This thesis is divided into five chapters. The first chapter begins with a discussion of the basic principles of electron spin resonance and concludes with a description of the theoretical interpretation of electron spin resonance spectra in terms of the Spin Hamiltonian. The first part of the second chapter is a general discussion of the physical properties of diamond and includes reasons for the classification of diamond into various types. The second part of the chapter is devoted to a brief historical survey of the developments in the production of synthetic diamond. The final part of the chapter is an outline of the experiments which have led to the identification of nitrogen as a major impurity in natural and synthetic diamond. The third chapter combines and describes some of the experimental studies which have been made on diamond using the technique of electron spin resonance. Particular emphasis is placed on theories which have been put forward to explain the electron spin resonance signals associated with substitutional nitrogen in natural diamond. Electron spin resonance associated with synthetic diamond is discussed under a separate heading. The fourth chapter is devoted entirely to a description of the experiments carried out in this work and is concerned mainly with electron spin resonance from five different types of commercially available synthetic diamond. Those resonances, which are due to the nitrogen and ferromagnetic impurities, are shown to depend markedly on the nature of the diamond as well as its temperature. Experiments on samples which have been treated either by heating or crushing or by a combination of both, are also described.

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