Quantum chemical studies of biochemical reaction mechanisms
Title: |
Quantum chemical studies of biochemical reaction mechanisms |
DNr: |
SNIC 2015/1-460 |
Project Type: |
SNIC Medium Compute |
Principal Investigator: |
Per Siegbahn <ps@organ.su.se> |
Affiliation: |
Stockholms universitet |
Duration: |
2016-01-01 – 2017-01-01 |
Classification: |
10407 |
Keywords: |
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Abstract
This application concerns computer resources for studying mechanisms
of redox active enzymes. During the past period, the studies have been
performed in about equal parts at the Ferlin cluster at PDC and at
Triolith at NSC. Using hybrid density functional theory and active
site models of 100-400 atoms, potential energy surfaces for different
mechanisms are calculated. The computed results are compared to
experimental reaction rates and other observations. There have been
two major projects the past decade. The first one is water oxidation
in photosystem II, for which results superior to experiments for both
structures and mechanisms have ben obtained. The second one is oxygen
reduction and proton pumping in cytochrome c oxidase in the
respiratory chain. During recent years a mechanism has been obtained,
which so far is the only one that stands all experimental
observations. During the past year, new very conclusive experimental
studies have been published in Science and JACS, by leading
experimental groups in this area. The mechanism proposed by our group
is confirmed in utmost detail. Other examples of enzyme redox mechanisms
have been described in a recent comprehensive review in Chemical
Reviews this year. It is of utmost importance that these projects,
which are at the top of similar projects in the world, continues to be
substantially supported by computer funding.