Abstract. Several recent studies have observed systematic differences between measurements in the 183.31 GHz water vapor line by space-borne sounders and calculations using radiative transfer models, with inputs from either radiosondes (radiosonde observations, RAOBs) or short-range forecasts by numerical weather prediction (NWP) models. This paper discusses all the relevant categories of observation-based or model-based data, quantifies their uncertainties and separates biases that could be common to all causes from those attributable to a particular cause. Reference observations from radiosondes, Global Navigation Satellite System (GNSS) receivers, differential absorption lidar (DIAL) and Raman lidar are thus overviewed. Biases arising from their calibration procedures, NWP models and data assimilation, instrument biases and radiative transfer models (both the models themselves and the underlying spectroscopy) are presented and discussed. Although presently no single process in the comparisons seems capable of explaining the observed structure of bias, recommendations are made in order to better understand the causes.
The rotational spectrum of water vapour highly enriched in 18 O has been studied by high resolution (≈ 0.001 cm -1 ) Fourier transform spectroscopy at the AILES beam line of the SOLEIL synchrotron. The room temperature absorption spectrum has been recorded between 40 and 700 cm -1 . The 18 O enrichment of the sample was about 97% while the gas pressure and the absorption pathlength were set to 0.97 mbar and 151.75 m, respectively. The spectrum contains more than 4800 rotational transitions from seven water isotopologues (H2 18 O, H2 16 O, H2 17 O, HD 18 O, HD 16 O, HD 17 O, D2 18 O). The assignments were performed using known experimental energy levels as well as calculated line lists based on the results of Schwenke and Partridge. The amount and accuracy of the reported line positions represent an important extension compared to previous works. Overall, lines of about 2570 transitions are observed for the first time and 35, 41, 50, and 16 new energy levels are determined for H2 18 O, H2 17 O, HD 18 O, and HD 17 O, respectively. The set of derived energy levels shows a number of important differences from those recommended by an IUPAC-task group. Compared to the HITRAN2016 database, numerous deviations of line positions (up to 0.15 cm -1 ) are found for the H2 17 O, H2 18 O, HD 17 O, and HD 18 O species. Incomplete and wrong HITRAN's assignments of more than 90 transitions for H2 18 O, H2 17 O and HD 18 O are identified. Overall, the measured line positions will allow to significantly refine and complete the sets of empirical energy levels of H2 18 O, H2 17 O, HD 18 O and HD 17 O in the ground vibrational state.
New experimental results regarding "warm" water dimer spectra under equilibrium conditions are presented. An almost equidistant series of six peaks corresponding to the merged individual lines of the bound dimer with consecutive rotational quantum numbers is studied in the 188-258 GHz frequency range in water vapour over a broad range of pressures and temperatures relevant to the Earth's atmosphere. The series is a continuation of the sequence detected earlier at lower frequencies at room temperature. The signal-to-noise ratio of the observed spectra allowed investigating their evolution, when water vapour was diluted by atmospheric air with partial pressure from 0 up to 540 Torr. Analysis of the obtained spectra permitted determining the dimerization constant as well as the hydrogen bond dissociation energy and the dimer spectral parameters, including the average coefficient of collisional broadening of individual lines by water vapour and air. The manifestation of metastable states of the dimer in the observed spectra is assessed. The contribution of three possible pair states of water molecules to the second virial coefficient is evaluated over the broad range of temperatures. The work supports the significant role of the water dimer in atmospheric absorption and related processes.
Line intensities for carbon dioxide are measured with a novel spectroscopic approach, assisted by an optical frequency comb synthesizer for frequency calibration purposes. The main feature of the spectrometer consists in the exploitation of optical feedback from a V-shaped high-finesse optical resonator to effectively narrow a distributed feedback diode laser at the wavelength of 2 μm. Laser-gas interaction takes place inside an isothermal cell, which is placed on the transmission from the cavity. High quality, self-calibrated, absorption spectra are observed in pure CO samples at different gas pressures, in coincidence with three lines of the R-branch of the ν + 2ν + ν band. Line intensities are determined using a global fitting approach in which a manifold of spectra are simultaneously analyzed across the range of pressures between 5 and 100 Torr, sharing a restricted number of unknown parameters. Various sources of uncertainty have been identified and carefully quantified, thus leading to an overall uncertainty ranging between 0.17% and 0.23%. The measured values are in a very good agreement with recent ab initio predictions.
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