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Recently, the extremely sensitive torsion-rotation transitions in methanol have been used to set a tight constraint on a possible variation of the proton-to-electron mass ratio over cosmological time scales. In order to improve this constraint, laboratory data of increased accuracy will be required. Here, we explore the possibility for performing high-resolution spectroscopy on methanol in a Stark-deflected molecular beam. We have calculated the Stark shift of the lower rotational levels in the ground torsion-vibrational state of CH3OH and CD3OH molecules, and have used this to simulate trajectories through a typical molecular beam resonance setup. Furthermore, we have determined the efficiency of non-resonant multi-photon ionization of methanol molecules using a femtosecond laser pulse. The described setup is in principle suited to measure microwave transitions in CH3OH at an accuracy below 10^{-8}.

A spectrometer for the measurement of spontaneous Rayleigh-Brillouin scattering line profiles at ultraviolet wavelengths from gas phase molecules has been developed, employing a high-power frequency-stabilized UV laser with narrow bandwidth (2 MHz). The UV light from a frequency-doubled titanium:sapphire laser is further amplified in an enhancement cavity, delivering a 5 Watt UV-beam propagating through the interaction region inside a scattering cell. The design of the RB-scattering cell allows for measurements at gas pressures in the range 0-4 bar and at stably controlled temperatures from -30 to 70 degree Celsius. A scannable Fabry-Perot analyzer with instrument resolution of 232 MHz probes the Rayleigh-Brillouin profiles. Measurements on N2 and SF6 gases demonstrate the high signal-to-noise ratio achievable with the instrument, at the 1% level at the peak amplitude of the scattering profile., Comment: 8 double column pages, 9 figures

The sensitivity of rotational transitions in CH and CD to a possible variation of fundamental constants has been investigated. Largely enhanced sensitivity coefficients are found for specific transitions which are due to accidental degeneracies between the different fine-structure manifolds. These degeneracies occur when the spin-orbit coupling constant is close to four times the rotational constant. CH and particularly CD match this condition closely. Unfortunately, an analysis of the transition strengths shows that the same condition that leads to an enhanced sensitivity suppresses the transition strength, making these transitions too weak to be of relevance for testing the variation of fundamental constants over cosmological time scales. We propose a test in CH based on the comparison between the rotational transitions between the e and f components of the Omega'=1/2,J=1/2 and Omega'=3/2,J=3/2 levels at 532 and 536 GHz and other rotational or Lambda-doublet transitions in CH involving the same absorbing ground levels. Such a test, to be performed by radioastronomy of highly redshifted objects, is robust against systematic effects.

An extensive survey of the D2 absorption spectrum has been performed with the high-resolution VUV Fourier-transform spectrometer of the DESIRS beamline at the SOLEIL synchrotron. The frequency range of 90 000-119 000 cm-1 covers the full depth of the potential wells of the B 1{\Sigma}+u, B' 1{\Sigma}+u, and C 1{\Pi}u electronic states up to the D(1s) + D(2\ell) dissociation limit. Improved level energies of rovibrational levels have been determined up to respectively v = 51, v = 13, and v = 20. Highest resolution is achieved by probing absorption in a molecular gas jet with slit geometry, as well as in a liquid helium cooled static gas cell, resulting in line widths of ~0.35 cm-1. Extended calibration methods are employed to extract line positions of D2 lines at absolute accuracies of 0.03 cm-1. The D1{\Pi}u and B" 1{\Sigma}+u electronic states correlate with the D(1s) + D(3\ell) dissociation limit, but support a few vibrational levels below the second dissociation limit, respectively v = 0-3 and v = 0-1, and are also included in the presented study. The complete set of resulting level energies is the most comprehensive and accurate data set for D2. The observations are compared with previous studies, both experimental and theoretical., Comment: 13 pages, 6 figures. The second set of Tables (Tables I-IV after the references), is auxiliary material

We determine the sensitivity to a possible variation of the proton-to-electron mass ratio \mu for torsion-wagging-rotation transitions in the ground state of methylamine (CH3NH2). Our calculation uses an effective Hamiltonian based on a high-barrier tunneling formalism combined with extended-group ideas. The \mu-dependence of the molecular parameters that are used in this model are derived and the most important ones of these are validated using the spectroscopic data of different isotopologues of methylamine. We find a significant enhancement of the sensitivity coefficients due to energy cancellations between internal rotational, overall rotational and inversion energy splittings. The sensitivity coefficients of the different transitions range from -19 to +24. The sensitivity coefficients of the 78.135, 79.008, and 89.956 GHz transitions that were recently observed in the disk of a z = 0.89 spiral galaxy located in front of the quasar PKS 1830-211 [S. Muller et al. Astron. Astrophys. 535, A103 (2011)] were calculated to be -0.87 for the first two and -1.4 for the third transition, respectively. From these transitions a preliminary upper limit for a variation of the proton to electron mass ratio of \Delta \mu/\mu< 9 x 10^{-6} is deduced.

Molecular hydrogen (H2) absorption features observed in the line-of-sight to Q2348-011 at redshift zabs = 2.426 are analysed for the purpose of detecting a possible variation of the proton-to-electron mass ratio mu=mp/me. By its structure Q2348-011 is the most complex analysed H2 absorption system at high redshift so far, featuring at least seven distinctly visible molecular velocity components. The multiple velocity components associated with each transition of H2 were modeled simultaneously by means of a comprehensive fitting method. The fiducial model resulted in dmu/mu = (-0.68 +/- 2.78) x 10^-5, showing no sign that mu in this particular absorber is different from its current laboratory value. Although not as tight a constraint as other absorbers have recently provided, this result is consistent with the results from all previously analysed H2-bearing sight-lines. Combining all such measurements yields a constraint of dmu/mu < 10^-5 for the redshift range z = (2--3)., Comment: 7 pages, 4 figures. Accepted by MNRAS

Recently, methanol was identified as a sensitive target system to probe variations of the proton-to-electron mass ratio $\mu$ [Jansen \emph{et al.} Phys. Rev. Lett. \textbf{106}, 100801 (2011)]. The high sensitivity of methanol originates from the interplay between overall rotation and hindered internal rotation of the molecule -- i.e. transitions that convert internal rotation energy into overall rotation energy, or vice versa, give rise to an enhancement of the sensitivity coefficient, $K_{\mu}$. As internal rotation is a common phenomenon in polyatomic molecules, it is likely that other molecules display similar or even larger effects. In this paper we generalize the concepts that form the foundation of the high sensitivity in methanol and use this to construct an approximate model which allows to estimate the sensitivities of transitions in internal rotor molecules with $C_{3v}$ symmetry, without performing a full calculation of energy levels. We find that a reliable estimate of transition sensitivities can be obtained from the three rotational constants ($A$, $B$, and $C$) and three torsional constants ($F$, $V_3$ and $\rho$). This model is verified by comparing obtained sensitivities for methanol, acetaldehyde, acetamide, methyl formate and acetic acid with a full analysis of the molecular Hamiltonian. From the molecules considered, methanol appears to be the most suitable candidate for laboratory and cosmological tests searching for a possible variation of $\mu$., Comment: submitted to PRA

UV frequency metrology has been performed on the a3Pi - X1Sigma+ (0,0) band of various isotopologues of CO using a frequency-quadrupled injection-seeded narrow-band pulsed Titanium:Sapphire laser referenced to a frequency comb laser. The band origin is determined with an accuracy of 5 MHz (delta \nu / \nu = 3 * 10^-9), while the energy differences between rotational levels in the a3Pi state are determined with an accuracy of 500 kHz. From these measurements, in combination with previously published radiofrequency and microwave data, a new set of molecular constants is obtained that describes the level structure of the a3Pi state of 12C16O and 13C16O with improved accuracy. Transitions in the different isotopologues are well reproduced by scaling the molecular constants of 12C16O via the common mass-scaling rules. Only the value of the band origin could not be scaled, indicative of a breakdown of the Born-Oppenheimer approximation. Our analysis confirms the extreme sensitivity of two-photon microwave transitions between nearly-degenerate rotational levels of different Omega-manifolds for probing a possible variation of the proton-to-electron mass ratio, \mu=m_p/m_e, on a laboratory time scale.

The operation of a frequency comb at extreme ultraviolet (XUV) wavelengths based on pair-wise amplification and nonlinear upconversion to the 15th harmonic of pulses from a frequency comb laser in the near-infrared range is reported. Following a first account of the experiment [Kandula et al., Phys. Rev. Lett. 105, 063001 (2010)], an extensive review is given of the demonstration that the resulting spectrum at 51 nm is fully phase coherent and can be applied to precision metrology. The pulses are used in a scheme of direct-frequency-comb excitation of helium atoms from the ground state to the 1s4p and 1s5p 1P_1 states. Laser ionization by auxiliary 1064 nm pulses is used to detect the excited state population, resulting in a cosine-like signal as a function of the repetition rate of the frequency comb with a modulation contrast of up to 55%. Analysis of the visibility of this comb structure yields an estimated timing jitter between the two upconverted comb laser pulses of 50 attoseconds, whch indicates that extension to even shorter wavelengths should be feasible. The helium metrology investigation results in transition frequencies of 5740806993(10) MHz and 5814248672(6) MHz for excitation of the 1s4p and 1s5p 1P_1 states, respectively. This constitutes the first absolute frequency measurement in the XUV, attaining unprecedented accuracy in this windowless part of the electromagnetic spectrum. From the measured transition frequencies an eight-fold improved 4He ionization energy of 5945204212(6) MHz is derived. Also a new value for the 4He ground state Lamb shift is found of 41247(6) MHz. This experimental value is in agreement with recent theoretical calculations up to order m\alpha^6 and m^2/(M\alpha^5), but with a six times higher precision, therewith providing a stringent test of quantum electrodynamics in bound two-electron systems., Comment: 18 pages, 13 figures

Molecular hydrogen transitions in quasar spectra can be used to constrain variation in the proton-to-electron mass ratio, $\mu\equiv m_p/m_e$, at high redshifts ($z\gtrsim 2$). We present here an analysis of a new spectrum of the quasar Q0528$-$250, obtained on VLT/UVES (the Ultraviolet and Visual Echelle Spectrograph, on the Very Large Telescope), and analyse the well-known H$_2$ absorber at $z=2.811$ in this spectrum. For the first time we detect HD (deuterated molecular hydrogen) in this system with a column density of $\log_{10}(N/\mathrm{cm^{-2}})=13.27 \pm 0.07$; HD is sensitive to variation in $\mu$, and so we include it in our analysis. Using 76 H$_2$ and 7 HD transitions we constrain variation in $\mu$ from the current laboratory value to be $\Delta\mu/\mu = (0.3\pm 3.2_\mathrm{stat} \pm 1.9_\mathrm{sys})\times 10^{-6}$, which is consistent with no cosmological variation in $\mu$, as well as with previous results from other H$_2$/HD absorbers. The main sources of systematic uncertainty relate to accurate wavelength calibration of the spectra and the re-dispersion of multiple telescope exposures onto the one pixel grid., Comment: 30 pages, 6 figures + 14 supplementary figures. Accepted for publication for MNRAS

A high signal-to-noise spectrum covering the largest number of hydrogen lines (90 H2 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$-$005 with the UVES spectrograph on the ESO Very Large Telescope (Paranal, Chile). This delivers a constraint on a possible variation of the proton-to-electron mass ratio of Dmu/mu = (8.5 \pm 3.6_{stat} \pm 2.2_{syst}) x 10^{-6} at redshift z=2.059$, which agrees well with a recently published result on the same system observed at the Keck telescope yielding Dmu/mu = (5.6 \pm 5.5_{stat} \pm 2.9_{syst}) x 10^{-6}. Both analyses used the same robust absorption line fitting procedures with detailed consideration of systematic errors., Comment: Accepted

Observations of H2 spectra in the line-of-sight of distant quasars may reveal a variation of the proton-electron mass ratio mu=m_p/m_e at high redshift, typically for z>2. Currently four high-quality systems (Q0347-383, Q0405-443, Q0528-250 and J2123-005) have been analyzed returning a constraint Dmu/mu < 1 x 10^{-5}. We present data and a mu-variation analysis of another system, Q2348-011 at redshift z_{abs}=2.42, delivering dmu/mu = (-1.5 \pm 1.6) x 10^{-5}. In addition to observational data the status of the laboratory measurements is reviewed. The future possibilities of deriving a competitive constraint on Dmu/mu from the known high-redshift H2 absorbers is investigated, resulting in the identification of a number of potentially useful systems for detecting mu-variation., Comment: 13 Pages, 4 Figures, JENAM conference (Lisbon); accepted

The remarkable precision of frequency comb (FC) lasers is transferred to the extreme ultraviolet (XUV, wavelengths shorter than 100 nm), a frequency region previously not accessable to these devices. A frequency comb at XUV wavelengths near 51 nm is generated by amplification and coherent upconversion of a pair of pulses originating from a near-infrared femtosecond FC laser. The phase coherence of the source in the XUV is demonstrated using Helium atoms as a ruler and phase detector. Signals in the form of stable Ramsey-like fringes with high contrast are observed when the FC laser is scanned over P states of Helium, from which the absolute transition frequency in the XUV can be extracted. This procedure yields a 4He ionization energy at h 5945204212(6) MHz, improved by nearly an order of magnitude in accuracy, thus challenging QED calculations of this two-electron system., Comment: 4 pages, 3 figures, acknowledgements added, fixed typos

Molecular transitions recently discovered at redshift z_abs=2.059 toward the bright background quasar J2123-0050 are analysed to limit cosmological variation in the proton-to-electron mass ratio, mu=m_p/m_e. Observed with the Keck telescope, the optical echelle spectrum has the highest resolving power and largest number (86) of H_2 transitions in such analyses so far. Also, (seven) HD transitions are used for the first time to constrain mu-variation. These factors, and an analysis employing the fewest possible free parameters, strongly constrain mu's relative deviation from the current laboratory value: dmu/mu =(+5.6+/-5.5_stat+/-2.9_sys)x10^{-6}, indicating an insignificantly larger mu in the absorber. This is the first Keck result to complement recent null constraints from three systems at z_abs>2.5 observed with the Very Large Telescope. The main possible systematic errors stem from wavelength calibration uncertainties. In particular, distortions in the wavelength solution on echelle order scales are estimated to contribute approximately half the total systematic error component, but our estimate is model dependent and may therefore under or overestimate the real effect, if present. To assist future mu-variation analyses of this kind, and other astrophysical studies of H_2 in general, we provide a compilation of the most precise laboratory wavelengths and calculated parameters important for absorption-line work with H_2 transitions redwards of the hydrogen Lyman limit., Comment: 15 pages, 8 figures (8 EPS files), 3 tables. Accepted by MNRAS. ArXiv copy includes full version of Fig. 1 (additional 8 pages, 7 EPS files). Complete version of Table 1 available at http://astronomy.swin.edu.au/~mmurphy/pub.html

Molecular transitions recently discovered at redshift z_abs=2.059 toward the bright background quasar J2123-0050 are analysed to limit cosmological variation in the proton-to-electron mass ratio, mu=m_p/m_e. Observed with the Keck telescope, the optical spectrum has the highest resolving power and largest number (86) of H_2 transitions in such analyses so far. Also, (7) HD transitions are used for the first time to constrain mu-variation. These factors, and an analysis employing the fewest possible free parameters, strongly constrain mu's relative deviation from the current laboratory value: dmu/mu =(+5.6+/-5.5_stat+/-2.7_sys)x10^{-6}. This is the first Keck result to complement recent constraints from three systems at z_abs>2.5 observed with the Very Large Telescope., Comment: 6 pages, 3 figures (3 EPS files). Contribution to Proc. IAU XXVIIth General Assembly, Joint Discussion 9, "Are the fundamental constants varying with time?". In P. Molaro, E. Vangioni-Flam, eds, Memorie della Societa Astronomica Italiana (MmSAIt), Vol. 80, pp. 882-887 (2009)