Excitation energy-dependent photocurrent switching in a single-molecule photodiode

Author:

Shan Bing,Nayak Animesh,Williams Olivia F.,Yost Dillon C.,Polizzi Nicholas F.,Liu Yanming,Zhou Ninghao,Kanai Yosuke,Moran Andrew M.,Therien Michael J.ORCID,Meyer Thomas J.ORCID

Abstract

The direction of electron flow in molecular optoelectronic devices is dictated by charge transfer between a molecular excited state and an underlying conductor or semiconductor. For those devices, controlling the direction and reversibility of electron flow is a major challenge. We describe here a single-molecule photodiode. It is based on an internally conjugated, bichromophoric dyad with chemically linked (porphyrinato)zinc(II) and bis(terpyridyl)ruthenium(II) groups. On nanocrystalline, degenerately doped indium tin oxide electrodes, the dyad exhibits distinct frequency-dependent, charge-transfer characters. Variations in the light source between red-light (∼1.9 eV) and blue-light (∼2.7 eV) excitation for the integrated photodiode result in switching of photocurrents between cathodic and anodic. The origin of the excitation frequency-dependent photocurrents lies in the electronic structure of the chromophore excited states, as shown by the results of theoretical calculations, laser flash photolysis, and steady-state spectrophotometric measurements.

Funder

U.S. Department of Energy

National Science Foundation

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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