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

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At least 1,675 records · Page 93
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Time-resolved ion imaging at free-electron lasers using TimepixCam

In this paper, the application of a novel fast optical-imaging camera, TimepixCam, to molecular photoionization experiments using the velocity-map imaging technique at a free-electron laser is described. TimepixCam is a 256 × 256 pixel CMOS camera that is able to detect and time-stamp ion hits with 20 ns timing resolution, thus making it possible to record ion momentum images for all fragment ions simultaneously and avoiding the need to gate the detector on a single fragment. This allows the recording of significantly more data within a given amount of beam time and is particularly useful for pump–probe experiments, where drifts, for example, in the timing and pulse energy of the free-electron laser, severely limit the comparability of pump–probe scans for different fragments taken consecutively. Finally, in principle, this also allows ion–ion covariance or coincidence techniques to be applied to determine angular correlations between fragments.

47 OTHER INSTRUMENTATION↗
DOE OSTI2018

Study of Triple Ar Gas Puff Z-Pinches on 0.9-MA, 200-ns COBRA

Ar gas puff z-pinch experiments were conducted on the 0.9 MA, 200 ns COBRA generator at Cornell University. In the experiments, a triple-nozzle gas valve was used to produce the zpinch load with concentric outer and inner gas puffs and a central gas jet. We used Planer Laser Induced Fluorescence (PLIF) to measure the initial gas profile of the load, two 4-frame 4-ns gated XUV cameras to image the imploding plasma, and filtered Photo- Conducting Diamond Detectors (PCDs) to measure the x-ray output. We have observed shock heating and/or photoionization of the dense center jet by the imploding plasma. With an outer to inner plenum pressure ratio of 1:3, de-acceleration of the imploding plasma occurred when the outer plasma shell imploded on the inner shell resulting in a stable implosion. By varying the plenum pressure for the center jet, the x-ray emission was optimized. In conclusion, an Ar K-shell x-ray (3-4 keV) yield of 77±17 J was produced at a current level of 0.87±0.2 MA and an implosion time of 200-ns.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2017

Tailoring Charge Reactivity Using In-Cylinder Generated Reformate for Gasoline Compression Ignition Strategies

In-cylinder reforming of injected fuel during a negative valve overlap (NVO) recompression period can be used to optimize main-cycle combustion phasing for low-load low-temperature gasoline combustion (LTGC). The objective of this work is to examine the effects of reformate composition on main-cycle engine performance. An alternate-fire sequence was used to generate a common exhaust temperature and composition boundary condition for a cycle-of-interest, with performance metrics measured for these custom cycles. NVO reformate was also separately collected using a dump valve apparatus and characterized by both gas chromatography and photoionization mass spectroscopy. To facilitate gas sample analysis, sampling experiments were conducted using a five-component gasoline surrogate (isooctane, n-heptane, ethanol, 1-hexene, and toluene) that matched the molecular composition, 50% boiling point, and ignition characteristics of the research gasoline. For the gasoline, it was found that an advance of the NVO start-of-injection (SOI) led to a corresponding advance in main-period combustion phasing as the combination of longer residence times and lower amounts of liquid spray piston impingement led to a greater degree of fuel decomposition. The effect was more pronounced as the fraction of total fuel injected in the NVO period increased. Main-period combustion phasing was also found to advance as the main-period fueling decreased. Slower kinetics for leaner mixtures were offset by a combination of increased bulk-gas temperature from higher charge specific heat ratios and increased fuel reactivity due to higher charge reformate fractions.

42 ENGINEERING↗
DOE OSTI2020

Accuracy limitations for composition analysis by XPS using relative peak intensities: LiF as an example

Although precision in XPS can be excellent, allowing small changes to be easily observed, obtaining accurate absolute elemental composition of a solid material from relative peak intensities is generally much more problematical, involving many factors: background removal; differing analysis depths at different photoelectron kinetic energies; possible angular distribution effects; calibration of the instrument transmission function, and variations of the distribution of the photoelectron intensity between “main” peaks (those usually used for analysis) and associated substructure following the main peak, as a function of the chemical bonding of the elements concerned. The last item, coupled with the use of photoionization cross-sections and/or relative sensitivity factors, is the major subject of this paper, though it is necessary to consider the other items also, using LiF as a test case. The results show that the above issues, which are relevant to differing degrees in most XPS analyses, present significant challenges to highly accurate XPS quantification.

Brundle, Christopher R.↗
DOE OSTI2018

Reconstruction of the time-dependent electronic wave packet arising from molecular autoionization

Autoionizing resonances are paradigmatic examples of two-path wave interferences between direct photoionization, which takes a few attoseconds, and ionization via quasi-bound states, which takes much longer. Time-resolving the evolution of these interferences has been a long-standing goal, achieved recently in the helium atom owing to progress in attosecond technologies. However, already for the hydrogen molecule, similar time imaging has remained beyond reach due to the complex interplay between fast nuclear and electronic motions. We show how vibrationally resolved photoelectron spectra of H2 allow one to reconstruct the associated subfemtosecond autoionization dynamics by using the ultrafast nuclear dynamics as an internal clock, thus forgoing ultrashort pulses. Our procedure should be general for autoionization dynamics in molecules containing light nuclei, which are ubiquitous in chemistry and biology.

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

Bond-length dependence of attosecond ionization delays in O 2 arising from electron correlation to a shape resonance

We experimentally and theoretically demonstrate that electron correlation can cause the bond-length sensitivity of a shape resonance to induce an unexpected vibrational state–dependent ionization delay in a nonresonant channel. This discovery was enabled by a high-resolution attosecond-interferometry experiment based on a 400-nm driving and dressing wavelength. The short-wavelength driver results in a 6.2–electron volt separation between harmonics, markedly reducing the spectral overlap in the measured interferogram. We demonstrate the promise of this method on O 2 , a system characterized by broad vibrational progressions and a dense photoelectron spectrum. We measure a 40-attosecond variation of the photoionization delays over the X 2 Π g vibrational progression. Multichannel calculations show that this variation originates from a strong bond-length dependence of the energetic position of a shape resonance in the b 4 Σ$^{-}_{g}$ channel, which translates to the observed effects through electron correlation. The unprecedented energy resolution and delay accuracies demonstrate the promise of visible-light–driven molecular attosecond interferometry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Direct Observation of Ultrafast Dissociation Dynamics of (R–I){sub n}-Type Iodide Clusters as a Result of UV Excitation below the Ionization Threshold

The dynamics of dissociation of (IF{sub 2}CCOF){sub n}, (CF{sub 3}I){sub n}, and (CH{sub 3}I){sub n} clusters induced by femtosecond UV radiation (λ = 266 nm) is investigated. The method of UV excitation and photoionization probing (λ = 400 nm) combined with the time-of-flight mass spectrometry is applied. It is found that clusters excited to Rydberg states lying below the ionization threshold are decomposed, as a result of subsequent relaxation processes, giving rise to free neutral molecules. A mechanism of electronic–vibrational relaxation process is proposed, and data on the characteristic times of different stages of this process are obtained.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2011

Ultrafast Dynamics of 1,3-Cyclohexadiene in Highly Excited States

The ultrafast dynamics of 1,3-cyclohexadiene has been investigated via structurally sensitive Rydberg electron binding energies and shown to differ upon excitation to the 1B state and the 3p Rydberg state. Excitation of the molecule with 4.63 eV photons into the ultrashort-lived 1B state yields the well-known ring opening to 1,3,5-hexatriene, while a 5.99 eV photon lifts the molecule directly into the 3p-Rydberg state. Excitation to 3p does not induce ring opening. In both experiments, time-dependent shifts of the Rydberg electron binding energy reflect the structural dynamics of the molecular core. Structural distortions associated with 3p-excitation cause a dynamical shift in the - and -binding energies by 10 and 26 meV/ps, respectively, whereas after excitation into 1B, more severe structural transformations along the ring-opening coordinate produce shifts at a rate of 40 to 60 meV/ps. The experiment validates photoionization-photoelectron spectroscopy via Rydberg states as a powerful technique to observe structural dynamics of polyatomic molecules.

Bühler, Christine C.↗
DOE OSTI2024

Nonlinear propagation of chirped laser pulses through a dispersive and turbulent atmosphere

The evolution of ultrashort laser pulses in dispersive, turbulent, nonlinear, and dissipative media is discussed in connection with nonlinear self-focusing collapse and the onset of laser filamentation. In quiescent air, a laser pulse propagating with a peak power greater than a critical power for self-focusing will undergo a catastrophic, transverse collapse until the intensity is large enough for photoionization. At this point, self-focusing is arrested and balanced by plasma refraction, forming a laser filament. By applying an appropriate chirp, the dispersive properties of the medium can be used to enhance this process and control its onset, and to counter dissipative effects such as molecular absorption and atmospheric scattering. This paper presents an analysis of the effect of atmospheric turbulence on the propagation of nonlinear pulses with dispersion compensation (chirp). Furthermore, the analytical results are compared with wave optics simulations and found to be in reasonable agreement as long as the pulse maintains a near-Gaussian spatiotemporal profile.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Measuring an ultrashort, ultraviolet pulse in a slowly responding, absorbing medium

Frequency-resolved optical gating (FROG) is a common technique for measuring ultrashort laser pulses using an instantaneous, nonlinear-optical interaction as a fast time-gate to measure the pulse intensity and phase. But at high frequencies, materials are often absorbing and it is not always possible to find a medium with a fast nonlinear-optical response. Here we show that an ultrashort, ultraviolet (UV) pulse can be measured in a strongly absorbing medium, using the absorption as the nonlinear-optical time-gate. To do this, we build on our recent implementation of FROG, known as induced-grating cross-correlation FROG (IG XFROG), where an unknown, higher-frequency pulse creates a transient grating that is probed with a lower-frequency, more easily detectable reference pulse. We demonstrate this with an 800 nm reference pulse to characterize 400 nm or 267 nm pulses using ZnS as the nonlinear-optical medium, which is absorptive at and below 400 nm. By scanning the delay between the two UV pulses which create the transient grating, we show that the phase-sensitive instantaneous four-wave-mixing contribution to the nonlinear signal field can be detected and separated from the slower, incoherent part of the response. Measuring a spectrally-resolved cross-correlation in this way and then applying a simple model for the response of the medium, we show that a modified generalized projections (GP) phase-retrieval algorithm can be used to extract the pulse amplitude and phase. We test this approach by measuring chirped UV pulses centered at 400 nm and 267 nm. Since interband absorption (or even photoionization) is not strongly wavelength-dependent, we expect IG XFROG to be applicable deeper into the UV.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Cross-polarized common-path temporal interferometry for high-sensitivity strong-field ionization measurements

Absolute density measurements of low-ionization-degree or low-density plasmas ionized by lasers are very important for understanding strong-field physics, atmospheric propagation of intense laser pulses, Lidar etc. A cross-polarized common-path temporal interferometer using balanced detection was developed for measuring plasma density with a sensitivity of ∼0.6 mrad, equivalent to a plasma density-length product of ∼2.6 × 10 13 cm −2 if using an 800 nm probe laser. By using this interferometer, we have investigated strong-field ionization yield versus intensity for various noble gases (Ar, Kr, and Xe) using 800 nm, 55 fs laser pulses with both linear (LP) and circular (CP) polarization. The experimental results were compared to the theoretical models of Ammosov-Delone-Krainov (ADK) and Perelomov-Popov-Terent’ev (PPT). We find that the measured phase change induced by plasma formation can be explained by the ADK theory in the adiabatic tunneling ionization regime, while PPT model can be applied to all different regimes. We have also measured the photoionization and fractional photodissociation of molecular (MO) hydrogen. By comparing our experimental results with PPT and MO-PPT models, we have determined the likely ionization pathways when using three different pump laser wavelengths of 800 nm, 400 nm, and 267 nm.

47 OTHER INSTRUMENTATION↗
DOE OSTI2013

Standoff Trace Chemical Sensing via Manipulation of Excited Electronic State Lifetimes

We present a technique for standoff trace chemical sensing that is based on the dependence of excited electronic state lifetimes on the amount of internal vibrational energy. Time resolved photoionization measurements show that the lifetime of the S1 state in N,N-dimethylisopropylamine (DMIPA) decreases exponentially with the amount of energy deposited into vibrational degrees of freedom. This property is employed to acquire spectral signatures of the molecule. Two nanosecond laser pulses are used, one (266 nm) to ionize the molecule through the S1 state and another, with tunable wavelength, to alter the lifetime of the S1 state by depositing energy into vibrations. Reduction of the S1 state lifetime results in a dip in ionization efficiency that is observed by remotely probing the laser-induced plasma with microwave radiation.

Rudakov, Fedor M↗
DOE OSTI2021

Spectroscopy of GR1 centers in synthetic diamonds

We report on the spectroscopic characterization, absorption saturation, and excited-state dynamics of GR1 centers in synthetic diamonds. The non-linear optical measurements reveal an efficient bleaching of the GR1 center’s ground level under ns-pulsed 633 nm excitation. The maxima of absorption and emission cross sections were estimated to be 4.5 × 10 −17 cm 2 and 9 × 10 −17 cm 2 at 630 nm and 780 nm, respectively. The radiative lifetime of the excited level was estimated to be 8.5 ns. The 658 nm probe kinetics uncovered relaxation of 1 T 2 excited level going predominantly to a metastable state with a lifetime of 220 μs. An induced absorption detected with the use of a highly concentrated diamond sample could be due to up-conversion and photoionization processes in additional impurity-vacancy center with absorption at the short-wavelength tail of GR1. The results presented here indicate that synthetic diamonds with GR1 centers could serve as near infrared gain media or passive Q-switchers for laser cavities over the 633–750 nm spectral range. Optimization of the center concentration and the crystal parameters are required to minimize the induced absorption at the lasing wavelengths.

36 MATERIALS SCIENCE↗
DOE OSTI2023

One dimensional temperature measurements by resonantly ionized photoemission thermometry of molecular nitrogen

This paper presents an extensive parameter study of a non-intrusive and non-seeded laser diagnostic method for measuring one dimensional (1D) rotational temperature of molecular nitrogen (N 2 ) at 165 - 450 K. Compared to previous efforts using molecular oxygen, here resonantly ionized and photoelectron induced fluorescence of molecular nitrogen for thermometry (N 2 RIPT) was demonstrated. The RIPT signal is generated by directly probing various rotational levels within the rovibrational absorption band of N 2 , corresponding to the 3-photon transition of N 2 ( X 1 Σ g + , v =0→ b 1 Π u , v ′ =6) near 285 nm, without involving collisional effects of molecular oxygen and nitrogen. The photoionized N 2 produces strong first negative band of N 2 + ( B 2 Σ u + − X 2 Σ g + ) near 390 nm, 420 nm, and 425 nm. Boltzmann analyses of various discrete fluorescence emission lines yield rotational temperatures of molecular nitrogen. By empirically choosing multiple rotational levels within the absorption band, non-scanning thermometry can be accurately achieved for molecular nitrogen. It is demonstrated that the N 2 RIPT technique can measure 1D temperature profile up to ∼5 cm in length within a pure N 2 environment. Multiple wavelengths are thoroughly analyzed and listed that are accurate for RIPT for various temperature ranges.

McCord, Walker (ORCID:0000000179747550)↗
DOE OSTI2021

All-optical single-shot complete electric field measurement of extreme ultraviolet free electron laser pulses

Recent advances in ultrafast extreme ultraviolet (EUV) and x-ray light sources provide direct access to fundamental time and length scales for biology, chemistry, and materials physics. However, such light pulses are challenging to measure due to the need for femtosecond time resolution at difficult-to-detect wavelengths. Also, single-shot measurements are needed because severe pulse-to-pulse fluctuations are common. Here we demonstrate single-shot, complete field measurements by applying a novel version of frequency resolved optical gating. An EUV free electron laser beam creates a transient grating containing the pulse’s electric field information, which is read out with a 400 nm probe pulse. By varying the time delay between two copies of the EUV pump, rather than between the pump and the probe, we separate the needed coherent wave mixing from the slow incoherent response. Because this approach uses photoionization, it should be applicable from the vacuum ultraviolet to hard x rays.

36 MATERIALS SCIENCE↗
DOE OSTI2015

An Experimental and Kinetic Modeling Study of Premixed Laminar Flames of Methyl Pentanoate and Methyl Hexanoate

Detailed chemical structures of stoichiometric and rich premixed laminar flames of methyl pentanoate and methyl hexanoate were investigated over a flat burner at 20 Torr and for methyl pentanoate at 1 atm. Molecular beam mass spectrometry was used with tunable synchrotron vacuum ultraviolet (VUV) photoionization for low pressure flames of both methyl pentanoate and methyl hexanoate, and soft electron-impact ionization was used for atmospheric pressure flames of methyl pentanoate. Mole fraction profiles of stable and intermediate species, as well as temperature profiles, were measured in the flames. A detailed chemical kinetic high temperature reaction mechanism for small alkyl ester oxidation was extended to include combustion of methyl pentanoate and methyl hexanoate, and the resulting model was used to compare computed values with experimentally measured values. Reaction pathways for both fuels were identified, with good agreement between measured and computed species profiles. Implications of these results for future studies of larger alkyl ester fuels are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Reaction of Chlorine Molecules with Unsaturated Submicron Organic Particles

Here, the reaction of closed shell Cl 2 molecules with sub-micron droplets composed of unsaturated molecules, oleic acid (OA), linoleic acid (LA), linolenic acid (LNA), or squalene (Sqe), are investigated in an atmospheric pressure flow tube reactor in conjunction with a vacuum ultraviolet photoionization aerosol mass spectrometer and a scanning mobility particle sizer. Cl 2 is found to react with all particles, and the reactive uptake coefficients depend on the number of unsaturated reaction sites, e.g., γ Cl2 Sqe = (0.66 ± 0.03) × 10 –4 versus γ Cl2 OA = (0.23 ± 0.01) × 10 –4 . In addition, the chemical evolution of squalene and its chlorinated products reveal that the reaction becomes slower for higher chlorinated products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Beam Profile Measurements Utilizing an Amplitude Modulated Pulsed Fiber Laser at PIP2IT

Fermilab is undertaking the development of a new 800 MeV superconducting RF linac to replace its present normal conducting 400 MeV linac. The PIP-II linac consists of a warm front-end generating 2 mA of 2.1 MeV H⁻ followed immediately by a series of superconducting RF cryomodules to 800 MeV. To limit the potential damage to the superconducting RF cavities, PIP-II will utilize laser-based monitors to obtain beam profiles via photoionization. This paper will present the results of transverse and longitudinal beam profile measurements using a prototype profile monitor that was tested with 2.1 MeV H⁻ beam at the PIP-II Injector Test (PIP2IT) accelerator. This prototype profile monitor utilizes a high repetition rate fiber laser and fiber optic transport into the PIP2IT enclosure. In addition, results will be shown of narrow-band electron detection from amplitude modulated laser pulses.

43 PARTICLE ACCELERATORS↗