Computers for chemistry and chemistry for computers: From computational prediction of reaction selectivities to novel molecular wires for electrical devices
type: CreativeWork
description: Taking advantage of cutting-edge technologies in computational and experimental chemistry, my Ph. D. research aimed to bridge both of these chemical subdivisions. Therefore, while part I of this dissertation focuses on new structure-based computational methodologies to predict selectivities of organic and enzymatic reactions, part II is concerned with the design, the synthesis and the electrical properties of novel, single molecular wires. These single molecule technologies described in part II are likely to contribute to more powerful computer chips in the future, which will in turn lead to faster and more accurate computational predictions for chemical problems. Part I: Computers for Chemistry: Progress towards the design of accurate computational tools to predict the selectivity of chemical reactions. The first fully quantum mechanical study to predict enantioselectivities for a large dataset of organic reactions has been reported. Enantioselectivities were calculated for a diverse set of 46 dioxirane catalyzed epoxidation reactions. Comparison to experiments showed that our methodology is able to accurately predict the free energy differences between transition states leading to enantiomeric products. To further improve the predictive performance, we have also developed a new correction scheme, which increases the accuracy of density functional theory (DFT) for non-covalent interactions. Our new correction scheme accurately estimates interaction energies of non-covalent complexes not only with large, but also with small basis sets at lower computational cost. The improved enantioselectivity prediction protocol containing our latest non-covalent corrections has now been fully automated in a user-friendly fashion. We are currently testing its accuracy for other asymmetric reactions, such as CBS reductions and are also trying to use our methodology to design new asymmetric organocatalysts. In collaboration with Dr. Jianing Li, a structure based computational method…
abstract: Taking advantage of cutting-edge technologies in computational and experimental chemistry, my Ph. D. research aimed to bridge both of these chemical subdivisions. Therefore, while part I of this dissertation focuses on new structure-based computational methodologies to predict selectivities of organic and enzymatic reactions, part II is concerned with the design, the synthesis and the electrical properties of novel, single molecular wires. These single molecule technologies described in part II are likely to contribute to more powerful computer chips in the future, which will in turn lead to faster and more accurate computational predictions for chemical problems. Part I: Computers for Chemistry: Progress towards the design of accurate computational tools to predict the selectivity of chemical reactions. The first fully quantum mechanical study to predict enantioselectivities for a large dataset of organic reactions has been reported. Enantioselectivities were calculated for a diverse set of 46 dioxirane catalyzed epoxidation reactions. Comparison to experiments showed that our methodology is able to accurately predict the free energy differences between transition states leading to enantiomeric products. To further improve the predictive performance, we have also developed a new correction scheme, which increases the accuracy of density functional theory (DFT) for non-covalent interactions. Our new correction scheme accurately estimates interaction energies of non-covalent complexes not only with large, but also with small basis sets at lower computational cost. The improved enantioselectivity prediction protocol containing our latest non-covalent corrections has now been fully automated in a user-friendly fashion. We are currently testing its accuracy for other asymmetric reactions, such as CBS reductions and are also trying to use our methodology to design new asymmetric organocatalysts. In collaboration with Dr. Jianing Li, a structure based computational method…
author: Schneebeli, Severin Thomas
language: English
keywords: Chemistry, Chemistry, Organic, Chemistry, Physical and theoretical
date published: 2011
date modified: 2026-07-24T01:44:14Z
provider: Columbia University
publisher: Networked Digital Library of Theses and Dissertations
type: WebPage
source organization: Columbia University

PropertyValue
property ID: DOI
value: 10.7916/D8V4125M