The possibilities for the extension of spectroscopy to two dimensions are discussed. Applications to nuclear magnetic resonance are described. The basic theory of two-dimensional spectroscopy is developed. Numerous possible applications are mentioned and some of them treated in detail, including the elucidation of energy level diagrams, the observation of multiple quantum transitions, and the recording of highresolution spectra in inhomogenous magnetic fields. Experimental results are presented for some simple spin systems.

In NMR Fourier transform spectroscopy, rf pulses are periodically applied to a spin system to generate a sequence of free induction decays which form the basis of spectroscopic measurements. In inhomogeneous magnetic fields, distortions of the free induction decay arise from superimposed spin-echo effects. They are strongly dependent on molecular diffusion which is also responsible for the nonexponential envelope of the echo train observed in a stopped pulse experiment. These effects are investigated by means of two independent methods, the Fourier expansion method and the partition method. The results are discussed and used to explain measurements made on a one-spin system. The influence of echoes on the sensitivity of Fourier transform spectroscopy is considered, and it is concluded that the achievable gain does not normally outweigh the complications arising from retention or enhancement of echoes. Experimental parameters are derived for efficient suppression of echoes by means of a periodically pulsed magnetic field gradient.

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