The CO A-X System for Constraining Cosmological Drift of the Proton-Electron Mass Ratio

The $\textrm{A}^1\Pi-\textrm{X}^1\Sigma^+$ band system of carbon monoxide, which has been detected in six highly redshifted galaxies ($z=1.6-2.7$), is identified as a novel probe method to search for possible variations of the proton-electron mass ratio ($\mu$) on cosmological time scales. Laboratory wavelengths of the spectral lines of the A-X ($v$,0) bands for $v=0-9$ have been determined at an accuracy of $\Delta\lambda/\lambda=1.5 \times 10^{-7}$ through VUV Fourier-transform absorption spectroscopy, providing a comprehensive and accurate zero-redshift data set. For the (0,0) and (1,0) bands, two-photon Doppler-free laser spectroscopy has been applied at the $3 \times 10^{-8}$ accuracy level, verifying the absorption data. Sensitivity coefficients $K_{\mu}$ for a varying $\mu$ have been calculated for the CO A-X bands, so that an operational method results to search for $\mu$-variation.Comment: 7 pages (main article), 3 figures, includes supplementary materia

Novel techniques in VUV high-resolution spectroscopy

Novel VUV sources and techniques for VUV spectroscopy are reviewed. Laser-based VUV sources have been developed via non-linear upconversion of laser pulses in the nanosecond (ns), the picosecond (ps), and femtosecond (fs) domain, and are applied in high-resolution gas phase spectroscopic studies. While the ns and ps pulsed laser sources, at Fourier-transform limited bandwidths, are used in wavelength scanning spectroscopy, the fs laser source is used in a two-pulse time delayed mode. In addition a Fourier-transform spectrometer for high resolution gas-phase spectroscopic studies in the VUV is described, exhibiting the multiplex advantage to measure many resonances simultaneously.Comment: 17 Pages, 8 figures, Conference proceedings of the VUV/X-ray 2013 at Hefei, Chin

Size effect in the ionization energy of PAH clusters

We report the first experimental measurement of the near-threshold photo-ionization spectra of polycyclic aromatic hydrocarbon clusters made of pyrene C16H10 and coronene C24H12, obtained using imaging photoelectron photoion coincidence spectrometry with a VUV synchrotron beamline. The experimental results of the ionization energy are confronted to calculated ones obtained from simulations using dedicated electronic structure treatment for large ionized molecular clusters. Experiment and theory consistently find a decrease of the ionization energy with cluster size. The inclusion of temperature effects in the simulations leads to a lowering of this energy and to a quantitative agreement with the experiment. In the case of pyrene, both theory and experiment show a discontinuity in the IE trend for the hexamer

High-resolution Fourier-transform XUV photoabsorption spectroscopy of 14N15N

The first comprehensive high-resolution photoabsorption spectrum of 14N15N has been recorded using the Fourier-transform spectrometer attached to the Desirs beamline at the Soleil synchrotron. Observations are made in the extreme ultraviolet (XUV) and span 100,000-109,000 cm-1 (100-91.7 nm). The observed absorption lines have been assigned to 25 bands and reduced to a set of transition energies, f values, and linewidths. This analysis has verified the predictions of a theoretical model of N2 that simulates its photoabsorption and photodissociation cross section by solution of an isotopomer independent formulation of the coupled-channel Schroedinger equation. The mass dependence of predissociation linewidths and oscillator strengths is clearly evident and many local perturbations of transition energies, strengths, and widths within individual rotational series have been observed.Comment: 14 pages, 8 figures, one data archiv

Vibrationally induced inversion of photoelectron forward-backward asymmetry in chiral molecule photoionization by circularly polarized light

Electron–nuclei coupling accompanying excitation and relaxation processes is a fascinating phenomenon in molecular dynamics. A striking and unexpected example of such coupling is presented here in the context of photoelectron circular dichroism measurements on randomly oriented, chiral methyloxirane molecules, unaffected by any continuum resonance. Here, we report that the forward-backward asymmetry in the electron angular distribution, with respect to the photon axis, which is associated with photoelectron circular dichroism can surprisingly reverse direction according to the ion vibrational mode excited. This vibrational dependence represents a clear breakdown of the usual Franck–Condon assumption, ascribed to the enhanced sensitivity of photoelectron circular dichroism (compared with other observables like cross-sections or the conventional anisotropy parameter-β) to the scattering phase off the chiral molecular potential, inducing a dependence on the nuclear geometry sampled in the photoionization process. Important consequences for the interpretation of such dichroism measurements within analytical contexts are discussed

Effect of electronic angular momentum exchange on photoelectron anisotropy following the two-colour ionization of krypton atoms

We present photoelectron energy and angular distributions for resonant two-photon ionization via several low-lying Rydberg states of atomic Kr. The experiments were performed by using synchrotron radiation to pump the Rydberg states and a continuous wave laser to probe them. Photoelectron images, recorded with both linear and circular polarized pump and probe light, were obtained in coincidence with mass-analyzed Kr ions. The photoelectron angular distributions and branching ratios for direct ionization into the Kr+ 2P3/2 and 2P1/2 spin-orbit continua show considerable dependence on the intermediate level, as well as on the polarizations of the pump and probe light. Photoelectron angular distributions were also recorded with several polarization combinations following two-colour excitation of the (2P1/2)5f[5/2]2 autoionizing resonance. These results are compared with the results of recent work on the corresponding autoionizing resonance in atomic Xe

VUV photoionization dynamics of the C 60 buckminsterfullerene: 2D-matrix photoelectron spectroscopy in an astrophysical context

Laboratory astrophysics and astrochemistr

Oscillator strengths for transitions to Rydberg levels in 12C16O^{12}C^{16}O, 13C16O^{13}C^{16}O and 13C18O^{13}C^{18}O between 967 and 972 A

Absorption oscillator strengths have been determined from high-resolution spectra in the 967-972 \AA region of three CO isotopomers for transitions to the Rydberg levels 4{\it p$\pi$}(0), 3{\it d$\pi$}(1) and 4{\it p$\sigma$}(0), as well as to the mixed {\it E(6)} level recently characterized by Eidelsberg et al. (2004). Synchrotron radiation from the Super-ACO electron storage ring at Orsay (LURE) was used as a light source. Oscillator strengths were extracted from the recorded spectra by least-squares fitting of the experimental profiles with synthetic spectra taking into account the homogeneous and heterogeneous interactions of the four levels. Column densities were derived from fits to the 3{\it p$\pi$}(0) absorption band whose oscillator strength is well established. These are the first reported measurements for $^{13}$C$^{18}$O. For $^{12}$C$^{16}$O, our results are consistent with the larger values obtained in the most recent laboratory and astronomical studies.Comment: 9 pages 7 figures 3 tables. Accepted in A&A, date of acceptance 11/05/200