TY - JOUR
T1 - Charge transport in photofunctional nanoparticles self-assembled from zinc 5,10,15,20-tetrakis(perylenediimide)porphyrin building blocks
AU - Van der Boom, Tamar
AU - Hayes, Ryan T.
AU - Zhao, Yongyu
AU - Bushard, Patrick J.
AU - Weiss, Emily A.
AU - Wasielewski, Michael R.
PY - 2002/8/14
Y1 - 2002/8/14
N2 - Molecules designed to carry out photochemical energy conversion typically employ several sequential electron transfers, as do photosynthetic proteins. Yet, these molecules typically do not achieve the extensive charge transport characteristic of semiconductor devices. We have prepared a large molecule in which four perylene-3,4:9,10-tetracarboxydiimide (PDI) molecules that both collect photons and accept electrons are attached to a central zinc 5,10,15,20-tetraphenylporphyrin (ZnTPP) electron donor. This molecule self-assembles into ordered nanoparticles both in solution and in the solid-state, driven by van der Waals stacking of the PDI molecules. Photoexcitation of the nanoparticles results in quantitative charge separation in 3.2 ps to form ZnTPP+PDI- radical ion pairs, in which the radical anion rapidly migrates to PDI molecules that are, on average, 21 Å away, as evidenced by magnetic field effects on the yield of the PDI triplet state that results from radical ion pair recombination. These nanoparticles exhibit charge transport properties that combine important features from both photosynthetic and semiconductor photoconversion systems.
AB - Molecules designed to carry out photochemical energy conversion typically employ several sequential electron transfers, as do photosynthetic proteins. Yet, these molecules typically do not achieve the extensive charge transport characteristic of semiconductor devices. We have prepared a large molecule in which four perylene-3,4:9,10-tetracarboxydiimide (PDI) molecules that both collect photons and accept electrons are attached to a central zinc 5,10,15,20-tetraphenylporphyrin (ZnTPP) electron donor. This molecule self-assembles into ordered nanoparticles both in solution and in the solid-state, driven by van der Waals stacking of the PDI molecules. Photoexcitation of the nanoparticles results in quantitative charge separation in 3.2 ps to form ZnTPP+PDI- radical ion pairs, in which the radical anion rapidly migrates to PDI molecules that are, on average, 21 Å away, as evidenced by magnetic field effects on the yield of the PDI triplet state that results from radical ion pair recombination. These nanoparticles exhibit charge transport properties that combine important features from both photosynthetic and semiconductor photoconversion systems.
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U2 - 10.1021/ja026286k
DO - 10.1021/ja026286k
M3 - Article
C2 - 12167053
AN - SCOPUS:0037077547
SN - 0002-7863
VL - 124
SP - 9582
EP - 9590
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 32
ER -