Solvent independent symmetry-breaking charge separation in terrylenediimide guanine-quadruplex nanoparticles

Powers-Riggs, Natalia E.; Zuo, Xiaobing; Young, Ryan M.; Wasielewski, Michael R.

doi:10.1063/5.0027471

Title: Solvent independent symmetry-breaking charge separation in terrylenediimide guanine-quadruplex nanoparticles

Journal Article · Sat Nov 28 00:00:00 EST 2020 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0027471· OSTI ID:1797959

^[1]; Zuo, Xiaobing ^[2];

^[1];

^[1]

Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)

G-quadruplex assemblies are a promising tool for self-assembling π-stacked chromophore arrays to better understand their photophysics. We have shown that coupling a single guanine moiety to terrylenediimide (TDI) produces a structure (GTDI) that self-assembles in tetrahydrofuran (THF) into a nearly monodisperse guanine-quadruplex structure having 16 π-stacked layers (GTDI₄)₁₆. The TDI surfaces were determined to have a high degree of cofacial overlap and underwent quantitative symmetry-breaking charge separation (SB-CS) upon photoexcitation. Here, we more deeply examine the relationship between solvent and aggregate formation and develop insights into structure–function relationships over a variety of solvent polarities and hydrogen-bonding capabilities. At high concentrations, GTDI assembles into guanine-quadruplex structures (GTDI₄)₁₆ in THF and toluene, as well as (GTDI₄)₉ in pyridine and benzonitrile. Here, transient absorption spectroscopy shows that SB-CS occurs in all solvents, regardless of their static dielectric constants, but the SB-CS yield is determined by structure. Solvent polarity independent SB-CS generation is also observed in GTDI films, where there is a complete absence of solvent.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); NSF Graduate Research Fellowship

Grant/Contract Number:: AC02-06CH11357; DGE-1324585; FG02-99ER14999, DE-AC02-06CH11357

OSTI ID:: 1797959

Alternate ID(s):: OSTI ID: 1970602

Journal Information:: Journal of Chemical Physics, Vol. 153, Issue 20; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
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Transient-absorption spectroscopy
G-quadruplex
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Title: Solvent independent symmetry-breaking charge separation in terrylenediimide guanine-quadruplex nanoparticles

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