TWO-PHOTON MICROWAVE TRANSITIONS WITHIN A TWO-LEVEL SYSTEM

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1990

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Ohio State University

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Two-photon pure rotational transitions in the symmetric top CF3CCH have been observed with a pulsed beam Fourier transform crossed-cavity spectrometer modified to allow the application of a static Stark field. Transient one-photon emission signals at νo=17267 MHz for transitions between the levels (J=3,K,M) and (2,K.M) are generated for KM≠0 by the application of intense pulses at ν0/2. It has been demonstrated that the two-photon transitions occur within an effectively isolated two-level system as a result of the first order ac Stark effect. Quantitative studies of the intensities as a function of pulse length and power show that the two-photon transition probability in the microwave region is well represented by the theoretical model used earlier1 to treat multiphoton transitions in a two-level system whose one-photon frequency is ≲1MHz. A description is given of the spectrometer with emphasis on the modifications made for two-photon studies.

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1 W. L. Meerts, I. Ozier, and J. T. Hougen, J. Chem. Phys. 90,4681 (1989).


Author Institution: Laboratorium f""{u}r Physikalische Chemie, Eidgen""{o}ssische Technische; Department of Physics, University of British Columbia

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