The two‐color laser‐induced grating (TC‐LIG) technique has been employed to probe the predissociative Rydberg states (4pσ) M 2Σ+ (v=1) and (3dσ,π) H 2Σ+, H′ 2Π± (v=2) and the non‐Rydberg B 2Π (v=26) state of nitric oxide. The ultraviolet pump laser frequency is fixed to a specific rotational line of the A 2Σ+ (v′=1 and 2)←X 2Π3/2 (v″=0) transition of NO. Interference of two pump laser beams crossing at a small angle in the gas sample forms a population grating. Then, the visible probe laser beam is diffracted off the grating as the signal beam when the probe laser frequency is resonant to a transition from the rotational level excited by the pump laser. Term values and rotational assignments of the H 2Σ+, H′ 2Π± (v=2)–B 2Π3/2 (v=26) states have been established for the first time, resulting in the value of ∼1.77 cm−1 for the l‐uncoupling constant. Line broadenings due to predissociation are observed in the TC‐LIG spectra for the M 2Σ+ (v=1) and H 2Σ+, H′ 2Π+ (v=2) states. The linewidths of the M 2Σ+ (v=1) state show no marked rotational dependence except for the N=4 level which is locally perturbed. On the other hand, the predissociative lifetimes of the H 2Σ+ and H′ 2Π+ (v=2) states exhibit a significant rotational dependence: The linewidth of the former state decreases with N, while the reverse tendency is seen for the latter. The mixing between the H 2Σ+ and H′ 2Π+ states caused by l‐uncoupling explains the observed rotational dependence successfully.
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15 June 1995
Research Article|
June 15 1995
Predissociative linewidths of (4pσ) M 2Σ+ (v=1) and (3dσ,π) H 2Σ+, H′ 2Π (v=2) Rydberg states of NO studied by the two‐color laser‐induced grating technique
Juntarou Ishii;
Juntarou Ishii
Department of Physics, Faculty of Science and Technology, Keio University, Hiyoshi, Kohoku‐ku, Yokohama, Kanagawa 223, Japan
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Kiyoji Uehara;
Kiyoji Uehara
Department of Physics, Faculty of Science and Technology, Keio University, Hiyoshi, Kohoku‐ku, Yokohama, Kanagawa 223, Japan
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Koichi Tsukiyama
Koichi Tsukiyama
The Institute of Physical and Chemical Research (RIKEN), Hirosawa, Wako, Saitama 351‐01, Japan
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J. Chem. Phys. 102, 9174–9182 (1995)
Article history
Received:
October 24 1994
Accepted:
March 17 1995
Citation
Juntarou Ishii, Kiyoji Uehara, Koichi Tsukiyama; Predissociative linewidths of (4pσ) M 2Σ+ (v=1) and (3dσ,π) H 2Σ+, H′ 2Π (v=2) Rydberg states of NO studied by the two‐color laser‐induced grating technique. J. Chem. Phys. 15 June 1995; 102 (23): 9174–9182. https://doi.org/10.1063/1.468866
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