Palmer, Jeremy C.2019-11-07August 2012019-08August 201Portions of this document appear in: Chawla, Aseem, Rui Li, Rishabh Jain, R. John Clark, James G. Sutjianto, Jeremy C. Palmer, and Jeffrey D. Rimer. "Cooperative effects of inorganic and organic structure-directing agents in ZSM-5 crystallization." Molecular Systems Design & Engineering 3, no. 1 (2018): 159-170. And in: Olafson, Katy N., R. John Clark, Peter G. Vekilov, Jeremy C. Palmer, and Jeffrey D. Rimer. "Structuring of Organic Solvents at Solid Interfaces and Ramifications for Antimalarial Adsorption on β-Hematin Crystals." ACS applied materials & interfaces 10, no. 35 (2018): 29288-29298.https://hdl.handle.net/10657/5288Crystallization is relevant to a variety of important applications ranging from chemical refinement and pharmaceutical formulation to the design of novel materials for electronics and photonics applications. In these applied settings, successful outcomes require the ability to produce the desired crystal polymorph or structure that exhibits the critical functional properties needed for a particular application. Additionally, in many scenarios, material performance is strongly affected by the size, shape, and morphology of the produced crystallites. Unfortunately, controlling polymorph selection and crystal size and shape is often very synthetically challenging, providing a significant barrier to designing materials with optimal performance characteristics for targeted applications. In this thesis, we show that computer simulation methods can be used to complement experiment and aid in the development of rational crystal design strategies based on the use of molecular additives. Specifically, we show several instances of how molecular simulation can be used to elucidate the mechanisms of molecular additives such as crystal growth modifiers and structure directing agents, which can be used to control crystal morphology and polymorph selection during synthesis, respectively. These insights provide fundamental understanding that can help with \emph{a prior} identification of effective additives to achieve desired synthesis outcomes. Moreover, they suggest promising future directions in applying these computational methods to screen large libraries of compounds to identify effective molecular additives and thereby accelerate material design.application/pdfengThe author of this work is the copyright owner. UH Libraries and the Texas Digital Library have their permission to store and provide access to this work. UH Libraries has secured permission to reproduce any and all previously published materials contained in the work. Further transmission, reproduction, or presentation of this work is prohibited except with permission of the author(s).Molecular dynamicsZeolitesMolecular-SievesZeolite ZSM-5Zeolite LZeolite TONCrystal MorphologyB-HematinFrameworkMFISilicaUmbrella Samplin2019-11-07Thesisborn digital