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Title: Two-proton laser spectroscopy of small molecules
Author: Zhiyuan, M.
Awarding Body: University of Edinburgh
Current Institution: University of Edinburgh
Date of Award: 1997
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An innovative optical-optical double resonance scheme (bound-free-bound) which employs resonant continuum intermediate states has been developed. A full quantum explanation has been suggested for the development of the vibronic envelope of the final states excited through such bound-free-bound pathways with two-colour pulsed layers. This scheme has been applied to observing extended vibrational progressions of some 0+g and 1g ion-pair states of I2 and C12, and the [2II1/2]6s;0 Rydberg state of methyl iodide (along the C-I stretching mode, v3). The vibrational structures of the E0+g and f0+g ion-pair states of I2 are simulated by using the resultant Franck-Condon calculation. The vibrational structure of the 0+g and 1g ion-pair states of C12 also agrees with the predictions from the Franck-Condon calculations. The curtailment at v1 = 5 of the v3 vibrational progression of the methyl iodide [2II1/2]6s;0 Rydberg state has been attributed to the sudden onset of predissociation. The two-photon Hönl-London factors for (a) a well defined intermediate (Ji, Mi), (b) a coherently superposed (Ji, Mi) and (c) a full set of coherent virtual states, are discussed. The simulation of the observed rotational contours of the 0+g ion-pair states of I2 and C12 in the bound-free-bound scheme reveals the dominant character of the intermediate electronic states. Similar deductions cannot be made for the 1g ion-pair states of C12 and the reason is discussed. The two-colour two-photon nonresonant excitation of the 000 vibronic band of the (2A"2)3pz Rydberg state of CD3 has been observed and its rotational contour has also been simulated on the basis of established Hönl-London factors. The dynamics of the virtual intermediate states can be revealed by considering the observed parallel and perpendicular polarization spectra. A relative resonant enhancement of the 213 vibronic band of the (2A112)4pz Rydberg state, in the out-of-plane mode (v2), occurred when the protons were turned on and off resonances with the intermediate (2A11)3s state which is strongly predissocated by tunnelling.
Supervisor: Not available Sponsor: Not available
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID:  DOI: Not available