期刊
JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS
卷 50, 期 18, 页码 -出版社
IOP PUBLISHING LTD
DOI: 10.1088/1361-6455/aa8696
关键词
solar radiation; open system quantum mechanics; PC645; light harvestng
资金
- US Air Force Office of Scientific Research [FA9550-13-1-0005]
- Comite para el Desarrollo de la Investigacion (CODI) of Universidad de Antioquia, Colombia under Estrategia de Sostenibilidad
- Purdue-UdeA Seed Grant Program
- Departamento Administrativo de Ciencia, Tecnologia e Innovacion (COLCIENCIAS) of Colombia [111556934912]
The nature of excited states of open quantum systems produced by incoherent natural thermal light is analyzed based on a description of the quantum dynamical map. Natural thermal light is shown to generate long-lasting coherent dynamics because of (i) the super-Ohmic character of the radiation, and (ii) the absence of pure dephasing dynamics. In the presence of an environment, the long-lasting coherences induced by suddenly turned-on incoherent light dissipate and stationary coherences are established. As a particular application, dynamics in a subunit of the PC645 light-harvesting complex is considered where it is further shown that aspects of the energy pathways landscape depend on the nature of the exciting light and number of chromophores excited. Specifically, pulsed laser and natural broadband incoherent excitation induce significantly different energy transfer pathways. In addition, we discuss differences in perspective associated with the eigenstate versus site basis, and note an important difference in the phase of system coherences when coupled to blackbody radiation or when coupled to a phonon background. Finally, an appendix contains an open systems example of the loss of coherence as the turn-on time of the light assumes natural time scales.
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