temporal-acceleration schemes, can efficiently handle stiff reaction-transport networks when fast processes rapidly relax to quasi-equilibrium on a fixed lattice. However, in glassy anion-exchange membranes (AEM), rare and irreversible chemical degradation events continuously reshape the nanoscale morphology, and the associated hydration and transport degrees of freedom remain far from a well-defined local equilibrium. This combination of evolving state space and nonequilibrated fast dynamics lies outside the scope of existing kMC acceleration frameworks. Here, to address this challenge, we introduce an auxiliary-particle kinetic Monte Carlo (AP-kMC) scheme. In AP-kMC, short-lived mobile particles spawned at degradation sites execute hop, water-elimination, and decay moves, enforcing rapid local relaxation of the hydration structure while preserving the stochastic rules of kMC. Parameterized with molecular-dynamics morphologies and experimental solution degradation kinetics, AP-kMC reproduces the evolution of ion-exchange capacity, water uptake, and conductivity, and reveals a feedback loop in which poorly hydrated sites degrade first and each degradation event induces further local dehydration. The resulting thinning and fragmentation of water channels cause loss of hydrophilic percolation and abrupt conductivity collapse well before complete charge loss. AP-kMC thus reframes AEM durability as a coupled degradation–drying–percolation problem and provides a transferable strategy to simulate reactive, out-of-equilibrium polymer electrolytes where local solvation controls reactivity.

organic↗

Sculpting 2D Crystals via Membrane Contractions before and during Solidification

When phospholipids crystallize within the otherwise fluid membranes of giant unilamellar vesicles, the resulting molecularly thin “2D” solids exhibit great variety in their morphology evolution. For example, within membranes containing moderate amounts of the crystallizing component, crystals grow with a fixed morphology depending on vesicle size. Conversely for membranes containing large amounts of the crystallizing species, we find small compact crystals on vesicles of all sizes. However, on large vesicles, growing crystals sprout flower petals that lengthen progressively. These behaviors result from two combined mechanisms: first, like other 2D solids, the shear rigidity of phospholipid crystals renders them intolerant to morphologies with nonzero Gaussian curvature. As a result and especially at elevated membrane tension, the cost of bending elasticity is reduced at the expense of line energy by the formation of flowers as opposed to compact crystals. Second, the composition-dependent tension rise during cooling relaxes via water permeation of the membrane with a time constant scaling as R2. The amount of crystal formed for a small decrease in temperature determines this composition-dependent increase in stress from thermal contractions versus solidification. Surface Evolver computations were motivated using the predicted tension evolution to develop a processing space that maps to experimental observations for initial and growing crystal morphology. Important variable groups are identified, including a scaled ratio of bending to line energy, a vesicle-size-independent group for membrane contractions, and a time constant for stress relaxation. Though processing stresses ultimately relax, the crystal morphology persists well beyond the processing window.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Real-Time KMC Simulation of Vacancy-Mediated Intermixing in Au@Ag Octahedral Core–Cubic Shell Nanocrystals with Ab Initio-Guided Kinetics

Utilization of core–shell rather than monometallic nanocrystals (NCs) facilitates fine-tuning of NC properties for applications. However, compositional evolution via intermixing can degrade these properties prompting recent experimental studies. We develop an atomistic-level stochastic model for vacancy-mediated intermixing exploiting a formalism which allows incorporation at an ab initio density functional theory level of not just the thermodynamics of vacancy formation, but also relevant diffusion barriers for a vast number of possible local environments (in the core and in the shell, at the interface, and in the intermixed phase). This facilitates a predictive treatment and comprehensive understanding of intermixing on the relevant time scale (e.g., 10 1 –10 3 s). In contrast, previous modeling at the atomistic level utilized only unrealistic generic prescriptions of barriers or employed simplified continuum treatments. For Au@Ag octahedral core–cubic shell NCs, our modeling not only captures the experimentally observed rate or time scale for intermixing of ~100 s at 450 °C for 60 nm NCs, but also elucidates the underlying rate controlling processes and the effective intermixing barrier.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Continuous operation of a coherent 3,000-qubit system

Neutral atoms are a promising platform for quantum science, enabling advances in areas ranging from quantum simulations and computation to metrology, atomic clocks and quantum networking. Although atom losses typically limit these systems to a pulsed mode, continuous operation could substantially enhance cycle rates, remove bottlenecks in metrology and enable deep-circuit quantum evolution through quantum error correction. Here we demonstrate an experimental architecture for high-rate reloading and continuous operation of a large-scale atom-array system while realizing coherent storage and manipulation of quantum information. Our approach utilizes a series of two optical lattice conveyor belts to transport atom reservoirs into the science region, where atoms are repeatedly extracted into optical tweezers without affecting the coherence of qubits stored nearby. Using a reloading rate of 300,000 atoms in tweezers per second, we create over 30,000 initialized qubits per second, which we leverage to assemble and maintain an array of over 3,000 atoms for more than 2 hours. Furthermore, we demonstrate persistent refilling of the array with atomic qubits in either a spin-polarized or a coherent superposition state while preserving the quantum state of stored qubits. Our results pave the way for the realization of large-scale continuously operated atomic clocks, sensors and fault-tolerant quantum computers.

atomic and molecular physics↗