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

Dillon, Robert J.; Alibabaei, Leila; Meyer, Thomas J.; Papanikolas, John M.

doi:10.1021/acsami.7b05856

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

Journal Article · Sun Jul 21 00:00:00 EDT 2019 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.7b05856· OSTI ID:1469824

Dillon, Robert J. ^[1]; Alibabaei, Leila ^[1]; ^[1]; ^[1]

Univ. of North Carolina, Chapel Hill, NC (United States)

The hole-injection and recombination photophysics for NiO sensitized with RuP ([Ru^II(bpy)₂(4,4'-(PO₃H₂)₂-bpy)]²⁺) are explored. Ultrafast transient absorption (TA) measurements performed with an external electrochemical bias reflect 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 results indicate a new design paradigm for NiO photocathodes and devices centered on the avoidance of this recombination pathway.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Solar Fuels (UNC EFRC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0001011

OSTI ID:: 1469824

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 32 Vol. 9; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
42 ENGINEERING
applied bias
dye-sensitized nickel oxide NiO
hole-injection
photocathode
recombination
solar fuels
transient absorption

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

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