Experimental and computational studies on the design of dyes for water-splitting dye-sensitized photoelectrochemical tandem cells 0.99) with very good predictive abilities (rmsd < 50 mV) were found when using density functional theory (DFT) combined with a continuum solvent model. DFT was also used to aid in the elucidation of the mechanism of the thermal relaxation observed for the charge-separated state of a molecular triad that mimics the photo-induced proton coupled electron transfer of the tyrosine-histidine redox relay in the reaction center of Photosystem II. It was found that the inclusion of explicit solvent molecules, hydrogen bonded to specific sites within the molecular triad, was essential to explain the observed thermal relaxation. These results are relevant for both advancing the knowledge about natural photosynthesis and for the future design of new molecules for WSDSPETCs.]]>autMéndez-Hernández, Dalvin DthsMoore, Ana LthsMujica, VladimirodgcGust, Devens J.dgcGould, IanpblArizona State UniversityengPartial requirement for: Ph.D., Arizona State University, 2014Includes bibliographical references (p. 105-113)Field of study: Chemistryby Dalvin D. Méndez-Hernándezhttps://hdl.handle.net/2286/R.I.2499800Doctoral DissertationAcademic thesesix, 113 p. : ill. (some col.)114023411151630348489152655adminIn CopyrightAll Rights Reserved2014TextChemistryenergyDFT calculationsPhotoelectrochemical tandem cellsPorphyrins and phthalocyaninesWater splittingPhotoelectrochemistryPhotoelectric cellsWater--Electrolysis.