Long-lived photoinduced polaron formation in conjugated polyelectrolyte-fullerene assemblies by Rachel C. Huber, Amy S. Ferreira, Robert Thompson, Daniel.

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Long-lived photoinduced polaron formation in conjugated polyelectrolyte-fullerene assemblies by Rachel C. Huber, Amy S. Ferreira, Robert Thompson, Daniel Kilbride, Nicholas S. Knutson, Lekshmi Sudha Devi, Daniel B. Toso, J. Reddy Challa, Z. Hong Zhou, Yves Rubin, Benjamin J. Schwartz, and Sarah H. Tolbert Science Volume 348(6241):1340-1343 June 19, 2015 Copyright © 2015, American Association for the Advancement of Science

Fig. 1 PFT and charged fullerene structure and assembly. PFT and charged fullerene structure and assembly. PFT structure (A); cartoon of a PFT micelle (B); charged fullerenes (C). CryoEM images of pure PFT (D), PFT:mixed-bis adducts (E), and PFT:high adducts (F). Rachel C. Huber et al. Science 2015;348:1340-1343 Copyright © 2015, American Association for the Advancement of Science

Fig. 2 SAXS data for PFT and PFT/fullerene mixtures. SAXS data for PFT and PFT/fullerene mixtures. (A) Data for PFT:high-adducts are reasonably approximated by a sum of PFT + high-adducts. (B) The PFT:mixed-bis profile overlap mass-scaled PFT data. (C) Raw scattering data for all PFT and PFT:bis-fullerene samples are similar. (D) Distance distribution functions, P(r), obtained by Fourier transformation of the data in (C) show different fullerene environments for trans-1,2 and trans-3,4, with PFT:mix-bis corresponding to the sum of the two. Rachel C. Huber et al. Science 2015;348:1340-1343 Copyright © 2015, American Association for the Advancement of Science

Fig. 3 Formation of P+ and N– polarons requires intimate assembly of the polymer and fullerene. Formation of P+ and N– polarons requires intimate assembly of the polymer and fullerene. (A) PL of PFT, PFT:high adducts, and PFT:mixed-bis; (B) pump-probe spectroscopy for dilute PFT:mixed-bis solutions excited at 470 nm showing the rapid formation of both excitons and polarons; (C) time decays for the stimulated emission and the polaronic absorption from (B). Absorption from a green concentrated PFT/fullerene solution showing both P+ and N- polarons (D). EPR from a similar green solution, again showing both P+ and N– polarons (E). PL for various concentrated PFT:mixed-bis solutions showing that polarons quench luminescence, but the addition of THF, which, destroys the PFT/fullerene assembly, restores PL intensity (F). Rachel C. Huber et al. Science 2015;348:1340-1343 Copyright © 2015, American Association for the Advancement of Science

Fig. 4 Spectroscopic evidence for long-lived charged species in solution. Spectroscopic evidence for long-lived charged species in solution. Chemical structures of trans-1 bis (A), trans-2 bis (B), trans-3 bis (C), and trans-4 bis (D) fullerene derivatives with color emphasizing the hydrophobic regions. Cartoon depicting the assembly of trans-1,2 (orange) and trans-3,4 (purple) bis fullerenes with PFT (red). Photoexcitation of the PFT backbone leads to charge transfer first to trans-3,4 and then to trans-1,2, where the electron remains due to stabilization by the reorganization of water. The hole (green, h+) remains on PFT (E). PL of PFT, PFT:mixed-bis, PFT:trans-3,4 bis, and PFT:trans-1,2 bis (F). Time-resolved luminescence for assembled concentrated PFT:trans-3,4 bis and PFT:trans-1,2 bis samples (G). Rachel C. Huber et al. Science 2015;348:1340-1343 Copyright © 2015, American Association for the Advancement of Science