Abstract
We explore various design principles for efficient excitation energy transport in complex quantum systems. We investigate energy transfer efficiency in randomly disordered geometries consisting of up to 20 chromophores to explore spatial and spectral properties of small natural/artificial Light-Harvesting Complexes (LHC). We find significant statistical correlations among highly efficient random structures with respect to ground state properties, excitonic energy gaps, multichromophoric spatial connectivity, and path strengths. These correlations can even exist beyond the optimal regime of environment-assisted quantum transport. For random configurations embedded in spatial dimensions of 30 Å or 50 Å, we observe that the transport efficiency saturates to its maximum value if the systems contain around 7 or 14 chromophores, respectively. Remarkably, these optimum values coincide with the number of chlorophylls in the Fenna-Matthews-Olson protein complex and LHC II monomers, respectively, suggesting a potential natural optimization with respect to chromophoric density.
Highlights
Monitoring and quantifying the effects of condensed phase environments on the quantum dynamics of charge and energy transfer has been one of central issues in chemical physics.1,2 One problem of fundamental and practical relevance is to engineer excitonic energy migration in disordered materials and nano-structures by exploiting the interplay of quantum effects and environmental interactions
By careful inspection of these results two main questions arise: How does the energy transfer efficiency (ETE) behave as a function of the chromophoric density? What are the possible classical and/or quantum correlations, in the spatial and energetic structure of these random multichromophoric geometries, discriminating ultrahigh or ultralow efficiencies in any fixed diameter? We addressed the former question in details in the Ref. 12 by examining the variation of the average transport efficiency for random configurations of up to 20 chromophores in two different compactness level
We studied the energy transport capability of random arrangements of chromophores in volumes of various diameters as a function of chromophoric density, reorganization energy, and their interplay
Summary
Monitoring and quantifying the effects of condensed phase environments on the quantum dynamics of charge and energy transfer has been one of central issues in chemical physics. One problem of fundamental and practical relevance is to engineer excitonic energy migration in disordered materials and nano-structures by exploiting the interplay of quantum effects and environmental interactions. One problem of fundamental and practical relevance is to engineer excitonic energy migration in disordered materials and nano-structures by exploiting the interplay of quantum effects and environmental interactions This rational design approach can be influenced by recent observations of Environment-Assisted Quantum Transport (ENAQT) in biological light-harvesting systems.. We compute the energy transfer efficiency (ETE) of the uniform distributions of random complexes consisting of 7 chromophores encapsulated in spherical dimension of various diameters interacting with a phononic bath. This allows us to compare our results with the performance of a well-characterized natural LHC such as the FMO complex. IV, we explore the role of chromophoric density in energy transfer as a dominating parameter. In the subsequent sections we explore the roles of other physical parameters in transport including, ground state energy properties, average excitonic energy, structure and strength of chromophoric connectivity
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