TY - JOUR
T1 - Proton transfer and dissociation of GlyLysH + following O-H and N-H stretching mode excitations
T2 - Dynamics simulations
AU - Shmilovits-Ofir, Michaela
AU - Gerber, R. Benny
PY - 2011/10/19
Y1 - 2011/10/19
N2 - Proton transfer and dissociation processes following excitation of the OH or NH stretching modes of the proton-bound complex GlyLysH + are studied by classical trajectories. "On the fly" simulations with the PM3 semiempirical electronic structure method for the potential surface are used. Initial conditions are sampled to correspond to the v=1 excited state of the OH or NH stretching modes. Five different conformers of the complex are studied as initial structures. The main findings are (1) Photoinduced proton transfer is on the picosecond time scale. (2) Proton transfer is much faster than the processes of dissociation. (3) Proton transfer involves different sites. Most trajectories show sequences of two proton transfer events. (4) The proton transfer events show high selectivity with regard to the initially excited vibration and the initial structure. (5) Photodissociation of the complex occurs on a typical time scale of 100 ps. (6) Conformational transitions are found to be often faster than proton transfer. These results have implications for the mass spectrometry of complexes, for dynamics of proton wires, and for proton migration in proteins.
AB - Proton transfer and dissociation processes following excitation of the OH or NH stretching modes of the proton-bound complex GlyLysH + are studied by classical trajectories. "On the fly" simulations with the PM3 semiempirical electronic structure method for the potential surface are used. Initial conditions are sampled to correspond to the v=1 excited state of the OH or NH stretching modes. Five different conformers of the complex are studied as initial structures. The main findings are (1) Photoinduced proton transfer is on the picosecond time scale. (2) Proton transfer is much faster than the processes of dissociation. (3) Proton transfer involves different sites. Most trajectories show sequences of two proton transfer events. (4) The proton transfer events show high selectivity with regard to the initially excited vibration and the initial structure. (5) Photodissociation of the complex occurs on a typical time scale of 100 ps. (6) Conformational transitions are found to be often faster than proton transfer. These results have implications for the mass spectrometry of complexes, for dynamics of proton wires, and for proton migration in proteins.
UR - http://www.scopus.com/inward/record.url?scp=80054748783&partnerID=8YFLogxK
U2 - 10.1021/ja205634b
DO - 10.1021/ja205634b
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C2 - 21877725
AN - SCOPUS:80054748783
SN - 0002-7863
VL - 133
SP - 16510
EP - 16517
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 41
ER -