Systematic parameterization of lignin for the CHARMM force field

摘要: Lignin is an abundant aromatic biopolymer within plant cell walls formed through radical coupling chemistry, whose composition and topology can vary greatly depending on the biomass source. Computational modeling provides a complementary approach to traditional experimental techniques probe lignin interactions, structure, material properties. However, current approaches are limited based subset of chemistries covered by existing force fields. To fill gap, we developed comprehensive field that accounts for more lignin–lignin lignin–carbohydrate interlinkages than fields, also expands monomer be modeled beyond simple alcohols into rich mixture natural varieties. The development this utilizes recent developments in parameterization methodology, synthesizes them workflow combines target data from multiple molecules simultaneously single consistent parameter set. set represents significant improvement alternatives atomic diverse topologies, accurately reproducing observables while significantly reducing error relative quantum calculations. improved energetics, as well rigid adherence CHARMM philosophy, enables simulation its biological context with greater accuracy was previously possible. presented here therefore crucial first step towards structure across broad range environments, including where complexed carbohydrates deconstructed bacterial or fungal enzymes, it exists industrial solvent mixtures. Future simulations enabled updated will thus lead better chemical structural understanding lignin, providing new insight role recalcitrance probing potential used processes.