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Temperature-dependent pressure broadened line shape measurements in the ν 1+ν 3 band of acetylene using a diode laser referenced to a frequency comb

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Abstract

Using an extended cavity diode laser referenced to a femtosecond frequency comb, the P(11) absorption line in the ν 1+ν 3 combination band of the most abundant isotopologue of pure acetylene was studied at temperatures of 296, 240, 200, 175, 165, 160, 155, and 150 K to determine pressure-dependent line shape parameters at these temperatures. The laser emission profile, the instrumental resolution, is a Lorentz function characterized by a half width at half the maximum emission (HWHM) of 8.3×10−6 cm−1 (or 250 kHz) for these measurements. Six collision models were tested in fitting the experimental data: Voigt, speed-dependent Voigt, Rautian–Sobel’man, Galatry, and two Rautian–Galatry hybrid models (with and without speed-dependence). Only the speed-dependent Voigt model was able to fit the data to the experimental noise level at all temperatures and for pressures between 3 and nearly 360 torr. The variations of the speed-dependent Voigt profile line shape parameters with temperature were also characterized, and this model accurately reproduces the observations over their entire range of temperature and pressure.

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Acknowledgements

Acknowledgment is made to the Donors of the American Chemical Society Petroleum Research Fund for partial support of this research. We are grateful for Program Development Funding awarded to TJS by Brookhaven National Laboratory which provided funds for some of the equipment used in this work. CPM gratefully acknowledges support by DOE EPSCoR grant DOE-07ER46361 for work conducted at the University of Oklahoma. AWM gratefully acknowledges support by NASA EPSCoR Grant No. PS 4990 for supporting the development of low temperature cells. The measurements and analyses were performed under grants NNX09AJ93G and NNX08AO78G from the NASA Planetary and Atmospheres program. Work at Brookhaven National Laboratory was carried out under Contract No. DE-AC02-98CH10886 with the US Department of Energy, Office of Science, and supported by its Division of Chemical Sciences, Geosciences and Biosciences within the Office of Basic Energy Sciences.

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Authors and Affiliations

  1. Department of Chemistry, Stony Brook University, Stony Brook, NY, 11794, USA

    M. J. Cich, G. V. Lopez & T. J. Sears

  2. Chemistry Department, Brookhaven National Lab, Bldg. 555A, P.O. Box 5000, Upton, NY, 11973, USA

    C. P. McRaven & T. J. Sears

  3. Service de Chimie Quantique et de Photophysique (Atomes, Molécules et Atmosphères), Université Libre de Bruxelles, 50 Av F. D. Roosevelt CPi 160/09, 10050, Bruxelles, Belgium

    D. Hurtmans

  4. Department of Physics, Astronomy and Astrophysics, Connecticut College, 270 Mohegan Avenue, New London, CT, 06320, USA

    A. W. Mantz

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  1. M. J. Cich
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  3. G. V. Lopez
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Correspondence to T. J. Sears.

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Cich, M.J., McRaven, C.P., Lopez, G.V. et al. Temperature-dependent pressure broadened line shape measurements in the ν 1+ν 3 band of acetylene using a diode laser referenced to a frequency comb. Appl. Phys. B 109, 373–384 (2012). https://doi.org/10.1007/s00340-011-4829-0

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