3 years ago

Enabling Efficient Creation of Long-Lived Charge-Separation on Dye-Sensitized NiO Photocathodes

Enabling Efficient Creation of Long-Lived Charge-Separation on Dye-Sensitized NiO Photocathodes
John M. Papanikolas, Robert J. Dillon, Leila Alibabaei, Thomas J. Meyer
The hole-injection and recombination photophysics for NiO sensitized with RuP ([RuII(bpy)2(4,4′-(PO3H2)2-bpy)]2+) are explored. Ultrafast transient absorption (TA) measurements performed with an external electrochemical bias reveal the efficiency for productive hole-injection, that is, quenching of the dye excited state that results in a detectable charge-separated electron–hole pair, is linearly dependent on the electronic occupation of intragap states in the NiO film. Population of these states via a negative applied potential increases the efficiency from 0% to 100%. The results indicate the primary loss mechanism for dye-sensitized NiO is rapid nongeminate recombination enabled by the presence of latent holes in the surface of the NiO film. Our findings suggest a new design paradigm for NiO photocathodes and devices centered on the avoidance of this recombination pathway.

Publisher URL: http://dx.doi.org/10.1021/acsami.7b05856

DOI: 10.1021/acsami.7b05856

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