Semiclassical approach for all-atom nonadiabatic simulations of excitation energy transfer processes in photosynthetic complexes Young Min Rhee Department.

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Presentation transcript:

Semiclassical approach for all-atom nonadiabatic simulations of excitation energy transfer processes in photosynthetic complexes Young Min Rhee Department of Chemistry POSTECH (Pohang University of Science and Technology)

Young Min Rhee, Quantum coherence in photosynthesis Debates, debates, debates, …

Young Min Rhee, 2013 Detailed look? Theoretical approaches!

Young Min Rhee, Quantum coherence vs hopping Classical hopping

Young Min Rhee, Quantum coherence vs hopping Classical hopping

Young Min Rhee, Quantum coherence vs hopping Coherent transfer Can be faster!

Young Min Rhee, Classroom chaos…

Young Min Rhee, Class I constant H + abstract model bath Class II more realistic H, but ground state-like bath Class III bath relaxation upon electronic changes Classes of theoretical approaches H.W. Kim; A. Kelly; J.W. Park; YMR, JACS 134, (2012)

Young Min Rhee, 2013 Importance of the model consistency What if the potential is switched for better accuracy?  Potential exaggeration in One potential model should be adopted all the time

Young Min Rhee, Class I constant H + abstract model bath Class II more realistic H but ground state-like bath Class III bath relaxation upon electronic changes Classes of theoretical approaches

Young Min Rhee, Class I constant H + abstract model bath Class II more realistic H but ground state-like bath Class III bath relaxation upon electronic changes Classes of theoretical approaches

Young Min Rhee, Modeling for the chromophore complex Diagonals: force-field approach Off-diagonals: transition charge electrostatic potential (TrESP) [Madjet et al. JPCB 110, (2006)]  Fluctuations with all-atom interaction

Young Min Rhee, Electronic structure theory  Direct passage toward studying dynamics Modeling for the chromophore complex

Young Min Rhee, 2013 Can this be reliable?  Decent to good agreement!

Young Min Rhee, mapping formalism All atom  Semiclassical approach H. Kim; A. Nassimi; R. Kapral, JCP 129, (2008) A. Kelly; YMR, JPCL 2, 808 (2011) Partial Wigner transform

Young Min Rhee, Semiclassical approach: PBME Mapping approach: N quantum states  N fictitious harmonic oscillator  Dynamics of electronic states : Dynamics of (r, p) with Hamiltonian (Classical-looking) Newton-like mechanics toward multiple surface dynamics! Modeling efforts

Young Min Rhee, Confinement versus electrostatics Mutation study Confinement dominates over electrostatics for FMO Wild type ALA-mutant Electrostatic mutant H.W. Kim; A. Kelly; J.W. Park; YMR, JACS 134, (2012)

Young Min Rhee, Nature of initial state When started from non-oscillatory initial state Fluctuation “kicks” stationary into oscillatory Still becomes oscillatory after ~20 fs

Young Min Rhee, Vibrational effects? With active chromophore vibration With silenced chromophore vibration No coherence??? Classical nature: exaggeration of vibrational effect (faster decoherence) H.W. Kim; A. Kelly; J.W. Park; YMR, JACS 134, (2012)

Young Min Rhee, Ensemble versus single molecules Each is coherent in its own manner “Rigid” protein keeps coherence Coherent even with classical vibrations

Young Min Rhee, Future prospects Better QCLE than PBME? Semi-classical but yet classical Zero-point energy leaking Currently, horrible when states are largely separated Better potential for more reliable modeling? Different systems with QM effects?

Young Min Rhee, Conclusions All-atom level insight: POSSIBLE!!! Rigid nature of protein Chromophore alignment maintenance Coherent coupling Fidelity in photosynthesis? Flexible nature of protein Coupling fluctuation Diversity? H.W. Kim; A. Kelly; J.W. Park; YMR, JACS 134, (2012)

Young Min Rhee, Acknowledgements Aaron Kelly: PBME Hyun Woo Kim: MD interface Jae Woo Park: IM/MM Sun Mi Choi Weon-Gyu Lee Chang Woo Kim Postech (equipment) KOSEF / KRF / IBS ( \$ ) KISTI (CPU time) Q-Chem And YOU!!!