Angular momentum is essential to any advanced discussion of magnetic resonance spectroscopy. A brief history of the modern sub-atomic particle-spin concept is presented. The origin of the spin-1/2 angular momentum quantum number is detailed and angular momentum operators are constructed for spin-1/2 nuclei using the postulates of quantum mechanics which are then used to produce a set of very useful eigenvalue formulas. Angular momentum operators in spherical coordinate form are developed and operator matrices are constructed from Cartesian operators. The time-evolution of these operators is of much interest in later chapters and is explored in some detail here.