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A methane molecule (CH4) has a permanent electric dipole moment (PEDM) in the excited state of the triply-degenerate vibrational modesa,b. The rotational ...
EXTENSIVE MEASUREMENTS OF VIBRATION-INDUCED PERMANENT ELECTRIC DIPOLE MOMENTS OF METHANE SHOKO OKUDA, HIROYUKI SASADA, Department of Physics, Faculty of Science and Technology, Keio University, Yokohama, Japan. A methane molecule (CH4 ) has a permanent electric dipole moment (PEDM) in the excited state of the triply-degenerate vibrational modesa,b . The rotational dependence of the PEDM was reported in the 2ν3 bandc . However, in the ν3 band, it was only determined on the P (7)E transition which fortunately lies in the tunable range of a 3.4 µm He-Ne laser. We have developed a mid-infrared broadband sub-Doppler resolution spectrometer consisting of a difference-frequencygeneration source and an optical frequency comb linked to International Atomic Time. This spectrometer enables us to measure the Stark effects of 20 transitions in the ν3 band of methane from 87.7 to 92.8 THz (2927∼3095 cm−1 ). The observed linewidth is 0.5 MHz, and the frequency scale is absolutely calibrated. The figure depicts the Stark modulation spectrum of the P (4)E transition. The applied DC electric field was 3.5 kV/cm. We determined Stark coefficients with a relative uncertainty of 1 %. Our goal is to reveal the rotational dependence of the PEDM. For this end, we yield molecular constants which reproduce the transition frequencies by a least-square method and determine the mixing of the wave functions. a M.
Mizushima and P. Venkateswarlu, J. Chem. Phys. 21, 705 (1953). Uehara, K. Sakurai and K. Shimoda, J. Phys. Soc. Jpn. 26, 1018 (1969). c H. Sasada, K. Suzumura and C. Ishibashi, J. Chem. Phys. 105, 9027 (1996).
