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High resolution rotational spectra of ¹⁰BH₃CO, ¹¹BH₃CO, ¹¹BD₃CO, PH₂D and CD₃CN were studied to obtain information concerning the electronic and magnetic properties of these molecules. From the analysis of the hyperfine structure of the rotational spectra of the molecules the following constants were determined: rotational constants (B₀), nuclear quadrupole coupling constants (eOq [x], spin-spin constants D (X-Y) and spin rotation constants (C[x]). The two instruments used in these experiments were a Stark modulated microwave spectrometer and a molecular beam maser spectrometer. The J = 0 to 1, F₁ = 3 to 3 and F₁ = 3 to 4 transitions of ¹⁰BH₃CO were studied. The molecular constants in KHz which were derived from the spectral analysis were: B(,0) = 8980060.3 (+/-) 1.0, eQqₐₐ (¹⁰B) = 3463.- (+/-) 8.0, C(¹⁰B) = .2 (+/-) .2, D(¹⁰B-H) = -2.8 (+/-) .2, D(H-H) = -7.2 (+/-) .5 and C(H) = 0.0 (+/-) .7. All three of the F₁ components of the J = 0 to 1 rotational transition of ¹¹BH₃CO were observed. The molecular constants in KHz which were obtained from the data analysis were: B₀ = 8657333.8 (+/-) .6, eQqₐₐ (¹¹B) = 1661.9 (+/-) 2.3, C(¹¹B) = .7 (+/-) .3, D(¹¹B-H) = 8.3 (+/-) .4, D(H-H) = -6.8 (+/-) .2 and C(H) = .4 (+/-) .4. Only spectra of the J = 0 to 1, F₁ = 3/2 to 3/2 transition of ¹¹BD₃CO were obtained. From the analysis of the spectra the following molecular constants were derived: eQqₐₐ (D) = -48.5 (+/-) 2.3, eQq(,zz)(D) = 116.9 (+/-) 5.4, C(D) = 0.0 (+/-) .8 and D(¹¹B-H) = -1.2 (+OR-) .3. The investigation of the 4₀₄ to 4₁₄ and 1₁₁ to 1₀₁ rotational transitions of PH₂D was unsuccessful in determining any molecular parameters. The spectra of the 4₀₄ to 4₁₄ rotational transition were not amenable to analysis and no spectra were obtained for the 1₁₁ to 1₀₁ rotational transitions. The three components of the J = 0 to 1 rotational transitions of CD₃CN were studied with the maser in the two cavity configuration. The constants in KHz which were determined were: B₀ = 7857978.7 (+/-) .1, eQqₐₐ(N) = -4229.2 (+/-) .6, eQqₐₐ(D) = -55.1 (+/-) .4, eQq(,zz)(D) = 165.5 (+/-) 5.0, C(,N) = 1.7 (+/-) .1 and C(,D) = 0.0 (+/-) .03.

H. H. Stroke, R. J. Blin-Stoyle and V. Jaccarino. / "August 15, 1961." "Reprinted from The Physical Review, vol. 123, no. 4, 1326-1348, August 15, 1961." / Includes bibliographical references. / Army Signal Corps Contract No. DA36-039-sc-78108. Dept. of the Army Task 3-99-20-001 and Project 3-99-00-000.

This thesis aims at the methodological developments in Nuclear Magnetic Resonance (NMR). The methodological developments in NMR has a long and successful history. The present thesis attempts to contribute some novel methods in this direction. This thesis restricts itself to two methodological developments, namely, (1) effects of cross-correlations between the chemical shift anisotropy (CSA) and dipole-dipole interactions in the relaxation of various nuclei and experiments which utilize spatial encoding. The cross-correlation has been successfully utilized to investigate the anisotropic motions of liquid crystals, and to understand the chemical shift anisotropy of fluorine atoms of Fluorine substituted ring compounds. Spatial encoding schemes have been developed to facilitate single scan measurements of longitudinal spin lattice relaxation times and implementations of parallel search algorithms.