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At least 37 records · Page 2

Time-resolved quantum beats in the fluorescence of helium resonantly excited by XUV radiation

Abstract We report on the observation of time-resolved quantum beats in the helium fluorescence from the transition 1 s 3 p → 1 s 2 s , where the initial state is excited by XUV free electron laser radiation. The quantum beats originate from the Zeeman splitting of the magnetic substates due to an external magnetic field. We perform a systematic study of this effect and discuss the possibilities of studying this phenomenon in the XUV and x-ray regime.

Optics↗

Imaging multiphoton ionization dynamics of CH 3 I at a high repetition rate XUV free-electron laser

XUV multiphoton ionization of molecules is commonly used in free-electron laser experiments to study charge transfer dynamics. However, molecular dissociation and electron dynamics, such as multiple photon absorption, Auger decay, and charge transfer, often happen on competing time scales, and the contributions of individual processes can be difficult to unravel. We experimentally investigate the Coulomb explosion dynamics of methyl iodide upon core–hole ionization of the shallow inner-shell of iodine (4d) and classically simulate the fragmentation by phenomenologically introducing ionization dynamics and charge transfer. Under our experimental conditions with medium fluence and relatively long XUV pulses (~75 fs), we find that fast Auger decay prior to charge transfer significantly contributes to the charging mechanism, leading to a yield enhancement of higher carbon charge states upon molecular dissociation. Furthermore, we argue for the existence of another charging mechanism for the weak fragmentation channels leading to triply charged carbon atoms. This study shows that classical simulations can be a useful tool to guide the quantum mechanical description of the femtosecond dynamics upon multiphoton absorption in molecular systems.

Optics↗

UV-induced dissociation of CH 2 BrI probed by intense femtosecond XUV pulses

The ultraviolet (UV)-induced dissociation and photofragmentation of gas-phase CH 2 BrI molecules induced by intense femtosecond extreme ultraviolet (XUV) pulses at three different photon energies are studied by multi-mass ion imaging. Using a UV-pump–XUV-probe scheme, charge transfer between highly charged iodine ions and neutral CH 2 Br radicals produced by C–I bond cleavage is investigated. In earlier charge-transfer studies, the center of mass of the molecules was located along the axis of the bond cleaved by the pump pulse. In the present case of CH 2 BrI, this is not the case, thus inducing a rotation of the fragment. We discuss the influence of the rotation on the charge transfer process using a classical over-the-barrier model. Our modeling suggests that, despite the fact that the dissociation is slower due to the rotational excitation, the critical interatomic distance for charge transfer is reached faster. Furthermore, we suggest that charge transfer during molecular fragmentation may be modulated in a complex way.

74 ATOMIC AND MOLECULAR PHYSICS↗

Time-Resolved XUV Opacity Measurements of Warm Dense Aluminum

The free-free opacity in plasmas is fundamental to our understanding of energy transport in stellar interiors and for inertial confinement fusion research. However, theoretical predictions in the challenging dense plasma regime are conflicting and there is a dearth of accurate experimental data to allow for direct model validation. Here we present time-resolved transmission measurements in solid-density Al heated by an XUV free-electron laser. We use a novel functional optimization approach to extract the temperaturedependent absorption coefficient directly from an oversampled pool of single-shot measurements, and find a pronounced enhancement of the opacity as the plasma is heated to temperatures of order of the Fermi energy. Plasma heating and opacity enhancement are observed on ultrafast timescales, within the duration of the femtosecond XUV pulse. We attribute further rises in the opacity on ps timescales to melt and the formation of warm dense matter

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Time-resolving state-specific molecular dissociation with XUV broadband absorption spectroscopy

The electronic and nuclear dynamics inside molecules are essential for chemical reactions, where different pathways typically unfold on ultrafast timescales. Extreme ultraviolet (XUV) light pulses generated by free-electron lasers (FELs) allow atomic-site and electronic-state selectivity, triggering specific molecular dynamics while providing femtosecond resolution. Yet, time-resolved experiments are either blind to neutral fragments or limited by the spectral bandwidth of FEL pulses. Here, we combine a broadband XUV probe pulse from high-order harmonic generation with an FEL pump pulse to observe dissociation pathways leading to fragments in different quantum states. We temporally resolve the dissociation of a specific O 2 + state into two competing channels by measuring the resonances of ionic and neutral fragments. This scheme can be applied to investigate convoluted dynamics in larger molecules relevant to diverse science fields.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Theoretical analysis of the role of complex transition dipole phase in XUV transient-absorption probing of charge migration

We theoretically investigate the role of complex dipole phase in the attosecond probing of charge migration. The iodobromoacetylene ion (ICCBr + ) is considered as an example, in which one can probe charge migration by accessing both the iodine and bromine ends of the molecule with different spectral windows of an extreme-ultraviolet (XUV) pulse. The analytical expression for transient absorption shows that the site-specific information of charge migration is encoded in the complex phase of cross dipole products for XUV transitions between the I-4 d and Br-3 d spectral windows. Ab-initio quantum chemistry calculations on ICCBr + reveal that there is a constant π phase difference between the I-4 d and Br-3 d transient-absorption spectral windows, irrespective of the fine-structure energy splittings. Transient absorption spectra are simulated with a multistate model including the complex dipole phase, and the results correctly reconstruct the charge-migration dynamics via the quantum beats in the two element spectral windows, exhibiting out-of-phase oscillations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Space-resolved spectra of laser-produced plasmas in the XUV

The design and imaging properties of an XUV (extreme ultraviolet, 200-550 A) normal-incidence slitless spectrograph, the spectrum obtained from laser-generated plasmas, and the monochromatic plasma images are described. The electron temperature of the plasmas, electron density as a function of position in the plasma, and the thickness of material penetrated by the laser pulse are determined. Elements from Z = 6 to Z = 28 were investigated, in addition to Nb. Secondary plasma-emission regions were observed 2-3 mm from the flat (thick or thin) targets. Time-integrated photographs of the expanding plasmas were recorded by the slitless spectrograph. A technique for obtaining time-resolved images of the plasmas in picosecond time intervals is proposed, and problems in the design of a stigmatic XUV spectrograph are discussed.

Feldman, U.↗

The analysis of XUV emission lines

A technique for analyzing measurements of XUV spectral-line intensities is described. Application of the technique to OSO-4 and OSO-6 spectra indicates that the mean coronal temperature is 2.1 million K in typical active solar regions and that the mean coronal temperature in typical quiet regions ranges from 1.5 to 2.1 million K. One active-region spectrum shows evidence for substantial quantities of coronal material with temperatures between 2 and 3.5 million K. Measurements from limb spectra show evidence that (1) coronal abundances of N and O are low relative to heavier elements; or (2) that the ionization-equilibrium calculations used may contain systematic errors; or (3) that the XUV intensity measurements may be incorrectly calibrated.

Withbroe, G. L.↗

Channel electron multipliers - Detection efficiencies with opaque MgF2 photocathodes at XUV wavelengths

Detection efficiencies of channel electron multipliers (CEM) with opaque MgF2 photocathodes obtained in the extreme ultraviolet (XUV), 44 A to 990 A, are reported. A stable highly efficient response is reported for that interval, with no adverse effects on CEM performance. Efficiencies twice those of uncoated CEMs are obtained for 50 A to 350 A. The Mullard B419BL and Galileo 4510WL single-stage cone-cathode CEMs were used in the experiments. A rare-gas double ionization chamber was employed as absolute standard detector for 406 A to 990 A, and a flow Geiger counter filled with 96% argon and 4% isobutane for 44 A to 256 A. Absolute detection efficiencies are 10% higher from 67 A to 990 A when photocathodes are illuminated at an angle of incidence 45 deg. The photocathodes suffered no loss of response in storage (in vacuum or air) after an initial aging period. Effects of scattered UV radiation are greatly reduced when MgF2-coated CEMs are used in the XUV.

Lapson, L. B.↗

Thin aluminum filters for use on the Apollo Telescope Mount XUV spectrographs

Thin, unbacked, aluminum film filters were used on two extreme ultraviolet (XUV) instruments flown on the Apollo Telescope Mount of Skylab by the Naval Research Laboratory to transmit the XUV radiation while blocking the longer wavelength radiation that would saturate the detector. The requirements placed on these filters - large size, resistance to degradation by high acoustic and vibration fields, and low pinhole transmittances - were far more severe than those placed on any filters previously flown. Special techniques were developed for vacuum evaporation of the aluminum, removal of the films from the substrates, supporting the films and mounting them to obtain finished filters, and storing them so that no degradation took place. A description of these techniques will be given.

Schumacher, R. J.↗

Structure and dynamics of a solar flare - X-ray and XUV observations

Results are presented for an analysis of X-ray and XUV emission from the solar flare that occurred on September 5, 1973. X-ray emission was monitored by ionization chambers aboard the Solrad 9 satellite, and the XUV emission in the wavelength range 170-345 A was recorded by a slitless objective-grating spectroheliograph on Skylab. The physical parameters of the flare plasma, including temperature, density, volume, and magnetic-field configuration, are evaluated. A geometrical loop model is used to determine the volumes of the various emitting regions. The structure of the flare in the rise and decay phases is examined in detail, and conclusions about the effect of various dynamic processes in the flare plasma are made. A major finding is that continued energy release is required well into the flare decay phase. In the rise phase, energy is apparently released only along a small portion of a loop, and in the decay phase apparently throughout most of its length.

Dere, K. P.↗

Anti-Stokes scattering as an XUV radiation source

Harris (1977) has shown that laser induced scattering from atoms stored in a metastable level may be used to produce an XUV radiation source with several unique properties, including narrow linewidth, tunability, linear polarization, picosecond pulsewidth, and relatively high peak spectral brightness. The present investigation provides a summary concerning the progress made on the use of this radiation source as a unique instrument for XUV spectroscopy, and as a possible flashlamp for a 200 A laser. Zych et al. (1978) demonstrated that the maximum spectral brightness of the source is that of a blackbody with a temperature of the metastable storage level. The peak count rate and peak spectral brightness of the anti-Stokes emission at 569 A are 17 times and 139 times greater than those of the 584 A resonance line. The anti-Stokes process was employed as an external source of radiation for high resolution spectroscopy of the 3p6 shell of potassium. Attention is also given to emission spectroscopy of lithium, metastable levels which are appropriate for storage, and a hollow cathode discharge.

Harris, S. E.↗

Plasma diagnostics for the outer solar corona - UV and XUV Fe XII lines

The formation of the UV and XUV spectral lines of Fe XII in the outer corona was investigated. The results indicate that these lines can be an important tool for probing the physical conditions in the coronal regions where the solar wind is generated. The Fe XII lines can be particularly useful for determining outflow velocities of heavy ions in the solar wind and for providing critical empirical constraints on energy transport and dissipation mechanisms in the solar wind acceleration region. Application of the theoretical calculations to existing UV, EUV, and XUV observations of the low corona provide evidence that: (1) the inclusion of the effects of resonances in the collision strengths for the low-lying levels of Fe XII is important, (2) that the contributions of resonances for these levels are even larger than the estimates given in the present paper, and (3) that the collision strengths used here yield populations for these levels which are accurate to a factor of 2. These results have implications concerning the accuracy of abundances and densities derived from observations of the Fe XII lines in the low corona.

Withbroe, G. L.↗

The Ultra High Resolution XUV Spectroheliograph

The Ultra High Resolution XUV Spectroheliograph (UHRXS), a solar observatory planned for the Space Station Freedom, is described. The UHRXR instruments include nine XUV Ritchey-Chretien telescopes covering a spectral range of 70-350 A, which will provide images of solar atmosphere structures ranging in temperature from 50,000 to 20,000,000 K. The images will be obtained with spatial resolution that is an order of magnitude better than any other currently planned solar satellite experiment.

Walker, Arthur B. C., Jr.↗

The Ultra High Resolution XUV Spectroheliograph. III - A modified configuration for a free flying platform

The Ultra-High Resolution XUV Spectroheliograph (UHRXS) is a comprehensive solar observatory capable of studying solar phenomena at soft X-ray, XUV, EUV, and VUV wavelengths with normal incidence imaging multilayer telescopes capable of very high angular resolution (about 0.1 arcsec), and spectrographs able to achieve high spectral resolution. This instrument has been selected by NASA for flight as an attached payload on the Space Station Freedom. Recent developments have made it clear that accommodations for attached payloads on Freedom will not become available during the initial operations of Freedom and may never be available. We have studied the changes that must be made to place the UHRXS instrument on a Free Flying Plafform such as the Delta Launched Explorer Bus. We report on the configuration, performance, and accommodation on a free flying platform of the revised UHRXS concept.

Walker, Arthur B. C., Jr.↗

Time-resolved relaxation and fragmentation of polycyclic aromatic hydrocarbons investigated in the ultrafast $\mathrm{XUV}$-$\mathrm{IR}$ regime

Polycyclic aromatic hydrocarbons (PAHs) play an important role in interstellar chemistry and are subject to high energy photons that can induce excitation, ionization, and fragmentation. Previous studies have demonstrated electronic relaxation of parent PAH monocations over 10–100 femtoseconds as a result of beyond-Born-Oppenheimer coupling between the electronic and nuclear dynamics. Here, we investigate three PAH molecules: fluorene, phenanthrene, and pyrene, using ultrafast XUV and IR laser pulses. Simultaneous measurements of the ion yields, ion momenta, and electron momenta as a function of laser pulse delay allow a detailed insight into the various molecular processes. We report relaxation times for the electronically excited PAH * , PAH +* and PAH 2+* states, and show the time-dependent conversion between fragmentation pathways. Additionally, using recoil-frame covariance analysis between ion images, we demonstrate that the dissociation of the PAH 2+ ions favors reaction pathways involving two-body breakup and/or loss of neutral fragments totaling an even number of carbon atoms.

79 ASTRONOMY AND ASTROPHYSICS↗

Effect of Auger recombination on transient optical properties in XUV and soft X-ray irradiated silicon nitride

Spatially encoded measurements of transient optical transmissivity became a standard tool for temporal diagnostics of free-electron-laser (FEL) pulses, as well as for the arrival time measurements in X-ray pump and optical probe experiments. The modern experimental techniques can measure changes in optical coefficients with a temporal resolution better than 10 fs. This, in an ideal case, would imply a similar resolution for the temporal pulse properties and the arrival time jitter between the FEL and optical laser pulses. However, carrier transport within the material and out of its surface, as well as carrier recombination may, in addition, significantly decrease the number of carriers. This would strongly affect the transient optical properties, making the diagnostic measurement inaccurate. Below we analyze in detail the effects of those processes on the optical properties of XUV and soft X-ray irradiated Si 3 N 4 , on sub-picosecond timescales. Si 3 N 4 is a wide-gap insulating material widely used for FEL pulse diagnostics. Theoretical predictions are compared with the published results of two experiments at FERMI and LCLS facilities, and with our own recent measurement. The comparison indicates that three body Auger recombination strongly affects the optical response of Si 3 N 4 after its collisional ionization stops. By deconvolving the contribution of Auger recombination, in future applications one could regain a high temporal resolution for the reconstruction of the FEL pulse properties measured with a Si 3 N 4 -based diagnostics tool.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗