The results reported in Part III consist of joint work with Martín Escardó . All the other results reported in this thesis are due to the author, except for background results, which are clearly stated as such. Some of the results in Part IV have already appeared as . Note This version of the thesis, produced on October 31, 2006, is the result of completing all the minor modifications as suggested by both the examiners in the viva report (Ref: CLM/AC/497773). We develop an operational domain theory to reason about programs in sequential functional languages. The central idea is to export domaintheoretic techniques of the Scott denotational semantics directly to the study of contextual pre-order and equivalence. We investigate to what extent this can be done for two deterministic functional programming languages: PCF (Programming-language for Computable Functionals) and FPC (Fixed Point Calculus).