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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 829 records · Page 46
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DOE OSTI2017

Probing autoionizing states of molecular oxygen with XUV transient absorption: Electronic-symmetry-dependent line shapes and laser-induced modifications

In this paper, we used extreme ultraviolet (XUV) transient absorption spectroscopy to study the autoionizing Rydberg states of oxygen in an electronically- and vibrationally-resolved fashion. XUV pulse initiates molecular polarization and near-infrared pulse perturbs its evolution. Transient absorption spectra show positive optical-density (OD) change in the case of $ns{{\sigma}}_{g}$ and $nd{{\pi}}_{g}$ autoionizing states of oxygen and negative OD change for $nd{{\sigma}}_{g}$ states. Multiconfiguration time-dependent Hartree-Fock (MCTDHF) calculations are used to simulate the transient absorption and the resulting spectra and temporal evolution agree with experimental observations. We model the effect of near-infrared perturbation on molecular polarization and find that the laser-induced phase-shift model agrees with the experimental and MCTDHF results, while the laser-induced attenuation model does not. Finally, we relate the electronic-state-symmetry-dependent sign of the OD change to the Fano parameters of the static absorption line shapes.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2017

Spatial and temporal control of populations, branching ratios, and electronic coherences in LiH by a single one-cycle infrared pulse

Dynamical computations demonstrate considerable selectivity over the fragmentation channels of the LiH molecule via the polarization and the carrier envelope phase (CEP) of a single ultrashort one-cycle strong IR pulse. For aligned molecules, control of the CEP allows building nonstationary coherent electronic wave packets of contrasting ionic character, either Li δ +H δ - or Li δ -H δ +. Furthermore, the complementary coherences are maintained all the way to dissociation. The direction of the electric field at its maximum points either towards the Li or towards the H atom, which selectively steers the nuclear dynamics to specific dissociation products.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2017

Vibrationally assisted below-threshold ionization

Here, we perform time-resolved UV pump (4.77 eV) and VUV probe (7.94 eV) measurements of internal conversion of 1,3-cyclohexadiene (CHD). Our measurements reveal a substantial ionization of the “hot” ground state following internal conversion despite the fact that our probe photon energy is below the ionization potential (8.21 eV). With the aid of electronic structure calculations, we interpret our results in terms of vibrationally assisted below-threshold ionization, where vibrational energy is converted to electronic energy. The effect relies on both having vibrational modes which allow for this vibrational-electronic coupling and exciting these modes during the internal conversion. We contrast our measurements in CHD with another similar molecule, cis,cis-1,3-cyclooctadiene (cis,cis-COD), for which we do not see the effect.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2017

High-order-harmonic generation by Laguerre-Gaussian laser modes: Control of the spectra by manipulating the spatial medium distribution

In this work, we study high-order-harmonic generation (HHG) by the incident laser beam in the Laguerre-Gaussian mode with a nonzero topological charge. We find that the harmonic signal in the central spot on the beam axis does not always vanish and depends on the distribution of the medium in the focal region of the incident laser beam. The HHG spectra on the beam axis can be controlled by changing the spatial medium distribution. General theoretical results are confirmed by calculations of HHG in the medium of argon atoms, with the single-atom response obtained by means of the time-dependent density functional theory.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2017

Resonant two- or three-photon ionization of noble-gas atoms captured by time-resolved photoelectron momentum spectroscopy

In this work, we present an all-electron, ab initio calculation of time-resolved photoelectron momentum distributions (PMDs) induced by resonant two-color, two- or three-photon ionization of helium and neon atoms, as recently measured by Villeneuve et al. [Science 356, 1150 (2017)] using a femtosecond infrared (IR) laser pulse and an attosecond pulse train (APT) produced with high harmonic generation as an extreme ultraviolet (XUV) photon source. In contrast to a monochromatic XUV pulse commonly used at the free-electron laser facilities, an APT is broadband and ultrashort (<1 fs), so that it could induce nonresonant one-photon transitions above ionization threshold as well as a resonantly excited state. They may interfere with each other upon subsequent absorption or emission of an IR photon, so that the resultant PMD loses clear orbital symmetry. Our time-dependent density functional calculation demonstrates that the selection of a particular excited state in the time-resolved PMD is nevertheless possible if energy and timing of an APT are adjusted properly.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2018

Quadruple coincidence measurement of electron correlation in strong-field molecular double ionization

Here, we study strong-field dissociative molecular double ionization with momentum-resolved quadruple coincidence measurements, measuring the two electrons and two ionic fragments produced with a coincidence velocity map imaging apparatus. We contrast measurements for two different molecules. In one case, our measurements reveal anticorrelation in the momentum for the two electrons. In the other, we find no anticorrelation, indicating differences in the underlying ionization dynamics.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2018

Controlling electron quantum paths for generation of circularly polarized high-order harmonics by H 2 + subject to tailored (ω, 2ω) counter-rotating laser fields

Recently, studies of high-order harmonics (HHG) from atoms driven by bichromatic counter-rotating circularly polarized laser fields as a source of coherent circularly polarized extreme ultraviolet (XUV) and soft-x-ray beams in a tabletop-scale setup have received considerable attention. Here, we demonstrate the ability to control the electron recollisions giving three returns per one cycle of the fundamental frequency ω by using tailored bichromatic (ω, 2ω) counter-rotating circularly polarized laser fields with a molecular target. The full control of the electronic pathway is first analyzed by a classical trajectory analysis and then extended to a detailed quantum study of H 2 + molecules in bichromatic (ω, 2ω) counter-rotating circularly polarized laser fields. The radiation spectrum contains doublets of left- and right-circularly polarized harmonics in the XUV ranges. Finally, we study in detail the below-, near-, and above-threshold harmonic regions and describe how excited-state resonances alter the ellipticity and phase of the generated harmonic peaks.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2018

Energy-resolved attosecond interferometric photoemission from Ag(111) and Au(111) surfaces

Photoelectron emission from solid surfaces induced by attosecond pulse trains into the electric field of delayed phase-coherent infrared (IR) pulses allows the surface-specific observation of energy-resolved electronic phase accumulations and photoemission delays. Here, we quantum-mechanically modeled interferometric photoemission spectra from the (111) surfaces of Au and Ag, including background contributions from secondary electrons and direct emission by the IR pulse, and adjusted parameters of our model to energy-resolved photoelectron spectra recently measured at a synchrotron light source by Roth et al. [J. Electron Spectrosc. 224, 84 (2018)]. Our calculated spectra and photoelectron phase shifts are in fair agreement with the experimental data of Locher et al. [Optica 2, 405 (2015)]. Our model's not reproducing the measured energy-dependent oscillations of the Ag(111) photoemission phases may be interpreted as evidence for subtle band-structure effects on the final-state photoelectron-surface interaction not accounted for in our simulation.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2018

State-selective dissociation dynamics of an oxygen molecular ion studied with single-harmonic pump and infrared-probe pulses

Laser-induced dissociation of a photoionized oxygen molecule is studied employing an extreme-ultraviolet-pump–near-infrared-probe (EUV-NIR pump-probe) technique. A combination of a narrow-band 11th harmonic pump centered at 17.3 eV and a moderate-intensity NIR probe restricts the dissociation dynamics to the pair of low-lying cationic states, a 4 Π u and f 4 Π g . The measured kinetic energies of the O + fragments reveal contributions from one-, two-, and three-photon dissociation pathways ( 1 ω , 2 ω , and 3 ω ) involving these two states. While the yields of the two- and three-photon channels initially rise and then decrease as a function of EUV-NIR delay, the yield of the single-photon pathway rises slower but keeps increasing over the whole delay range studied. Furthermore, this behavior reflects the evolving probability density of the ionic nuclear wave packet at the internuclear distances, where it can undergo resonant 3 ω and 1 ω transitions from the a 4 Π u to the f 4 Π g state of O 2 + .

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2019

Limits on magnetically induced Faraday rotation from polarized He 3 atoms

Faraday rotation has become a powerful tool in a large variety of physics applications. Most prominently, Faraday rotation can be used in precision magnetometry. Here we report measurements of gyromagnetic Faraday rotation on a dense, hyperpolarized 3 He gas target. Here, theoretical calculations predict the rotations of linearly polarized light due to the magnetization of spin-1/2 particles on the scale of 10 –7 radians. To maximize the signal, a 3 He target designed to use with a multipass cavity is combined with a sensitive apparatus for polarimetry that can detect optical rotations on the order of 10 –8 radians. Although the expected results are well above the sensitivity for the given experimental conditions, no nuclear-spin-induced rotation was observed.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2019

Pulse-duration dependence of the double-to-single ionization ratio of Ne by intense 780-nm and 800-nm laser fields: Comparison of simulations with experiments

Accurate ab initio calculations of the ratio of double-to-single ionization of Ne atoms in strong laser fields are difficult due to the many-electron nature of the target. Here, with accurate total cross sections carefully evaluated by using the state-of-the-art many-electron R-matrix theory for both electron-impact ionization and electron-impact excitation of Ne + , we simulate the total double-ionization yields of Ne 2+ in strong laser fields at 780 and 800 nm for pulse durations in the range from 7.5 to 200 fs based on the improved quantitative rescattering model. The corresponding single-ionization yields of Ne + are calculated within the nonadiabatic tunneling model of Perelomov, Popov, and Terent'ev. The ratio of double-to-single ionization of Ne is then obtained from the calculated double- and single-ionization yields. By normalizing the ratio to the one calculated from solving the time-dependent Schrödinger equation for a short few-cycle pulse, we make quantitative comparisons of our results with experimental data to show that our model predicts the experimental findings very well. Lastly, we analyze the pulse-duration dependence of the double-to-single ionization ratio.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2019

Photoionization and photofragmentation of singly charged positive and negative Sc 3 N @ C 80 endohedral fullerene ions

Photoprocesses of the endohedral fullerene ions $\mathrm{Sc_3N@C_{80}^{+}}$ and $\mathrm{Sc_3N@C_{80}-}$ in the gas phase have been investigated in the photon energy ranges 30-50 eV and 280-420 eV. Single and double ionization as well as single ionization accompanied by the release of a C 2 dimer were observed as a function of the photon energy for the positive parent ion and double detachment was measured for the negative parent ion. The emphasis of the experiments was on the specific effects of the encapsulated trimetallic nitride cluster Sc 3 N on the observed reactions. Clear evidence of photoexcitation near the Sc L edge is obtained with the dominating contributions visible in the one- and two-electron-removal channels. K-vacancy production in the encapsulated central nitrogen atom is seen in the single ionization of $\mathrm{Sc_3N@C_{80}^{+}}$ but is much less pronounced in the photoionization-with-fragmentation channel. Comparison of the cross sections near the carbon K edge with the corresponding channels measured previously in the photoionization of $\mathrm{Lu_3N@C_{80}^+}$ reveal strong similarities. Previously predicted sharp resonance features in the ionization of $\mathrm{Sc_3N@C_{80}^{+}}$ ions below the Sc M edge are not confirmed. Finally, the experiments are accompanied by quantum-chemistry calculations in the Hartree-Fock approximation and by model calculations employing density functional theory (DFT).

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Alignment of Polarization against an Electric Field in van der Waals Ferroelectrics

Polarization in ferroelectrics can be switched in the direction of an applied electric field by dipole reorientation, enabling numerous applications and fundamental phenomena. In this study, we demonstrate that, in the van der Waals (vdW) layered ferrielectric Cu In P 2 S 6 , a unique mechanism exists where polarization aligns against the direction of the applied electric field, seemingly in violation of the fundamental properties of a dipolar solid. The mechanism is the result of the electric field driving the Cu atoms unidirectionally across the vdW gaps, which is distinctively different from dipole reorientation. The crossing of Cu atoms is the fundamental process of ionic conductivity, yet it is compatible with the existence of polarization. These phenomena are confirmed by nanoscale imaging and spectroscopy of ferroelectric capacitors, coupled with dynamic density-functional-theory simulations. The symbiotic relationship of ferroelectric and ionic phenomena enables alternative approaches to control polarization and necessitates a change in perspective on nucleation, domain-wall dynamics, and other ferroelectric and electromechanical characteristics in material systems where ionic and ferroelectric phenomena manifest.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Quadratic Zeeman effect in hydrogen at 2–3 MG magnetic fields

The Zeeman effect is used for measurement of magnetic fields in astrophysical and laboratory plasmas. Magnetic fields in atmospheres of magnetic white dwarf stars are in the range 40 kG–1 GG. The quadratic Zeeman effect results in the additional split and shift of lines for magnetic fields >2 MG. Hydrogen Balmer lines were studied in magnetic fields delivered by a 1 MA pulse power generator. The magnetic field was generated by rod loads 0.8–1 mm in diameter. A droplet of CH oil on the load center was the source of hydrogen. A low ionized oil layer was backlit by blackbody emission from the rod with a temperature of 0.5–0.6 eV. Zeeman splitting of H-alpha and H-beta absorption lines were with a grating spectrometer. A spectral shift of the central component of the triplet indicated the quadratic Zeeman effect in hydrogen lines.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2011

Electrical Breakdown in Water Vapor

In this paper investigations of the voltage required to break down water vapor are reported for the region around the Paschen minimum and to the left of it. In spite of numerous applications of discharges in biomedicine, and recent studies of discharges in water and vapor bubbles and discharges with liquid water electrodes, studies of the basic parameters of breakdown are lacking. Paschen curves have been measured by recording voltages and currents in the low-current Townsend regime and extrapolating them to zero current. The minimum electrical breakdown voltage for water vapor was found to be 480 V at a pressure times electrode distance (pd) value of around 0.6 Torr cm ({approx}0.8 Pa m). The present measurements are also interpreted using (and add additional insight into) the developing understanding of relevant atomic and particularly surface processes associated with electrical breakdown.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Dynamic Scaling and Island Growth Kinetics in Pulsed Laser Deposition of SrTiO 3

We use real-time diffuse surface x-ray diffraction to probe the evolution of island size distributions and its effects on surface smoothing in pulsed laser deposition (PLD) of SrTiO 3 . In this study, we show that the island size evolution obeys dynamic scaling and two distinct regimes of island growth kinetics. Our data show that PLD film growth can persist without roughening despite thermally driven Ostwald ripening, the main mechanism for surface smoothing, being shut down. The absence of roughening is concomitant with decreasing island density, contradicting the prevailing view that increasing island density is the key to surface smoothing in PLD. We also report a previously unobserved crossover from diffusion-limited to attachment-limited island growth that reveals the influence of nonequilibrium atomic level surface transport processes on the growth modes in PLD. We show by direct measurements that attachment-limited island growth is the dominant process in PLD that creates step flowlike behavior or quasistep flow as PLD “self-organizes” local step flow on a length scale consistent with the substrate temperature and PLD parameters.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Helicity-Selective Enhancement and Polarization Control of Attosecond High Harmonic Waveforms Driven by Bichromatic Circularly Polarized Laser Fields

High harmonics driven by two-color counter-rotating circularly-polarized laser fields are a unique source of bright, circularly-polarized, extreme ultraviolet and soft x-ray beams, where the individual harmonics themselves are completely circularly polarized. Here, we demonstrate the ability to preferentially select either the right or left circularly polarized harmonics simply by adjusting the relative intensity ratio of the bichromatic circularly polarized driving laser field. In the frequency domain, this significantly enhances the harmonic orders that rotate in the same direction as the higher intensity driving laser. In the time domain, this helicity-dependent enhancement corresponds to control over the polarization of the resulting attosecond waveforms. Here, this helicity control enables the generation of circularly-polarized high harmonics with a user-defined polarization of the underlying attosecond bursts. In the future, this technique should allow for the production of bright highly elliptical harmonic supercontinua as well as the generation of isolated elliptically polarized attosecond pulses.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2018

Real-Time Observation of Molecular Spinning with Angular High-Harmonic Spectroscopy

We demonstrate an angular high-harmonic spectroscopy method to probe the spinning dynamics of a molecular rotation wave packet in real time. With the excitation of two time-delayed, polarization-skewed pump pulses, the molecular ensemble is impulsively kicked to rotate unidirectionally, which is subsequently irradiated by another delayed probe pulse for high-order harmonic generation (HHG). The spatiotemporal evolution of the molecular rotation wave packet is visualized from the time-dependent angular distributions of the HHG yields and frequency shift measured at various polarization directions and time delays of the probe pulse. Here, the observed frequency shift in HHG is demonstrated to arise from the nonadiabatic effect induced by molecular spinning. Different from the previous spectroscopic and Coulomb explosion imaging techniques, the angular high-harmonic spectroscopy method can reveal additionally the electronic structure and multiple orbitals of the sampled molecule. All the experimental findings are well reproduced by numerical simulations. Further extension of this method would provide a powerful tool for probing complex polyatomic molecules with HHG spectroscopy.

74 ATOMIC AND MOLECULAR PHYSICS↗