We found a match
Your institution may have access to this item. Find your institution then sign in to continue.
- Title
Multichromophoric Perylenediimide-Silicon Phthalocyanine-C<sub>60</sub> System as an Artificial Photosynthetic Analogue.
- Authors
Martín‐Gomis, Luis; Peralta‐Ruiz, Francisco; Thomas, Michael B.; Fernández‐Lázaro, Fernando; D'Souza, Francis; Sastre‐Santos, Ángela
- Abstract
Sequential photoinduced energy transfer followed by electron transfer and the formation of charge-separated states, which are primary events of natural photosynthesis, have been demonstrated in a newly synthesized multichromophoric covalently linked triad, PDI-SiPc-C60. The triad comprises a perylenediimide (PDI), which primarily fulfils antenna and electron-acceptor functionalities, silicon phthalocyanine (SiPc) as an electron donor, and fulleropyrrolidine (C60) as a second electron acceptor. The multi-step convergent synthetic procedure developed here produced good yields of the triad and control dyads, PDI-SiPc and SiPc-C60. The structures and geometries of the newly synthesized donor-acceptor systems have been established from spectral, computational, and electrochemical studies with reference to appropriate control compounds. Ultrafast energy transfer from 1PDI* to SiPc in the case of PDI-SiPc and PDI-SiPc-C60 was witnessed. An energy-level diagram established from spectral and electrochemical data suggested the formation of two types of charge-separated states, that is, PDI-SiPc.+-C60.− and PDI.−-SiPc.+-C60 from the 1SiPc* in the triad, with generation of the latter being energetically more favorable. However, photochemical studies involving femtosecond transient spectroscopy revealed the formation of PDI-SiPc.+-C60.− as a major charge-separated product. This observation may be rationalized in terms of the closer spatial proximity to SiPc of C60 compared to PDI in the triad. The charge-separated state persisted for a few nanoseconds prior to populating the 3SiPc* state during charge recombination.
- Subjects
PHOTOINDUCED electron transfer; ENERGY transfer; PERYLENE derivatives; FEMTOSECOND pulses; ELECTROCHEMICAL analysis
- Publication
Chemistry - A European Journal, 2017, Vol 23, Issue 16, p3863
- ISSN
0947-6539
- Publication type
Article
- DOI
10.1002/chem.201606033