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We report the two-photon absorption laser-induced fluorescence rotational spectrum of the CO B 1Σ+ ← X 1Σ+ Hopfield–Birge system (v′ = 0, v″ = 0) Q-branch in an ∼4850 K, atmospheric pressure plasma torch plume at thermal equilibrium in both the quenching-dominated (low laser intensity) and photoionization-dominated (high laser intensity) regimes. We provide a detailed analysis of the photophysics in these two regimes using a rate equation approach and propose modeling considerations for them as well. In the experimental spectra, distinct rotational transitions up to J″ = 83 are observed, allowing analysis over a very large range of rotational states. Evidence of predissociation is observed for J′ ≥ 64 and is likely due to the interaction with the D′1Σ+ electronic state, which has been proposed in the literature but never observed in the v′ = 0 state. The line positions of higher rotational states show disagreement with line positions calculated from molecular constants in the available literature, suggesting the need for modifications to the constants, which are reported here. A shift in the B 1Σ+ ← X 1Σ+ absorption spectrum toward higher two-photon energy as a result of the second-order Stark shift was observed in the photoionization-dominated spectrum, and the second-order Stark shift cross section was estimated to be 7 ± 3 × 10−18 cm2. The mean photoionization cross section of the excited upper state was inferred by comparing the line broadening of the two spectra and was estimated to be 11 ± 7 × 10−18 cm2. In addition, weak J′-dependent variations of the photoionization cross section were observed and are reported here. [ABSTRACT FROM AUTHOR]

The contribution of atomic nitrogen is fairly possible in plasma-assisted catalytic synthesis of ammonia since it has high adsorption probabilities on solid surfaces. On the other hand, recently, the contribution of vibrational excited molecular nitrogen to ammonia synthesis has been discussed. In this work, we compared the fluxes of atomic nitrogen and vibrational excited molecular nitrogen with the rate of plasma-assisted ammonia synthesis. We employed an atmospheric-pressure nitrogen plasma jet, and the spatial afterglow of the plasma jet and a hydrogen flow irradiated the surface of a ruthenium catalyst. The fluxes of atomic nitrogen and vibrational excited molecular nitrogen were measured by two-photon absorption laser-induced fluorescence spectroscopy and laser Raman scattering, respectively. The synthesis rate of ammonia had a positive correlation with the flux of vibrational excited molecular nitrogen, while the variation of the synthesis rate with the gas flow rate was opposite to the flux of atomic nitrogen. The experimental results indicate the contribution of vibrational excited molecular nitrogen to the synthesis of ammonia using the atmospheric-pressure plasma, where the flux of vibrational excited molecular nitrogen is more than four orders of magnitude higher than that of atomic nitrogen. [ABSTRACT FROM AUTHOR]

This study was focused on the photochemistry of OAlOH and three possible pathways, which were studied with high-level multireference configuration interaction ab initio calculations. We computed cuts of the six-dimensional potential energy surfaces for the ground, the lowest singlet and triplet excited states, and probed the photodissociation mechanisms and the stabilities. The OAlOH electronic spectrum, with an energy reaching 7.15 eV, contained four prominent peaks. Photodissociation to AlO, OH, and AlOH constituted a plausible mechanism within the deep-UV range (λ = 250.4 nm). Our data indicated the photostability of OAlOH in the near-UV‒Vis region, so detection with laser-induced fluorescence is possible. Fluorescence and phosphorescence may occur upon excitation at 363.5 nm. The roles of OAlOH in the photochemical reactions of Al-bearing molecules in the upper atmosphere and VY Canis Majoris are discussed. [ABSTRACT FROM AUTHOR]

An IR–vacuum ultraviolet (VUV) ion-dip spectroscopy method is utilized to examine the IR spectrum of acetaldehyde oxide (CH3CHOO) in the overtone CH stretch (2νCH) spectral region. IR activation creates a depletion of the ground state population that reduces the VUV photoionization signal on the parent mass channel. IR activation of the more stable and populated syn-CH3CHOO conformer results in rapid unimolecular decay to OH + vinoxy products and makes the most significant contribution to the observed spectrum. The resultant IR–VUV ion-dip spectrum of CH3CHOO is similar to that obtained previously for syn-CH3CHOO using IR action spectroscopy with UV laser-induced fluorescence detection of OH products. The prominent IR features at 5984 and 6081 cm−1 are also observed using UV + VUV photoionization of OH products. Complementary theoretical calculations utilizing a general implementation of second-order vibrational perturbation theory provide new insights on the vibrational transitions that give rise to the experimental spectrum in the overtone CH stretch region. The introduction of physically motivated small shifts of the harmonic frequencies yields remarkably improved agreement between experiment and theory in the overtone CH stretch region. The prominent features are assigned as highly mixed states with contributions from two quanta of CH stretch and/or a combination of CH stretch with an overtone in mode 4. The generality of this approach is demonstrated by applying it to three different levels of electronic structure theory/basis sets, all of which provide spectra that are virtually indistinguishable despite showing large deviations prior to introducing the shifts to the harmonic frequencies. [ABSTRACT FROM AUTHOR]

A femtosecond laser induced photofragmentation fluorescence (fs-LIPF) scheme for the sensitive detection and imaging of water vapor is presented. Two photons of 244.3 nm excite water to the D ̃ state and produce hydroxyl radicals in the fluorescing A ̃ state. Two more photons promote electrons from the D ̃ state to a neutral Rydberg state of the (1b2)−1 ionic core through a 2 + 2 doubly resonant process. The resulting high-lying Rydberg state undergoes neutral dissociation, and the energetic hydrogen fragments are detected from their Balmer series fluorescence. These channels (in the low-pressure limit) have detection sensitivities around 1012 molecules per cubic centimeters, orders of magnitude more sensitive than laser-induced fluorescence based approaches, allowing for sensitive non-invasive detection and imaging of water density for many important processes. [ABSTRACT FROM AUTHOR]

Rotationally resolved Fourier-transform spectra of laser-induced fluorescence A 1 Σ u + ∼ b 3 Π u → X 1 Σ g + of K2 molecules were recorded and analyzed, yielding 4053 term values of the spin–orbit (SO) coupled A ∼ b complex of the 39K2 isotopologue with ∼0.01 cm−1 accuracy. Their compilation with 1739 term values from previously published sources allowed them to cover the energy range [9955, 17 436] cm−1 from the bottom of the lower-lying b3Πu state up to the vicinity of the atomic asymptote 4 s 2 S 1 2 + 4 p 2 P 1 2 , with a rotational quantum number J ∈ [0, 149]. The experimental data were processed by a direct 6 × 6 coupled-channel (CC) deperturbation treatment, which accounted explicitly for both SO and electronic-rotational interactions between all six e-symmetry states: A 1 Σ u + ( 0 u + ), b3Πu( 0 u + , 1 u , 2 u ), c3Σu(1u), and B1Πu(1u). The initial parameters of the global deperturbation model have been estimated in the framework of ab initio electronic structure calculations applying multi-reference configuration-interaction and coupled-clusters methods. The interatomic potentials analytically defined for A and b states, as well as SO-splitting of the triplet b state and A ∼ b SO-coupling functions, have been particularly refined to fit the 5792 term values of the 39K2 isotopologue, whereas the rest parameters were fixed on their ab initio values. The resulting mass-invariant parameters of the 6 × 6 CC model reproduced the overall rovibronic term energies of the A ∼ b complex of 39K2 with accuracy, which is well within the experimental errors. The quality of the deperturbation analysis was independently confirmed by comparison with the present obtained 705 and 14 term values of respective 39K41K and 41K2 isotopologues, as well as by agreement between measured and predicted relative intensity distributions in long A ∼ b → X(vX) band progressions. This deperturbation analysis provided the refined dissociation energy Tdis = 17 474.569(5) cm−1 and the long-range coefficient C 3 Σ = 5.501(4) × 105 cm−1 Å3 relevant to the non-relativistic atomic limit 4s + 4p. The derived Tdis yielded the accurate well depth De = 4450.910(5) cm−1 for the ground X 1 Σ g + state, whereas the new C 3 Σ value yielded the improved estimates for atomic K(4 p 2 P 1 2 ; 3 2 ) radiative lifetimes, τ 1 2 = 26.67(3) and τ 3 2 = 26.32(3) ns. [ABSTRACT FROM AUTHOR]

GaCH2, a free radical thought to play a role in the chemical vapor deposition of gallium-containing thin films and semiconductors, has been spectroscopically detected for the first time. The radical was produced in a pulsed discharge jet using a precursor mixture of trimethylgallium vapor in high pressure argon and studied by laser-induced fluorescence and wavelength resolved emission techniques. Partially rotationally resolved spectra of the hydrogenated and deuterated species were obtained, and they exhibit the nuclear statistical weight variations and subband structure expected for a 2A2–2B1 electronic transition. The measured spectroscopic quantities have been compared to our own ab initio calculations of the ground and excited state properties. The electronic spectrum of gallium methylene is similar to the corresponding spectrum of the aluminum methylene radical, which we reported in 2022. [ABSTRACT FROM AUTHOR]

A π-type hydrogen bonding between the OH group and the π electron is a crucial factor for the conformational preference of the molecular structure with a flexible group. However, the information on the effect of the substituent on the OH/π interaction is insufficient. The laser-induced fluorescence (LIF) excitation, the dispersed fluorescence (DF), the IR–UV hole-burning, and the IR dip spectra of jet-cooled 2-(4-methoxyphenyl)ethanol were measured for the first time. Almost all bands observed in the spectral region of 35 550–36 500 cm−1 in the LIF excitation spectrum were successfully assigned with the DF and the IR–UV hole-burning spectra coupled with the quantum chemical calculation at M06-2x/6-311G and MP2/6-311G levels. Five conformers were found in the LIF excitation spectrum. The most stable conformer was Ggπ, and the second most stable conformer was Ggπ′ (the trans rotamer of the methoxy group for Ggπ). Ggπ and Ggπ′ had the OH group directed toward the π electron system of the benzene ring. The OH stretching frequency of Ggπ/Ggπ′ of MPE in the IR dip spectra was red-shifted against that of Ggπ of phenylethanol, indicating that the introduction of the methoxy group would enhance the intramolecular OH/π interaction. In addition, the torsional vibration between the benzene ring and the side chain (−CH2CH2OH) (mode 63) was observed in the DF spectra of the Ggπ–00 and Ggπ′–00 band excitation, but their intensities were rather different, resulting from the different orientation of the OH group for each conformer toward the π electron system. The methoxy group would increase the negative charge on the benzene ring and would enhance the intramolecular OH/π interaction through the electrostatic interaction. [ABSTRACT FROM AUTHOR]

Gas–liquid two-phase stratified flow exists in many industrial processes. Although the flow pattern is simple, the interfacial shear prediction of stratified flow is still the focus of the study. The calculation of the shear stress at the gas–liquid interface is closely related to the measurement of the void fraction and pressure drop of the stratified flow. In this study, a new method for the calculation of interfacial shear stress of gas–liquid two-phase stratified flow is proposed. Differential pressure measurement and planar laser-induced fluorescence technology are combined to obtain important parameters for stratified flow under low-speed flow conditions (Ql = 0.10–0.25 m3/h, Qg = 0.35–1.00 m3/h). The interfacial shear stress is successfully calculated using macroparameters. The uncertainty associated with the calculated parameters using the proposed method is 2.67%, and this study verifies the accuracy of the linear relationship. The method provides a new way to obtain the interfacial shear stress of gas–liquid stratified flow. [ABSTRACT FROM AUTHOR]

We have analyzed the effects of the spreads in experimental parameters on the reliability of speeds and angular distributions extracted from a generic surface-scattering experiment based on planar laser-induced fluorescence detection. The numerical model assumes a pulsed beam of projectile molecules is directed at a surface. The spatial distribution of the scattered products is detected by imaging the laser-induced fluorescence excited by a thin, pulsed sheet of laser light. Monte Carlo sampling is used to select from realistic distributions of the experimental parameters. The key parameter is found to be the molecular-beam diameter, expressed as a ratio to the measurement distance from the point of impact. Measured angular distributions are negligibly distorted when this ratio is <∼10%. Measured most-probable speeds are more tolerant, being undistorted when it is <∼20%. In contrast, the spread of speeds or of corresponding arrival times in the incident molecular beam has only very minor systematic effects. The thickness of the laser sheet is also unimportant within realistic practical limits. These conclusions are broadly applicable to experiments of this general type. In addition, we have analyzed the specific set of parameters designed to match the experiments on OH scattering from a liquid perfluoropolyether (PFPE) surface in the Paper I [Roman et al., J. Chem. Phys. 158, 244704 (2023)]. This reveals that the detailed form of the molecular-beam profile is important, particularly on apparent angular distributions, for geometric reasons that we explain. Empirical factors have been derived to correct for these effects. [ABSTRACT FROM AUTHOR]

Inelastic collisions of OH with an inert liquid perfluoropolyether (PFPE) surface have been studied experimentally. A pulsed molecular beam of OH with a kinetic energy distribution peaking at 35 kJ mol−1 was directed at a continually refreshed PFPE surface. OH molecules were detected state-selectively with spatial and temporal resolution by pulsed, planar laser-induced fluorescence. The scattered speed distributions were confirmed to be strongly superthermal, regardless of the incidence angle (0° or 45°). Angular scattering distributions were measured for the first time; their reliability was confirmed through extensive Monte Carlo simulations of experimental averaging effects, described in Paper II [A. G. Knight et al., J. Chem. Phys. 158, 244705 (2023)]. The distributions depend markedly on the incidence angle and are correlated with scattered OH speed, consistent with predominantly impulsive scattering. For 45° incidence, the angular distributions are distinctly asymmetric to the specular side but peak at sub-specular angles. This, along with the breadth of the distributions, is incompatible with scattering from a surface that is flat on a molecular scale. New molecular dynamics simulations corroborate the roughness of the PFPE surface. A subtle but unexpected systematic dependence of the angular distribution on the OH rotational state was found, which may be dynamical in origin. The OH angular distributions are similar to those for kinematically similar Ne scattering from PFPE and hence not strongly perturbed by OH being a linear rotor. The results here are broadly compatible with prior predictions from independent quasiclassical trajectory simulations of OH scattering from a model-fluorinated self-assembled monolayer surface. [ABSTRACT FROM AUTHOR]

The isoelectronic molecules UN and UO+ are known to have Ω = 3.5 and Ω = 4.5 ground states, respectively (where Ω is the unsigned projection of the electronic angular momentum along the internuclear axis). A ligand field theory model has been proposed to account for the difference [Matthew and Morse, J. Chem. Phys. 138, 184303 (2013)]. The ground state of UO+ arises from the U3+(5f3(4I4.5))O2− configuration. Owing to the higher nominal charge of the N3− ligand, the U3+ ion in UN is stabilized by promoting one of the 5f electrons to the more polarizable 7s orbital, reducing the repulsive interaction with the ligand and rendering U3+(5f27s(4H3.5))N3− the lowest energy configuration. In the present work, we have advanced the characterization of the UN ground state through studies of two electronic transitions, [18.35]4.5-X(1)3.5 and [18.63]4.5-X(1)3.5, using sub-Doppler laser excitation techniques with fluorescence detection. Spectra were recorded under field-free conditions and in the presence of static electric or magnetic fields. The ground state electric dipole moment [μ = 4.30(2) D] and magnetic ge-factor [2.160(9)] were determined from these data. These values were both consistent with the 5f27s configurational assignment. Dispersed fluorescence measurements were used to determine vibrational constants for the ground and first electronically excited states. Electric dipole moments and magnetic ge-factors are also reported for the higher-energy electronically excited states. [ABSTRACT FROM AUTHOR]

The current work investigates the effects of oblique Lorentz force and Navier's slip boundary condition on unsteady hybrid nanoliquid flow with three different base liquids (H2O, CH3OH and H2O–EG) across a nonlinearly elongating surface set in a porous medium. This research considers the effects of viscous–Ohmic dissipation, nonlinearly variable thermal radiation, internal heat source, the Soret effect, first-order chemical reaction and thermal and solutal jump conditions at the boundary. Proper thermo-physical relationships for the hybrid nanoliquid have been established. Rosseland's estimate for an optically thick regime is used when calculating the heat flow owing to radiation. The dimensional governing equations are translated into nondimensional forms using appropriate similarity transformations. The velocity, energy and concentration fields are numerically solved using a shooting strategy based on the secant iteration and the Runge–Kutta–Fehlberg method. The physical implications of several essential parameters on the hybrid nanoliquid velocity, temperature and concentration are investigated using graphical and tabular representations of numerical data. Furthermore, the multiple (quadratic) regression analysis reveals that physical parameters strongly influence the local skin friction coefficient, Sherwood and Nusselt numbers. For continuously growing values of the unsteadiness parameter, the velocity, thermal and concentration scattering declined everywhere within the boundary layer region. [ABSTRACT FROM AUTHOR]

Laser-induced fluorescence (LIF) Doppler spectroscopy using an optical vortex beam with an asymmetric intensity distribution, referred to as aOVLIF, is proposed as a new method to measure plasma flow velocity. LIF spectra were calculated numerically using typical laboratory low-temperature plasma parameters, and it was revealed that an ion flow across the beam produces a frequency shift of the spectra. This method also has the capability of temperature measurements. The propagation effects of asymmetric optical vortex beams are discussed assuming an actual experiment, and it is found that the sensitivity to the transverse flow velocity is approximately unchanged. The aOVLIF method, which exploits the inhomogeneous phase structure of optical vortices, can be applied to the determination of three-dimensional velocity vectors and promises to enhance the usefulness of conventional LIF spectroscopy using plane waves. [ABSTRACT FROM AUTHOR]

Ammonia (NH 3), hydrogen (H 2) and methane (CH 4) as zero- or low-carbon fuels are considered as highly promising alternative fuels. Turbulent non-premixed jet combustion is a prospective way in practical combustion devices for ammonia, hydrogen and methane, but the relevant experimental researches are rare, while such information is critical for the development and validation of numerical models. In this paper, the laser diagnostic studies are carried out in a constant volume combustion chamber to investigate the characteristics of the 50%NH 3 +50%H 2 blend jet with or without ignition in comparison to H 2 , CH 4 and NH 3 jets. Firstly, the morphological developments and concentration distributions of the four gas jets without ignition are compared. Then, the OH or NO distributions in the non-premixed gas jet flames are clarified by the planar laser-induced fluorescence techniques. The generation and consumption processes of OH and NO are elucidated by the one-dimensional simulation. The results show that the four jets exhibit a similar morphological development with the nearly same jet angles, except for a little slower tip penetration of 50%NH 3 +50%H 2 blend. The equivalence ratio of the 50%NH 3 +50%H 2 blend and NH 3 jets along the jet axis are lower than those in the CH 4 and H 2 jets due to the difference in the flow rate and stoichiometric number. The H 2 jet exhibits the highest combustion intensity, featuring faster flame propagation, the shortest lift-off length and an apparently higher OH radical intensity, while the NH 3 jet fails to develop a stable flame. The mixture in the 50%NH 3 +50%H 2 blend jet is too lean, resulting in a weaker combustion intensity than the H 2 and CH 4 jets. However, the NO intensity in the 50%NH 3 +50%H 2 jet flame is remarkably stronger than those of the H 2 and CH 4 jet, due to the much higher amount of fuel-type NO converted from NH 3 than that of thermal NO. A self-reducing (SR) zone can be observed where OH is produced and then consumed in the 50%NH 3 +50%H 2 blend, H 2 and CH 4 jet flames. However, the NO SR zone is only observable in the 50%NH 3 +50%H 2 blend jet flames, probably owing to the consumption by the NH 2 and NH radicals. • The laser diagnostic was used to obtained the OH and NO distributions. • The 50%NH 3 +50%H 2 , H 2 , CH 4 and NH 3 jets exhibit a similar morphologic development. • The equivalence ratios of the 50%NH 3 +50%H 2 blend and NH 3 jets are the lowest. • The fuel-type NO makes the strongest NO intensity in 50%NH 3 +50%H 2 blend flames. • For the first time a self-reducing zone was observed for the OH and NO. [ABSTRACT FROM AUTHOR]

This study explores the stabilization of non-premixed NH 3 /CH 4 flames using gradient magnetic fields, overcoming challenges like low flame speed and instability inherent in ammonia—a carbon-free fuel and efficient hydrogen carrier. The action of the magnetic field modified the flame flow field, resulting in the suppression of emissions. By applying magnetic fields, the blending ratio of ammonia in the diffusion flame was elevated, resulting in an increase of 69% in the limit concentration to a near-pure level of 0.914. Measurements with Particle Image Velocimetry and schlieren system, alongside computational fluid dynamics, reveal how gradient magnetic fields mitigate flame detachment, lift-off, and blowout by altering flame root stabilization mechanisms. Specifically, gradient magnetic fields reduce localized flow velocity at the flame root and improve mass transfer. This indicates that gradient magnetic fields can significantly enhance the stability of NH 3 /CH 4 flames, suggesting a promising route toward cleaner energy production and environmental sustainability. [Display omitted] • Achieves near-pure ammonia combustion in diffusion flames by imposing gradient magnetic fields. • Identified critical impact of magnetic fields on flame structure and reactant species distribution. • Investigates gradient magnetic field effects on flame root dynamics, offering new stabilization insights. • Integrates PIV, schlieren photography, and simulations to detail magnetic fields' role in sustaining ammonia flames. [ABSTRACT FROM AUTHOR]

Single‐molecule localization microscopy (SMLM) has revolutionized optical microscopy by exceeding the diffraction limit and revealing previously unattainable nanoscale details of cellular structures and molecular dynamics. This super‐resolution imaging capability relies on fluorophore photoswitching, which is crucial for optimizing the imaging conditions and accurately determining the fluorophore positions. To understand the general on and off photoswitching mechanisms of single dye molecules, various photoswitching reagents were evaluated. Systematic measurement of the single‐molecule‐level fluorescence on and off rates (kon and koff) in the presence of various photoswitching reagents and theoretical calculation of the structure of the photoswitching reagent‐fluorophore pair indicated that the switch‐off mechanism is mainly determined by the nucleophilicity of the photoswitching reagent, and the switch‐on mechanism is a two‐photon‐induced dissociation process, which is related to the power of the illuminating laser and bond dissociation energy of this pair. This study contributes to a broader understanding of the molecular photoswitching mechanism in SMLM imaging and provides a basis for designing improved photoswitching reagents with potential applications extending to materials science and chemistry. [ABSTRACT FROM AUTHOR]

Ytterbium‐doped lanthanum titanate glasses were prepared by levitation melting for the detailed characterization of the Yb3+${\rm Yb}^{3+}$ spectroscopic properties in the rare‐earth titanate glass host. Low‐temperature fluorescence spectroscopy reveals distinct site‐selectivity in both static and lifetime fluorescence measurements suggesting an absence of clustering as well as significant variation of local ytterbium environments. Typical site‐selectivity behavior of a shrinking Stark manifold with lower excitation energy is observed. At 77 K, both the mean emission frequency and the fluorescence lifetime initially increase as the excitation energy decreases from about 11100 to 10750 cm−1${\rm cm}^{-1}$ and then slightly decrease at lower excitation energy. Temperature‐dependent lifetime measurements between 77 and 420 K show a decreasing lifetime with increasing temperature and are well described by a two‐level thermal activation model. The temperature‐dependent fluorescence spectroscopy coupled with a room temperature white light absorption measurement allow the determination of the Stark energy levels of Yb3+${\rm Yb}^{3+}$ in lanthanum titanate glass as well as the calculation of the laser cross‐sections. [ABSTRACT FROM AUTHOR]

AbstractAccurate models of turbulent buoyant flows are essential for the design of the cooling circuit of nuclear reactors and passive safety systems. However, available models fail to fully capture the physics of turbulent mixing when buoyancy becomes predominant with respect to momentum. Therefore, high-fidelity experiments of well-controlled fundamental flows are needed to develop and validate more accurate models. We analyze experiments of positive and negative turbulent buoyant jets, both in uniform and stratified environments, with the aim of understanding the thermal hydraulics of turbulent mixing with variable density and providing high-fidelity data for the development and validation of turbulence models. Non-intrusive, simultaneous particle image velocimetry and laser-induced fluorescence measurements were carried out to acquire instantaneous velocity and concentration fields on a vertical section parallel to the axis of a jet in the self-similar region. The refractive index matching method was applied to measure high-resolution buoyant jets with up to 8.6% density difference. These data are free of the typical errors that characterize optical measurements of buoyancy-driven flows (e.g. natural and mixed convection) where the refractive index of the fluid is inhomogeneous throughout the measurement domain. Turbulent statistics and entrainment of buoyant jets in uniform and stratified environments are presented. These data are compared with non-buoyant jets in a uniform environment, as a reference to investigate the effects of buoyancy and stratification on turbulent mixing. The results will be used for the assessment of current turbulence models and as a basis for the development of a new model that captures turbulent mixing. [ABSTRACT FROM AUTHOR]

Digital PCR (dPCR) holds immense potential for precisely detecting nucleic acid markers essential for personalized medicine. However, its broader application is hindered by high consumable costs, complex procedures, and restricted multiplexing capabilities. To address these challenges, an all‐in‐one dPCR system is introduced that eliminates the need for microfabricated chips, offering fully automated operations and enhanced multiplexing capabilities. Using this innovative oscillation‐induced droplet generation technique, OsciDrop, this system supports a comprehensive dPCR workflow, including precise liquid handling, pipette‐based droplet printing, in situ thermocycling, multicolor fluorescence imaging, and machine learning‐driven analysis. The system's reliability is demonstrated by quantifying reference materials and evaluating HER2 copy number variation in breast cancer. Its multiplexing capability is showcased with a quadruplex dPCR assay that detects key EGFR mutations, including 19Del, L858R, and T790M in lung cancer. Moreover, the digital stepwise melting analysis (dSMA) technique is introduced, enabling high‐multiplex profiling of seven major EGFR variants spanning 35 subtypes. This innovative dPCR system presents a cost‐effective and versatile alternative, overcoming existing limitations and paving the way for transformative advances in precision diagnostics. [ABSTRACT FROM AUTHOR]

The behavior of ions in the plasma is an essential component in the process of industrial etching. We studied the motions and energy distribution of argon ions in a inductively coupled plasma (ICP) etching tool, by the method of laser induced fluorescence (LIF). The silicon wafer clamped to a chuck at the bottom of the chamber was biased with a 1 MHz 1–1.2 kV peak-to-peak sinusoidal voltage. The plasma is formed with a 2 MHz ICP coil pulsed at 10 Hz. Sheath thickness was measured at different phases of the bias waveform. The experiment also compared the ion motions with and without wafer bias, as well as different switch-on time of wafer bias. For all cases, ion energy distribution functions and the two-dimensional flow pattern were studied near the center and edge of the wafer. Significant vortex flows were observed near the wafer edge. Experiments in which the wafer was biased in the plasma afterglow resulted in a narrow distribution of ion energy close to the bias voltage at the vicinity of the wafer, and the ion incident angle on the wafer was the smallest. The results were compared to simulations using the Hybrid Plasma Equipment Model code. [ABSTRACT FROM AUTHOR]

The objective of this paper is to assess the capabilities of the Conditional Source-term Estimation (CSE) approach applied to a laboratory scaled turbulent buoyant flame without extinction. CSE is coupled with the Large Eddy Simulation (LES) solver, FireFOAM. Tabulated detailed chemistry is included. Radiation is treated using the optically thin model using four different implementations and the effect of subgrid scale (sgs) Turbulence-Radiation Interactions (TRI) is considered. Predictions of time-averaged temperatures and corresponding root mean square (rms) are compared with the experimental measurements at several locations. Further, flame shape, unconditional and conditional species mass fractions, axial velocity and mixture fraction are also examined for qualitative analysis. The predicted temperatures are in good agreement with the experimental data, except very close to the fuel inlet. The predicted temperatures increase more slowly compared to the experimental data in the first 0.09 m above the burner. The temperature rms is in reasonable agreement with experimental data with the peak being overpredicted by approximately 17%. The predicted flame height closely matches the experimental value. The temperature predictions are consistent with previously published results. Best predictions are obtained when the effect of sgs TRI is included. For this flame, the optically thin assumption is found to be valid, in agreement with previous investigations. The calculated radiative fraction is found to be close to the experimental value, but the postprocessed heat release rate is larger than the experimental finding. This first LES-CSE study provides a good foundation for further developments, for example more detailed radiation models, for more complex fire cases. [ABSTRACT FROM AUTHOR]

This paper delves into the methodology employed in examining lean premixed turbulent flame fronts extracted from Planar Laser Induced Fluorescence (PLIF) images at elevated pressures. In such flow regimes, the PLIF signal suffers from significant collisional quenching, typically resulting in image data with low signal-to-noise ratio (SNR). This poses severe difficulties for conventional flame front extraction algorithms based on intensity gradients and requires intense user intervention to yield acceptable results. In this work, we propose Convolutional Neural Network (CNN)-based Deep Learning (DL) models as an alternative to problem specific conventional methods. The pretrained DL models were fine-tuned, employing data augmentation, on a small annotated dataset including a variety of conditions between SNR ≈ 1.6 to 2.6 and subsequently evaluated. All DL models significantly outperformed the best-scoring conventional implementation both quantitatively and visually, while having similar inference times. IoU-scores and Recall values were found to be up to a factor ≈ 1.2 and ≈ 2.5 higher, respectively, with ≈ 1.15 times improved Precision. Small-scale structures were captured much better with fewer erroneous predictions, becoming particularly pronounced for the lower SNR data investigated. Moreover, by applying artificially modeled noise, it was shown that the range of image conditions in terms of SNR that can be reliably processed extends well beyond the images included in the training data, and satisfactory segmentation performances were found for SNR as low as ≈ 1.1. The presented DL-based flame front detection algorithm marks a methodology with significantly increased detection performance, while a similar computational effort for inference is achieved and the need for user-based parameter tuning is eliminated. It enables a very accurate extraction of instantaneous flame fronts in large image datasets where supervised processing is infeasible, unlocking unprecedented possibilities for the study of flame dynamics and instability mechanisms at industry-relevant conditions. [ABSTRACT FROM AUTHOR]

The process of Infrared Multiphoton Dissociation (IRMPD) was studied in a mixture of vinyl bromide/chlorodifluoromethane (VBr, C2H3Br/CF2HCl) using single and double infrared pulsed transverse excitations atmospheric CO2 laser beams. The dissociation of VBr was investigated using FTIR, and the product composition was analysed, and various dissociation routes were proposed. The study found that the VBr molecules were more heavily dissociated when exposed to the CF2HCl environment than without it. By using a time-resolved LIF, the kinetics reactions with CF2HCl were explored under pseudo-first-order conditions, and the quenching rate constant for the interaction between CF2HCl and C 2 d 3 Π g was published using the classical Stern–Volmer model. The impact of pulsed laser heating on the generation of C 2 a 3 Π u radicals was also observed. The decrease in the intensity of the C 2 (a 3 Π u) LIF signal was due to faster recombination of the C 2 a 3 Π u radicals, together with a decrease in V - V ′ energy transfer and the pressure oscillations produced by the effect of pulsed laser heating in the irradiated volume and the experimental conditions. [ABSTRACT FROM AUTHOR]

The existence of pathogenic microorganisms is a significant contributor to high morbidity rates in both developed and developing countries. Numerous human diseases have been related to Escherichia coli and Enterococcus faecalis. Fast diagnosis of these bacteria is crucial for limiting the progress of the associated diseases. The current study investigated the potential application of femtosecond laser-induced fluorescence spectroscopy (LIF) in monitoring bacteria. The INSPIRE HF100 laser system, which was pumped by a mode-locked femtosecond Ti: sapphire MAI TAI HP laser, delivered 100 femtosecond laser pulses to the samples. E. coli and E. faecalis were exposed to femtosecond laser pulses, and a spectrometer was used to monitor the fluorescence emission spectra. The measured LIF spectra of the two bacteria showed that E. coli and E. faecalis had fluorescence peaks at 502 and 512.5 nm, respectively. When the excitation wavelength varied from 350 to 400 nm, E. coli and E. faecalis fluorescence peak intensities linearly decreased. Furthermore, the LIF peaks revealed that the full width at half maximum of E. coli is 91.9 nm and that of E. faecalis is 101.3 nm. The current study findings suggest that femtosecond laser-induced fluorescence spectroscopy is a reliable, accurate, and sensitive approach for rapidly and directly identifying pathogenic bacteria. [ABSTRACT FROM AUTHOR]

Blending hydrogen with natural gas is useful for reducing CO 2 emissions, but this alters the flame structure, creating challenges for flame stability. Numerous researches on methane-hydrogen flame structure have been carried out based on two-dimensional combustion diagnostic techniques such as flame chemiluminescence and planar laser-induced fluorescence. In this paper, a low-cost OH* chemiluminescence imaging system consisting of 8 ultraviolet (UV) cameras is proposed to reconstruct the three-dimensional (3D) structure of methane-hydrogen flames, and validated through use of the correlation coefficient. Further experimental investigations of the low-swirl methane-hydrogen flames are performed by this computed tomography of chemiluminescence (CTC) system. The flame properties are determined to evaluate the effects of various fractions of blended hydrogen on the flame structure, including the flame center of mass, flame surface density and fractal dimension. Results showed that the flame initially has bowl-shape structure. The flame height gradually decreases and the flame cross-sectional area increases as the blended hydrogen fraction increases. Meanwhile, the bottom of the flame moves toward the nozzle outlet. Nevertheless, when the blended hydrogen fraction reaches 50%, the flame transforms into a cup-shaped flame and shows a double-layer flame structure. When the flame is bowl-shaped, the flame center of mass moves away from the nozzle center axis with increasing blended hydrogen fraction, but the fractal dimension and flame surface density are not sensitive to the blended hydrogen fraction. In contrast, when the flame is cup-shaped, the flame center of mass moves towards the nozzle center axis, and the flame surface density and fractal dimension increase significantly, indicating the increase of flame wrinkling. These results reveal that blending hydrogen leads to two distinct flame structures and characteristics in low-swirl flame, also demonstrate that the proposed 3D low-cost CTC system based on multiple UV cameras is well-suited for combustion diagnostics. • A low-cost 3D computed tomography of OH* chemiluminescence system is proposed. • Two distinct low-swirl CH 4 –H 2 flame shapes are observed and reconstructed. • The change in flame shape is accompanied by a significant change in flame wrinkling. [ABSTRACT FROM AUTHOR]

Clean-burning oxygenated and synthetic fuels derived from renewable power, so-called e-fuels, are a promising pathway to decarbonize compression–ignition engines. Polyoxymethylene dimethyl ethers (PODEs or OMEs) are one candidate of such fuels with good prospects. Their lack of carbon-to-carbon bonds and high concentration of chemically bound oxygen effectively negate the emergence of polycyclic aromatic hydrocarbons (PAHs) and even their precursors like acetylene (C2H2), enabling soot-free combustion without the soot-NOx trade-off common for diesel engines. The differences in the spray combustion process for OMEs and diesel-like reference fuels like n-dodecane and their potential implications on engine applications include discrepancies in the observed ignition delay, the stabilized flame lift-off location, and significant deviations in high-temperature flame morphology. For CFD simulations, the accurate modeling and prediction of these differences between OMEs and n-dodecane proved challenging. This study investigates the spray combustion process of an OME3 − 5 mixture and n-dodecane with advanced optical diagnostics, Reynolds-Averaged Navier–Stokes (RANS), and Large-Eddy Simulations (LESs) within a constant-volume vessel. Cool-flame and high-temperature combustion were measured simultaneously via high-speed (50 kHz) imaging with formaldehyde (CH2O) planar laser-induced fluorescence (PLIF) representing the former and line-of-sight OH* chemiluminescence the latter. Both RANS and LES simulations accurately describe the cool-flame development process with the formation of CH2O. However, CH2O consumption and the onset of high-temperature reactions, signaled by the rise of OH* levels, show significant deviations between RANS, LES, and experiments as well as between n-dodecane and OME. A focus is set on the quality of the simulated results compared to the experimentally observed spatial distribution of OH*, especially in OME fuel-rich regions. The influence of the turbulence modeling is investigated for the two distinct ambient temperatures of 900 K and 1200 K within the Engine Combustion Network Spray A setup. The capabilities and limitations of the RANS simulations are demonstrated with the initial cool-flame propagation and periodic oscillations of CH2O formation/consumption during the quasi-steady combustion period captured by the LES. [ABSTRACT FROM AUTHOR]

Silicon carbide ceramic matrix composites (SiC CMC) have excellent properties for applications but is challenging to precisely process, in particular for curved surfaces and deep through-holes. A long interaction range of femtosecond laser filament with sufficiently high intensity may open the opportunity. In this work, femtosecond laser filament was used to ablate grooves on the surface of SiC CMC. The effects of different filament positions, pulse energies, scanning speeds and scanning times on filament ablated grooves were investigated. The plasma fluorescence from filament ablated SiC CMC was collected to monitor filament micro-grooving processes. The variation of fluorescence spectral lines of SiⅠ390.55 nm reflects the removal rate of material surface with different processing parameters, which helps understand the filament ablated grooves processes. Although using plasma fluorescence to monitor filament ablated SiC CMC was demonstrated by the intensity measurement, the method can be in principle extended for online imaging the laser ablation process. [ABSTRACT FROM AUTHOR]

Through comprehensive experimental and modeling efforts, this work unravels the underlying mechanisms governing flame development and misfire at advanced engine conditions that are representative of low-load and lean blow-out operations. Toward this, preliminary heat release, autoignition, and flame developing patterns are characterized, via a case study of n-heptane, at ultra-lean conditions in a well-controlled optical engine under various combustion modes including homogeneous charge compression ignition (HCCI), partially premixed combustion (PPC), and reactivity-controlled compression ignition (RCCI). Changes in preliminary heat release and flame developing patterns at three overall equivalence ratios (0.12, 0.18, and 0.24) are first characterized under the PPC mode. Flame development characteristics including flame areas and number of initial flame kernels at close-to-misfire conditions are further extracted and compared across the HCCI, RCCI, and three PPC modes, with two distinctive and one transition regimes identified. Further analyses indicate that sustainable flame development and misfire are largely controlled by the spatial distribution of local equivalence ratio (phi) and local temperature in the mixture, which dictate the initial flame kernel generation and the subsequent flame propagation through localized preliminary heat release and autoignition. Chemical kinetic modeling is also undertaken, using a recently updated gasoline chemistry model, in conjunction with a backpropagation neural network, where the predicted ignition delay map well captures the different regions of flame development. Further kinetic analysis and heat rate of production per reaction analysis corroborate the CH2O planar laser-induced fluorescence experiments and highlight the important chemical kinetics that govern the initial flame development patterns. [ABSTRACT FROM AUTHOR]

Lead in any food is harmful even at low concentrations. In this study, a direct and highly sensitive lead analysis technique was developed for wheat flour using laser-induced fluorescence combined with laser-induced breakdown spectroscopy. Wheat flour was pressed into small pellets and ablated by a low-energy ultraviolet 266-nm laser. A tunable dye laser constructed in our laboratory was used to resonantly excite the lead. The optimized interpulse time delay was 400 ns. A calibration curve was constructed and the detection limit for lead was 73.8 ppb. This method could be used to directly and sensitively analyze wheat flour for trace concentrations of lead. [ABSTRACT FROM AUTHOR]

In interfacial science and microfluidics, there is an increasing need for improving the ability to measure flow velocity profiles in the sub-micrometer range to better understand transport phenomena at interfaces, such as liquid–solid interfaces. Current standard methods of velocimetry typically use particles as tracers. However, seed particles can encounter issues at liquid and solid interfaces, where charge interactions between particles and surfaces can limit their ability to measure near-wall flows accurately. Furthermore, in many flows, seed particles have a different velocity from that of their surrounding fluid, which the particles are intended to represent. Several molecular tracer-based velocimeters have been developed which can bypass these issues. However, they either have limited resolution for measurement near solid surfaces, such as for slip flows, or require pre-calibration. Laser-induced fluorescence photobleaching anemometry (LIFPA) is one such technique that is noninvasive and has achieved unprecedented nanoscopic resolution for flow velocity profile measurement. However, it also requires pre-calibration, which is unavailable for unknown flows. Here, we present a novel, calibration-free technique called travel time after photobleaching (TTAP) velocimetry, which can measure flow velocity profiles and near-wall flow with high spatiotemporal resolution. Furthermore, TTAP velocimetry is compatible with LIFPA, and thus, the two systems can be coupled to satisfy LIFPA's long-anticipated need for pre-calibration, enabling measurement of flow velocity profiles in unknown flows with salient resolution. [ABSTRACT FROM AUTHOR]

In this work, we establish a quantitative relationship between the fluorescence signal intensity of acetone and toluene and their concentration, and acetone/toluene planar laser‐induced fluorescence (PLIF) is developed to measure the concentrations of two components simultaneously, providing an equivalent ratio distribution of the flow field. Due to a thorough consideration of the tracer effect on each other's fluorescence signals, the uncertainty in the PLIF concentration measurement is reduced to 10.4%. Experimental results of OH‐PLIF and acetone/toluene PLIF indicate that the equivalence ratio distribution obtained by acetone/toluene PLIF in cold‐state flow fields can be employed to predict and analyze the trend of equivalence ratio distribution in the combustion field. [ABSTRACT FROM AUTHOR]

Controlling the ion velocity in an ion sheath by applying an alternating current (AC) voltage to an electrode and/or a substrate is critical in plasma material processes. To externally control the velocity distribution of incident ions on a substrate, the application of tailored-waveform AC voltages instead of sinusoidal voltages has garnered interest in recent years. In this study, to investigate temporal changes in ion-velocity distributions, we developed a time-resolved laser-induced fluorescence spectroscopy (LIF) system using a continuous-wave diode laser as an excitation-laser source. A time-resolved LIF system entails the capture of temporally continuous and spectrally discrete LIF spectra during an AC voltage cycle. By measuring temporal changes in the LIF signal intensity at various excitation-laser wavelengths, the argon-ion velocity distribution near the electrode following the AC voltage can be characterized. The results of applying sinusoidal, triangular, and rectangular bias waveforms indicate that the LIF measurement scheme proposed herein can be used to investigate the dynamic behavior of ion-velocity distributions controlled by tailored-waveform AC voltages. [ABSTRACT FROM AUTHOR]

Plastic pollution is a rising environmental issue, with millions of tons of plastic debris collecting in the world's seas and on its shores. Hyperspectral imaging (HSI) has become increasingly widely used as a more precise approach that can identify targets in remote sensing aquatic missions. The interference from other beach materials, and the need for proper identification of litter types can make identifying dumped plastics on sand-surrounded beaches challenging. This study lays the groundwork for a physical laboratory setting for images captured by a hyperspectral (HS) imager. The suggested testing setup included the development of a fluorescence signature for the target theater of operations (low-density polyethylene (LD-PE) and wood surrounded by sand) for detecting polymers in a simulated beach environment using the laser-induced fluorescence (LIF) approach. Initially using broadband-spectrum light, strong sample diffuse reflectance contrast is observed in the imaging at wavelengths between 400 and 460 nm. Next, a dedicated LIF system for plastic litter discovery was developed using an ultraviolet (UV) laser source. Initial findings show that there is a distinct fluorescence signal for plastics at 450 nm and at 750 nm for wood. Our pilot studies support current efforts to determine the optimum spectral signature that these polymers will appear with clarity on shorelines using an inexpensive imagery combined with our UV LIF approach, which may have an impact on applications for the detection of beach pollution. The knowledge gained from this study can be used to construct reliable aerial conventional cameras for plastic waste environmental monitoring and management. [ABSTRACT FROM AUTHOR]

In addressing the substantial greenhouse gas emissions produced by the energy-intensive Haber–Bosch synthesis, this study investigates the viability of sustainable nitrogen fixation (NF) via low-temperature plasma systems energized by renewable sources. Utilizing vibrational coherent anti-Stokes Raman scattering as a diagnostic tool, we probed the nitrogen rovibrational temperature and population dynamics within a DC glow discharge in atmospheric air, a setting with considerable promise for eco-friendly fertilizer production. Besides, density for atomic N , O , and NO was quantified by laser-induced fluorescence (LIF) or two-photon absorbed LIF methods. Our findings reveal a quasi-equilibrium between rotational and vibrational energy states in the DC glow discharge environment, reaching an approximate value of 3500 K at the discharge core. The discharge parameters, discharge current, air flow rate, and discharge gap influence the rovibrational temperature, density distribution of species of interest, and the NF energy cost. However, the influences induced by these parameters are of limitations. Further analysis implies that the high gas temperature and its induced significant vibrational-rotational and vibrational-translational energy exchange are mainly responsible for the non-ideal NF energy cost. [ABSTRACT FROM AUTHOR]

In this study, we explore the potential of using laser-induced photo-fragmentation of O3 by UV radiation as a quantitative diagnostic tool in non-thermal O2-mixed plasmas. We analyze the optical processes of O3 using a comprehensive kinetic model with a 226 nm laser, which is typically used in the two-photon absorption laser-induced fluorescence (TALIF) measurement of O atoms. Our model demonstrates that the fluorescence intensity from atomic O fragments produced by the same laser is directly proportional to the population of precursor O3. This makes various diagnostic purposes achievable through the proposed O3 full photo-fragmentation (FPF) TALIF spectroscopy, including calibration of TALIF signals of O atoms and quantification of both O and O3 in O2-mixed plasmas. We present detailed theoretical principles, technical requirements, and successful examples of implementation for different diagnostic aims using the proposed O3 FPF-TALIF spectroscopy. However, we also specify the limitations of the developed diagnostic methods, particularly under low E/N conditions (<30 Td), where other interferential species such as the vibrationally excited ground-state O 2 ( X 3 Σ g − , v ≠ 0) are abundantly produced. [ABSTRACT FROM AUTHOR]

We present the first experimental application of coherent Raman spectroscopy (CRS) on the ro-vibrational ν2 mode spectrum of methane (CH4). Ultrabroadband femtosecond/picosecond (fs/ps) CRS is performed in the molecular fingerprint region from 1100 to 2000 cm−1, employing fs laser-induced filamentation as the supercontinuum generation mechanism to provide the ultrabroadband excitation pulses. We introduce a time-domain model of the CH4ν2 CRS spectrum, including all five ro-vibrational branches allowed by the selection rules Δv = 1, ΔJ = 0, ±1, ±2; the model includes collisional linewidths, computed according to a modified exponential gap scaling law and validated experimentally. The use of ultrabroadband CRS for in situ monitoring of the CH4 chemistry is demonstrated in a laboratory CH4/air diffusion flame: CRS measurements in the fingerprint region, performed across the laminar flame front, allow the simultaneous detection of molecular oxygen (O2), carbon dioxide (CO2), and molecular hydrogen (H2), along with CH4. Fundamental physicochemical processes, such as H2 production via CH4 pyrolysis, are observed through the Raman spectra of these chemical species. In addition, we demonstrate ro-vibrational CH4v2 CRS thermometry, and we validate it against CO2 CRS measurements. The present technique offers an interesting diagnostics approach to in situ measurement of CH4-rich environments, e.g., in plasma reactors for CH4 pyrolysis and H2 production. [ABSTRACT FROM AUTHOR]

In this work, we investigated non-equilibrium plasma produced by nanosecond repetitively pulsed glow discharges applied across a lean premixed methane-air flame. The flame is stationary, axisymmetric, and laminar. The discharges are applied on the symmetry axis crossing the reactant gases, flame front, and product gases, allowing phase-locked averaged measurements and comparisons with axisymmetric numerical simulations. The thermal effect and methyl radical production are quantified in the discharge in the reactant gas region. One-dimensional, two-beam, hybrid, femtosecond-picosecond, coherent anti-Stokes Raman scattering is used to acquire spatial and temporal profiles of temperature and oxygen-to-nitrogen concentration ratio. Photo-fragmentation laser-induced fluorescence is used to acquire quantitative two-dimensional profiles of methyl radicals in the discharge providing the first quantitative imaging of methyl produced ahead of a flame by plasma-induced methane dissociation. The spatial profiles of temperature and oxygen-to-nitrogen concentration ratio are in steady state, indicating that individual discharges have an insignificant heating effect. Upper and lower bounds of the produced mole fraction of methyl radicals in the plasma are obtained due to uncertainties in the collisional quenching rates of excited state methylidyne radicals in the plasma. The discharges produce a maximum of 600–1100 ppm of methyl radicals upstream of the flame front within 25 ns. This amount is similar to the predicted methyl mole fraction for the flame without plasma and thus represents a significant chemical perturbation to the reactants upstream of the flame front. The produced methyl follows an exponential decay in the first microsecond after the discharge with a decay constant of 8 µs close to the flame, and 0.8 µs further from the flame. The decay then deviates from the exponential curve and the methyl persists for tens of microseconds. The results suggest that for the tested configuration, the thermal effect of individual discharges through fast gas heating is negligible, while active chemical species are produced in large quantities in the reactant gases, upstream of the flame front. [ABSTRACT FROM AUTHOR]

The formation and transportation of short-lived species on/within the plasma-liquid interfacial layer plays a crucial role in various applications because of their high chemical reactivity. However, the experimental detection and quantification of these short-lived species, such as ˙OH radicals, at the gas–liquid interface still pose formidable challenges. This study confronts this challenge by employing incident microscopic laser-induced fluorescence (mLIF) method to capture the OH-LIF signals on the interfacial layer at different time moments of the post-discharge phase under high spatial resolution. The temporal evolution of ˙OH density is subsequently quantified by fitting the OH-LIF decay behavior to a reaction-dissolution model. Results reveal that increasing the pulse width serves better to enhance ˙OH generation on liquid surface, reaching a density of 1.25 × 1016 cm−3. Furthermore, the cathode-solution interface demonstrates significantly enhanced ˙OH production compared to the anode-solution interface. These results underscore the efficacy of incident mLIF in quantitatively probing short-lived ˙OH-radical production at the interfacial layer in pulsed-driven plasma-solution interactions, with potential applicability to other reactive species. [ABSTRACT FROM AUTHOR]

Sulfur–chlorine cycles play a role in the atmosphere of Venus. It is thought that many sulfur–chlorine bearing molecules could be present in Venus's atmosphere and play an important role in its chemical processes. The goal of this work is to provide new insight into the electronic structure and spectroscopy of the [Cl, S, S, O] molecular system. Eight isomers could be formed, but only three were found to be thermodynamically stable relative to the first dissociation limit. We spectroscopically characterized the two lowest energy stable isomers, C1–ClSSO and trans-ClSSO, using the accurate CCSD(T)-F12/aug-cc-pVTZ method. The dipole moments of the two lowest energy stable isomers are predicted to be 1.90 and 1.60 debye, respectively. The C1–ClSSO isomer is suitable for laser induced fluorescence detection since the lowest excited electronic states absorb in the visible, ∼610 nm, and near UV region, 330 nm. We mapped the evolution of the low-lying excited electronic states along the ClS, SS, and SO bond lengths to find that the production of ClS, SO, or S2O is plausible, whereas the production of ClS2 is not allowed. [ABSTRACT FROM AUTHOR]

The H2CSn and D2CSn molecules have been detected for the first time by laser-induced fluorescence (LIF) and emission spectroscopic techniques through the B ̃ 1 B 2 − X ̃ 1 A 1 electronic transition in the 425–400 nm region. These reactive species were prepared in a pulsed electric discharge jet using (CH3)4Sn or (CD3)4Sn diluted in high-pressure argon. Transitions to the electronic excited state of the jet-cooled molecules were probed with LIF, and the ground state and low-lying A ̃ 1 A 2 state energy levels were measured from single vibronic level emission spectra. We supported the experimental studies by a variety of ab initio calculations that predicted the energies, geometries, and vibrational frequencies of the ground and lower excited electronic states. The spectroscopy of stannylidene (H2CSn) is in many aspects similar to that of silylidene (H2CSi) and germylidene (H2CGe). [ABSTRACT FROM AUTHOR]

The blood flow through our microvascular system is a renowned difficult process to understand because the complex flow behavior of blood is intertwined with the complex geometry it has to flow through. Conventional 2D microfluidics has provided important insights, but progress is hampered by the limitation of 2-D confinement. Here we use selective laser-induced etching to excavate non-planar 3-D microfluidic channels in glass that consist of two generations of bifurcations, heading towards more physiological geometries. We identify a cross-talk between the first and second bifurcation only when both bifurcations are in the same plane, as observed in 2D microfluidics. Contrarily, the flow in the branch where the second bifurcation is perpendicular to the first is hardly affected by the initial distortion. This difference in flow behavior is only observed when red blood cells are aggregated, due to the presence of dextran, and disappears by increasing the distance between both generations of bifurcations. Thus, 3-D structures scramble in-plane flow distortions, exemplifying the importance of experimenting with truly 3D microfluidic designs in order to understand complex physiological flow behavior. [ABSTRACT FROM AUTHOR]

Phase change materials based on organics and salt hydrates with large latent heats of transition are used extensively in energy storage systems; those based on low melting alloys exhibiting electrical/optical characteristics switching with amorphous‐crystalline (A ↔ C) transformations are of major interest in information storage devices. The direct laser write‐read‐erase is reported using a functional molecular phase change material. Facile and reversible A ↔ C transformations with concomitant switching of fluorescence emission color and intensity are demonstrated in polymer thin films doped with a diaminodicyanoquinodimethane based fluorophore using thermal operations as well as laser irradiation. In the mask‐less direct write‐erase process developed, the laser power and irradiation time are tuned to write and erase; the reading is carried out by exploiting the characteristic fluorescence signature. This work opens up a novel avenue to develop sensors and encryption systems exploiting organic molecule based optical materials encapsulated in polymer thin films. [ABSTRACT FROM AUTHOR]

Enhancement of fluorescence emission in a flexible and free‐standing fluorescing film is a key requirement for sensing platforms with augmented sensitivity. In this context, a study on the enhanced fluorescence emission from nitrogen‐doped carbon dots (NCDs) embedded on a flexible free‐standing photonic crystal hydrogel film prepared via photopolymerization, is presented. The composite structure utilizes the photonic crystal enhanced fluorescence (PCEF) technique and incorporates a self‐assembled 3D photonic crystal (3D PC) onto a photopolymerizable hydrogel matrix containing the NCDs. The 3D PC template is prepared through vertical deposition self‐assembly using monodisperse polystyrene (PS) spheres. By leveraging the enhanced excitation and extraction effect in a PC‐fluorophore composite, the authors' structure exhibits a fourfold enhancement in fluorescence emission compared to the control sample. The relative positioning of the photonic stopband with the excitation and emission spectra of the fluorophore (NCDs) is thoroughly studied by selecting four different 3D PCs with varied lattice parameters. In addition, the hydrogel matrix offers improved photostability and enhanced lifetime for the NCDs. This structure can be further modified into an efficient sensor through appropriate functionalization. [ABSTRACT FROM AUTHOR]

The statistical behaviour and modelling of turbulent fluxes of the reaction progress variable and non-dimensional temperature in the context of Reynolds-Averaged Navier–Stokes (RANS) simulations have been analysed for flame–wall interactions within turbulent boundary layers. Three-dimensional Direct Numerical Simulation (DNS) databases of two different flame–wall interaction configurations—(i) statistically stationary oblique wall quenching (OWQ) of a V-flame in a turbulent channel flow and (ii) unsteady head-on quenching (HOQ) of a statistically planar flame propagating across a turbulent boundary layer—have been considered for this analysis. Scalar fluxes of both the temperature and reaction progress variable exhibit counter-gradient behaviour at all times during unsteady HOQ of statistically planar turbulent premixed flames considered here. In the case of statistically stationary V-flame OWQ, the scalar fluxes of both reaction progress variable and temperature exhibit counter-gradient behaviour before quenching, but gradient behaviour has been observed close to the wall once the flame begins to quench. The weakening of the effects of thermal expansion close to the wall as a result of flame quenching gives rise to a gradient type of transport for the streamwise component in the oblique quenching of the V-flame. It has been found that the relative orientation of the flame normal vector with respect to the wall normal vector needs to be accounted for in the algebraic scalar flux closure, which can be applied to different flame/flow configurations. An existing algebraic scalar flux model has been modified in this analysis for flame–wall interaction within turbulent boundary layers, and it has been demonstrated to capture the turbulent fluxes of the reaction progress variable and non-dimensional temperature reasonably accurately for both configurations considered here based on a priori DNS analysis. [ABSTRACT FROM AUTHOR]

In this study, the fluorescence properties of Lumisis, a phosphor that can be easily applied to ultrafine wires, were evaluated. By evaluating the wavelength characteristics of Lumisis phosphor, we investigated the possibility of applying it to a dual-wavelength laser-induced fluorescence (LIF) measurement system and evaluated the accuracy of temperature measurements. The difference between the decrease in the percentage intensities of the red and green fluorescence of Lumisis phosphors showed that two-color LIF was possible. The Lumisis phosphor–mixture ratio was optimized as 1:1.25, and the average measurement error of the fluorescent wire was 0.20 K, as evaluated through uncertainty analysis. Finally, the application of this measurement method to hot air jet phenomena showed that this method accurately captures the temperature changes in hot air, thus proving its validity. [ABSTRACT FROM AUTHOR]

Effective cleaning of tin contamination on the collecting mirrors in extreme ultraviolet source is one of the key techniques to improve throughput and cost performance of extreme ultraviolet lithography. Hydrogen radicals produced in hydrogen plasma that is induced by wideband extreme ultraviolet radiation are expected to be utilized for in situ tin contamination cleaning in extreme ultraviolet sources. In this Letter, we clarified absolute density and cleaning ability of the hydrogen radicals produced by intense extreme ultraviolet pulse through ground state population density measurement by laser-induced fluorescence technique. The experimentally obtained radical parameters coincided well with simulation results and collisional radiative model. It was found that the extreme ultraviolet induced plasma was in quasi-steady state with abundant amount of hydrogen radicals in ground state. Further, it was found that the in situ tin contamination cleaning in extreme ultraviolet lithography source would become more practical with increase in operational parameters, such as extreme ultraviolet emission intensity, gas pressure, and radical production cross section. [ABSTRACT FROM AUTHOR]

A time-resolved experimental investigation was undertaken on the temperature evolution of Rayleigh–Bénard convection (RBC) in a slender convection cell with aspect ratio of Γ = 0.1. Experiments were conducted for Rayleigh numbers of R a = 5.3 × 10 7 , 7.6 × 10 7 , and 9.5 × 10 7 and Prandtl number of P r ≈ 6 within the non-Oberbeck–Boussinesq (NOB) condition with a temperature difference variation in the range of 30 ° C ≤ Δ T ≤ 40 ° C. Measurement of the temperature was by applying time-resolved two-color planar laser-induced fluorescence over the initial 2400 s. Experimental observations showed that the lateral confinement of the convection cell leads to the development of a single large-scale thermal plume instead of multiple plumes. Results showed that contrary to expectations, lateral confinement was found to be ineffective in suppressing temperature oscillations near thermal boundaries. Results also indicated that for R a = 5.3 × 10 7 , 7.6 × 10 7 , the temperature oscillations had a frequency of f ≈ 0.028 Hz similar to the frequency of the oscillations in Oberbeck–Boussinesq (OB) RBC. For R a = 9.5 × 10 7 , however, it was found that the frequency of the oscillations was much lower than the OB RBC with a relatively wide range of the oscillations in the vicinity of f ≈ 0.006 Hz. It is also found that the lateral confinement and formation of singular high-energy thermal plumes leads to an increase in the nonsymmetrical temperature distribution of NOB RBC with a bimodal distribution of the temperature field, deviating significantly from the Gaussian distribution temperature field found in OB RBC. [ABSTRACT FROM AUTHOR]