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 $CF_{3}CCH$ 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 $\nu_{o}=17267$ MHz for transitions between the levels $(J=3,K,M)$ and (2,K.M) are generated for $KM \neq 0$ by the application of intense pulses at $\nu_{0}/2$. 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 $earlier^{1}$ to treat multiphoton transitions in a two-level system whose one-photon frequency is $\lesssim 1 MHz$. 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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