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복잡계 자기조립 연구단
복잡계 자기조립 연구단
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Excitonic energy transfer of cryptophyte phycocyanin 645 complex in physiological temperature by reduced hierarchical equation of motion

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Title
Excitonic energy transfer of cryptophyte phycocyanin 645 complex in physiological temperature by reduced hierarchical equation of motion
Author(s)
Weon-Gyu Lee; Young Min Rhee
Publication Date
2014-03
Journal
BULLETIN OF THE KOREAN CHEMICAL SOCIETY, v.35, no.3, pp.858 - 864
Publisher
KOREAN CHEMICAL SOC
Abstract
Recently, many researches have shown that even photosynthetic light-harvesting pigment-protein complexes can have quantum coherence in their excitonic energy transfer at cryogenic and physiological temperatures.Because the protein supplies such noisy environment around pigments that conventional wisdom expects veryshort lived quantum coherence, elucidating the mechanism and searching for an applicability of the coherence have become an interesting topic in both experiment and theory. We have previously studied the quantum coherence of a phycocyanin 645 complex in a marine algae harvesting light system, using Poisson mappingbracket equation (PBME). PBME is one of the applicable methods for solving quantum-classical Liouville equation, for following the dynamics of such pigment-protein complexes. However, it may suffer from many defects mostly from mapping quantum degrees of freedom into classical ones. To make improvements againstsuch defects, benchmarking targets with more accurately described dynamics is highly needed. Here, we fall back to reduced hierarchical equation of motion (HEOM), for such a purpose. Even though HEOM is knownto applicable only to simplified system that is coupled to a set of harmonic oscillators, it can provide ultimateaccuracy within the regime of quantum-classical description, thus providing perfect benchmark targets for certain systems. We compare the evolution of the density matrix of pigment excited states by HEOM against the PBME results at physiological temperature, and observe more sophisticated changes of density matrixelements from HEOM. In PBME, the population of states with intermediate energies display only monotonically increasing behaviors. Most importantly, PBME suffers a serious issue of wrong population in the longtime limit, likely generated by the zero-point energy leaking problem. Future prospects for developments are briefly discussed as a concluding remark.
URI
https://pr.ibs.re.kr/handle/8788114/1092
ISSN
0253-2964
Appears in Collections:
Center for Self-assembly and Complexity(복잡계 자기조립 연구단) > Journal Papers (저널논문)
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