A comprehensive investigation of the frequency-noise spectral density of a free-running midinfrared quantum-cascade laser is presented for the first time. It provides direct evidence of the leveling of this noise down to a white-noise plateau, corresponding to an intrinsic linewidth of a few hundred hertz. The experiment is in agreement with the most recent theory on the fundamental mechanism of line broadening in quantum-cascade lasers, which provides a new insight into the Schawlow-Townes formula and predicts a narrowing beyond the limit set by the radiative lifetime of the upper level.
We report on a new implementation of Doppler broadening thermometry based on precision absorption spectroscopy by means of a pair of offset-frequency locked extended-cavity diode lasers at 1.39 μm. The method consists in the highly accurate observation of the shape of the 4(4,1)→4(4,0) line of the H2(18)O ν1+ν3 band, in a water vapor sample at thermodynamic equilibrium. A sophisticated and extremely refined spectral analysis procedure is adopted for the retrieval of the Doppler width as a function of the gas pressure, taking into account the Dicke narrowing effect, the speed dependence of relaxation rates, and the physical correlation between velocity-changing and dephasing collisions. A spectroscopic determination of the Boltzmann constant with a combined (type A and type B) uncertainty of 24 parts over 10(6) is reported. This is the best result obtained so far by means of an optical method. Our determination is in agreement with the recommended CODATA value.
We present a fully ab initio model and calculations of the spectral shapes of absorption lines in a pure molecular gas under conditions where the influences of collisions and of the Doppler effect are significant. Predictions of the time dependence of dipole autocorrelation functions (DACFs) are made for pure CO 2 at room temperature using requantized classical molecular dynamics simulations. These are carried, free of any adjusted parameter, on the basis of an accurate anisotropic intermolecular potential. The Fourier-Laplace transforms of these DACFs then yield calculated spectra which are analyzed, as some measured ones, through fits using Voigt line profiles. Comparisons between theory and various experiments not only show that the main line-shape parameters (Lorentz pressure-broadening coefficients) are accurately predicted, but that subtle observed non-Voigt features are also quantitatively reproduced by the model. These successes open renewed perspectives for the understanding of the mechanisms involved (translational-velocity and rotational-state changes and their dependences on the molecular speed) and the quantification of their respective contributions. The proposed model should also be of great help for the test of widely used empirical line-shape models and, if needed, the construction of more physically based ones.
We report on a new optical implementation of primary gas thermometry based on laser-absorption spectrometry in the near infrared. The method consists in retrieving the Doppler broadening from highly accurate observations of the line shape of the R(12) nu1+2nu2(0)+nu3 transition in CO2 gas at thermodynamic equilibrium. Doppler width measurements as a function of gas temperature, ranging between the triple point of water and the gallium melting point, allowed for a spectroscopic determination of the Boltzmann constant with a relative accuracy of approximately 1.6 x 10(-4).
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