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Results for “angular distributions”

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

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At least 505 records · Page 28
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Unveiling the orbital texture of 1T-TiTe 2 using intrinsic linear dichroism in multidimensional photoemission spectroscopy

The momentum-dependent orbital character in crystalline solids, referred to as orbital texture, is of capital importance in the emergence of symmetry-broken collective phases, such as charge density waves as well as superconducting and topological states of matter. By performing extreme ultraviolet multidimensional angle-resolved photoemission spectroscopy for two different crystal orientations linked to each other by mirror symmetry, we isolate and identify the role of orbital texture in photoemission from the transition metal dichalcogenide 1T-TiTe 2 . By comparing our experimental results with theoretical calculations based on both a quantitative one-step model of photoemission and an intuitive tight-binding model, we unambiguously demonstrate the link between the momentum-dependent orbital orientation and the emergence of strong intrinsic linear dichroism in the photoelectron angular distributions. Our results represent an important step towards going beyond band structure (eigenvalues) mapping and learning about electronic wavefunction and orbital texture of solids by exploiting matrix element effects in photoemission spectroscopy.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Asymmetries in ionization of atomic superposition states by ultrashort laser pulses

Abstract Progress in ultrafast science allows for probing quantum superposition states with ultrashort laser pulses in the new regime where several linear and nonlinear ionization pathways compete. Interferences of pathways can be observed in the photoelectron angular distribution and in the past they have been analyzed for atoms and molecules in a single quantum state via anisotropy and asymmetry parameters. Those conventional parameters, however, do not provide comprehensive tools for probing superposition states in the emerging research area of bright and ultrashort light sources, such as free-electron lasers and high-order harmonic generation. We propose a new set of generalized asymmetry parameters which are sensitive to interference effects in the photoionization and the interplay of competing pathways as the laser pulse duration is shortened and the laser intensity is increased. The relevance of the parameters is demonstrated using results of state-of-the-art numerical solutions of the time-dependent Schrödinger equation for ionization of helium atom and neon atom.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Towards isolated attosecond electron bunches using ultrashort-pulse laser-solid interactions

We investigate MeV-level attosecond electron bunches from ultrashort-pulse laser-solid interactions through similarities between experimental and simulated electron energy spectra. We show measurements of the bunch duration and temporal structure from particle-in-cell simulations. The experimental observation of such bunches favors specular reflection direction when focusing the laser pulse onto a subwavelength boundary of thick overdense plasmas at grazing incidence. Particle-in-cell simulation further reveals that the attosecond duration is a result of ultra-thin (~tenth of a micron) gaps of zero electromagnetic energy density in the modulated reflected radiation, while the bunching (locally peaked electron concentration) comes from the highly-directional electron angular distribution acquired by the electrons in a grazing incidence setup. To isolate a single electron bunch, we perform simulations using 1-cycle laser pulses and analyze the effect of carrier-envelop phase with particle tracking. The duration of the electron bunch can be further decreased by increasing the laser intensity and the focal spot size, while its direction can be changed by tuning the preplasma density gradient.

High-harmonic generation↗
DOE OSTI2023

Golden ratio in venation patterns of dragonfly wings

Abstract The vein pattern in insect wings allows this lightweight structure to carry multiple biological functions. Here, an investigation of the angular distribution of the vein struts in dragonfly wings revealed that the golden angle or golden ratio dominates the venation patterns. We find that the golden angle dominates the intervein angles in regions where thin veins and membranes demand strength reinforcement. A golden ratio partition method has thus been developed that explains a set of preferred intervein angles in distorted polygon-shaped venation cells throughout the venation pattern in dragonfly wings. These observations provide new evidence that the wing structure is spatially optimized, by the golden rule in nature, for supporting biomechanical functions of dragonfly wings.

36 MATERIALS SCIENCE↗
DOE OSTI2023

A multi-MeV alpha particle source via proton-boron fusion driven by a 10-GW tabletop laser

Nuclear fusion between protons and boron-11 nuclei has undergone a revival of interest thanks to the rapid progress in pulsed laser technology. Potential applications of such reaction range from controlled nuclear fusion to radiobiology and cancer therapy. A laser-driven fusion approach consists in the interaction of high-power, high-intensity pulses with H- and B-rich targets. We report on an experiment exploiting proton-boron fusion in CN-BN targets to obtain high-energy alpha particle beams (up to 5 MeV) using a very compact approach and a tabletop laser system with a peak power of ~10 GW, which can operate at high-repetition rate (up to 1 kHz). The secondary resonance in the cross section of proton-boron fusion (~150 keV in the center-of-mass frame) is exploited using a laser-based approach. The generated alpha particles are characterized in terms of energy, flux, and angular distribution using solid-state nuclear-track detectors, demonstrating a flux of ~10 5 particles per second at 10 Hz, and ~10 6 per second at 1 kHz. Hydrodynamic and particle-in-cell numerical simulations support our experimental findings. Potential impact of our approach on future spread of ultra-compact, multi-MeV alpha particle sources driven by moderate intensity (10 16 -10 17 W/cm 2 ) laser pulses is anticipated.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Subpicosecond HI elimination in the 266 nm photodissociation of branched iodoalkanes

Here, the 266 nm photodissociation dynamics of 1-iodopropane and 2-iodopropane were studied using photofragment translational energy spectroscopy using vacuum ultraviolet (VUV) photoionization and electron impact ionization detection of products. The photochemistry of 1-iodopropane was found to be similar to that of iodomethane and iodoethane, with dominant production of I*( 2 P 1/2 ), and no evidence (<0.21%) for HI + alkene formation. Significantly different behavior was observed for 2-iodopropane, with dominant production of ground state I( 2 P 3/2 ), and a HI yield >10.5%. The anisotropy (β) parameters for all channels approached the limiting value of 2.0, indicating that 1,2-HI elimination occurs on subpicosecond timescales, like direct C–I bond fission, following excitation to 3 Q 0 . The HI translational energy and angular distributions were similar to those for I( 2 P 3/2 ), suggesting that motion of the heavy I atom in HI is largely derived from the repulsive nature of the 1 Q 1 surface correlating to R + I with the light H atom picked up by ground state I late in the exit channel producing highly vibrationally excited HI.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Selective bond-breaking in formic acid by dissociative electron attachment

We report the results of a joint experimental and theoretical study of dissociative electron attachment to formic acid (HCOOH) in the 6–9 eV region, where H- fragment ions are a dominant product. Breaking of the C–H and O–H bonds is distinguished experimentally by deuteration of either site. We show that in this region H- ions can be produced by formation of two or possibly three Feshbach resonance (doubly-excited anion) states, one of which leads to either C–H or O–H bond scission, while the other can only produce formyloxyl radicals by O–H bond scission. Comparison of experimental and theoretical angular distributions of the anion fragment allows the elucidation of state specific pathways to dissociation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Photodissociation of iso-propoxy (i-C 3 H 7 O) radical at 248 nm

Photodissociation of the i-C 3 H 7 O radical is investigated using fast beam photofragment translational spectroscopy. Neutral i-C 3 H 7 O radicals are produced through the photodetachment of a fast beam of i-C 3 H 7 O - anions and are subsequently dissociated at 248 nm (5.0 eV). Furthermore, the dominant product channels are CH 3 + CH 3 CHO and OH + C 3 H 6 with some contribution from H + C 3 H 6 O. The CH 3 and H loss channels are attributed to dissociation on the ground electronic state of i-C 3 H 7 O, but in a nonstatistical manner because calculated RRKM dissociation rates exceed the rate of energy randomization. Translational energy and angular distributions for OH loss are consistent with ground state dissociation, but the branching ratio for this channel is considerably higher than predicted from RRKM rate calculations. Additionally, i-C 3 H 7 O undergoes three-body fragmentation to CH 3 + CH 3 + HCO and CH 3 + CH 4 + CO. These three-body channels are attributed to dissociation of i-C 3 H 7 O to CH 3 + CH 3 CHO, followed by secondary dissociation of CH 3 CHO on its ground electronic state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

X-ray photoelectron spectroscopy of surfactants on sub-micron aqueous aerosols

Organic molecules at the aqueous interfaces of droplets and aerosols can influence multiphase chemistry and cloud condensation nuclei activity. While surface tension measurements on flat surfaces are commonly used to quantify organic partitioning and structure, extending these measurements to more realistic aerosols that might exist in metastable, supercooled and supersaturated states remains a challenge. Here, we use aerosol velocity map imaging X-ray photoelectron spectroscopy (A-VMI-XPS), a surface-sensitive and in situ technique, to study the partitioning and structure of a model surfactant (n-octyl β-D-thioglucopyranoside, OTG) in submicron aqueous aerosols with a mean radius of 116 nm. After accounting for finite size effects and evaporative cooling, we find the bulk concentrations of OTG in the aerosol are depleted 600-fold relative to macroscopic solutions. At the low temperatures of the experiment (ca. ∼188 K), we obtain a Langmuir equilibrium constant of 700 m3 mol-1, which corresponds to 4.9 m3 mol-1 at room temperature; a value that is consistent with prior literature reports. Analysis of photoelectron angular distributions, peak areas, and secondary electron escape barriers indicates a transition from a disordered surfactant layer at low [OTG] to a more structured layer at high [OTG]. These results link macroscopic surface tension measurements to nanoparticle surfactant behavior and demonstrate the utility of A-VMI-XPS in probing surfactant coating structure on free aerosols, with implications for understanding the impact of organic coatings on cloud formation and atmospheric chemistry.

Deal, Alexandra M↗
DOE OSTI2020

Opportunities for detailed fission studies using light charged particle reactions

Since its discovery in 1939, the nuclear fission process has provided much insight into the behavior of nuclei under many different conditions. As part of the nuclear chain reaction, the fission process has had a profound impact on modern society and it has consequently attracted much attention to the field of nuclear physics. In this talk, I will argue that the time is ripe for a resumption of studies of the fission process induced by light charged particle reactions. Although fission can be induced in heavy nuclei by several means, in some cases these methods suffer from the complication that fission can occur at several points during the decay chain thus mixing up contributions from different excitation energies. Using instead light charged particle reactions to excite the nuclei in question, the precise excitation energy from which fission takes place, can be determined. In fact, a number of such studies were carried out previously, and a first set of results on fission barrier heights, mass, energy and angular distributions were obtained. Applying detection techniques developed over the last decades will allow researchers to obtain detailed, high-quality data from which to probe and refine our present understanding of the process. Based on these observations, I suggest that substantial advances in the study of this process can be achieved by using simple light charged particle reactions.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Experiments with neutron induced neutron emission from U-235, Pu-239, and graphite

A neutron induced neutron emission experiment was conducted as the Los Alamos Neutron Science Center (LANSCE) facility at Los Alamos National Laboratory (LANL). In this experiment, a sample was placed in a well collimated neutron beam and was surrounded by an array of 28 fast neutron detectors (EJ-309). The experiment was performed with a neutron flight path of 21.5 m from the source to the sample, and 1 m from the sample to the detectors. The neutron emission from the sample was measured as a function of neutron time of flight covering an incident energy range from 0.7- 20 MeV. The samples included U-235, Pu-239, carbon (graphite), and blanks that matched the encapsulation of the sample. The measured samples were constantly cycled in and out of the neutron beam. This type of experiment measures neutron emission from all reactions occurring in the sample such as fission and elastic and inelastic scattering. Similar to the methodology previously developed at RPI, the measurements were compared with detailed simulations of the experiment using different cross section evaluations for the sample. The observed differences can be attributed to the evaluated neutron cross section and angular distributions. The carbon sample was used as a reference to validate both the experiment and simulation methodology and showed good agreement between experiments and simulations. A review of the experimental setup, analysis methods, and some of the results will be presented.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Photoinduced charge transfer in the Zn-methanol cation studied with selected-ion photofragment imaging

The Zn + (methanol) ion molecule complex produced by laser vaporization is studied with photofragment imaging at 280 and 266 nm. Photodissociation produces the methanol cation CH 3 OH + via excitation of a charge-transfer excited state. Surprisingly, excitation of bound excited states produces the same fragment via a curve crossing prior to separation of products. Significant kinetic energy release is detected at both wavelengths with isotropic angular distributions. Similar experiments are conducted on the perdeuterated methanol complex. The Zn + cation is a minor product channel that also exhibits significant kinetic energy release. Finally, an energetic cycle using the ionization energies of zinc and methanol together with the kinetic energy release produces an upper limit on the Zn + -methanol bond energy of 33.7 ± 4.2 kcal/mol (1.46 ± 0.18 eV).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Strongly coupled intermediate electronic states in one-color two-photon single valence ionization of O 2

Here, we present an experimental and theoretical energy- and angle-resolved investigation on the non-dissociative photoionization dynamics of near-resonant, one-color, two-photon, single valence ionization of neutral O 2 molecules. Using 9.3 eV femtosecond pulses produced via high harmonic generation and a 3-D momentum imaging spectrometer, we detect the photoelectrons and O$^{+}_{2}$ cations produced from one-color, two-photon ionization in coincidence. The measured and calculated photoelectron angular distributions show agreement, which indicates that a superposition of two intermediate electronic states is dominantly involved and that wavepacket motion on those near-resonantly populated intermediate states does not play a significant role in the measured two-photon ionization dynamics. Here, we find greater utility in the diabatic representation compared to the adiabatic representation, where invoking a single valence-character diabat is sufficient to describe the underlying two-photon ionization mechanism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Self-consistent integrated modeling of combined hybrid discharge-laser produced plasma devices for extreme ultraviolet metrology

Discharge- and laser-produced plasma (DLPP) devices are being used as light sources for extreme ultraviolet (EUV) generation. A key challenge for both, DPP and LPP, is achieving sufficient brightness to support the throughput requirements of nanometrology tools. To simulate the environment of a hybrid DLPP device and optimize the EUV output, we have developed an integrated HEIGHTS-DLPP computer simulation package. The package integrates simulation of two evolving plasmas (DPP and LPP) and includes modeling of a set of integrated self-consistent processes: external power source and plasma energy balance, plasma resistive magnetohydrodynamics, plasma heat conduction, detailed radiation transport (RT), and laser absorption and refraction. We simulated and optimized DLPP devices using Xe gas as a target material. We synchronized the external circuit parameters, chamber gas parameters, and laser beam temporal and spatial profiles to achieve maximum EUV output. The full 3D Monte Carlo scheme was integrated for detailed RT and EUV output calculations in Xe using more than 3600 spectral groups. The modeling results are in good agreement with Julich Forschungszentrum experimental data. Theoretical models, developed and integrated into the HEIGHTS package, showed wide capabilities and flexibility. In conclusion, the models and package can be used for optimization of the experimental parameters and settings, investigation of DLPP devices with complex design, analyzing the impact of integrated spatial effects and working timeline arrangement on the final EUV output, and EUV source size, shape, and angular distribution.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Wave packet dynamics and control in excited states of molecular nitrogen

Wave packet interferometry with vacuum ultraviolet light has been used to probe a complex region of the electronic spectrum of molecular nitrogen, N 2 . Wave packets of Rydberg and valence states were excited by using double pulses of vacuum ultraviolet (VUV), free-electron-laser (FEL) light. These wave packets were composed of contributions from multiple electronic states with a moderate principal quantum number (n ~ 4-9) and a range of vibrational and rotational quantum numbers. The phase relationship of the two FEL pulses varied in time, but as demonstrated previously, a shot-by-shot analysis allows the spectra to be sorted according to the phase between the two pulses. The wave packets were probed by angle-resolved photoionization using an infrared pulse with a variable delay after the pair of excitation pulses. The photoelectron branching fractions and angular distributions display oscillations that depend on both the time delays and the relative phases of the VUV pulses. The combination of frequency, time delay, and phase selection provides significant control over the ionization process and ultimately improves the ability to analyze and assign complex molecular spectra.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Voltage waveform tailoring for high aspect ratio plasma etching of SiO 2 using Ar/CF 4 /O 2 mixtures: Consequences of low fundamental frequency biases

The use of non-sinusoidal waveforms in low pressure capacitively coupled plasmas intended for microelectronics fabrication has the goal of customizing ion and electron energy and angular distributions to the wafer. One such non-sinusoidal waveform uses the sum of consecutive harmonics of a fundamental sinusoidal frequency, f 0 , having a variable phase offset between the fundamental and even harmonics. In this paper, we discuss results from a computational investigation of the relation between ion energy and DC self-bias when varying the fundamental frequency f 0 for capacitively coupled plasmas sustained in Ar/CF 4 /O 2 and how those trends translate to a high aspect ratio etching of trenches in SiO 2 . The fundamental frequency, f 0 , was varied from 1 to 10 MHz and the relative phase from 0° to 180°. Two distinct regimes were identified. Average ion energy onto the wafer is strongly correlated with the DC self-bias at high f 0 , with there being a maximum at φ = 0° and minimum at φ = 180°. In the low frequency regime, this correlation is weak. Average ion energy onto the wafer is instead dominated by dynamic transients in the applied voltage waveforms, with a maximum at φ = 180° and minimum at φ = 0°. The trends in ion energy translate to etch properties. In both, the high and low frequency regimes, higher ion energies translate to higher etch rates and generally preferable final features, though behaving differently with phase angle.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Resonant Auger decay of dissociating CH 3 I near the I 4d threshold

Resonant Auger processes provide a unique perspective on electronic interactions and excited vibrational and electronic states of molecular ions. Here, new data are presented on the resonant Auger decay of excited CH 3 I in the region just below the I 4d -1 ionization threshold. The resonances include the Rydberg series converging to the five spin–orbit and ligand-field split CH 3 I (I 4d -1 ) thresholds, as well as resonances corresponding to excitation from the I 4d 5/2,3/2 orbitals into the σ* lowest unoccupied molecular orbital. This study focuses on participator decay that populates the lowest lying states of CH 3 I + , in particular, the X̃ 2 E 3/2 and 2 E 1/2 states, and on spectator decay that populates the lowest-lying (CH 3 I 2+ )σ* states of CH 3 I + . The CH 3 I (I 4d -1 )σ* resonances are broad, and dissociation to CH 3 + I competes with the autoionization of the core-excited states. Auger decay as the molecule dissociates produces a photoelectron spectrum with a long progression (up to v 3 + ~ 25) in the C–I stretching mode of the X̃ 2 E 3/2 and 2 E 1/2 states, providing insights into the shape of the dissociative core-excited surface. Further, the observed spectator decay processes indicate that CH 3 I + is formed on the repulsive wall of the lower-lying (CH 3 I 2+ )σ* potentials, and the photon-energy dependence of the processes provides insights into the relative slopes of the (4d -1 )σ* and (CH 3 I 2+ )σ* potential surfaces. Data are also presented for the spectator decay of higher lying CH 3 I (I 4d -1 )nl Rydberg resonances. Photoelectron angular distributions for the resonant Auger processes provide additional information that helps distinguish these processes from the direct ionization signal.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Proton rings from late-forming ballistic sheath fields

Many laser-driven ion experiments have seen ring-like patterns in the proton angular distribution across a wide array of laser and target parameters. These rings can impede measurement due to the small acceptance angle of detectors and often inhibit potential applications. A myriad of explanations for their formation have been proposed, yet most studies attribute them to some aspect of the laser–plasma interaction. Using 3D particle-in-cell simulations, we show that late-forming strong radial electric fields can arise due to charge separation while the beam is in flight, long after the laser–plasma interaction. These fields can accelerate ions to significant divergences (≈ 10°) as they propagate away from the target. We compare our results to a recent experiment where a high intensity, short pulse laser (I 0 ≈ 10 21 W/cm 2 , τ ≈ 30 fs) was incident upon thin (≈ 1 μm) liquid crystal targets. Our simulations capture all the main features of the experimental results—namely, robust ring formation and larger rings for higher energy protons. In addition, we show that rings do not form for sufficiently short preplasma scale lengths. Finally, we develop a phenomenological model to describe the spatiotemporal structure of the radial electric field and use this to explain the proton rings' energy and preplasma dependencies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗