Investigation of a bacteriochlorin-containing pentad array for panchromatic light-harvesting and charge separation

Jing, Haoyu; Magdaong, Nikki Cecil M.; Diers, James R.; Kirmaier, Christine; Bocian, David F.; Holten, Dewey; Lindsey, Jonathan S.

doi:10.1039/d2cp05400k

Title: Investigation of a bacteriochlorin-containing pentad array for panchromatic light-harvesting and charge separation

Journal Article · Wed Jan 04 00:00:00 EST 2023 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/d2cp05400k· OSTI ID:2263524

Jing, Haoyu ^[1];

^[2]; Diers, James R. ^[3];

^[2]; Bocian, David F. ^[3];

^[2];

^[1]

North Carolina State University, Raleigh, NC (United States)
Washington University, St. Louis, MO (United States)
University of California, Riverside, CA (United States)

A new pentad array designed to exhibit panchromatic absorption and charge separation has been synthesized and characterized. The array is composed of a triad panchromatic absorber (a bis(perylene-monoimide)-porphyrin) to which are appended an electron acceptor (perylene-diimide) and an electron donor/hole acceptor (bacteriochlorin) in a crossbar arrangement. The motivation for incorporation of the bacteriochlorin versus a free-base or zinc chlorin utilized in prior constructs was to facilitate hole transfer to this terminal unit and thereby achieve a higher yield of charge separation across the array. The intense S₀ → S₁ (Q_y) band of the bacteriochlorin also enhances absorption in the near-infrared spectral region. Due to synthetic constraints, a phenylethyne linker was used to join the bacteriochlorin to the core porphyrin of the panchromatic triad rather than the diphenylethyne linker employed for the prior chlorin-containing pentads. Static and time-resolved photophysical studies reveal enhanced excited-state quenching for the pentad in benzonitrile and dimethyl sulfoxide compared to the prior chlorin-containing analogues. Success was only partial, however, as a long-lived charge separated state was not observed despite the improved energetics for the final ground-state hole/electron-shift reaction. The apparent reason is more facile competing charge-recombination due to the shorter bacteriochlorin – porphyrin linker that increases electronic coupling for this process. Furthermore, the studies highlight design criteria for balancing panchromatic absorption and long-lived charge separation in molecular architectures for solar-energy conversion.

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Research Organization:: Washington Univ., St. Louis, MO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE

Grant/Contract Number:: FG02-05ER15661; DEFG02- 05ER15661

OSTI ID:: 2263524

Alternate ID(s):: OSTI ID: 1907913

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Vol. 25, Issue 3; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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