Date of Award
8-2009
Document Type
Dissertation
Degree Name
Doctor of Philosophy (PhD)
Legacy Department
Chemical and Biomolecular Engineering
Committee Chair/Advisor
Bruce, David A
Committee Member
Hirt , Douglas E
Committee Member
Latour , Robert A
Committee Member
Stuart , Steven J
Committee Member
Thies , Mark C
Abstract
In this work, existing force field descriptions of poly (lactic acid), or PLA, were improved by modifying the torsional potential energy terms to more accurately model the bond rotational behavior of PLA. Extensive calculations were carried out using density functional theory (DFT), for small PLA molecules in vacuo, and also using DFT with a continuum model to approximate the electronic structure of PLA in its condensed phase. From these results, improved force field parameters were developed using a combination of the OPLS and CHARMM force fields. The new force field, PLAFF2, is an update to the previously developed PLAFF model developed in David Bruce's group, and results in more realistic conformational distributions during simulation of bulk amorphous PLA. It is demonstrated that the PLAFF2 model retains the accuracy of the original PLAFF in simulating the crystalline α polymorph of PLA. The PLAFF2 model has superior performance to any other publicly available force field for use with PLA; hence, we recommend its use in future modeling studies on the material, whether in its crystalline or amorphous form.
Recommended Citation
Mcaliley, James, "Development of Improved Torsional Potentials in Classical Force Field Models of Poly (Lactic Acid)" (2009). All Dissertations. 433.
https://tigerprints.clemson.edu/all_dissertations/433