  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.
