Absolute measurements of state-to-state rotational energy transfer between CO and 
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 at interstellar temperatures

Labiad, Hamza; Fournier, Martin; Mertens, Laura A.; Fauré, Alexandre; Carty, David; Stoecklin, Thierry; Jankowski, Piotr; Szalewicz, Krzysztof; Picard, Sébastien D. Le; Sims, Ian

doi:10.1103/physreva.105.l020802

Phys. Rev. A

2022

DOI: 10.1103/physreva.105.l020802

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Absolute measurements of state-to-state rotational energy transfer between CO and H2 at interstellar temperatures

Hamza Labiad

Martin Fournier

Laura A. Mertens

et al.

Abstract: Experimental measurements and theoretical calculations of state-to-state rate coefficients for rotational energy transfer of CO in collision with H 2 are reported at the very low temperatures prevailing in dense interstellar clouds (5-20 K). Detailed agreement between quantum state-selected experiments performed in cold supersonic flows using time-resolved infrared-vacuum-ultraviolet double-resonance spectroscopy and close-coupling quantum scattering calculations confirms the validity of the calculations for c… Show more

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Cited by 4 publications

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Measurements and calculations of collisional line parameters for Raman lines of CO perturbed by H2

Thibault,

Paredes-Roibás,

Viel

et al. 2024

Journal of Quantitative Spectroscopy and Radiative Transfer

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Measurements and calculations of collisional line parameters for Raman lines of CO perturbed by H2

Thibault,

Paredes-Roibás,

Viel

et al. 2024

Journal of Quantitative Spectroscopy and Radiative Transfer

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Experimental study of rotational relaxation for D2(1,12) in collisions with N2

Mao,

Liu,

Habibulla

et al. 2024

The Journal of Chemical Physics

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The rotational relaxation behavior of D2(1,12) in a D2–N2 mixture was investigated using coherent anti-Stokes Raman scattering (CARS) technique. The rovibrational level v = 1 and J = 12 of D2 was selectively excited through stimulated Raman pumping while monitoring the temporal evolution of population for D2(1, J ≤ 12) molecules using time-resolved CARS spectroscopy. The results demonstrate that the rotational relaxation processes of D2(1,12) encompass both multi-quantum relaxation and continuous single-quantum relaxation. When α, the molar ratio of N2, is less than 0.5, D2(1,12) predominantly undergoes a single quantum relaxation process transition. However, when α ≥ 0.5, the multi-quantum relaxation mechanism gradually predominates. The total rotational relaxation rate coefficients of D2(1,12) collisions with N2 and D2 at 295 K were determined to be 3.974 × 10−14 and 1.179 × 10−14 cm3 s−1, respectively. The temperature dependence of rotational relaxation rate of D2(1,12) was investigated within the temperature range of 295–453 K. With increasing temperature, the dominant relaxation process exhibited an accelerated behavior, while the minor relaxation process remained largely unaffected. The rotational temperature of the D2 molecule at various N2 molar ratios was determined through the utilization of Boltzmann plots. The rotational temperature undergoes a rapid decline within 2 μs, corresponding to the near-resonant rotation–vibration relaxation process of D2(1,12) collisions with N2. The system reaches a quasi-equilibrium state when the delay time is 3 μs. The findings of this study can serve as a valuable empirical basis for further validation of the kinetic theory and simulation.

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Product-specific reaction kinetics in continuous uniform supersonic flows probed by chirped-pulse microwave spectroscopy

Guillaume,

Hays,

Gupta

et al. 2024

The Journal of Chemical Physics

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Experimental studies of the products of elementary gas-phase chemical reactions occurring at low temperatures (<50 K) are very scarce, but of importance for fundamental studies of reaction dynamics, comparisons with high-level quantum dynamical calculations, and, in particular, for providing data for the modeling of cold astrophysical environments, such as dense interstellar clouds, the atmospheres of the outer planets, and cometary comae. This study describes the construction and testing of a new apparatus designed to measure product branching fractions of elementary bimolecular gas-phase reactions at low temperatures. It combines chirped-pulse Fourier transform millimeter wave spectroscopy with continuous uniform supersonic flows and high repetition rate laser photolysis. After a comprehensive description of the apparatus, the experimental procedures and data processing protocols used for signal recovery, the capabilities of the instrument are explored by the study of the photodissociation of acrylonitrile and the detection of two of its photoproducts, HC3N and HCN. A description is then given of a study of the reactions of the CN radical with C2H2 at 30 K, detecting the HC3N product, and with C2H6 at 10 K, detecting the HCN product. A calibration of these two products is finally attempted using the photodissociation of acrylonitrile as a reference process. The limitations and possible improvements in the instrument are discussed in conclusion.

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Absolute measurements of state-to-state rotational energy transfer between CO and H2 at interstellar temperatures

Cited by 4 publications

References 29 publications

Measurements and calculations of collisional line parameters for Raman lines of CO perturbed by H2

Measurements and calculations of collisional line parameters for Raman lines of CO perturbed by H2

Experimental study of rotational relaxation for D2(1,12) in collisions with N2

Product-specific reaction kinetics in continuous uniform supersonic flows probed by chirped-pulse microwave spectroscopy

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