Computational Study Using Tensile Force and Torque to Manipulate Axial Chirality in Biaryl Molecules

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Neal, Mathew

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thesis

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eng

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Chemistry , Mechanochemistry , Chirality , Computational

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Abstract

Biaryl molecules are widely studied systems that have applications in a broad selection of fields including pharmaceuticals, environmental protection, liquid crystal synthesis, and metal organic framework synthesis. Extra care is required in consideration of the axial chirality they often exhibit. Careful control of axial chirality in biaryl molecules is a blossoming area of study which remains open to fresh interpretation. This study, employing quantum chemical calculations and first principles molecular dynamics simulations, has demonstrated that a mechanochemical scheme may be employed wherein mechanical work introduced by the application of tensile forces and torques can be used to promote enantiomeric excess in a number of axially chiral substituted biaryl molecules. Furthermore, quantitative control over the timescales of biphenyl rotation and chiral purification is offered. Subsequently, a system incorporating Taylor series approximations has been employed to approximate the effects of mechanical work on the potential energy surface, reducing the number of quantum chemical calculations required in order to identify a suitable range of tensile forces and torques in order to achieve enantiomeric excess.

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