Supramolecular polymers (SPs) have received great attention because of their potential for various practical applications. As part of our search for SPs that are highly fluorescent in aqueous media, we designed a system based on a cucurbit[8]uril (CB[8]) host and a newly designed cyanostilbene guest. Fluorescence quantum yields of ≈0 % in the disassembled monomer state and 91 % in the CB[8]-induced SP state were obtained. The intriguing photophysical properties of the SP are elucidated through detailed experimental and computational analysis, paving the way towards a fascinating class of water-soluble fluorescent SPs.
A novel system of light-harvesting supramolecular block copolymers (SBCPs) in water is demonstrated. To realize cucurbit[8]uril (CB[8])-based SBCPs generating artificial light-harvesting in water, finely color-tuned supramolecular homopolymers (SHPs) comprising CB[8] host and different cyanostilbene guests (named as B, G, Y, and R) emitting blue, green, yellow, and red fluorescence are first synthesized and characterized, respectively. Light-harvesting SBCPs with mixed guest emitters are then simply produced by mixing blue and red-emitting SHPs according to the dynamic host-guest exchange interaction. The light-harvesting SBCPs show highly efficient energy transfer from B (donor D) to R (acceptor A) attributed to the D/A proximity and parallel orientation of their transition dipoles secured in the block copolymer structure. It is comprehensively shown that cyanostilbene/CB[8]-based fluorescent SBCPs represent a novel and fascinating class of eco-friendly artificial light-harvesting system.
Highly efficient red-green-blue (RGB) tricolor luminescence switching was demonstrated in a bicomponent solid film consisting of (2Z,2'Z)-2,2'-(1,4-phenylene)bis(3-(4-butoxyphenyl)acrylonitrile) (DBDCS) and (2Z,2'Z)-3,3'-(2,5-bis(6-(9H-carbazol-9-yl)hexyloxy)-1,4-phenylene)bis(2-(3,5-bis(trifluoromethyl)phenyl)acrylonitrile) (m-BHCDCS). Reversible RGB luminescence switching with a high ratiometric color contrast (λ(em)=594, 527, 458 nm for red, green, and blue, respectively) was realized by different external stimuli such as heat, solvent vapor exposure, and mechanical force. It was shown that Förster resonance energy transfer in the bicomponent mixture could be efficiently switched on and off through supramolecular control.
Highlights d The cryo-EM analysis on normal (Q23) and disease (Q78) HTT are described d The polyQ expansion alters the relative movement of HTT domains d The polyQ expansion at N terminus alters the global phosphorylation pattern of HTT d Ser2116 phosphorylation affects the global structure and function of HTT
Organic photodetectors (OPDs) exhibit superior spectral responses but slower photoresponse times compared to inorganic counterparts. Herein, we study the light-intensity-dependent OPD photoresponse time with two small-molecule donors (planar MPTA or twisted NP-SA) co-evaporated with C60 acceptors. MPTA:C60 exhibits the fastest response time at high-light intensities (>0.5 mW/cm2), attributed to its planar structure favoring strong intermolecular interactions. However, this blend exhibits the slowest response at low-light intensities, which is correlated with biphasic photocurrent transients indicative of the presence of a low density of deep trap states. Optical, structural, and energetical analyses indicate that MPTA molecular packing is strongly disrupted by C60, resulting in a larger (370 meV) HOMO level shift. This results in greater energetic inhomogeneity including possible MPTA-C60 adduct formation, leading to deep trap states which limit the low-light photoresponse time. This work provides important insights into the small molecule design rules critical for low charge-trapping and high-speed OPD applications.
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