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We demonstrate similarity rules for inductively coupled plasmas with thermohydrodynamic coupling effects using two-dimensional fluid simulations and theoretical analyses of the gas flow and heat transfer equations. The results confirm the validity of conventional similarity laws, e.g., the similarity relation for electron density, which can be violated by the nonlinear gas heating effects from exothermic and endothermic reactions. The nonlinear gas heating can obviously perturb the invariance of spatial distributions of the gas flow velocity, resulting in the electron density decreasing nonproportionally with different scaling factors. Adding an external heat source can mitigate the violation of the gas temperature scaling law, thus maintaining the validity of similarity relations to some extent. In addition, two kinds of scaling relations for excited-state argon atoms are identified with and without the consideration of nonlinear collisions. [ABSTRACT FROM AUTHOR]

We demonstrate similarity-based scaling networks for capacitive radio frequency (RF) plasmas, which extensively correlate discharge characteristics under varied conditions, incorporating the transition from original to similarity states. Based on fully kinetic particle-in-cell simulations, similar RF discharges in argon are demonstrated with three external control parameters (gas pressure, gap distance, and driving frequency) simultaneously tuned. A complete set of scaling pathways regarding fundamental discharge parameters is obtained, from which each plasma state finds its neighboring node with only one control parameter tuned. The results from this study provide a promising strategy for plasma multi-parameter mapping, enabling effective cross-comparisons, prediction, and manipulation of RF discharge plasmas. [ABSTRACT FROM AUTHOR]

Resonance mechanisms have been found to be essential for the generation of high-density rf plasmas at low pressures, in which electrons can be continuously accelerated through multiple interactions with the oscillating rf sheaths. In this work, we report the scale-invariant resonance mechanisms, such as bounce resonance heating and plasma series resonance, in low-pressure capacitive rf plasmas in the presence of an external magnetic field. The generation conditions for the resonance mechanisms are determined via fully kinetic simulations. It is found that the resonance dynamical properties of single-frequency plasmas (e.g., a double-peak electron density vs magnetic field curve) can be exactly replicated at different scales when three combined control parameters, i.e., the reduced gap distance pd (pressure × distance), reduced driving frequency f/p (frequency divided by pressure), and reduced magnetic field B/p (magnetic field divided by pressure), are kept constant. The similarity relations for the electron density and electron power absorption in magnetized rf plasmas are numerically confirmed. Furthermore, the similarity and scale-invariant resonance characteristics are elucidated through the scaling of the Boltzmann equation with collisional terms for weakly ionized rf plasmas with a magnetic field, which is proven to be theoretically exact. [ABSTRACT FROM AUTHOR]

Both direct and indirect drive concepts of inertial confinement fusion rely on targets with cryogenic thermonuclear fuel shells for ignition. Experiments on the Shenguang-III prototype laser facility using laser-driven gas-filled hohlraums show distinct differences between cryogenic (20 K) and warm hohlraums. Although the measured x-ray flux in the photon range from 1.6 to 4.4 keV (Au M-band) is identical between cryogenic and warm hohlraums, the cryogenic hohlraum has a much slower rate of rise and is 20% lower in peak intensity of x-ray flux in the photon range from 0.1 to 4 keV. The reasons for this drive deficit between cryogenic and warm hohlraums are investigated using a similar series of hohlraum experiments. The experiments employ three types of hohlraums to distinguish the effect of a shroud window membrane and condensates. Warm hohlraums with a shroud window membrane replicate the slower rate of rise of radiation flux of cryogenic targets. When the shroud window is present, the measured x-ray flux in the hohlraum shows a drive deficit that decreases with time. However, the measured deficit increases as the viewing angle increases. All of these results indicate that the portion of the shroud not illuminated by the lasers absorbs the outgoing x-ray flux from the hohlraum. [ABSTRACT FROM AUTHOR]

A Ce atom reaction with propene is carried out in a pulsed laser vaporization molecule beam source. Several Ce–hydrocarbon species formed by the C—H and C—C bond activation of propene are observed by time-of-flight mass spectrometry, and Ce(C3Hn) (n = 4 and 6) are characterized by mass-analyzed threshold ionization (MATI) spectroscopy and density functional theory, multiconfiguration, and relativistic quantum chemical calculations. The MATI spectrum of each species consists of two vibronic band systems, each with several vibronic bands. Ce(C3H6) is identified as an inserted species with Ce inserting into an allylic C—H bond of propene and Ce(C3H4) as a metallocycle through 1,2-vinylic dehydrogenation. Both species have a Cs structure with the Ce 4f16s1 ground valence electron configuration in the neutral molecule and the Ce 4f1 configuration in the singly charged ion. The two vibronic band systems observed for each species are attributed to the ionization of two pairs of the lowest spin–orbit coupled states with each pair being nearly degenerate. [ABSTRACT FROM AUTHOR]

Although lithium-sulfur (Li-S) batteries are widely regarded as one of the most promising next-generation high energy density storage systems, their large-scale applications are seriously impeded by rapid capacity fading and poor Coulombic efficiency owing to the shuttling of lithium polysulfides (LiPSs) and irreversible discharge product Li2S. Here, by means of first principles calculations, we studied defective black phosphorene (BP) as a host material to realize high-performance Li-S batteries, including Stone Wales [SW(55-77)], single, and double vacancy [SV(5-9) and DV(5-9-5)] defects. Our results demonstrate that while BP has moderate adsorption energies towards LiPSs, the presence of defects could enhance the adsorption strength between LiPSs and BP because of increased charge transfer. Particularly, defective BP could strike a good balance between adsorption energy and integrity of LiPSs, which is beneficial to prevent the shuttling of LiPSs. Moreover, during the lithiation process, defective BP not only has narrow bandgaps but also decreases the dissociation energy of Li2S, facilitating the catalytic oxidation of Li2S back to sulfur. Therefore, it is highly desirable to fabricate defective BP to improve the reversible capacity and cycle stability of Li-S batteries. [ABSTRACT FROM AUTHOR]

To investigate the decomposition law of SF6 under negative direct current partial discharge (PD) at different energies, a SF6 PD hybrid numerical model based on fluid dynamics and plasma chemical reaction models, in which 14 particle species and 24 chemical reactions are considered, is proposed. The effectiveness of the proposed model is validated with the current pulse waveform and the V–I discharge curve obtained by experiment. The influence of discharge energy on SF6 PD characteristic quantities and SF6 decomposition products is investigated with simulation and experiment. The results show that most of the discharge area of SF6 is neutral, and the cation clouds only exist in the ionosphere (4.79–5 mm). With the increase in applied voltage, the electric field intensity of the needle plate gap does not increase completely and even decreases in some areas. Moreover, different from the traditional opinion, the generation of SO2F2 under PD is mainly generated by the hydrolysis reaction of SOF4, which is formed by [SF5], [SF4], and [OH], [O]. The reaction path of [SF2] with O2 is not important. Thus, c(SO2F2)/c(SOF2 + SO2) can be used as the energy characteristic component ratio because of its ability to represent the low-fluorine sulfide ratio n([SF5])/n([SF4]). [ABSTRACT FROM AUTHOR]

The generic problem of low-frequency acoustic radiation through quiescent air from a circular pipe that is inclined with respect to its exit flange is studied in this work. The exit flange is taken to extend as an infinite plane away from the pipe opening. The analysis implements a hybrid method that combines modal expansions with the boundary element method. The reflection coefficient and pipe end correction for Helmholtz numbers (based on the pipe radius) less than 2.5 are calculated for various inclination angles up to 75°. Calculations are validated using simulations from the finite-element solver of the commercial software package COMSOL. The reflection coefficient and end correction predictions agree closely with the validation simulations yet differ notably from the results available in the literature. The solution obtained from the hybrid method is subsequently used to analyse the acoustic field at the pipe exit and in the downstream space. The key aspects of the governing physics pertaining to practical engineering applications at low frequencies are captured in a low-order approximation, which significantly reduces the degrees of freedom of the problem and provides generally good estimates of the reflection coefficient and end correction, as well as the downstream acoustic field. [ABSTRACT FROM AUTHOR]

In order to study the laser plasma instabilities (LPIs) in the context of some novel six-side laser-driven indirect designs like the six-cylinder-port hohlraum and the three-axis cylindrical hohlraum, where the laser beams inject in hohlraum with a large angle. LPI experiments in cylindrical hohlraum with only outer beams were designed and performed based on the current laser arrangement condition of SGIII laser facility for the first time. Stimulated Brillouin backscatter (SBS) was found to be the dominant instability with high instantaneous reflectivity in experiments. A typical feature was obtained in the time-resolved spectra of SBS, which maintained similar for different laser intensities of the interaction beam. The experimental data are analyzed by the hydrodynamic simulations combined with HLIP code, which is based on the ray-tracing model. By analysis of experimental data, it is argued that the mixture of gas and Au in the region of their interface is important to SBS, which indicates the need for the mixture model between the filled gas and the high Z plasma from hohlraum wall in the hydrodynamic simulations. Nonlinear saturation of SBS as well as the smoothed beam are also discussed here. Our effective considerations of the ions pervasion effect and the smoothed beam provide utilitarian ways for improvement of the current ray-tracing method. [ABSTRACT FROM AUTHOR]

In the present work, we report exploitation of spatial symmetry in calculations of ground state energy and analytic first derivatives of closed-shell molecules based on our previously developed coupled-cluster (CC) approach with spin-orbit coupling. Both time-reversal symmetry and spatial symmetry for D2h and its subgroups are exploited in the implementation. The symmetry of a certain spin case for the amplitude, intermediate, or density matrix is determined by the symmetry of the corresponding spin functions and the direct product decomposition method is employed in computations involving these quantities. The reduction in computational effort achieved through the use of spatial symmetry is larger than the order of the molecular single point group. Symmetry exploitation renders application of the CC approaches with spin-orbit coupling to larger closed-shell molecules containing heavy elements with high accuracy. [ABSTRACT FROM AUTHOR]

Metal-pyridine (metal=Li, Ca, and Sc) complexes are produced inlaser-vaporization molecular beams and studied by pulsed-field-ionization zero-electron-kinetic-energy (ZEKE) spectroscopy and theoretical calculations. Both σ and π structures are considered for the three complexes by theory, and preferred structures are determined by the combination of the ZEKE spectra and calculations. The Li and Ca complexes prefer a σ bonding mode, whereas the Sc complex favors a π mode. Adiabatic ionization energies and metal-ligand vibrational frequencies are determined from the ZEKE spectra. Metal-ligand bond dissociation energies of the neutral complexes are obtained from a thermodynamic cycle. The ionization energies follow the trend of Li-pyridine (32 460 cm-1)≤Ca-pyridine(39 043 cm-1)≤Sc-pyridine(42 816 cm-1), whereas the bond energies are in the order of Ca-pyridine (27.0 kJ mol-1)≤Li-pyridine(49.1 kJ mol-1)≤Sc-pyridine(110.6 kJ mol-1). The different bonding modes between the main group metals and transition element are discussed in terms of Sc 3d orbital involvement. The bond energy differences between the Li and Ca metals are explained by the number of valence s electrons and the size of the metal atoms. [ABSTRACT FROM AUTHOR]

Vibrational frequencies of three niobium normal modes of triniobium dicarbide neutral and cation have been determined from pulsed field ionization-zero electron kinetic energy photoelectron spectra. The niobium stretching mode has a frequency of 326 cm[SUP-1]in the neutral and 339 cm[SUP-1]in the ion. The two deformation modes have frequencies of 238 and 82 cm[SUP-1]in the neutral and a degenerate frequency of 258 cm[SUP-1]in the ion. The geometry of the triniobium dicarbide has been established by comparing the experimental spectra with theoretical calculations. The cluster has a trigonal bipyramid geometry with carbon atoms capping on each face of the metal frame. The cation cluster has D[SUB3h] symmetry whereas the neutral cluster has lower symmetry resulting from a Jahn-Teller distortion. A second low-lying structure with doubly bridging carbon atoms has been identified by the calculations but has not yet been observed. [ABSTRACT FROM AUTHOR]

The geometrical structures of the ground states of triniobium monoxide, Nb3O, and its cation, Nb3O+, have been determined by an experimental and theoretical study. Vibrationally resolved photoelectron spectra of an Nb3O cluster beam were obtained at 100 and 300 K using the pulsed field ionization-zero electron kinetic energy technique. The spectra were simulated by calculating multidimensional Franck–Condon factors using the geometries and harmonic vibrational frequencies obtained from density functional theory for the minimum energy structures of the ion and neutral molecule. The rather remarkable agreement between the experiment and the simulated spectra establishes that Nb3O and Nb3O+ have planar C2v structures with the oxygen atom bridging two niobium atoms. These are the most complex transition metal cluster structures to date to be characterized by gas phase spectroscopic techniques. © 1995 American Institute of Physics. [ABSTRACT FROM AUTHOR]

The technique of pulsed-field-ionization zero-kinetic-energy (PFI-ZEKE), photoelectron spectroscopy was employed to probe the electronic structure of the V+2 cation. Rotationally resolved PFI-ZEKE spectra of the V+2 ground state were obtained by two color excitation via the 700 nm A 3Πu←X 3Σ-g system. The observation of transitions from the A 3Π2u state to two spin–orbit components with Ω=1/2 and Ω=3/2, confirms that the cation ground state has 4Σg- symmetry, in accordance with previous experimental and theoretical work. Striking differences were observed in the rotational selection rules for the 4Σg-←A 3Π1u and the 4Σg-←A 3Π2u transitions. The adiabatic ionization potential of V2 was determined to be 51 271.14(50) cm-1. From an analysis of the rotational structure of the PFI-ZEKE spectra, the following molecular constants were determined for the 4Σg- state: r0=1.7347(24) Å, second order spin–orbit splitting, λ=5.248(17) cm-1, spin–rotation constant, γ=0.0097(87) cm-1, T0=51 282.20(50) cm-1 (1σ error bounds). © 1995 American Institute of Physics. [ABSTRACT FROM AUTHOR]

Although it plays a critical role in the photophysics and catalysis of lanthanides, spin–orbit coupling of electrons on individual lanthanide atoms in small clusters is not well understood. The major objective of this work is to probe such coupling of the praseodymium (Pr) 4f and 6s electrons in Pr2O2 and Pr2O2+. The approach combines mass-analyzed threshold ionization spectroscopy and spin–orbit multiconfiguration second-order quasi-degenerate perturbation theory. The energies of six ionization transitions are precisely measured; the adiabatic ionization energy of the neutral cluster is 38 045 (5) cm−1. Most of the electronic states involved in these transitions are identified as spin–orbit coupled states consisting of two or more electron spins. The electron configurations of these states are 4f46s2 for the neutral cluster and 4f46s for the singly charged cation, both in planar rhombus-type structures. The spin–orbit splitting due to the coupling of the electrons on the separate Pr atoms is on the order of hundreds of wavenumbers. [ABSTRACT FROM AUTHOR]

Metal-mediated N–H and C–H bond activation of aliphatic amines is an effective strategy for synthesizing biologically important molecules. Ln (Ln = La and Ce) atom reactions with dimethylamine are carried out in a pulsed-laser vaporization supersonic molecular beam source. A series of dehydrogenation species are observed with time-of-flight mass spectrometry, and the dehydrogenated Ln-containing species in the formula Ln(CH2NCH3) are characterized by single-photon mass-analyzed threshold ionization (MATI) spectroscopy and quantum chemical calculations. The theoretical calculations include density functional theory for both Ln species and multiconfiguration self-consistent field and quasi-degenerate perturbation theory for the Ce species. The MATI spectrum of La(CH2NCH3) consists of a single vibronic band system, which is assigned to the ionization of the doublet ground state of N-methyl-lanthanaaziridine. The MATI spectrum of Ce(CH2NCH3) displays two vibronic band systems, which are attributed to the ionization of two-pair lowest-energy spin–orbit coupling states of N-methyl-ceraaziridine. Both metallaaziridines are three-membered metallacycles and formed by the thermodynamically and kinetically favorable concerted dehydrogenation of the amino group and one of the methyl groups. [ABSTRACT FROM AUTHOR]

The local structure of La[SUB0.7]Ca[SUB0.3-x]Ba[SUBx]MnO[SUB3] (x = 0; 0.03; 0.06;...; and 0.3) lanthanum manganites were studied by extended x-ray absorption fine structure analysis. Dispersion, σ[SUP2][SUBMn-O], and asymmetry, σ[SUP3][SUBMn-O], of the pair distribution function for the Mn-O bond distances of MnO[SUB6] octahedron showed a maximum on x dependence. The maximum of σ[SUP2][SUBMn-O] is caused by an increase of dynamic displacements of the Mn-O bond distances near the Curie temperature, T[SUBC]. The observed x dependence of σ[SUP3][SUBMn-O] is caused by a reduction in mobility of the charge carriers approaching T[SUBC] from low as well as high temperatures. [ABSTRACT FROM AUTHOR]

There are several methods for treating aortic stenosis including transcatheter valve implantation (TAVI) and surgical aortic valve replacement. Among these, TAVI is highly recommended for elderly patients with high surgical risk or a life expectancy of less than 10 yr. However, recent research findings indicate that thrombosis after TAVI leads to the malfunction of TAVI leaflets, which increases the risk of stroke and heart attack. Since the mechanism of thrombus formation is unclear, this study aimed to investigate the sinus hemodynamics after TAVI in different configurations using particle image velocimetry. The results showed that compared with SAV, the TAV resulted in a relatively low velocity at the sinus owing to the native leaflet and skirt of the TAV. The native leaflet length, covering over 75% of TAV, significantly increased the flow stasis and particle residence. In addition, a larger sinus diameter corresponded to a larger stasis area of the same length as that of the native leaflet. According to this study, patients with long native leaflets in their aortic sinus are at a higher risk of developing thrombosis and may require a higher deployment during treatment. [ABSTRACT FROM AUTHOR]

Hybrid organic–inorganic perovskite (HOIP) materials have attracted significant attention in photovoltaics, light emission, photodetection, etc. Based on the prototype metal halide perovskite crystal, there is a huge space for tuning the composition and crystal structure of this material, which would provide great potential to render multiple physical properties beyond the ongoing emphasis on the optoelectronic property. Recently, the two-dimensional (2D) HOIPs have emerged as a potential candidate for a new class of ferroelectrics with high Curie temperature and spontaneous polarization. Room-temperature solution-processability further makes HOIP a promising alternative to traditional oxide ferroelectrics such as BaTiO3 and PbTiO3. In this perspective, we focus on the molecular aspects of 2D HOIPs, their correlation with macroscopic properties, as well as the material design rules assisted by advanced simulation tools (e.g., machine learning and atomistic modeling techniques). The perspective provides a comprehensive discussion on the structural origin of ferroelectricity, current progress in the design of new materials, and potential opportunities and challenges with emerging materials. We expect that this perspective will provide inspiration for innovation in 2D HOIP ferroelectrics. [ABSTRACT FROM AUTHOR]

Ln (Ln = La and Ce) atom reactions with methylamine are carried out in a pulsed-laser vaporization supersonic molecular beam source. A series of dehydrogenation species are observed with time-of-flight mass spectrometry, and the dehydrogenated Ln-containing species in the formula Ln(NCH3) are characterized by mass-analyzed threshold ionization (MATI) spectroscopy and density functional theory and multiconfiguration spin–orbit coupling computations. The MATI spectrum of La(NCH3) consists of two vibronic band systems that are assigned to the ionization of the 2A1 ground state of the C3v isomer La(N–CH3) and the 2A′ ground state of the Cs isomer La(NH–CH2). The MATI spectrum of Ce(NCH3) also displays two band systems, which are attributed to the ionization of the low-energy spin–orbit coupling states of the C3v isomer Ce(N–CH3). Ln(N–CH3) is formed by the concerted dehydrogenation of the amino group, while La(NH–CH2) is formed by the dehydrogenation of both amino and methyl groups. Ce(NH–CH2) is presumably formed in the reaction based on the computational predictions but not observed by the spectroscopic measurements. [ABSTRACT FROM AUTHOR]

Ce atom reactions with ethylene, 2-butene, and isobutene are carried out in a pulsed laser vaporization molecule beam source. Ce-containing species are observed with time-of-flight mass spectrometry, and Ce(C4H6) is characterized with mass-analyzed threshold ionization (MATI) spectroscopy and relativistic quantum chemical calculations. Two structural isomers are identified for Ce(C4H6): one is the tetrahedronlike Ce[C(CH2)3] in C3v symmetry and the other is the five-membered metallocyclic Ce(CH2CHCHCH2) in Cs. The MATI spectrum of the C3v isomer exhibits two vibronic band systems separated by 88 cm−1, while that of the Cs isomer displays three split by 60 and 101 cm−1. The multiple band systems are attributed to spin-orbit splitting and vibronic transitions involving metal-hydrocarbon and hydrocarbon-based vibrations. The splitting in the C3v isomer arises from interactions of two triplet and two singlet states at the lowest energies, while each splitting in the Cs isomer involves two triplets and a singlet. Although the Ce atom has ground electron configuration 4f15d16s2, Ce valence electron configurations in both isomers are 4f16s1 in the neutral ground state and 4f1 in the ion. The remaining Ce 5d electrons in the isolated atom are spin paired in molecular orbitals that are a bonding combination between Ce 5dπ and hydrocarbon π* orbitals. [ABSTRACT FROM AUTHOR]

In recent years, there have been reports of gas leakage accidents during the transportation of gas tankers in tunnels, potentially leading to destructive explosions. However, the overall distribution of gas concentration in the entire tunnel has not been experimentally investigated. This study presents a series of brine-water experiments to explore the characteristics of buoyant gas flow in tunnel leakage accidents. The gas distribution is categorized into a stably stratified longitudinal current and a source region. Gas concentration in the tunnel is correlated with the dimensionless reduced gravity, which increases with the source buoyancy flux but decreases with the source release velocity. A model is proposed to estimate the maximum gas concentration of the longitudinal current. The spatial range of the explosive region is influenced by the source buoyancy flux and the leakage velocity. However, the propagation velocity of the longitudinal current is primarily controlled by the source buoyancy flux, with the source momentum having a negligible effect. The thickness of the longitudinal gas flow, δ, linearly decreases from the source region to the tunnel ends. A dimensionless parameter, λ, is introduced to characterize δ. When λ < 1.25, δ rapidly increases with λ and then remains approximately constant when λ exceeds 1.25. This study contributes to a better understanding of buoyant gas flow in tunnel leakage accidents. [ABSTRACT FROM AUTHOR]

Ln (Ln = La and Ce) atom reactions with ammonia are carried out in a pulsed laser vaporization supersonic molecular beam source. Lanthanide-containing species are observed with time-of-flight mass spectrometry, and LnNH molecules are characterized by mass-analyzed threshold ionization (MATI) spectroscopy and quantum chemical calculations. The theoretical calculations include density functional theory for both Ln species and a scalar relativity correction, electron correlation, and spin-orbit coupling for the Ce species. The MATI spectrum of LaNH exhibits a single vibronic band system with a strong origin band and two weak vibronic progressions, whereas the spectrum of CeNH displays two band systems separated by 75 cm−1 with each being like the LaNH spectrum. By comparing with the theoretical calculations, both LaNH and CeNH are identified as linear molecules with C∞v symmetry, and the two vibronic progressions are attributed to the excitations of Ln–N stretching and Ln–N–H bending modes in the ions. The additional band system observed for CeNH is due to the spin-orbit splitting from the interactions of triplet and singlet states. The ground valence electron configurations of LaNH and CeNH are La 6s1 and Ce 4f16s1, and the ionization of each species removes the Ln 6s1 electron. The remaining two electrons that are associated with the isolated Ln atoms or ions are in a doubly degenerate molecular orbital that is a bonding combination between Ln 5dπ and N pπ orbitals. [ABSTRACT FROM AUTHOR]

La atom reaction with isoprene is carried out in a laser-vaporization molecular beam source. The reaction yields an adduct as the major product and C—C cleaved and dehydrogenated species as the minor ones. La(C5H8), La(C2H2), and La(C3H4) are characterized with mass-analyzed threshold ionization (MATI) spectroscopy and quantum chemical computations. The MATI spectra of all three species exhibit a strong origin band and several weak vibronic bands corresponding to La-ligand stretch and ligand-based bend excitations. La(C5H8) is a five-membered metallacycle, whereas La(C2H2) and La(C3H4) are three-membered rings. All three metallacycles prefer a doublet ground state with a La 6s1-based valence electron configuration and a singlet ion. The five-membered metallacycle is formed through La addition and isoprene isomerization, whereas the two three-membered rings are produced by La addition and insertion, hydrogen migration, and carbon-carbon bond cleavage. [ABSTRACT FROM AUTHOR]

Streak camera is widely used in continuous time diagnostics in fast physical process. To produce accurate result, it requires delicate calibration and a reliable analysis method. High quality sweep-rate data with uncertainty smaller than 0.5% are obtained over the full record area by a constrained fitting method of peak position measurement, with a short pulse laser and an etalon as the fiducial source. The temporal response is linearized by this full-screen sweep-rate data, which eliminates errors in measurement due to nonlinearity and space-distortion inherent in streak camera. [ABSTRACT FROM AUTHOR]

The precise ionization energy of praseodymium oxide (PrO) seeded in supersonic molecular beams is measured with mass-analyzed threshold ionization (MATI) spectroscopy. A total of 33 spin–orbit (SO) states of PrO and 23 SO states of PrO+ are predicted by second-order multiconfigurational quasi-degenerate perturbation (MCQDPT2) theory. Electronic transitions from four low-energy SO levels of the neutral molecule to the ground state of the singly charged cation are identified by combining the MATI spectroscopic measurements with the MCQDPT2 calculations. The precise ionization energy is used to reassess the ionization energies and the reaction enthalpies of the Pr + O → PrO+ + e− chemi-ionization reaction reported in the literature. An empirical formula that uses atomic electronic parameters is proposed to predict the ionization energies of lanthanide monoxides, and the empirical calculations match well with available precise experimental measurements. [ABSTRACT FROM AUTHOR]

Four-dimensional flow magnetic resonance imaging (4D flow MRI) offers a powerful tool for visualizing fluid flows, critical for both diagnosing cardiovascular diseases and analyzing engineering fluid dynamics. Despite its potential in medical research, the clinical applicability of 4D flow MRI often faces challenges due to inherent noise. To mitigate this, we introduce the split-and-overlap singular value decomposition (SOSVD) filter, a distinctive noise reduction approach. Unlike traditional singular value decomposition methods, the SOSVD filter partitions the primary data matrix into overlapping subdomains and then applies singular value decomposition to each subdomain, preserving only the dominant mode for noise attenuation. Evaluations on simulated and experimental flow data within a square duct revealed a significant decrease in root mean square noise metrics. Moreover, when applied to in vivo aortic data, the SOSVD filter enhanced various flow determinants, including divergence, velocity gradients, streamlines, and velocity coherence. Thus, the SOSVD method presents a promising avenue for augmenting noise reduction in 4D flow MRI, potentially elevating diagnostic accuracy and enriching cardiovascular disease research. [ABSTRACT FROM AUTHOR]

The structural and bonding properties of the Pt2C2n− (n = 1–3) complexes have been investigated by mass-selected photoelectron velocity-map imaging spectroscopy with quantum chemical calculations. The adiabatic detachment energies and vertical detachment energies of Pt2C2n− have been obtained from the measured photoelectron imaging spectra. Theoretical results indicate that the lowest-energy isomers of Pt2C2n− (n = 1–3) possess linear chain-shaped configurations. The binding motif in the most stable isomer of Pt2C2− has a linear cumulenic structure with a Pt=C=C=Pt configuration, and the structural characteristic persists up to all the lowest-energy isomers of the Pt2C4− and Pt2C6− anions. The chemical bonding analyses indicate that the Pt2C2n− (n = 1–3) complexes have multicenter two-electron characteristics. [ABSTRACT FROM AUTHOR]

Vibronic spectra of lutetium oxide (LuO) seeded in supersonic molecule beams are investigated with mass-analyzed threshold ionization (MATI) spectroscopy and second-order multiconfigurational quasi-degenerate perturbation (MCQDPT2) theory. Six states of LuO and four states of LuO+ are located by the MCQDPT2 calculations, and an a3Π(LuO+) ← C2Σ+ (LuΟ) transition is observed by the MATI measurement. The vibronic spectra show abnormal vibrational intervals for both the neural and cation excited states, and the abnormality is attributed to vibrational perturbations induced by interactions with neighboring states. [ABSTRACT FROM AUTHOR]

Ultraprecise fabrication of three-dimensional (3D) microstructures comes up to be one of the most important issues in two-photon induced photopolymerization. To date, it has been difficult to fabricate 3D microstructures without any deformation due to the surface tension between a rinsing material and solidified microstructures during the developing process: In general, the surface tension significantly affects the precision of the resulting 3D microstructures. To overcome this problem, the authors propose a simple and effective laser scanning method to reinforce the strength of 3D microstructures without loss of precision. Overall, a complex 3D artistic sculpture such as “The Thinker” was reproduced in the controlled ultraprecise form, which shows that the proposed method enables the fabrication of 3D patterns with dramatically improved precision and stability. [ABSTRACT FROM AUTHOR]

Ultraprecise fabrication of three-dimensional (3D) microstructures comes up to be one of the most important issues in two-photon induced photopolymerization. To date, it has been difficult to fabricate 3D microstructures without any deformation due to the surface tension between a rinsing material and solidified microstructures during the developing process: In general, the surface tension significantly affects the precision of the resulting 3D microstructures. To overcome this problem, the authors propose a simple and effective laser scanning method to reinforce the strength of 3D microstructures without loss of precision. Overall, a complex 3D artistic sculpture such as “The Thinker” was reproduced in the controlled ultraprecise form, which shows that the proposed method enables the fabrication of 3D patterns with dramatically improved precision and stability. [ABSTRACT FROM AUTHOR]

Polycyclic aromatic hydrocarbons are model systems for studying the mechanisms of lithium storage in carbonaceous materials. In this work, Li complexes of naphthalene, pyrene, perylene, and coronene were synthesized in a supersonic metal-cluster beam source and studied by zero-electron-kinetic-energy (ZEKE) electron spectroscopy and density functional theory calculations. The adiabatic ionization energies of the neutral complexes and frequencies of up to nine vibrational modes in the singly charged cations were determined from the ZEKE spectra. The metal-ligand bond energies of the neutral complexes were obtained from a thermodynamic cycle. Preferred Li/Li+ binding sites with the aromatic molecules were determined by comparing the measured spectra with theoretical calculations. Li and Li+ prefer the ring-over binding to the benzene ring with a higher π-electron content and aromaticity. Although the ionization energies of the Li complexes show no clear correlation with the size of the aromatic molecules, the metal-ligand bond energies increase with the extension of the π-electron network up to perylene, then decrease from perylene to coronene. The trends in the ionization and metal-ligand bond dissociation energies of the complexes are discussed in terms of the orbital energies, local quadrupole moments, and polarizabilities of the free ligands and the charge transfer between the metal atom and aromatic molecules. [ABSTRACT FROM AUTHOR]

Copper-diammonia, Cu(NH3)2, and its deuterated species, Cu(ND3)2, are produced in supersonic molecular beams and studied by pulsed-field ionization zero electron kinetic energy photoelectron spectroscopy and ab initio calculations. Structural isomers with a copper atom binding to an ammonia dimer or two ammonia molecules are obtained by the calculations. By comparing the experimental measurements to the theoretical calculations, the neutral and ionic forms of copper-diammonia are determined to be in a doubly bound linear conformation in their ground electronic states. The adiabatic ionization potentials of Cu(NH3)2 and Cu(ND3)2 are measured as 29 532 (5) and 29 313 (5) cm-1, respectively. The metal-ligand symmetric stretching frequencies are measured to be 436 cm-1 for Cu+–(NH3)2 and 398 cm-1 for Cu+–(ND3)2, and the metal-ligand bending frequencies 75/139 cm-1 for Cu/Cu+–(NH3)2 and 70/125 cm-1 for Cu/Cu+–(ND3)2. Moreover, the dissociation energy of Cu(NH3)2→CuNH3+NH3 is determined to be 11(3) kcal mol-1 through a thermodynamic relationship. [ABSTRACT FROM AUTHOR]

The yttrium complexes with one and two dimethyl ethers and their deuterated derivatives are prepared with laser vaporization molecular beam techniques, identified with photoionization time-of-flight mass spectrometry, and investigated with pulsed-field-ionization zero-electronkinetic-energy (ZEKE) photoelectron spectroscopy and ab initio calculations. Adiabatic ionization potentials and yttrium-oxygen stretch and ether-based vibrations are measured for the 1:1 and 1:2 complexes. Fermi interactions are observed from the ZEKE spectra of the 1:1 species. The ground electronic states of the monoligand complexes are determined to be [SUP2]A[SUB2] for the neutral and [SUP1]A[SUB1] for the singly charged positive ion, both in C[SUB2v] symmetry, with yttrium binding to oxygen. The coordination of a second ether forms a diligand complex with a linear oxygen-yttrium-oxygen configuration. This is the first electronic-vibrational spectroscopic study of yttrium-polyatomic molecule complexes and weakly bound metal complexes with two or more polyatomic molecules. [ABSTRACT FROM AUTHOR]

Aluminum-trimethylphosphine and trimethylarsine have been prepared by pulsed laser vaporization. Their electronic spectra have been obtained for the first time, using pulsed field ionization zero electron kinetic energy (ZEKE) photoelectron spectroscopy. The ZEKE spectra reveal the information about adiabatic ionization energies, intermolecular and ligand vibrations, and charge effects on molecular geometries. In coordination with the experimental measurements, density functional theory has been used to calculate equilibrium geometries, vibrational frequencies, and bond dissociation energies for the neutral and ionic complexes. The calculations predict that ionization causes the most significant geometry changes in the Al–P–C or Al–As–C angles, in agreement with the experimental observations. The aluminum ion and atom bind phosphorus more strongly than arsenic in these species. © 2002 American Institute of Physics. [ABSTRACT FROM AUTHOR]

A coil-unit barrel for a helical coil electromagnetic launcher is described. It provides better features of high structural strength and flexible adjustability. It is convenient to replace the damaged coil units and easy to adjust the number of turns in the stator coils due to the modular design. In our experiments, the highest velocity measured for a 4.5-kg projectile is 47.3 m/s and the mechanical reinforcement of the launcher could bear 35 kA peak current. The relationship between the energy conversion efficiency and the inductance gradient of the launcher is also studied. In the region of low inductance gradient, the efficiency is positively correlated with the inductance gradient. However, in the region of high inductance gradient, the inter-turn arc erosion becomes a major problem of limiting the efficiency and velocity of the launcher. This modular barrel allows further studies in the inter-turn arc and the variable inductance gradient helical coil launcher. [ABSTRACT FROM AUTHOR]

In laser driven hohlraums, laser beams on the same incident cone may have different beam and plasma conditions, causing beam-to-beam backscatter difference and subsequent azimuthal variations in the x-ray drive on the capsule. To elucidate the large variation of backscatter proportion from beam to beam in some gas-filled hohlraum shots on Shenguang-III, two 28.5° beams have been measured with the Stimulated Raman Scattering (SRS) time-resolved spectra. A bifurcated fiber is used to sample two beams and then coupled to a spectrometer and streak camera combination to reduce the cost. The SRS spectra, characterized by a broad wavelength, were further corrected considering the temporal distortion and intensity modulation caused by components along the light path. This measurement will improve the understanding of the beam propagation inside the hohlraum and related laser plasma instabilities. [ABSTRACT FROM AUTHOR]

Upconverting nanoparticles (UCNPs) composed of NaYF4 and doped with photoactive Yb3+ and Er3+ (NaYF4:Yb/Er) are highly desirable for many biological applications, but obtaining stable dispersions of UCNPs is challenging. Traditional synthetic methods often use complicated synthetic steps, produce toxic side products, and require post modifications to make UCNPs more dispersible in aqueous solutions. In this study, we demonstrate that laser ablation in liquid (LAL) is a novel approach to synthesize water-dispersible and -stable UCNPs with advantages of particle-size tuning, in situ coating of UCNPs with capping agents, no use of toxic or high boiling point solvents, and short reaction times. NaYF4:Yb/Er UCNPs were produced through LAL of annealed targets using water as the liquid, and their compositions and properties were investigated at a laser fluence of 0.57 J cm−2–6.22 J cm−2 by direct capping with citric acid and ethylene glycol and by comparing with the UCNPs prepared from the traditional hydrothermal method. Low laser fluences produced polydisperse particles consisting of no photoactive species through a thermal evaporation mechanism, while high laser fluences generated UCNPs with more uniform morphologies and compositions similar to the target material by an explosive ejection mechanism. The inclusion of capping agents during LAL allowed for direct coating of the UCNP surface without the need of post modifications, and the concentrations of capping agents affected the UCNP photoluminescence lifetimes. As compared to the hydrothermal method, the LAL-prepared samples showed better size control and no degradation of the capping agents. [ABSTRACT FROM AUTHOR]

An ultraviolet Thomson-scattering system has been designed and implemented on the Shenguang-III laser facility, a 48-beam, 3ω (351 nm), 180 kJ-level laser driver for high energy density physics and inertial confinement fusion researches. The 4ω (263.3 nm) probe beam of the Thomson-scattering system is injected from the north pole (top) of the target chamber, with an assistant beam-pointing monitor to achieve high pointing accuracy. The Thomson-scattered light is collected by a double-Cassegrain optical transmission system, which provides an achromatic image over a wide wavelength range of 200–800 nm. A novel on-line alignment method is developed and applied to the diagnostic system, ensuring a volumetric positioning accuracy of ∼30 μm for the scattering volume. An online calibration is also conducted to provide the wavelength benchmark and the spectral resolution of the system. This Thomson-scattering system has been tested in a complicated experimental environment with gas-filled hohlraums, and a high-quality ion feature of the scattered light has been obtained. [ABSTRACT FROM AUTHOR]

The analysis and detection of nucleic acid and specific antigens and antibodies are the most basic technologies for virus monitoring. However, the potential window for applying these technologies exists within a late specific period in the early monitoring and control of unknown viruses, especially human and animal pathogenic viruses transmitted via aerosols, e.g., SARS-CoV-2 and its variants. This is because early, real-time, and convenient monitoring of unknown viruses in the air or exhaled gas cannot be directly achieved through existing technologies. Herein, we report a weak light spectral imaging technology based on Tesla discharge (termed T-DAI) that can quickly monitor for viruses in real time in simulated aerosols with 71% sensitivity and 76% specificity for aerosol virus concentrations exceeding approximately 2800 vp/μl. This technology realizes the rapid detection of low concentrations of viruses in aerosols and could provide an important means for predicting, screening, and monitoring unknown or pandemic pathogenic viruses in the air or exhaled breath of humans and animals. [ABSTRACT FROM AUTHOR]

La atom reactions with 1-pentene and 2-pentene are carried out in a laser-vaporization molecular beam source. The two reactions yield the same metal-hydrocarbon products from the dehydrogenation and carbon–carbon bond cleavage of the pentene molecules. The dehydrogenated species La(C5H8) is the major product, whereas the carbon–carbon bond cleaved species La(C2H2) and La(C3H4) are the minor ones. La(C10H18) is also observed and is presumably formed by La(C5H8) addition to a second pentene molecule. La(C5H8) and La(C2H2) are characterized with mass-analyzed threshold ionization (MATI) spectroscopy and quantum chemical computations. The MATI spectra of each species from the two reactions exhibit the same transitions. Adiabatic ionization energies and metal-ligand stretching frequencies are determined for the two species, and additional methyl bending and torsional frequencies are measured for the larger one. Five possible isomers are considered for La(C5H8), and a C1 metallacyclopentene (Iso A) is identified as the most possible isomer. La(C2H2) is confirmed to be a C2v metallacyclopropene. The ground electronic state of each species is a doublet with a La 6s1-based electron configuration, and ionization yields a singlet state. The formation of the lanthanacyclopentene includes La addition to the C=C double bond, La insertion into two C(sp3)—H bonds, and concerted dehydrogenation. For the 2-pentene reaction, the formation of the five-membered ring may also involve 2-pentene to 1-pentene isomerization. In addition to the metal addition and insertion, the formation of the three-membered metallacycle from 1-pentene includes C(sp3)—C(sp3) bond breakage and hydrogen migration from La to C(sp3), whereas its formation from 2-pentene may involve the ligand isomerization. [ABSTRACT FROM AUTHOR]

La atom reactions with 1-butene, 2-butene, and isobutene are carried out in a laser-vaporization molecular beam source. The three reactions yield the same La-hydrocarbon products from the dehydrogenation and carbon-carbon bond cleavage and coupling of the butenes. The dehydrogenated species La(C4H6) is the major product, which is characterized with mass-analyzed threshold ionization (MATI) spectroscopy and quantum chemical computations. The MATI spectrum of La(C4H6) produced from the La+1-butene reaction exhibits two band systems, whereas the MATI spectra produced from the La+2-butene and isobutene reactions display only a single band system. Each of these spectra shows a strong origin band and several vibrational progressions. The two band systems from the spectrum of the 1-butene reaction are assigned to the ionization of two isomers: La[C(CH2)3] (Iso A) and La(CH2CHCHCH2) (Iso B), and the single band system from the spectra of the 2-butene and isobutene reactions is attributed to Iso B and Iso A, respectively. The ground electronic states are 2A1 (C3v) for Iso A and 2A′ (Cs) for Iso B. The ionization of the doublet state of each isomer removes a La 6s-based electron and leads to the 1A1 ion of Iso A and the 1A′ ion of Iso B. The formation of both isomers consists of La addition to the C=C double bond, La insertion into two C(sp3)—H bonds, and H2 elimination. In addition to these steps, the formation of Iso A from the La+1-butene reaction may involve the isomerization of 1-butene to isobutene prior to the C—H bond activation, whereas the formation of Iso B from the La+trans-2-butene reaction may include the trans- to cis-butene isomerization after the C—H bond activation. [ABSTRACT FROM AUTHOR]

The plasma arc caused by lightning overvoltage can significantly degrade the power grid reliability. Thus, it is essential to design an efficient arc extinguishing system. The modeling and analysis of the plasma arc in an arc extinguishing system can provide an essential theoretical basis for improving and optimizing its structure. However, the precision of the governing equation and boundary value of the plasma arc model chosen in previous studies can be entirely different from the corresponding practical values. This study develops an arc extinguishing system named "convective shock wave complex system." In order to further optimize its structure and achieve a better arc extinguishing effect, an appropriate model is established to analyze the plasma's operation characteristics inside the arc extinguishing device while stroking by lightning. Based on the magnetohydrodynamics theory, the COMSOL software is utilized to analyze the temperature of the plasma arc, the flow rate of gas in the cavity, and the conductivity and current density of some monitoring points to comprehensively analyze the plasma's physical characteristics in the system. Finally, a virtual lightning experiment is utilized to evaluate the simulation results. [ABSTRACT FROM AUTHOR]