Recently the finding of an indication for a decrease of the proton-to-electron mass ratio l = 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 theWerner band systems at an accuracy of (4-11) · 10
À8, depending on the wavelength region. This corresponds to an absolute accuracy of 0.000004-0.000010 nm. A database of 233 accurately calibrated H 2 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 0405À443 and Q 0347À383) resulted in 76 reliably determined transition wavelengths of H 2 lines at accuracies in the range 2 · 10 À7 to 1 · 10 À6 . 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 l. 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 X 1 R þ g ground electronic state and the presently determined level energies in the B 1 R þ u and C 1 P 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 Dl/l = (2.45 ± 0.59) · 10 À5 for a weighted fit and Dl/l = (1.99 ± 0.58) · 10 À5 for an unweighted fit. This result, indicating the decrease of l, has a statistical significance of 3.5r. 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 0405À443 and Q 0347À383. The statistical analysis is further documented and possible systematic shifts underlying the data, with the possibility of mimicking a non-zero Dl/l value, are discussed. The observed decrease in l corresponds to a rate of change of d lnl/dt = À2 · 10 À15 per year, if a linear variation with time is assumed. Expe...