Design principles and fundamental trade-offs in biomimetic light harvesting

Abstract

Recent developments in synthetic and supramolecular chemistry have created opportunities to design organic systems with tailored nanoscale structure for various technological applications. A key application area is the capture of light energy and its conversion into electrochemical or chemical forms for photovoltaic or sensing applications. In this work we consider cylindrical assemblies of chromophores that model structures produced by several supramolecular techniques. Our study is especially guided by the versatile structures produced by virus-templated assembly. We use a multi-objective optimization framework to determine design principles and limitations in light harvesting performance for such assemblies, both in the presence and absence of disorder. We identify a fundamental trade-off in cylindrical assemblies that is encountered when attempting to maximize both efficiency of energy transfer and absorption bandwidth. We also rationalize the optimal design strategies and provide explanations for why various structures provide optimal performance. Most importantly, we find that the optimal design strategies depend on the amount of energetic and structural disorder in the system. The aim of these studies is to develop a program of quantum-informed rational design for construction of organic assemblies that have the same degree of tailored nanoscale structure as biological photosynthetic light harvesting complexes, and also have the potential to reproduce their remarkable light harvesting performance.

35 pages, 8 figures. Published version

References in corpus (4)

• Environment-Assisted Quantum Transport
• Highly efficient energy excitation transfer in light-harvesting complexes: The fundamental role of noise-assisted transport
• Role of quantum coherence in chromophoric energy transport
• Efficiency of energy transfer in a light-harvesting system under quantum coherence

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• Optimal Dephasing for Ballistic Energy Transfer in Disordered Linear Chains
• Efficient light harvesting and photon sensing via engineered cooperative effects
• Efficient excitation transfer in an LH2-inspired nanoscale stacked ring geometry
• Environment-assisted modulation of heat flux in a bio-inspired system based on collision model
• Quantum walk in stochastic environment