This thesis focuses on the use of surface modifiers to tune the properties of both metals and metal oxides. Particular attention is given to examine the modification of transparent conducting oxides (TCOs) including indium tin oxide and zinc oxide both through the use of phosphonic acids as well as organic and metal-organic dopants. In this thesis a variety of known and new phosphonic acids are synthesized. A subset of these molecules are then used to probe the relationship between the ability of a phosphonic acid to tune the work function of ITO and how that interrelates with the coverage and molecular orientation of the modifier on the surface. Experimental techniques including XPS, UPS, and NEXAFS are coupled with theoretical DFT calculations in order to more closely examine this relationship. Literature surrounding the modification of zinc oxide with phosphonic acids is not as prevalent as that found for the modification of ITO. Thus, effort is placed on attempting to determine optimal modification conditions for phosphonic acids on zinc oxide. As zinc oxide is already a low work function metal oxide, modifiers were synthesized in an attempt to further decrease the work function of this substrate in an effort to minimize the barrier to carrier collection/injection. Etching of the substrate by phosphonic acids is also examined. In a related technique, n- and p-dopants are used to modify the surfaces of ITO, zinc oxide, and gold and it was found that the work function can be drastically altered, to approximately 3.3 – 3.6 eV for all three of the substrates examined. Surface reactions are straightforward to conduct typically taking only 60 s to achieve this change in work function.