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.

arXiv comment35 pages, 8 figures. Published version

References in corpus (8)

• Long-lived quantum coherence in photosynthetic complexes at physiological temperature
• 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
• Efficient energy transfer in light-harvesting systems, I: optimal temperature, reorganization energy, and spatial-temporal correlations
• Environmental correlation effects on excitation energy transfer in photosynthetic light harvesting
• Optical Spectra and Localization of Excitons in Inhomogeneous Helical Cylindrical Aggregates

Cited by in corpus (20)

• Rabi model as a quantum coherent heat engine: From quantum biology to superconducting circuits
• Observation of noise-assisted transport in an all-optical cavity-based network
• Cooperative Robustness to Static Disorder: Superradiance and localization in a nanoscale ring to model natural light-harvesting systems
• Quantum Diffusion on Molecular Tubes: Universal Scaling of the 1D to 2D Transition
• Universally Optimal Noisy Quantum Walks on Complex Networks
• Non-Hermitian Hamiltonian approach to quantum transport in disordered networks with sinks: validity and effectiveness
• Realistic and verifiable coherent control of excitonic states in a light harvesting complex
• Long-range coherent energy transport in Photosystem II
• Cooperative robustness to dephasing: single-exciton Superradiance in a nanoscale ring to model natural light-harvesting systems
• Interplay of different environments in open quantum systems: Breakdown of the additive approximation
• Opening-Assisted Coherent Transport in the Deep Classical Regime
• An analytical continuation approach for evaluating emission lineshapes of molecular aggregates and the adequacy of multichromophoric Förster theory
• Optimal Dephasing for Ballistic Energy Transfer in Disordered Linear Chains
• Ab-Initio Calculation of Molecular Aggregation Effects: a Coumarin-343 Case Study
• Efficient light harvesting and photon sensing via engineered cooperative effects
• Quantum stochastic transport along chains
• Efficient excitation transfer in an LH2-inspired nanoscale stacked ring geometry
• Breakdown of quantum-to-classical correspondence for diffusion in high temperature thermal environment
• Quantum walk in stochastic environment
• Environment-assisted modulation of heat flux in a bio-inspired system based on collision model