Mediating Reductive Charge Shift Reactions in Electron Transport Chains

Beitrag in einer Fachzeitschrift

Details zur Publikation

Autorinnen und Autoren: Wolf M, Villegas C, Trukhina O, Delgado JL, Torres T, Martin N, Clark T, Guldi DM
Zeitschrift: Journal of the American Chemical Society
Jahr der Veröffentlichung: 2017
Band: 139
Heftnummer: 48
Seitenbereich: 17474-17483
ISSN: 0002-7863


We report the synthesis of a full-fledged family of covalent electron donor-acceptor(1)-acceptor(2) conjugates and their charge-transfer characterization by means of advanced photophysical assays. By virtue of variable excited state energies and electron donor strengths, either Zn(II)Porphyrins or Zn(II)Phthalocyanines were linked to different electron-transport chains featuring pairs of electron accepting fullerenes, that is, C-60 and C-70. In this way, a fine-tuned redox gradient is established to power a unidirectional, long-range charge transport from the excited-state electron donor via a transient C-60(center dot-) toward C-70(center dot-). This strategy helps minimize energy losses in the reductive, short-range charge shift from C-60 to C-70. At the forefront of our investigations are excited-state dynamics deduced from femtosecond transient absorption spectroscopic measurements and subsequent computational deconvolution of the transient absorption spectra. These provide evidence for cascades of short-range charge-transfer processes, including reductive charge shift reactions between the two electron-accepting fullerenes, and for kinetics that are influenced by the nature and length of the respective spacer. Of key importance is the postulate of a mediating state in the charge-shift reaction at weak electronic couplings. Our results point to an intimate relationship between triplet-triplet energy transfer and charge transfer.

FAU-Autorinnen und Autoren / FAU-Herausgeberinnen und Herausgeber

Clark, Timothy apl. Prof. Dr.
Guldi, Dirk Michael Prof. Dr.
Lehrstuhl für Physikalische Chemie I
Wolf, Maximilian
Lehrstuhl für Physikalische Chemie I

Einrichtungen weiterer Autorinnen und Autoren

Universidad Autónoma de Madrid (UAM)
Universidad Complutense de Madrid (UCM)
University of Basque Country / Universidad del Pais Vasco (UPV) / Euskal Herriko Unibersitatea (EHU)


Wolf, M., Villegas, C., Trukhina, O., Delgado, J.L., Torres, T., Martin, N.,... Guldi, D.M. (2017). Mediating Reductive Charge Shift Reactions in Electron Transport Chains. Journal of the American Chemical Society, 139(48), 17474-17483.

Wolf, Maximilian, et al. "Mediating Reductive Charge Shift Reactions in Electron Transport Chains." Journal of the American Chemical Society 139.48 (2017): 17474-17483.


Zuletzt aktualisiert 2018-20-12 um 08:53