TY  - JOUR
A1  - Deniz, Erhan
A1  - Valiño Borau, Luis
A1  - Löffler, Jan Gerrit
A1  - Eberl, Katharina Barbara
A1  - Gulzar, Adnan
A1  - Wolf, Steffen
A1  - Durkin, Patrick M.
A1  - Kaml, Robert
A1  - Budisa, Nediljko
A1  - Stock, Gerhard
A1  - Bredenbeck, Jens
T1  - Through bonds or contacts? Mapping protein vibrational energy transfer using non-canonical amino acids
T2  - Nature Communications
N2  - Vibrational energy transfer (VET) is essential for protein function. It is responsible for efficient energy dissipation in reaction sites, and has been linked to pathways of allosteric communication. While it is understood that VET occurs via backbone as well as via non-covalent contacts, little is known about the competition of these two transport channels, which determines the VET pathways. To tackle this problem, we equipped the β-hairpin fold of a tryptophan zipper with pairs of non-canonical amino acids, one serving as a VET injector and one as a VET sensor in a femtosecond pump probe experiment. Accompanying extensive non-equilibrium molecular dynamics simulations combined with a master equation analysis unravel the VET pathways. Our joint experimental/computational endeavor reveals the efficiency of backbone vs. contact transport, showing that even if cutting short backbone stretches of only 3 to 4 amino acids in a protein, hydrogen bonds are the dominant VET pathway.
KW  - Computational biophysics
KW  - Energy transfer
KW  - Infrared spectroscopy
KW  - Proteins
Y1  - 2021
UR  - http://publikationen.ub.uni-frankfurt.de/frontdoor/index/index/docId/75070
UR  - https://nbn-resolving.org/urn:nbn:de:hebis:30:3-750703
SN  - 2041-1723
N1  - We acknowledge DFG funding (BR 3746/4-1; BU1404/9-1; INST 161/722-1; STO 247/10-2, INST 39/963-1 FUGG) as well as funding by the Canada Research Chairs Program (grant no. 950-231971).

This work has been supported by the DFG via the Research Unit FOR5099 “Reducing complexity of nonequilibrium systems”, the High Performance and Cloud Computing Group at the Rechenzentrum of the University of Freiburg, the state of Baden-Württemberg through bwHPC and the DFG (bwForCluster NEMO RV bw18A004), and the Black Forest Grid Initiative.

Open Access funding enabled and organized by Projekt DEAL.
VL  - 12
IS  - art. 3284
SP  - 1
EP  - 8
PB  - Nature Publishing Group
CY  - [London]
ER  -