Measurement of Atomic Oxygen Densities Using TALIF in Dielectric Barrier Discharge: Insights into the effluent of a micro cavity plasma array
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Steuer, David Frithjof↗
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Near-IR Laser Absorption Measurements of Atomic Nitrogen, Oxygen, and Carbon Concentrations in Shock-Heated Air.
Abstract not provided.
Jans, Elijah↗
Oxide– and Silicate–Water Interfaces and Their Roles in Technology and the Environment
Interfacial reactions drive all elemental cycling on Earth and play pivotal roles in human activities such as agriculture, water purification, energy production and storage, environmental contaminant remediation, and nuclear waste repository management. The onset of the 21st century marked the beginning of a more detailed understanding of mineral aqueous interfaces enabled by advances in techniques that use tunable high-flux focused ultrafast laser and X-ray sources to provide near-atomic measurement resolution, as well as by nanofabrication approaches that enable transmission electron microscopy in a liquid cell. This leap into atomic- and nanometer-scale measurements has uncovered scale-dependent phenomena whose reaction thermodynamics, kinetics, and pathways deviate from previous observations made on larger systems. A second key advance is new experimental evidence for what scientists hypothesized but could not test previously, namely, interfacial chemical reactions are frequently driven by “anomalies” or “non-idealities” such as defects, nanoconfinement, and other nontypical chemical structures. Third, progress in computational chemistry has yielded new insights that allow a move beyond simple schematics, leading to a molecular model of these complex interfaces. In combination with surface-sensitive measurements, we have gained knowledge of the interfacial structure and dynamics, including the underlying solid surface and the immediately adjacent water and aqueous ions, enabling a better definition of what constitutes the oxide– and silicate–water interfaces. This critical review discusses how science progresses from understanding ideal solid–water interfaces to more realistic systems, focusing on accomplishments in the last 20 years and identifying challenges and future opportunities for the community to address. Further, we anticipate that the next 20 years will focus on understanding and predicting dynamic transient and reactive structures over greater spatial and temporal ranges as well as systems of greater structural and chemical complexity. Closer collaborations of theoretical and experimental experts across disciplines will continue to be critical to achieving this great aspiration.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Noninvasive mid-circuit measurement and reset on atomic qubits
Mid-circuit measurement and reset of subsets of qubits are crucial ingredients of quantum error correction and many quantum information applications. Measurement of atomic qubits is accomplished through resonant fluorescence, which typically disturbs neighboring atoms due to photon scattering. We propose and prototype a scheme for measurement and reset that provides both spatial and spectral isolation by using tightly focused laser beams and narrow atomic transitions. The unique advantage of this scheme is that all operations are applied exclusively to the read-out qubit, with little overhead and negligible disturbance to the other qubits of the same species. In this paper, we pave the way for noninvasive and high-fidelity mid-circuit measurement and demonstrate all key building blocks on a single trapped barium ion.
atomic systems↗
Non-invasive mid-circuit measurement and reset on atomic qubits
Mid-circuit measurement and reset of subsets of qubits is a crucial ingredient of quantum error correction and many quantum information applications. Measurement of atomic qubits is accomplished through resonant fluorescence, which typically disturbs neighboring atoms due to photon scattering. We propose and prototype a new scheme for measurement that provides both spatial and spectral isolation by using tightly-focused individual laser beams and narrow atomic transitions. The unique advantage of this scheme is that all operations are applied exclusively to the read-out qubit, with negligible disturbance to the other qubits of the same species and little overhead. In this letter, we pave the way for non-invasive and high fidelity mid-circuit measurement and demonstrate all key building blocks on a single trapped barium ion.
Atomic Physics (physics.atom-ph)↗
Molecules Functionalized with Cycling Centers for Quantum Information Science
The ability for a single molecule to produce enough laser-induced fluorescence to control and detect its quantum state is known as optical cycling. This property has been used to great effect in atoms, where the relatively small number of states promotes their ability to repeatedly fluoresce, for applications such as laser cooling, precision measurement, atomic clocks, and quantum information processing. The extension of this capability to molecular species, however, has been difficult, primarily due to their propensity to become vibrationally excited during illumination. This project brought together experts from atomic physics, physical chemistry, and computational quantum chemistry to develop means to create molecules capable of optical cycling. In particular, this program sought to produce an optical cycling center (OCC), a quantum functional group capable of chemical attachment to a wide variety of molecular hosts while retaining (and thereby furnishing to its host) the ability to optically cycle. Following our team’s theoretical identification of promising species, including alkaline-earth phenoxides, we then created these species and in many cases confirmed their optical cycle closure. We now not only know of the existence of a handful of large, molecular species that can be deployed for applications in quantum technologies and measurement, but have improved our knowledge of the molecular mechanisms leading to this discovery, which will enable generalization in the future. The extension of these ideas for informed chemical design of cycling molecules with bespoke properties is now being pursued by multiple groups.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
X-ray diffraction and in situ pressurization of dentine apatite reveals nanocrystal modulus stiffening upon carbonate removal
Bone-like materials comprise carbonated-hydroxyapatite nanocrystals (c-Ap) embedding a fibrillar collagen matrix. The mineral particles stiffen the nanocomposite by tight attachment to the protein fibrils creating a high strength and toughness material. The nanometer dimensions of c-Ap crystals make it very challenging to measure their mechanical properties. Mineral in bony tissues such as dentine contains 2~6 wt.% carbonate with possibly different elastic properties as compared with crystalline hydroxyapatite. Here we determine strain in biogenic apatite nanocrystals by directly measuring atomic deformation in pig dentine before and after removing carbonate. Transmission electron microscopy revealed the platy 3D morphology while atom probe tomography revealed carbon inside the calcium rich domains. High-energy X-ray diffraction in combination with in situ hydrostatic pressurization quantified reversible c-Ap deformations. Additionally, crystal strains differed between annealed and ashed (decarbonated) samples, following 1 or 10 h heating at 250 °C or 550 °C respectively. Measured bulk moduli (K) and a-/c-lattice deformation ratios (η) were used to generate synthetic K syn and ηsyn identifying the most likely elastic constants C 33 and C 13 for c-Ap. These were then used to calculate the nanoparticle elastic moduli. For ashed samples, we find an average E 11 =107 GPa and E 33 =128 GPa corresponding to ~5% and ~17% stiffening of the a-/c-axes of the nanocrystals as compared with the biogenic nanocrystals in annealed samples. Ashed samples exhibit ~10% lower Poisson's ratios as compared with the 0.25~0.36 range of carbonated apatite. Carbonate in c-Ap may therefore serve for tuning local deformability within bony tissues.
36 MATERIALS SCIENCE↗
Local strain-dependent electronic structure and perpendicular magnetic anisotropy of a MnGaN 2D magnetic monolayer
Local strain-dependent spin-polarized electronic structure of a two-dimensional (2D) magnetic layer is an exciting property for practical applications. For example, it holds the promise for advanced ultrathin spintronic nanodevices with customized electronic and magnetic properties by local strain engineering. Here, we demonstrate that the spin-polarized electronic structure of a 2D manganese gallium nitride (MnGaN-2D) magnetic monolayer is sensitive to intrinsic local lattice strain, as proven by first-principles calculations and indicated by scanning tunneling spectroscopy measurements. Atomic resolution images reveal a highly non-Gaussian lattice spacing/strain distribution, while the spectroscopy reveals variations in the electronic density of states. Simulations of the MnGaN-2D monolayer based on first-principles calculations, including both isotropic and anisotropic strains, confirm a highly strain-dependent manganese partial density of states. Spin-orbit coupling is included which indicates either out-of-plane perpendicular magnetic anisotropy (PMA) or in-plane magnetic anisotropy, dependent on the type of strain whether compressive or tensile, suggesting that MnGaN-2D is magnetoelastic. The MnGaN-2D PMA is further supported by superconducting quantum interference device magnetometry measurements which reveal a high spin polarization of ~ 79 % at room temperature.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Tunable Infrared Laser Absorption Spectroscopy of Aluminum Monoxide $A^2\Pi_i $–$X^2\Sigma^+$.
We report the details of an infrared, laser absorption diagnostic capable of quantifying aluminum monoxide temperature and column density at 100 kHz repetition rate. This novel technique employs a near infrared MEMS-VCSEL to measure rotationally resolved optical absorption spectra of aluminum monoxide $A^2\Pi_i$ - $X^2\Sigma^+$ from approximately 7400 –7900 cm -1 . Temperatures and column densities are extracted from model regressions to provide temporally resolved thermochemical information on aluminum oxidation reactions. The measurement capability is demonstrated by performing 100 kHz measurement in the plume of an exploding bridgewire with measured temperatures of 3450–3100 K and column densities of 1– 11 x 10 16 cm -2 . To the authors knowledge, this is the first use of the AlO $A^2\Pi_i$ - $X^2\Sigma^+$ transition to characterize aluminum combustion environments. Details regarding signal extraction and calibration of MEMS-VCSEL spectra are also included. Although unsuccessful, efforts to extract kinetic temperature and column density from simultaneously measured, atomic aluminum 2 P 3/2,1/2 - 2 S 1/2 transitions at 7618 cm -1 and 7602 cm -1 are also described.
47 OTHER INSTRUMENTATION↗
A machine learning photon detection algorithm for coherent x-ray ultrafast fluctuation analysis
X-ray free electron laser experiments have brought unique capabilities and opened new directions in research, such as creating new states of matter or directly measuring atomic motion. One such area is the ability to use finely spaced sets of coherent x-ray pulses to be compared after scattering from a dynamic system at different times. This enables the study of fluctuations in many-body quantum systems at the level of the ultrafast pulse durations, but this method has been limited to a select number of examples and required complex and advanced analytical tools. By applying a new methodology to this problem, we have made qualitative advances in three separate areas that will likely also find application to new fields. As compared to the “droplet-type” models, which typically are used to estimate the photon distributions on pixelated detectors to obtain the coherent x-ray speckle patterns, our algorithm achieves an order of magnitude speedup on CPU hardware and two orders of magnitude improvement on GPU hardware. We also find that it retains accuracy in low-contrast conditions, which is the typical regime for many experiments in structural dynamics. Finally, it can predict photon distributions in high average-intensity applications, a regime which up until now has not been accessible. Our artificial intelligence-assisted algorithm will enable a wider adoption of x-ray coherence spectroscopies, by both automating previously challenging analyses and enabling new experiments that were not otherwise feasible without the developments described in this work.
47 OTHER INSTRUMENTATION↗
Satellites, core hole excitations, and spin-resolved electronic structure in the spectroscopy of half-metallic CrO 2
Photoelectron satellites—the structures appearing on the low kinetic or high binding-energy side of the “main” or “elastic” photopeak—betray the complex many-body interactions set in motion by the sudden creation of the core hole. In this work, we demonstrate, using the technologically important ferromagnetic half-metal CrO 2 , how such satellites can manifest themselves in other core-level spectroscopies of the material and how they can reveal important details pertinent to its electronic structure. Specifically, we identify a fluorescence satellite in the Cr 𝐿 3 resonant x-ray-emission spectra that radiates at a constant emission energy across the Cr 𝐿 3 x-ray edge with energy ≈1.3 eV above the ordinary valence fluorescence. Here, we provide evidence that this feature arises from the valence recombination of the Cr 2𝑝 core hole “dressed” by the same shakeup charge-transfer process present in both the Cr x-ray photoelectron and the Cr x-ray absorption spectra with its energy uniquely measuring the exchange splitting of the Cr 3𝑑 level. Further analysis of the x-ray emission data reveals three additional features that radiate at constant loss energy that are attributed to combinations of Cr 3𝑑(𝑡 2𝑔 ) → Cr 3𝑑(𝑡 2𝑔 ), charge-transfer O 2𝑝→Cr 3𝑑, and crystal-field Cr 3𝑑(𝑡 2𝑔 )→Cr 3𝑑(𝑒 𝑔 ) excitations. These assignments and their energies are supported by density-functional theory calculations, the accuracy of which we demonstrate by hard x-ray valence-photoemission measurements. Atomic multiplet calculations, which include crystal-field effects, help interpret x-ray photoelectron and x-ray absorption spectra of the covalently mixed Cr ion. Resonant Cr K-𝐿 2,3 𝐿 2,3 Auger-electron emission spectra support a ligand-to-metal nature of the charge-transfer process while highlighting the charge sensitivity differences between photon-in/electron-out and photon-in/photon-out spectroscopies.
36 MATERIALS SCIENCE↗
Growth of ultrathin Bi 2 Se 3 films by molecular beam epitaxy
Bi 2 Se 3 is a widely studied 3D topological insulator having potential applications in optics, electronics, and spintronics. When the thickness of these films decreases to less than approximately 6 nm, the top and bottom surface states couple, resulting in the opening of a small gap at the Dirac point. In the 2D limit, Bi 2 Se 3 may exhibit quantum spin Hall states. However, growing coalesced ultrathin Bi 2 Se 3 films with a controllable thickness and typical triangular domain morphology in the few nanometer range is challenging. Here, we explore the growth of Bi 2 Se 3 films having thicknesses down to 4 nm on sapphire substrates using molecular beam epitaxy that were then characterized with Hall measurements, atomic force microscopy, and Raman imaging. We find that substrate pretreatment—growing and decomposing a few layers of Bi 2 Se 3 before the actual deposition—is critical to obtaining a completely coalesced film. In addition, higher growth rates and lower substrate temperatures led to improvement in surface roughness, in contrast to what is observed for conventional epitaxy. Altogether, coalesced ultrathin Bi 2 Se 3 films with lower surface roughness enable thickness-dependent studies across the transition from a 3D-topological insulator to one with gapped surface states in the 2D regime.
36 MATERIALS SCIENCE↗
Dark Sector Physics at High-Intensity Experiments
Is Dark Matter part of a Dark Sector? The possibility of a dark sector neutral under Standard Model (SM) forces furnishes an attractive explanation for the existence of Dark Matter (DM), and is a compelling new-physics direction to explore in its own right, with potential relevance to fundamental questions as varied as neutrino masses, the hierarchy problem, and the Universe's matter-antimatter asymmetry. Because dark sectors are generically weakly coupled to ordinary matter, and because they can naturally have MeV-to-GeV masses and respect the symmetries of the SM, they are only mildly constrained by high-energy collider data and precision atomic measurements. Yet upcoming and proposed intensity-frontier experiments will offer an unprecedented window into the physics of dark sectors, highlighted as a Priority Research Direction in the 2018 Dark Matter New Initiatives (DMNI) BRN report. Support for this program -- in the form of dark-sector analyses at multi-purpose experiments, realization of the intensity-frontier experiments receiving DMNI funds, an expansion of DMNI support to explore the full breadth of DM and visible final-state signatures (especially long-lived particles) called for in the BRN report, and support for a robust dark-sector theory effort -- will enable comprehensive exploration of low-mass thermal DM milestones, and greatly enhance the potential of intensity-frontier experiments to discover dark-sector particles decaying back to SM particles.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
A diagnostic to measure neutral-atom density in fusion-research plasmas
For this study, a femtosecond two-photon-absorption laser-induced-fluorescence (TALIF) diagnostic was designed, installed, and operated on the Princeton-Field-Reversed Configuration-2 device to provide non-invasive measurements of the time and spatially resolved neutral-atom densities in its plasmas. Calibration of the H o density was accomplished by comparison with Kr TALIF. Measurements on plasmas formed of either H 2 or Kr fill gases allowed examination of nominally long and short ionization mean-free-path regimes. With multi-kW plasma heating and H 2 fill gas, a spatially uniform H o density of order 10 17 m –3 was measured with better than ±2 mm and 10 µs resolution. Under similar plasma conditions but with Kr fill gas, a 3-fold decrease in the in-plasma Kr density was observed.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Absolute atomic hydrogen density measurements in an atmospheric pressure plasma jet: generation, transport and recombination from the active discharge region to the effluent
Atomic hydrogen (H) generated by atmospheric pressure radio frequency (RF) plasma jet is investigated by two-photon absorption laser induced fluorescence in a He-H 2 mixture. The reported time and spatially resolved H density profiles enable a detailed analysis of the species generation, transport and decay along the axis of symmetry of the jet. Here, the H density distribution for a continuous RF plasma jet corresponds well with the outcome of a Pseudo-1D plug flow model. In addition, RF power modulation has a strong effect on the H density in the active discharge region but has a negligible effect on the H density in the far effluent.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Absolute Reactive Oxygen Species Densities in the Effluent of the COST Reference Source and Plasma-generated Atomic Oxygen Density Measurements in Liquid using TALIF
Reactive oxygen species are one of the most important species produced in a plasma. In particular the role of atomic oxygen and the hydroxyl radical OH has attracted many studies ranging from plasma medicine to plasma-driven biocatalysis and water treatment. Atomic oxygen and the hydroxyl radical OH are very reactive and react unselectively with many different substrates. The quantification of atomic oxygen and OH is challenging because of their reactivity and unknown reactions and rate constants.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Dynamic STEM-EELS for single-atom and defect measurement during electron beam transformations
This study introduces the integration of dynamic computer vision–enabled imaging with electron energy loss spectroscopy (EELS) in scanning transmission electron microscopy (STEM). This approach involves real-time discovery and analysis of atomic structures as they form, allowing us to observe the evolution of material properties at the atomic level, capturing transient states traditional techniques often miss. Rapid object detection and action system enhances the efficiency and accuracy of STEM-EELS by autonomously identifying and targeting only areas of interest. This machine learning (ML)–based approach differs from classical ML in that it must be executed on the fly, not using static data. We apply this technology to V-doped MoS 2 , uncovering insights into defect formation and evolution under electron beam exposure. This approach opens uncharted avenues for exploring and characterizing materials in dynamic states, offering a pathway to increase our understanding of dynamic phenomena in materials under thermal, chemical, and beam stimuli.
47 OTHER INSTRUMENTATION↗
Reconstruction of high-resolution atomic force microscopy measurements from fast-scan data using a Noise2Noise algorithm
Not Available
47 OTHER INSTRUMENTATION↗