Optical Intramolecular Electron Transfer in Opposite Directions through the Same Bridge That Follows Different Pathways
Abstract
The electrochemical and spectroscopic properties of eight bis(tridentate) cyclometalated RuII compounds covalently linked by a phenyl- or xylyl-thiophene bridge to a pendant triphenylamine (TPA) were characterized in fluid solution and immobilized on metal oxide surfaces. Upon surface immobilization, the TPA+/0 reduction potentials of the phenyl-bridged compounds exhibited large changes, ±100 mV, relative to solution-based values, yet those observed for the xylyl-bridged compounds were relatively unchanged. Additionally, the highest occupied molecular orbital of the surface-immobilized compounds was associated with either TPA or RuII, enabling the study of the electron transfer in opposite directions. Electron transfer in the mixed-valent states of the compounds was found to proceed by different optical pathways for RuII → TPA+ relative to TPA → RuIII. Mulliken–Hush analysis of intervalence charge transfer bands for the phenyl-bridged compounds revealed that the electronic coupling matrix element, HDA, was ~950 cm–1 for RuII → TPA+, while HDA for TPA → RuIII appeared to be 2500 cm–1. In contrast, the xylyl-bridged compounds were weakly coupled. A superexchange analysis, where unoccupied bridge orbitals were taken directly into account, led to a very different conclusion: HDA did not depend on the charge-transfer direction or path. In conclusion, the results imply that the electron-transfer directionmore »
- Authors:
-
[1];
[1];
[2];
[1]
- Univ. of North Carolina, Chapel Hill, NC (United States)
- Univ. of British Columbia, Vancouver, BC (Canada)
- 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)
- OSTI Identifier:
- 1470615
- Grant/Contract Number:
- SC0001011
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 140; Journal Issue: 23; 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 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (homogeneous); catalysis (heterogeneous); solar (photovoltaic); solar (fuels); photosynthesis (natural and artificial); hydrogen and fuel cells; electrodes - solar; charge transport; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly)
Citation Formats
Piechota, Eric J., Troian-Gautier, Ludovic, Sampaio, Renato N., Brennaman, M. Kyle, Hu, Ke, Berlinguette, Curtis P., and Meyer, Gerald J. Optical Intramolecular Electron Transfer in Opposite Directions through the Same Bridge That Follows Different Pathways. United States: N. p., 2018.
Web. doi:10.1021/jacs.8b02715.
Piechota, Eric J., Troian-Gautier, Ludovic, Sampaio, Renato N., Brennaman, M. Kyle, Hu, Ke, Berlinguette, Curtis P., & Meyer, Gerald J. Optical Intramolecular Electron Transfer in Opposite Directions through the Same Bridge That Follows Different Pathways. United States. https://doi.org/10.1021/jacs.8b02715
Piechota, Eric J., Troian-Gautier, Ludovic, Sampaio, Renato N., Brennaman, M. Kyle, Hu, Ke, Berlinguette, Curtis P., and Meyer, Gerald J. Mon .
"Optical Intramolecular Electron Transfer in Opposite Directions through the Same Bridge That Follows Different Pathways". United States. https://doi.org/10.1021/jacs.8b02715. https://www.osti.gov/servlets/purl/1470615.
@article{osti_1470615,
title = {Optical Intramolecular Electron Transfer in Opposite Directions through the Same Bridge That Follows Different Pathways},
author = {Piechota, Eric J. and Troian-Gautier, Ludovic and Sampaio, Renato N. and Brennaman, M. Kyle and Hu, Ke and Berlinguette, Curtis P. and Meyer, Gerald J.},
abstractNote = {The electrochemical and spectroscopic properties of eight bis(tridentate) cyclometalated RuII compounds covalently linked by a phenyl- or xylyl-thiophene bridge to a pendant triphenylamine (TPA) were characterized in fluid solution and immobilized on metal oxide surfaces. Upon surface immobilization, the TPA+/0 reduction potentials of the phenyl-bridged compounds exhibited large changes, ±100 mV, relative to solution-based values, yet those observed for the xylyl-bridged compounds were relatively unchanged. Additionally, the highest occupied molecular orbital of the surface-immobilized compounds was associated with either TPA or RuII, enabling the study of the electron transfer in opposite directions. Electron transfer in the mixed-valent states of the compounds was found to proceed by different optical pathways for RuII → TPA+ relative to TPA → RuIII. Mulliken–Hush analysis of intervalence charge transfer bands for the phenyl-bridged compounds revealed that the electronic coupling matrix element, HDA, was ~950 cm–1 for RuII → TPA+, while HDA for TPA → RuIII appeared to be 2500 cm–1. In contrast, the xylyl-bridged compounds were weakly coupled. A superexchange analysis, where unoccupied bridge orbitals were taken directly into account, led to a very different conclusion: HDA did not depend on the charge-transfer direction or path. In conclusion, the results imply that the electron-transfer direction can alter optical charge transfer pathways without influencing the electronic coupling.},
doi = {10.1021/jacs.8b02715},
journal = {Journal of the American Chemical Society},
number = 23,
volume = 140,
place = {United States},
year = {Mon May 07 00:00:00 EDT 2018},
month = {Mon May 07 00:00:00 EDT 2018}
}
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