Molecular photon upconversion, by way of triplet−triplet annihilation (TTA-UC), is an intriguing strategy to increase solar cell efficiencies beyond the Shockley−Queisser limit. Here we introduce self-assembled bilayers of acceptor and sensitizer molecules on high surface area electrodes as a means of generating an integrated TTA-UC dye-sensitized solar cell. Intensity dependence and IPCE measurements indicate that bilayer films effectively generate photocurrent by two different mechanisms: (1) direct excitation and electron injection from the acceptor molecule and (2) low-energy light absorption by the sensitizer molecule followed by TTA-UC and electron injection from the upconverted state. The power conversion efficiency from the upconverted photons is the highest yet reported for an integrated TTA-UC solar cell. Energy transfer and photocurrent generation efficiency of the bilayer device is also directly compared to the previously reported heterogeneous UC scheme.

Azobenzene polymers show promising photostrictive behavior for a broad range of applications in flow control, robotics, and energy harvesting applications. The conversion of solar energy directly into mechanical work provides unique capabilities in adaptive structures; however, the energy conversion of visible light into mechanical work presents several material chemistry challenges. Azobenzene strongly absorbs ultraviolet (UV) light and blue/green light which limits the efficiency of the photomechanical response under solar irradiation. Photon upconversion — combining two or more low energy photons (longer wavelength) to generate a higher energy excited state (shorter wavelength), provides an intriguing strategy to drive these high energy photochemical reactions with low energy light. We present an experimental study showing the feasibility to drive azobenzene photoisomerization using visible light via select up-conversion molecules in the fluidic state. Multi-physics modeling is then used to predict advances in photomechanical energy conversion when up-conversion molecules are introduced within an azobenzene polymer.