Structural Gating Enhances Long-Distance Light-Driven Interfacial Electron Transfer

Loague, Quentin R.; Heidari, Marzieh; Mann, Hayden J.; Danilov, Evgeny O.; Castellano, Felix N.; Galoppini, Elena; Meyer, Gerald J.

doi:10.1021/acscentsci.4c01106

Title: Structural Gating Enhances Long-Distance Light-Driven Interfacial Electron Transfer

Journal Article · 11 November 2024 · ACS Central Science

DOI: https://doi.org/10.1021/acscentsci.4c01106 · OSTI ID:2476764

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University of North Carolina at Chapel Hill, NC (United States)
Rutgers University, Newark, NJ (United States)
North Carolina State University, Raleigh, NC (United States)

Structural gating provides a molecular means to transfer electrons preferentially in one desired vectorial direction, a behavior needed for applications in artificial photosynthesis. At the interfaces utilized herein, visible-light absorption by a transition metal complex opens a “structural gate” by planarization of otherwise rotating phenyl rings in p-phenylene ethynylene (PE) bridge units. Planarization provides a conjugated pathway for electron flow toward a conductive oxide surface. Interfacial electron transfer to the oxide restores rotation and closes the gate to the unwanted recombination reaction. This structural gating results in nearly quantitative long-distance (>20 Å) interfacial electron transfer that occurs ~1000 times faster than transfer in the opposite direction. A comparative kinetic study of these complexes with those that contain ionic bridge units, without gating function, as a function of the applied potential and hence –ΔG° provided a physical basis for the structural gating. A small distancedependent reorganization energy with weak electronic coupling underlies the success of this gate that enables efficient long-distance electron transfer and slow recombination.

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Research Organization:: University of North Carolina at Chapel Hill, NC (United States)

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

Grant/Contract Number:: FG02-01ER15256; SC0011979; SC0013461

OSTI ID:: 2476764

Journal Information:: ACS Central Science, Journal Name: ACS Central Science Journal Issue: 11 Vol. 10; ISSN 2374-7943

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Charge transfer
Excited states
Kinetics
Metal to ligand charge transfer
Recombination

Title: Structural Gating Enhances Long-Distance Light-Driven Interfacial Electron Transfer

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