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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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
NASA NTRS1991

Study of Cluster Formation and its Effects on Rayleigh and Raman Scattering Measurements in a Mach 6 Wind Tunnel

Using a frequency-doubled Nd-YAG pulsed laser and a single-intensified CCD camera, Rayleigh scattering measurements have been performed to study the cluster formation in a Mach 6 wind tunnel at NASA Langley Research Center. These studies were conducted both in the free stream and in a model flow field for various flow conditions to gain an understanding of the dependence of the Rayleigh scattering (by clusters) on the local pressures and temperatures in the facility. Using the same laser system, we have also performed simultaneous measurements of the local temperature using the rotational Raman scattering of molecular nitrogen and determined the densities of molecular oxygen and nitrogen by using the vibrational Raman scattering from these species. Quantitative results will be presented in detail with emphasis on the applicability of the Rayleigh scattering for obtaining quantitative measurements of molecular densities both in the free stream and in the model flow field.

Shirinzadeh, B.↗
NASA NTRS1990

The C9 cluster - Structure and infrared frequencies

A structural characterization is presented for C9, the largest cluster predicted to have a linear ground state. IR laser diode absorption spectroscopy of a supersonic carbon jet is used to measure 51 lines of the nu6 (sigma u) antisymmetric stretch fundamental transition within the linear 1Sigma(g)+ ground electronic state of C9. The measured ground state rotational constant suggests an effective C-C bond length which is in good agreement with ab initio theory and consistent with cumulenic bonding in this cluster.

Heath, J. R.↗
DOE OSTI2020

Rapid Generation of Hierarchically Porous Metal–Organic Frameworks through Laser Photolysis

Abstract Hierarchically porous metal–organic frameworks (HP‐MOFs) facilitate mass transfer due to mesoporosity while preserving the advantage of microporosity. This unique feature endows HP‐MOFs with remarkable application potential in multiple fields. Recently, new methods such as linker labilization for the construction of HP‐MOFs have emerged. To further enrich the synthetic toolkit of MOFs, we report a controlled photolytic removal of linkers to create mesopores within microporous MOFs at tens of milliseconds. Ultraviolet (UV) laser has been applied to eliminate “photolabile” linkers without affecting the overall crystallinity and integrity of the original framework. Presumably, the creation of mesopores can be attributed to the missing‐cluster defects, which can be tuned through varying the time of laser exposure and ratio of photolabile/robust linkers. Upon laser exposure, MOF crystals shrank while metal oxide nanoparticles formed giving rise to the HP‐MOFs. In addition, photolysis can also be utilized for the fabrication of complicated patterns with high precision, paving the way towards MOF lithography, which has enormous potential in sensing and catalysis.

Wang, Kun‐Yu↗
DOE OSTI2020

Rapid Generation of Hierarchically Porous Metal–Organic Frameworks through Laser Photolysis

Hierarchically porous metal–organic frameworks (HP-MOFs) facilitate mass transfer due to mesoporosity while preserving the advantage of microporosity. This unique feature endows HP-MOFs with remarkable application potential in multiple fields. Recently, new methods such as linker labilization for the construction of HP-MOFs have emerged. To further enrich the synthetic toolkit of MOFs, we report a controlled photolytic removal of linkers to create mesopores within microporous MOFs at tens of milliseconds. Ultraviolet (UV) laser has been applied to eliminate “photolabile” linkers without affecting the overall crystallinity and integrity of the original framework. Presumably, the creation of mesopores can be attributed to the missing-cluster defects, which can be tuned through varying the time of laser exposure and ratio of photolabile/robust linkers. Upon laser exposure, MOF crystals shrank while metal oxide nanoparticles formed giving rise to the HP-MOFs. In addition, photolysis can also be utilized for the fabrication of complicated patterns with high precision, paving the way towards MOF lithography, which has enormous potential in sensing and catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2015

Feasibility of Rayleigh Scattering Flow Diagnostics in the National Transonic Facility

Laser-based Rayleigh light scattering (RLS) was performed in the National Transonic Facility (NTF) at NASA Langley Research Center. The goal was to determine if the free-stream flow undergoes clustering (early stage of condensation from gas to liquid) or remains in a pure diatomic molecular phase. Data indicate that clusters are not observable down to levels of 10% of the total light scatter for a variety of total pressures at one N2 cryogenic-mode total temperature (Tt = -50 F = 227 K) and one air-mode temperature (Tt = +130 F = 327 K). Thus RLS appears viable as a qualitative or quantitative diagnostic for flow density in NTF in the future. Particles are distinguished from optically unresolvable clusters because they are much larger and individually resolvable in the laser beam image with Mie scattering. The same RLS apparatus was also used, without modification, to visualize naturally occurring particles entrained in the flow for both cryogenic and air-modes. Estimates of the free-stream particle flux are presented, which may be important for interpretation of laminar-to-turbulent boundary-layer transition studies. 1

Herring, Gregory C.↗
NASA NTRS1991

Tunable far infrared laser spectrometers

The state of the art in far infrared (FIR) spectroscopy is reviewed. The development of tunable, coherent FIR radiation sources is discussed. Applications of tunable FIR laser spectrometers for measurement of rotational spectra and dipole moments of molecular ions and free radicals, vibration-rotation-tunneling spectra of weakly bound complexes, and vibration-rotation spectra of linear carbon clusters are presented. A detailed description of the Berkeley tunable FIR laser spectrometers is presented.

Blake, G. A.↗
DOE OSTI2021

Ab initio study and assignment of electronic states in molecular RaCl

Radium compounds have attracted recently considerable attention due to both development of experimental techniques for high-precision laser spectroscopy of molecules with short-lived nuclei and amenability of certain radium compounds for direct cooling with lasers. Currently, radium monofluoride (RaF) is one of the most studied molecules among the radium compounds, both theoretically and recently also experimentally. Complementary studies of further diatomic radium derivatives are highly desired to assess the influence of chemical substitution on diverse molecular parameters, especially on those connected with laser cooling, such as vibronic transition probabilities, and those related to violations of fundamental symmetries. Here in this article high-precision ab initio studies of electronic and vibronic levels of diatomic radium monochloride (RaCl) are presented. Recently developed approaches for treating electronic correlation with Fock-space coupled cluster methods are applied for this purpose. Theoretical results are compared to an early experimental investigation by Lagerqvist and used to partially reassign the experimentally observed transitions and molecular electronic levels of RaCl. Effective constants of $\mathscr{P}$-odd hyperfine interaction W a and $\mathscr{P, T}$-odd scalar-pseudoscalar nucleus-electron interaction Ws in the ground electronic state of RaCl are estimated within the framework of a quasirelativistic Zeroth-Order Regular Approximation approach and compared to parameters in RaF and RaOH.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1999

Laser ablation of persistent twist cells in Drosophila: muscle precursor fate is not segmentally restricted

In Drosophila the precursors of the adult musculature arise during embryogenesis. These precursor cells have been termed Persistent Twist Cells (PTCs), as they continue to express the transcription factor Twist after that gene ceases expression elsewhere in the mesoderm. In the larval abdomen, the PTCs are associated with peripheral nerves in stereotypic ventral, dorsal, and lateral clusters, which give rise, respectively, to the ventral, dorsal, and lateral muscle fiber groups of the adult. We tested the developmental potential of the PTCs by using a microbeam laser to ablate specific clusters in larvae. We found that the ablation of a single segmental PTC cluster does not usually result in the deletion of the corresponding adult fibers of that segment. Instead, normal or near normal numbers of adult fibers can form after the ablation. Examination of pupae following ablation showed that migrating PTCs from adjacent segments are able to invade the affected segment, replenishing the ablated cells. However, the ablation of homologous PTCs in multiple segments does result in the deletion of the corresponding adult muscle fibers. These data indicate that the PTCs in an abdominal segment can contribute to the formation of muscle fibers in adjacent abdominal segments, and thus are not inherently restricted to the formation of muscle fibers within their segment of origin.

NASA Discipline Neuroscience↗
DOE OSTI2020

In search of molecular ions for optical cycling: a difficult road

Optical cycling, a continuous photon scattering off atoms or molecules, plays a central role in the quantum information science. While optical cycling has been experimentally achieved for many neutral species, few molecular ions have been investigated. We present a systematic theoretical search for diatomic molecular ions suitable for optical cycling using equation-of-motion coupled-cluster methods. Inspired by the electronic structure patterns of laser-cooled neutral molecules, we establish the design principles for molecular ions and explore various possible cationic molecular frameworks. The results show that finding a perfect molecular ion for optical cycling is challenging, yet possible. Among various possible diatomic molecules we suggest several candidates, which require further attention from both theory and experiment: YF + , SiO + , PN + , SiBr + , and BO + .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1991

Infrared laser absorption spectroscopy of the nu4 (sigma u) fundamental and associated nu11(pi u) hot band of C7 - Evidence for alternating rigidity in linear carbon clusters

The first characterization of the bending potential of the C7 cluster is reported via the observation of the v = 1(1) and v = 2 deg levels of the nu11 (pi u) bend as hot bands associated with the nu4 (sigma u) antisymmetric stretch fundamental. The lower state hot band rotational constants are measured to be 1004.4(1.3) and 1123.6(9.0) MHz, constituting a 9.3 and 22 percent increase over the ground state rotational constant, 918.89 (41) MHz. These large increases are strong quartic and sextic centrifugal distortion constants determined for the ground and nu 4 = 1 states are found to be anomalously large and negative, evidencing strong perturbations between stretching and bending modes.

Heath, J. R.↗
NASA NTRS2022

Laser-Guided Space Interferometer

The mirrors of astronomical interferometers need to be aligned within a fraction of a wavelength relative to one another. This would be especially challenging for optical instruments with mirrors separated by hundreds of meters flying in Earth’s orbit. However, in this work, we show that this alignment can be achieved by means of: (i) flying the mirror cluster in a particular orbital configuration; (ii) closing a coarse positioning loop using GNSS (Global Navigation Satellite System); and (iii) closing a fine wavefront-control loop using light from a laser guide star. The orbital configuration is designed to keep the mirrors passively pointing at the target star (up to a small orbital perturbation) while the interferometer cluster is orbiting and changing its baseline. The laser guide star would be flying in the same orbit but in the opposite direction. In medium- or high-Earth orbit, the interferometer would be able to observe a star for several hours per orbit. In this work, we analyzed the performance of an optical space interferometer consisting of nine 20 cm mirrors mounted on CubeSats and flying 3 km apart (together with a combiner and a laser guide star small satellite). This configuration supports a resolution of 0.04 milliarcseconds - an order of magnitude better than current ground-based interferometers. We estimate the performance of this system imaging stellar surfaces assuming perfect wavefront estimation and control.

Leonid Pogorelyuk↗
DOE OSTI2025

Orientation-dependent enhanced ionization in acetylene revealed by ultrafast cross-polarized pulse pairs

We investigate the orientation dependence of enhanced ionization (EI) during strong-field-driven nuclear motion in acetylene (C 2 ⁢H 2 ). Here, we both initiate and probe molecular dynamics in acetylene with intense 6-fs cross-polarized pulse pairs, separated by a variable delay. Following multiple ionization by the first pulse, acetylene undergoes simultaneous elongation of the carbon-carbon and carbon-hydrogen bonds, enabling further ionization by the second pulse and the formation of a very highly charged state, [C 2 ⁢H 2 ] 6+ . At small interpulse delays (< 20 fs), this enhancement occurs when the molecule is aligned to the probe pulse. Conversely, at large delays (> 40 fs), formation of [C 2 ⁢H 2 ] 6+ occurs when the molecule is aligned to the pump pulse. By analyzing the polarization and time dependence of sequentially ionized [C 2 ⁢H 2 ] 6+ , we resolve two transient alignments that both contribute to a large increase in the multiple ionization yield. In conclusion, this cross-polarized pulse pair scheme uniquely enables selective probing of deeply bound orbitals, providing new insights on orientation-dependent EI in highly charged hydrocarbons.

Atomic & molecular clusters↗
DOE OSTI2023

Observation of Slow Eigen-Zundel Interconversion in H + (H 2 O) 6 Clusters upon Isomer-Selective Vibrational Excitation and Buffer Gas Cooling in a Cryogenic Ion Trap

The formation of isomers when trapping floppy cluster ions in a temperature-controlled ion trap is a generally observed phenomenon. This involves collisional quenching of the ions initially formed at high temperature by buffer gas cooling until their internal energies fall below the barriers in the potential energy surface that separate them. Here we explore the kinetics at play in the case of the two isomers adopted by the H + (H 2 O) 6 cluster ion that differ in the proton accommodation motif. One of these is most like the Eigen cation with a tricoordinated hydronium motif (denoted E), and the other is most like the Zundel ion with the proton equally shared between two water molecules (denoted Z). After initial cooling to about 20 K in the radiofrequency (Paul) trap, the relative populations of these two spectroscopically distinct isomers are abruptly changed through isomer-selective photoexcitation of bands in the OH stretching region with a pulsed (~6 ns) infrared laser while the ions are in the trap. We then monitor the relaxation of the vibrationally excited clusters and reformation of the two cold isomers by recording infrared photodissociation spectra with a second IR laser as a function of delay time from the initial excitation. The latter spectra are obtained after ejecting the trapped ions into a time-of-flight photofragmentation mass spectrometer, thus enabling long (~0.1 s) delay times. Excitation of the Z isomer is observed to display long-lived vibrationally excited states that are collisionally cooled on a ms time scale, some of which quench into the E isomer. These excited E species then display spontaneous interconversion to the Z form on a ~10 ms time scale. Furthermore, these qualitative observations set the stage for a series of experimental measurements that can provide quantitative benchmarks for theoretical simulations of cluster dynamics and the potential energy surfaces that underlie them.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2003

Therma1 Conductivity and Durability of Advanced Thermal Barrier Coatings

Thermal barrier coatings (TBCs) will play a crucial role in advanced gas turbine engines because of their ability to further increase engine operating temperature and reduce cooling, thus helping to achieve engine emission and efficiency goals. Future TBCs must be designed with increased phase stability, lower thermal conductivity, and improved sintering and thermal stress resistance in order to effectively protect engine hot-section components. Advanced low conductivity TBCs are being developed at NASA by incorporating multi-component oxide dopants into zirconia-yttria or hafnia-yttria to promote the formation of thermodynamically stable defect clusters within the coating structures. This presentation will primarily focus on thermal conductivity and durability of the novel defect cluster thermal barrier coatings for turbine airfoil and combustor applications, determined by a unique CO2 laser heat-flux approach. The laser heat-flux testing approach emphasizes the real-time monitoring and assessment of the coating thermal conductivity under simulated engine temperature and thermal gradient conditions. The conductivity increase due to coating sintering (and/or phase change) and the conductivity decrease due to coating delamination have been determined under steady-state, cyclic, uniform or non-uniform heat-flux conditions. The coating radiation flux resistance has been evaluated by varying coating thermal gradients, and also by using a laser-heated radiative-flux source. Advanced multi-component TBC systems have been shown to have significantly reduced thermal conductivity and improved high temperature stability due to the nano-sized, low mobility defect clusters associated with the paired rare earth dopant additions. The effect of oxide defect cluster dopants on coating thermal conductivity, thermal stability and furnace cyclic durability will also be discussed. The current low conductivity TBC systems have demonstrated long-term cyclic durability at very high temperatures which is far beyond the baseline ZrO2-Y2O3 capabilities.

Zhu, Dong-Ming↗
DOE OSTI2021

Fluorescence intensity correlation imaging with high spatial resolution and elemental contrast using intense x-ray pulses

We theoretically investigate the fluorescence intensity correlation (FIC) of Ar clusters and Mo-doped iron oxide nanoparticles subjected to intense, femtosecond, and sub-femtosecond x-ray free-electron laser pulses for high-resolution and elemental contrast imaging. We present the FIC of Kα and Kαh emission in Ar clusters and discuss the impact of sample damage on retrieving high-resolution structural information and compare the obtained structural information with those from the coherent diffractive imaging (CDI) approach. We found that, while sub-femtosecond pulses will substantially benefit the CDI approach, few-femtosecond pulses may be sufficient for achieving high-resolution information with the FIC. Furthermore, we show that the fluorescence intensity correlation computed from the fluorescence of the Mo atoms in Mo-doped iron oxide nanoparticles can be used to image dopant distributions in the nonresonant regime.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Extended x-ray emission times of clusters in intense x-ray pulses

Novel experimental spectroscopic and imaging techniques have been developed to exploit x-ray free-electron laser (XFEL) for studying structure and dynamic of non-periodic entities at atomic spatial resolution and femtosecond timescales.Recently, intensity correlation of x-ray fluorescence, based on the principle introduced by Hanbury Brown and Twiss [R. Hanbury Brown and R. Q. Twiss, Nature (London) 177, 27 (1956)], has been proposed for high-resolution imaging of a three-dimensional arrangement of atoms. To explore the applicability of this fluorescence approach, we theoretically investigate fluorescence dynamics of nonperiodic systems subject to x-ray free electron laser (XFEL) pulses over a range of fluences from the linear to nonlinear x-ray absorption regimes as a function of system size, from a single atom to a cluster of 149 171 atoms. Fluorescence dynamics in the nonlinear x-ray regime differs from that in the weak x-ray field in that intense x-ray pulses interrupt the fluorescence dynamics by multiphoton absorption creating a dense electron environment within the sample on a femtosecond timescale. In large systems, the presence of both recombination and photoionization pathways gives rise to an enhanced Kα and Kα h emission yield and an extended emission time beyond the lifetime of the core-excited states. Our analysis suggests that, in an intense x-ray pulse, the Kα h emission line can be a good candidate for fluorescence imaging as it has a higher yield and an emission time that is short relative to the x-ray-induced lattice distortion time.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS1986

Characterization of biogenic elements in interplanetary dust particles

Those particles that were designated cometary are aggregates of amorphous materials including carbon, iron-magnesium silicates, sulfides, metal and trace amounts of unusual phases. Most aggregates are carbon-rich with major and minor element abundances similar to a fine grained matrix of carbonaceous chondrites. Several particles were analyzed by a laser microprobe. The negative ionic species identified to date include carbon clusters, protonated carbon clusters, CN-, HCN-, CNO-, PO2-, PO3-, S-, S2- asnd OH-. These species are similar to those observed in cometary spectra and they support the assumption that organic materials are present. The occurance of phosphate ions suggests the presence of apatite or whitlockite. Cometary particle characteristics may indicate that the component grains represent primitive unaltered dust whose overall properties are extremely similar to altered primitive dust in carbonaceous chondrites.

Bunch, T. E.↗
DOE OSTI2024

Controlled molecule injector for cold, dense, and pure molecular beams at the European x-ray free-electron laser

A permanently available molecular-beam injection setup for controlled molecules (COMO) was installed and commissioned at the small quantum systems (SQS) instrument at the European x-ray free-electron laser (EuXFEL). A b-type electrostatic deflector allows for pure state-, size-, and isomer-selected samples of polar molecules and clusters. The source provides a rotationally cold (T ≈ 1 K) and dense (ρ ≈ 10 8 cm −3 ) molecular beam with pulse durations up to 100 µs generated by a new version of the Even-Lavie valve. Here, a performance overview of the COMO setup is presented along with characterization experiments performed both with an optical laser at the Center for Free-Electron-Laser Science and with x rays at EuXFEL under burst-mode operation. COMO was designed to be attached to different instruments at the EuXFEL, in particular, the SQS and single particles, clusters, and biomolecules (SPB) instruments. This advanced controlled-molecules injection setup enables x-ray free-electron laser studies using highly defined samples with soft and hard x-ray FEL radiation for applications ranging from atomic, molecular, and cluster physics to elementary processes in chemistry and biology.

He, Lanhai↗