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The Rotational Spectra of Propyne in the Ground, V₁₀=1, V₁₀=2, and V₉=1 Vibrational States
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The problem of a vibrating-rotating polyatomic molecule is treated, with emphasis given to the case of molecules with C_3v symmetry. It is shown that several of the gross features of the rotational spectra of polyatomic molecules in excited vibrational states can be predicted by group theoretical considerations. Expressions for the rotational transition frequencies of molecules of C_3v symmetry in the ground vibrational state, singly excited degenerate vibrational states, and doubly excited degenerate vibrational states are given. The derivation of these expressions by fourth order perturbation theory as given by Amat, Nielsen, and Tarrago is discussed. The ground and V_10=1 rotational spectra of propyne have been investigated in the 17 to 70 GHz, and 17 to 53 GHz regions, respectively, and compared with predictions based on higher frequency measurements. The V_9=1 and V_10=2 rotational spectra of propyne have been investigated and assigned for the first time. A perturbation of the V_9=1 rotational spectra for K=-l has been discovered and discussed.
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Nonlinear Absorption Techniques and Measurements in Semiconductors
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We have conducted a detailed experimental and theoretical study of nonlinear absorption in semiconductors. Experimental measurements were made on a variety of materials at wavelengths of 1.06 and 0.53 microns using a picosecond Nd:YAG laser. Both two- and three-photon processes were investigated. Values of nonlinear absorption coefficients extracted from these measurements show excellent agreement with recent theory and scaling rules. Our theoretical investigation has been carried out for two-, three-,and n-photon absorption, for both continuous and pulsed sources. Expressions are obtained for the transmission of the sample in terms of the incident irradiance for each case. The physical interpretation of these results is discussed. We have also considered the effects of the photogenerated carriers on the measurements. Equations are developed that include linear absorption by these carriers. We have observed severe distortions on the transmitted beam, caused by changes in the refractive index of the material, due to the presence of these carriers. We present a model that accurately describes these effects in terms of the photogenerated carrier density. We have developed several novel techniques for monitoring nonlinear absorption. In particular, we have adapted the photoacoustic technique to the measurement of nonlinear absorption in semiconductors. We have also developed a technique employing irradiance modulation to greatly enhance the sensitivity to nonlinear processes and simultaneously discriminate against linear background signals. A related technique has been used to observe coherent mixing effects in semiconductors with cw, modelocked dye lasers.