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Direct simulation of non-adiabatic dynamics in large-scale enzymatic systems

Kretchmer, Joshua and Miller, Thomas (2017) Direct simulation of non-adiabatic dynamics in large-scale enzymatic systems. In: 254th American Chemical Society National Meeting & Exposition, August 20-24, 2017, Washington, DC.

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The simulation of general non-adiabatic processes, such as electron transfer, proton-transfer, and protoncoupled electron transfer, in enzymic systems presents a challenge for theor. methods due to the large system-sizes, the coupling between classical and quantum mech. motions, and the multiple time-scales present in these systems. To address these challenges we have developed the kinetically-constrained ring-polymer mol. dynamics (KC-RPMD) method for the direct simulation of non-adiabatic processes in large-scale biol. and chem. systems. KC-RPMD, like the conventional ring-polymer mol. dynamics (RPMD), is based on Feynman's path-integral formulation of statistical mechanics and is able to simulate quantum dynamical processes using purely classical dynamics; KC-RPMD goes beyond conventional RPMD, allowing for the treatment of general, multi-electron non-adiabatic processes. We apply KC-RPMD in fully atomistic simulations (15,000 atoms in explicit solvent) to understand the long-range electron transfer in various mutants of the blue-copper protein Azurin. Through the anal. of the KC-RPMD trajectories, we show for the first time the importance of donor-acceptor compression and the role of dynamical hydrogen-bonding networks during the electron transfer process in Azurin.

Item Type:Conference or Workshop Item (Paper)
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URLURL TypeDescription Website
Kretchmer, Joshua0000-0003-3468-0481
Miller, Thomas0000-0002-1882-5380
Additional Information:© 2017 American Chemical Society.
Record Number:CaltechAUTHORS:20170915-075505817
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:81473
Deposited By: Tony Diaz
Deposited On:15 Sep 2017 16:43
Last Modified:09 Mar 2020 13:18

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