Through-Space Ultrafast Photoinduced Electron Transfer Dynamics of a C70-Encapsulated Bisporphyrin Covalent Organic Polyhedron in a Low-Dielectric Medium

Michael Ortiz; Sung Cho; Jens Niklas; Seonah Kim; Oleg G. Poluektov; Wei Zhang; Garry Rumbles; Jaehong Park

doi:10.1021/jacs.7b00220

Through-Space Ultrafast Photoinduced Electron Transfer Dynamics of a C₇₀-Encapsulated Bisporphyrin Covalent Organic Polyhedron in a Low-Dielectric Medium

Michael Ortiz, Sung Cho, Jens Niklas, Seonah Kim, Oleg G. Poluektov, Wei Zhang, Garry Rumbles, Jaehong Park

National Renewable Energy Laboratory

Research output: Contribution to journal › Article

24 Citations (Scopus)

Abstract

Ultrafast photoinduced electron transfer (PIET) dynamics of a C₇₀-encapsulated bisporphyrin covalent organic polyhedron hybrid (C₇₀@COP-5) is studied in a nonpolar toluene medium with fluorescence and transient absorption spectroscopies. This structurally rigid donor (D)-acceptor (A) molecular hybrid offers a new platform featuring conformationally predetermined cofacial D-A orientation with a fixed edge-to-edge separation, R_EE (2.8 Å), without the aid of covalent bonds. Sub-picosecond PIET (τ_ET ≤ 0.4 ps) and very slow charge recombination (τ_CR ≈ 600 ps) dynamics are observed. The origin of these dynamics is discussed in terms of enhanced D-A coupling (V = 675 cm^-1) and extremely small reorganization energy (λ ≈ 0.18 eV), induced by the intrinsic structural rigidity of the C₇₀@COP-5 complex.

Original language	English
Pages (from-to)	4286-4289
Number of pages	4
Journal	Journal of the American Chemical Society
Volume	139
Issue number	12
DOIs	https://doi.org/10.1021/jacs.7b00220
Publication status	Published - Mar 29 2017

ASJC Scopus subject areas

Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry

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Ortiz, M., Cho, S., Niklas, J., Kim, S., Poluektov, O. G., Zhang, W., Rumbles, G., & Park, J. (2017). Through-Space Ultrafast Photoinduced Electron Transfer Dynamics of a C₇₀-Encapsulated Bisporphyrin Covalent Organic Polyhedron in a Low-Dielectric Medium. Journal of the American Chemical Society, 139(12), 4286-4289. https://doi.org/10.1021/jacs.7b00220

Through-Space Ultrafast Photoinduced Electron Transfer Dynamics of a C₇₀-Encapsulated Bisporphyrin Covalent Organic Polyhedron in a Low-Dielectric Medium. / Ortiz, Michael; Cho, Sung; Niklas, Jens; Kim, Seonah; Poluektov, Oleg G.; Zhang, Wei; Rumbles, Garry; Park, Jaehong.

In: Journal of the American Chemical Society, Vol. 139, No. 12, 29.03.2017, p. 4286-4289.

Research output: Contribution to journal › Article

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abstract = "Ultrafast photoinduced electron transfer (PIET) dynamics of a C70-encapsulated bisporphyrin covalent organic polyhedron hybrid (C70@COP-5) is studied in a nonpolar toluene medium with fluorescence and transient absorption spectroscopies. This structurally rigid donor (D)-acceptor (A) molecular hybrid offers a new platform featuring conformationally predetermined cofacial D-A orientation with a fixed edge-to-edge separation, REE (2.8 {\AA}), without the aid of covalent bonds. Sub-picosecond PIET (τET ≤ 0.4 ps) and very slow charge recombination (τCR ≈ 600 ps) dynamics are observed. The origin of these dynamics is discussed in terms of enhanced D-A coupling (V = 675 cm-1) and extremely small reorganization energy (λ ≈ 0.18 eV), induced by the intrinsic structural rigidity of the C70@COP-5 complex.",

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