Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 109, Issue 39, Pages 15565-15571Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1113753109
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Funding
- Cluster of Excellence Engineering of Advanced Materials award
- MEC, Spain [CTQ2011-24187/BQU, CDS 2007-00010]
- CAM [MADRISOLAR-2, S2009/PPQ/1533]
- UAM
- Fonds der Chemischen Industrie
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In the current work, we have documented the use of two complementary supramolecular motifs, namely multipoint hydrogen bonding and metal complexation, as a means to control the step-by-step assembly of a panchromatically absorbing and highly versatile solar energy conversion system. On one hand, two different perylenediimides (1a/1b) have been integrated together with a metalloporphyrin (2) by means of the Hamilton receptor/cyanuric acid hydrogen bonding motif into energy transduction systems 1a center dot 2 or 1b center dot 2. Steady-state and time-resolved measurements corroborated that upon selective photoexcitation of the perylenediimides (1a/1b), an energy transfer evolved from the singlet excited state of the perylenediimides (1a/1b) to that of the metalloporphyrin (2). On the other hand, fullerene (3) and metalloporphyrin (2) form the electron donor-acceptor system 2 center dot 3 via axial complexation. Photophysical measurements confirm that an electron transfer prevails from the singlet excited state of 2 to the electron-accepting 3. The correspondingly formed radical ion pair state decays with a lifetime of 1.0 +/- 0.1 ns. As a complement to the aforementioned, the energy transduction features of 1a center dot 2 were combined with the electron donor-acceptor characteristics of 2 center dot 3 to afford 1a center dot 2 center dot 3. To this end, time-resolved measurements reveal that the initially occurring energy-transfer interaction (53 +/- 3 ps) between 1a/1b and 2 is followed by an electron transfer (12 +/- 1 ps) from 2 to 3. From multiwavelength analyses, the lifetime of the radical ion pair state in 1a center dot 2 center dot 3-as a product of a cascade of light-induced energy and electron transfer-was derived as 3.8 +/- 0.2 ns.
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