XUV-laser excitation of molecular fluorine

Excited states of the Fe₂ molecule are investigated in high resolution by means of 1 XUV + 1 UV resonance-enhanced photo-ionization. Perturbations in the C ¹Σ⁺_u valence state and the spectroscopy of the H ¹Π_u Rydberg state are studied in detail. It is shown that F₂ molecules may be state-selectively detected with a sensitivity of 5 × 10⁷ particles per cm³.     

Spectral redshift in harmonic generation from plasma dynamics in the laser focus

High-precision spectral measurements on the 9th harmonic generated in xenon gas are compared with calculations of the plasma dynamics resulting from multiphoton ionization in the laser focus. For the regime of 300 ps pulses and above-saturation intensities a novel mechanism producing redshifts in the harmonics is uncovered and explained. Ions play a double role: the nonlinear susceptibility of the ions is decisive for the harmonic intensity, while their mutual repulsion and the associated increase of the index of refraction is identified as the cause of the redshift.     

Narrow-band extreme-ultraviolet laser radiation tunable in the range 90.5–95 nm

Tunable, narrowband extreme ultraviolet radiation in the range 90.5–95 nm with only limited intensity variations is produced by frequency-tripling ultraviolet light from a frequency-doubled dye laser in a gas-jet of xenon. Acetylene gas is found to be an efficient medium for third-harmonic generation in this wavelength range as well. The extreme-ultraviolet radiation is applied in a spectroscopic study of the b ¹ II _u , v=6–8 and v=10–12, o ¹ II _u , v=0 and b¹ _u ⁺ , v=9 states of molecular nitrogen. From linewidth measurements a value k _p=6×10¹⁰ s^–1 for the predissociation rate of the b ¹ II _u , v=11 state is deduced.     

SBS pulse compression to 200 ps in a compact single-cell setup

Received: 14 September 1998 / Published online: 24 February 1999     

Double-well states of ungerade symmetry in H2: first observation and comparison with Ab initio calculations

The observation of a new class of long-lived outer well states of ungerade symmetry (B"B1Sigma+u) in molecular hydrogen, lying above the ionization threshold, is reported. Rovibrational levels within a potential extended over internuclear separations of R = 7-25 a.u. are experimentally investigated in a triple resonance scheme. Good agreement ( <0.5 cm(-1)) with updated ab initio calculations is found for vibrational levels up to v = 26, demonstrating that such calculations can now be extended to this energetic range above ionization, as long as interaction with the Rydberg manifolds is shielded by a barrier. The dynamical behavior (predissociation and autoionization) of this class of " u" symmetry states is remarkably different from similar outer well states of " g" symmetry; this phenomenon can be understood from the structure of doubly excited electronic states.     

Lifetime and predissociation yield of 14N2 b 1Piu(v=1)

The lifetime of the b 1Piu(v=1) state in 14N2 has been determined experimentally using a laser-based pump-probe scheme and an exceptionally long lifetime of 2.61 ns was found. Semiempirical close-coupling calculations of the radiative lifetime, which include Rydberg-valence interactions in the singlet manifold, are consistent with this large value, giving a value of 3.61 ns and suggesting a predissociation yield of approximately 28% for this level of the b state.     

First constraint on cosmological variation of the proton-to-electron mass ratio from two independent telescopes

A high signal-to-noise spectrum covering the largest number of hydrogen lines (90 H(2) lines and 6 HD lines) in a high-redshift object was analyzed from an observation along the sight line to the bright quasar source J2123-005 with the Ultraviolet and Visual Echelle Spectrograph on the European Southern Observatory Very Large Telescope (Paranal, Chile). This delivers a constraint on a possible variation of the proton-to-electron mass ratio of Δμ/μ=(8.5 ± 3.6(stat) ± 2.2(syst))×10(-6) at redshift z(abs) = 2.059, which agrees well with a recently published result on the same system observed at the Keck telescope yielding Δμ/μ=(5.6 ± 5.5(stat) ± 2.9(syst))×10(-6). Both analyses used the same robust absorption line fitting procedures with detailed consideration of systematic errors.     

On a possible variation of the proton-to-electron mass ratio: H2 spectra in the line of sight of high-redshift quasars and in the laboratory

Recently the finding of an indication for a decrease of the proton-to-electron mass ratio μ = m_p/m_e by 0.002% in the past 12 billion years was reported in the form of a Letter [E. Reinhold, R. Buning, U. Hollenstein, P. Petitjean, A. Ivanchik, W. Ubachs, Phys. Rev. Lett. 96 (2006) 151101]. Here we will further detail the methods that led to that result and put it in perspective. Laser spectroscopy on molecular hydrogen, using a narrow-band and tunable extreme ultraviolet laser system at the Laser Centre Vrije Universiteit Amsterdam, results in transition wavelengths of spectral lines in the Lyman and Werner band systems at an accuracy of (4-11) × 10⁻⁸, depending on the wavelength region. This corresponds to an absolute accuracy of 0.000004-0.000010 nm. A database of 233 accurately calibrated H₂ lines is presented here for future reference and comparison with astronomical observations. Recent observations of the same spectroscopic features in cold hydrogen clouds at redshifts z = 2.5947325 and z = 3.0248970 in the line of sight of two quasar light sources (Q 0405−443 and Q 0347−383) resulted in 76 reliably determined transition wavelengths of H₂ lines at accuracies in the range 2 × 10⁻⁷ to 1 × 10⁻⁶. Those observations were performed with the Ultraviolet and Visible Echelle Spectrograph at the Very Large Telescope of the European Southern Observatory at Paranal, Chile. A third ingredient in the analysis is the calculation of an improved set of sensitivity coefficients K_i, a parameter associated with each spectral line, representing the dependence of the transition wavelength on a possible variation of the proton-to-electron mass ratio μ. The new model for calculation of the K_i sensitivity coefficients is based on a Dunham representation of ground state and excited state level energies, derived from the most accurate data available in literature for the ground electronic state and the presently determined level energies in the and C¹Π_u states. Moreover, the model includes adiabatic corrections to electronic energies as well as local perturbation effects between B and C levels. The full analysis and a tabulation of the resulting K_i coefficients is given in this paper. A statistical analysis of the data yields an indication for a variation of the proton-to-electron mass ratio of Δμ/μ = (2.45 ± 0.59) × 10⁻⁵ for a weighted fit and Δμ/μ = (1.99 ± 0.58) × 10⁻⁵ for an unweighted fit. This result, indicating the decrease of μ, has a statistical significance of 3.5σ. Mass-variations as discussed relate to inertial or kinematic masses, rather than gravitational masses. Separate treatment of the data gives a similar positive result for each of the quasars Q 0405−443 and Q 0347−383. The statistical analysis is further documented and possible systematic shifts underlying the data, with the possibility of mimicking a non-zero Δμ/μ value, are discussed. The observed decrease in μ corresponds to a rate of change of d lnμ/dt = −2 × 10⁻¹⁵ per year, if a linear variation with time is assumed. Experiments for detecting a possible variation of μ in the modern epoch via ultra-precision experiments on H₂ quadrupole transitions are proposed.     

线形C5H自由基A2Δ电子态的自选轨道分裂和寿命展宽

重新研究了C₅H和C₅D自由基A²Δ-X2Π电子吸收谱带. 利用乙炔/氦混合气脉冲直流放电产生的碳氢等离子体制备气相C5H和C5D自由基,利用光腔衰荡光谱记录碳氢等离子体束的直接吸收光谱. 与之前工作相比,实验光谱的波长校准得到了改进. 通过对实验光谱的分析,首次实验确定了C₅H自由基A²Δ电子态的自旋-轨道分裂常数为-0.7(3) cm^-1. 这为标识A2￠电子态的提供了有力的实验证据. 通过对谱带寿命展宽的分析,A²Δ电子态的寿命估测为1.6±0.3 ps.