An electron momentum spectrometer at the Australian National University has been used to study various aspects of different solid state systems. EMS is a transmission mode technique and involves the collision of the incident electron with a bound electron, after which both electrons are ejected and measured in coincidence. Through well defined reaction kinematics the complete valence spectral momentum density A(ɛ,q) can be measured. The spectrometer has been used to measure the spectral momentum densities (spectral functions) of single crystal targets, as well as targets in disordered states. A new spin polarised electron source was constructed and implemented in the ANU spectrometer, which was used to measure spin dependent features of ferromagnetic samples.¶ This thesis is divided into seven chapters, the first chapter is an introduction into the field of electron momentum spectroscopy, highlighting what has been measured before and how the technique has progressed to its present state. Some comparisons to other experimental techniques will be made.¶ The second chapter describes the ANU EMS spectrometer in detail. The technique requires some technical and advanced equipment that is often used in novel ways. The production of thin (20 nm) free standing targets will be detailed, along with the experimental chamber and electronics used to run the apparatus and collect data. The determination of the energy and momentum resolution of the experiment is also described.¶ The third chapter will detail the design and construction of the new spin polarised electron source. The results of commissioning and characterizing the new source will be presented.¶ Chapters four through six will present the measured results. The fourth chapter will detail the single crystalline measurements for the group eleven noble metals (Cu, Ag and Au). Each sample was measured along three high symmetry directions and compared to a DFT calculation using the LDA and a FP-LMTO basis. The fifth chapter will include the results from samples that were in disordered states, a measurement which is unique to the EMS technique. The polycrystalline and amorphous states of the Si and Ge semiconductors are presented and conclusions are made to the degree of difference in the results and to which theoretical approach to the unique amorphous state of the semiconductors best matches the EMS results. The sixth chapter includes results of ferromagnetic iron, measured using the spin polarised electron source. The spectrometer was used to measure spin-polarised electron-energy-loss-spectroscopy (SPEELS) and magnetic electron-Compton profiles. A theoretical investigation is also presented in chapter six which details the advancements required in the spin polarised electron gun to measure an accurate spin-polarised EMS spectra of a ferromagnetic Fe sample.¶ Chapter 7 includes the summary of all the results presented and conclusions reached from the comparison of the measured EMS spectra and various theoretical calculations. A discussion is presented about the future directions and possibilities of the EMS technique.