Funneling and Enhancing Upconversion Emission by Light-Harvesting Molecular Wires

However, challenging issues exist in improving TTA upconversion efficiencies in solid-states, one of which is the back energy transfer from upconverted singlet annihilators to sensitizers resulting in decreasing upconversion emission. Here we present a light-harvesting molecular wire consisting of dendrons with 9,10-diphenylanthracene derivatives (DPAEH) at the periphery and para-phenylene ethynylene oligomers (PPE) as the wire core.

The peripheral DPAEH antenna funnels singlet excitonic energy to the wire on a 12 ps timescale. Incorporating the molecular wire into the TTA upconversion solid consisting of the DPAEH annihilator and the porphyrin sensitizer evidently improves the upconversion quantum yield from 1.5% to 2.7% upon 532 nm excitation by suppressing the back energy transfer from the singlet annihilator to the sensitizer. This finding offers a potential route to use singlet energy light-harvesting architecture for enhancing TTA upconversion.