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

Abstract

The hole-injection and recombination photophysics for NiO sensitized with RuP ([Ru II(bpy) 2(4,4'-(PO 3H 2) 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.

Authors:
 [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of North Carolina, Chapel Hill, NC (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Solar Fuels (UNC EFRC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1469824
Grant/Contract Number:  
SC0001011
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 9; Journal Issue: 32; Related Information: UNC partners with University of North Carolina (lead); Duke University; University of Florida; Georgia Institute of Technology; University; North Carolina Central University; Research Triangle Institute; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 42 ENGINEERING; hole-injection; recombination; dye-sensitized nickel oxide NiO; transient absorption; applied bias; solar fuels; photocathode

Citation Formats

Dillon, Robert J., Alibabaei, Leila, Meyer, Thomas J., and Papanikolas, John M. Enabling Efficient Creation of Long-Lived Charge-Separation on Dye-Sensitized NiO Photocathodes. United States: N. p., 2019. Web. doi:10.1021/acsami.7b05856.
Dillon, Robert J., Alibabaei, Leila, Meyer, Thomas J., & Papanikolas, John M. Enabling Efficient Creation of Long-Lived Charge-Separation on Dye-Sensitized NiO Photocathodes. United States. doi:10.1021/acsami.7b05856.
Dillon, Robert J., Alibabaei, Leila, Meyer, Thomas J., and Papanikolas, John M. Sun . "Enabling Efficient Creation of Long-Lived Charge-Separation on Dye-Sensitized NiO Photocathodes". United States. doi:10.1021/acsami.7b05856.
@article{osti_1469824,
title = {Enabling Efficient Creation of Long-Lived Charge-Separation on Dye-Sensitized NiO Photocathodes},
author = {Dillon, Robert J. and Alibabaei, Leila and Meyer, Thomas J. and Papanikolas, John M.},
abstractNote = {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 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.},
doi = {10.1021/acsami.7b05856},
journal = {ACS Applied Materials and Interfaces},
number = 32,
volume = 9,
place = {United States},
year = {2019},
month = {7}
}

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This content will become publicly available on July 21, 2020
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Works referencing / citing this record:

Promising sensitizers for dye sensitized solar cells: A comparison of Ru(II) with other earth's scarce and abundant metal polypyridine complexes
journal, April 2019

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