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Thermodynamic Integration Networks and Their Application to Charge Transfer Reactions within the AauDyPI Fungal
Anna Bauß1, Michael Langenmaier1, Eric Strittmatter2
1Institut für Physikalische Chemie, Universität Freiburg , Albertstraße 23a, D-79104 Freiburg im Breisgau, Germany.
Abstract:
We present a computer simulation study of the thermodynamics and kinetics of charge transfer reactions within the fungal peroxidase AauDyPI from Auricularia auriculae-judae. Driving forces and reorganization energies are obtained from a thermodynamic integration scheme based upon molecular dynamics simulations. To enhance the numerical accuracy, the free energies are analyzed within a least-squares scheme of a closely knit thermodynamic network. We identify Tyr147, Tyr229, and Trp105 as oxidative agents, and find Trp377 to be a long-lived reaction intermediate. The results are compared to recent experimental findings.
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