High-order harmonic generation yielding tunable extreme-ultraviolet radiation of high spectral purity

Production of extreme-ultraviolet radiation by high-order harmonic generation is demonstrated to yield unprecedented spectral purity of lambda/Delta lambda=2.5 x 10(5) at wavelengths covering the entire range 40-100 nm. Tunability and sub-cm(-1) bandwidth of the harmonics are demonstrated in recordings of the He (1s4p) and Ar (3p(5)3d') resonance lines at 52.2 and 86.6 nm. Frequency shift of the harmonics due to chirp-induced phenomena are investigated and found to be small, resulting in a frequency accuracy of about 5 x 10(-7) in the domain of extreme-ultraviolet radiation.     

A Dense Grid of Reference Iodine Lines for Optical Frequency Calibration in the Range 595-655 nm

A dense grid of reference lines in the hyperfine structure of the B-X transitions of molecular iodine ((127)I(2)) is presented. Frequencies of 481 "t"-hyperfine components in 15 vibrational bands covering the wavelength range 595-655 nm were determined with an absolute accuracy of 1.0 MHz (1varsigma uncertainty). Spectra were obtained by Doppler-free saturation spectroscopy using a cw ring-dye laser of 1-MHz bandwidth. Center-of-gravity frequencies of rovibronic lines, determined by correcting for the calculated hyperfine shift, are included separately in a least-squares parametrization for each band. From the obtained molecular constants a prediction is made for all t-hyperfine components of the 15 bands covering 595-655 nm. Hence a dense grid of reference lines of 1 MHz (1varsigma) absolute accuracy is created, with a line in each interval of 1 cm(-1) in the entire range. This spectral atlas of about 3400 lines may provide a useful calibration tool in many laboratories. Copyright 2000 Academic Press.     

QED effects in molecules: test on rotational quantum states of H2

Quantum electrodynamic effects have been systematically tested in the progression of rotational quantum states in the X?1Σ(g)(+), v=0 vibronic ground state of molecular hydrogen. High-precision Doppler-free spectroscopy of the EF?1Σ(g)(+)-X?1Σ(g)(+) (0,0) band was performed with 0.005 cm(-1) accuracy on rotationally hot H2 (with rotational quantum states J up to 16). QED and relativistic contributions to rotational level energies as high as 0.13 cm(-1) are extracted, and are in perfect agreement with recent calculations of QED and high-order relativistic effects for the H2 ground state.     

Methanol as a sensitive probe for spatial and temporal variations of the proton-to-electron mass ratio

The 6.7 and 12.2 GHz masers, corresponding to the 5(1) → 6(0)A+ and 2(0) → 3(-1)E transitions in methanol (CH3OH), respectively, are among the brightest radio objects in the sky. We present calculations for the sensitivity of these and other transitions in the ground state of methanol to a variation of the proton-to-electron mass ratio. We show that the sensitivity is greatly enhanced due to a cancellation of energies associated with the hindered internal rotation and the overall rotation of the molecule. We find sensitivities of K(μ) = -42 and K(μ) = -33, for the 5(1) → 6(0)A+ and 2(0) → 3(-1)E transitions, respectively. The sensitivities of other transitions in the different isotopologues of methanol range from -88 to 330. This makes methanol a sensitive probe for spatial and temporal variations of the proton-to-electron mass ratio.     

High-resolution Fourier-transform extreme ultraviolet photoabsorption spectroscopy of 14N15N

The first comprehensive high-resolution photoabsorption spectrum of (14)N(15)N has been recorded using the Fourier-transform spectrometer attached to the Desirs beamline at the Soleil synchrotron. Observations are made in the extreme ultraviolet 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 N(2) that simulates its photoabsorption and photodissociation cross section by solution of an isotopomer independent formulation of the coupled-channel Schro?dinger 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.     

Lifetimes and transition frequencies of several singlet ungerade states in N2 between 106 000 and 109 000 cm

Using a narrow-band tunable XUV source, ultra-high resolution 1 XUV + 1 UV two-photon ionisation spectra were recorded of transitions to several singlet ungerade states in ¹⁴N₂ and ¹⁵N₂ in the range 106 000-109 000 cm⁻¹. The natural linewidths of the individual rotational spectral lines were determined and the resulting lifetimes were found to depend on vibrational level and for the c₃¹Π_u (v = 1) level also on isotope. Furthermore, accurate transition frequencies were determined and for several bands, lines near bandhead regions were resolved for the first time.     

Deep-UV absorption and Rayleigh scattering of carbon dioxide

Cavity ring-down spectroscopy and pressure ramp measurements have been used to determine the extinction coefficients of CO₂ in the deep-ultraviolet wavelength region, between 198 and 270 nm. The observed optical extinction confirms that there is a clear absorption onset of CO₂ in the deep-UV wavelength region. This onset has been reported previously around 205 nm. The new set of measurements presented here shows that the onset actually starts at higher energy, around 202 nm. For longer wavelengths it is found that the optical extinction demonstrates a 1/λ⁴ like behavior, as typical for Rayleigh scattering.     

HD as a probe for detecting mass variation on a cosmological time scale

The strong electronic absorption systems of the B1 Sigma u+-X1 Sigma g+ Lyman and the C1Pi u-X1 Sigma g+ Werner bands can be used to probe possible mass-variation effects on a cosmological time scale from spectra observed at high redshift, not only in H2 but also in the second most abundant hydrogen isotopomer HD. High resolution laboratory determination of the most prominent HD lines at extreme ultraviolet wavelengths is performed at an accuracy of delta lambda/lambda approximately 5 x 10(-8), forming a database for comparison with astrophysical data. Sensitivity coefficients Ki = d ln lambda i/d ln mu are determined for HD from quantum ab initio calculations as a function of the proton-electron mass ratio mu. Strategies to deduce possible effects beyond first-order baryon/lepton mass ratio deviations are discussed.     

Observation of a Rydberg series in H+H-: a heavy Bohr atom

We report on the realization of a heavy "Bohr atom," through the spectroscopic observation of a Rydberg series of bound quantum states at principal quantum numbers n=140 to 230. The system is made heavy by replacing an electron inside a hydrogen atom by a composite H- particle, thus forming a H+H- Coulombically bound system obeying the physical laws of a generalized atom with appropriate mass scaling.     

Highly accurate H2 Lyman and Werner band laboratory measurements and an improved constraint on a cosmological variation of the proton-to-electron mass ratio

Transition wavelengths on a large set of H2 Lyman and Werner band spectral lines have been obtained at an accuracy of 5 x 10(-8), using a narrow band tunable extreme ultraviolet laser. The data are used to determine a constraint on a possible cosmological variation of the proton-to-electron mass ratio (mu=Mp/me) from a comparison with highly redshifted spectral data of quasistellar objects, yielding a fractional change in the mass ratio of Deltamu/mu=-0.5+/-3.6 x 10(-5) (2sigma), which would correspond to a temporal change of d/dt(Deltamu/mu)=-0.4+/-3.0 x 10(-15) per year (2sigma) if a linear cosmological expansion model is assumed.