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The spectrum of autoionizing states of xenon in the vacuum ultraviolet (VUV) was first observed by Beutler using a helium discharge lamp as the light source and a two-meter grating monochromator.
The goal of this project was to take a VUV laser system designed by Kapteyn-Murnane Labs (KMLabs)—the Hyperion VUV, and increase its functionality, efficiency, and applicability by further probing the fundamental physics taking place in the system and optimizing the system performance. More specifically, DOE accelerator applications—particularly for XFELs that require low-emittance electron beams, require precisely controlled ultrashort pulses in the deep-UV at 250-260 nm to drive the photocathode electron source. This is conventionally done using an ultrafast infrared laser, with subsequent stages of nonlinear upconversion in solid-state nonlinear-optical crystal media (principally BBO, which is commonly used for UV upconversion). However, maintaining high spatial mode beam quality, as well as precisely controlled temporal profile, has proven a persistent challenge. As a possible alternative to this approach, KMLabs has demonstrated a system that generates vacuum ultraviolet light (VUV) by upconverting pulses from an infrared ultrafast laser in a gas-filled hollow waveguide, driving a process of highly cascaded harmonic generation (HCHG). Because HCHG upconversion is done in a gas, rather than a solid, at high intensity in a guided-wave geometry, it retains an excellent beam spatial profile as well as a large spectral bandwidth that allows for control over the temperal structure of the pulse. A challenge, however, is in energy scaling of this HCHG technique to the ~1-20 μJ pulses required for photocathode applications. To-date, the pulse energies used in published HCHG work are sub-10-nJ. This project proposed to explore ways to generate higher-energy pulses using HCHG, as well as to investigate spectral and temporal shaping of the deep UV pulses by pulse shaping the infrared laser used to seed the process. Although we showed that our approach works for generating light at 259 nm, the total pulse energy achieved seems limited to approximately the same value as past work. However, the techniques we investigated may well have benefits for extending this source to much shorter wavelength output.
Doubly excited autoionizing states of alkaline earth atoms are explored by multistep laser spectroscopy, which is precisely the inverse process to dielectronic recombination, the recombination of hot electron with ions via an autoionizing state. Dielectronic recombination is an important mechanism leading to power loss in high temperature plasmas. Measurements included the autoionization rates of atoms in zero field and in the presence of electric and magnetic fields, as might be encountered in a plasma. To mimic the effects of the rapidly varying fields of electron collisions measurements were made in the presence of microwave electric fields. These experiments are analogous to experiments conducted with combined high intensity infrared and vuv laser fields, In laser/microwave experiments the effects of laser pulse envelope timing relative to the microwave phase were explored extensively.
The goal of this project was to probe fundamental kinetics questions regarding the gas phase reactive behavior of oxygenates. In order to succeed, our program necessitated both the development of new experimental tools and the development of theory based kinetic models to explain the chemistry of oxygenate fuels. By using advanced hybrid additive manufacturing/ traditional manufacturing techniques to create specialized ceramic micro-reactors, the team was able to simulate extreme high-temperature environments with much greater precision and durability than was previously possible. These tiny, high-tech tubes allow researchers to capture and identify "fleeting" chemical species—molecules that exist for only a fraction of a millisecond—using sophisticated light sources and mass spectrometry. Additionally, the team supported the development of a tabletop VUV laser system for isomer detection without a synchrotron. Through this work, we have successfully mapped out the specific chemical pathways of various oxygen-rich fuels, solving long-standing mysteries about how these substances break down kinetically. Ultimately, this research provides the fundamental knowledge needed to design next-generation engines and fuels that are better for the environment.
The interactions of VUV radiation with solids are explored in reviews and reports of recent theoretical and experimental investigations from the fields of atomic and molecular physics, solid-state physics, and VUV instrumentation. Topics examined include photoabsorption and photoionization, multiphoton processes, plasma physics, VUV lasers, time-resolved spectroscopy, synchrotron radiation centers, solid-state spectroscopy, and dynamical processes involving localized levels. Consideration is given to the fundamental principles of photoemission, spin-polarized photoemission, inverse photoemission, semiconductors, organic materials, and adsorbates.
Giant pulse Q switched lasers generated plasmas, noting VUV spectral line shifts, asymmetries and existence of satellite lines
The short wavelength operation of free-electron laser (FEL) oscillators is limited by the availability of high-reflectivity, thermally stable, and radiation-resistant FEL mirrors in the VUV wavelength. We report our recent work to extend the shortest lasing wavelength of the oscillator FEL to 168.6 nm using a storage ring FEL. This progress has been made possible by developing a new FEL configuration with substantially reduced undulator harmonic radiation on the FEL mirror, a thermally stable FEL optical cavity, and a new type of high-reflectivity fluoride-based multilayer coating with a protective capping layer. Using these fluoride-based mirrors, we have demonstrated storage ring FEL lasing from 168.6 to 179.7 nm with excellent beam stability. Employing this VUV FEL in Compton scattering, we have produced the first 120 MeV gamma rays at the High Intensity Gamma-ray Source (HIGS). Furthermore, operating the HIGS in this new high-energy region will create many new opportunities for photonuclear physics research, in particular, the low-energy QCD research.
The results of experiments performed to check the possibility of stimulated emission in the extreme vacuum ultraviolet (VUV) by an Al(+3) laser-generated plasma are reported. It is concluded that the spectral line intensity anomalies previously observed are not due to population inversion.
The spectrum of Al VII is re-examined in the vuv. A laser-produced plasma is used as a light source. Twenty-four newly classified lines are reported. No new energy levels have been determined.
Three classes of molecular electronic transition lasers produced by hybrid pumping of high pressure rate gas mixtures are discussed. These are (1) rare gas dimer lasers (such as excited Ar2, Kr2, and Xe2) lasing in the VUV, (2) rare gas halide lasers or excimer lasers (such as KrF, ArF, and XeCl excimers) lasing in the UV, and (3) the charge transfer molecular ion laser (such as N2/+/) lasing in the visible range. Laser excitation methods and kinetic sequences are examined for these lasers.
Laser beams operating in high order transverse modes, especially orbital angular momentum (OAM) modes, have been used increasingly in many frontier research areas. The characterization of these laser modes and the related component analysis can be carried out using the retrieved optical phase. However, conventional iterative phase retrieval methods, when applied to pure OAM modes, may fail because their convergence depends on the choice of the initial phase. Here, we present an improved phase retrieval method which can incorporate additional phase information obtained using knife-edge diffraction. Using no additional optics or few optics available in a wide spectral range, this method is particularly suitable for short wavelength lasers such as free-electron lasers (FELs) in the VUV, EUV, and X-ray regimes. Finally, this method has been tested using simulated beams, and successfully applied to experimentally generated beams from a HeNe laser and an FEL.
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.
Radiative lifetimes of the eight lowest even parity levels in the doublet system of B I are measured using time-resolved laser-induced fluorescence in the UV and VUV on an atomic beam of boron. The accurate lifetimes provide a base for improved determination of absolute transition probabilities in B I. The techniques described are broadly applicable to measurement of lifetimes of levels with transitions in the visible, UV, and VUV in almost any element.
We are currently developing an atomic oxygen diagnostic to study the degree of oxygen dissociation in ground-based facilities. The absorption of the (sub 3)P - (sup 3)S(sup 0) resonance triplet in the vacuum ultraviolet is a direct measure of the ground state number density of atomic oxygen. Although the integrated line strength is well known for these transitions, the line profile is not. We report the results of a series of experiments in which the line profile is measured in shock-heated oxygen. An ArF excimer laser and a hydrogen Raman shifter generate tunable VUV radiation at the resonance wavelength. The test gas is dissociated oxygen, generated in the Electric Arc Shock Tube (EAST) Facility at NASA-Ames Research Center. By measuring the absorption of known concentrations of atomic oxygen, we are able to study the absorption line profile. The results will serve as a calibration to apply this diagnostic in other flowfields.
Analytical and experimental studies of the rapid transfer of stored populations from metastable states to selected target states of a different species are reported. Both laser-induced or laser-switched collision and laser-induced two-photon spontaneous emission are described. It is shown that the laser-induced collision method is particularly useful in the visible and UV spectral regions. It has applications in photochemistry, gas-phase kinetics, and in high-power, high-energy gas-phase lasers. The anti-Stokes source is useful in the VUV and soft X-ray spectral regions.
An IR–vacuum ultraviolet (VUV) ion-dip spectroscopy method is utilized to examine the IR spectrum of acetaldehyde oxide (CH3CHOO) in the overtone CH stretch (2νCH) spectral region. IR activation creates a depletion of the ground state population that reduces the VUV photoionization signal on the parent mass channel. IR activation of the more stable and populated syn-CH3CHOO conformer results in rapid unimolecular decay to OH + vinoxy products and makes the most significant contribution to the observed spectrum. The resultant IR–VUV ion-dip spectrum of CH3CHOO is similar to that obtained previously for syn-CH3CHOO using IR action spectroscopy with UV laser-induced fluorescence detection of OH products. The prominent IR features at 5984 and 6081 cm−1 are also observed using UV + VUV photoionization of OH products. Complementary theoretical calculations utilizing a general implementation of second-order vibrational perturbation theory provide new insights on the vibrational transitions that give rise to the experimental spectrum in the overtone CH stretch region. The introduction of physically motivated small shifts of the harmonic frequencies yields remarkably improved agreement between experiment and theory in the overtone CH stretch region. The prominent features are assigned as highly mixed states with contributions from two quanta of CH stretch and/or a combination of CH stretch with an overtone in mode 4. The generality of this approach is demonstrated by applying it to three different levels of electronic structure theory/basis sets, all of which provide spectra that are virtually indistinguishable despite showing large deviations prior to introducing the shifts to the harmonic frequencies.
Aims: A tunable, high spectral resolution, high effective finesse, vacuum ultraviolet (VUV) Fabry-Perot interferometer (PPI) is designed for obtaining narrow-passband images, magnetograms, and Dopplergrams of the transition region emission line of CIV (155 nm). Methods: The integral part of the CIV narrow passband filter package (with a 2-10 pm FWHM) consists of a multiple etalon system composed of a tunable interferometer that provides high-spectral resolution and a static low-spectral resolution interferometer that allows a large effective free spectral range. The prefilter for the interferometers is provided by a set of four mirrors with dielectric high-reflective coatings. A tunable interferometer, a VUV piezoelectric-control etalon, has undergone testing using the surrogate F2 eximer laser line at 157 nm for the CIV line. We present the results of the tests with a description of the overall concept for a complete narrow-band CIV spectral filter. The static interferometer of the filter is envisioned as being hudt using a set of fixed MgF2 plates. The four-mirror prefilter is designed to have dielectric multilayer n-stacks employing the design concept used in the Ultraviolet Imager of NASA's Polar Spacecraft. A dual etalon system allows the effective free spectral range to be commensurate with the prefilter profile. With an additional etalon, a triple etalon system would allow a spectrographic resolution of 2 pm. The basic strategy has been to combine the expertise of spaceflight etalon manufacturing with VUV coating technology to build a VUV FPI which combines the best attributes of imagers and spectrographs into a single compact instrument. Results. Spectro-polarimetry observations of the transition region CIV emission can be performed to increase the understanding of the magnetic forces, mass motion, evolution, and energy release within the solar atmosphere at the base of the corona where most of the magnetic field is approximately force-free. The 2D imaging of the full vector magnetic field at the height of maximum magnetic influence (minimum plasma beta) can be accomplished, albeit difficult, by measuring the Zeeman splitting of the CIV resonance pair. Designs of multiple VUV FPIs can be developed for integration into future orbiting solar observatories to obtain rapid cadence, spectral imaging of the transition region.
Helium in the superfluid state emits copious amounts of radiation in the ultraviolet region when excited by an electron stream. Conventional laser action using mirrors is impossible in superfluid helium because there are no mirrors that will reflect VUV radiation. By utilizing the distributed feedback method, the superfluid helium can be made to lase. By setting up a standing wave in superfluid helium that has a wavelength equal to, or harmonically related to, half the wavelength of the photon radiation chosen to be emitted as laser radiation by the superfluid helium, the need for end mirrors to produce reflection of the laser radiation is eliminated and reflection occurs instead at the wavefronts of the standing wave. The photons leave the superfluid helium at right angles to the standing wave as coherent radiation having a very high intensity. The standing wave established in the superfluid helium may be an acoustical standing wave, a thermal standing wave (second sound), or an electric standing wave.