TY - JOUR
T1 - Inter-Backbone Charge Transfer as Prerequisite for Long-Range Conductivity in Perylene Bisimide Hydrogels
AU - Burian, Max
AU - Rigodanza, Francesco
AU - Demitri, Nicola
AU - D Ord Ević, Luka
AU - Marchesan, Silvia
AU - Steinhartova, Tereza
AU - Letofsky-Papst, Ilse
AU - Khalakhan, Ivan
AU - Mourad, Eléonore
AU - Freunberger, Stefan A
AU - Amenitsch, Heinz
AU - Prato, Maurizio
AU - Syrgiannis, Zois
PY - 2018/6/11
Y1 - 2018/6/11
N2 - Hydrogelation, the self-assembly of molecules into soft, water-loaded networks, is one way to bridge the structural gap between single molecules and functional materials. The potential of hydrogels, such as those based on perylene bisimides, lies in their chemical, physical, optical, and electronic properties, which are governed by the supramolecular structure of the gel. However, the structural motifs and their precise role for long-range conductivity are yet to be explored. Here, we present a comprehensive structural picture of a perylene bisimide hydrogel, suggesting that its long-range conductivity is limited by charge transfer between electronic backbones. We reveal nanocrystalline ribbon-like structures as the electronic and structural backbone units between which charge transfer is mediated by polar solvent bridges. We exemplify this effect with sensing, where exposure to polar vapor enhances conductivity by 5 orders of magnitude, emphasizing the crucial role of the interplay between structural motif and surrounding medium for the rational design of devices based on nanocrystalline hydrogels.
AB - Hydrogelation, the self-assembly of molecules into soft, water-loaded networks, is one way to bridge the structural gap between single molecules and functional materials. The potential of hydrogels, such as those based on perylene bisimides, lies in their chemical, physical, optical, and electronic properties, which are governed by the supramolecular structure of the gel. However, the structural motifs and their precise role for long-range conductivity are yet to be explored. Here, we present a comprehensive structural picture of a perylene bisimide hydrogel, suggesting that its long-range conductivity is limited by charge transfer between electronic backbones. We reveal nanocrystalline ribbon-like structures as the electronic and structural backbone units between which charge transfer is mediated by polar solvent bridges. We exemplify this effect with sensing, where exposure to polar vapor enhances conductivity by 5 orders of magnitude, emphasizing the crucial role of the interplay between structural motif and surrounding medium for the rational design of devices based on nanocrystalline hydrogels.
KW - Journal Article
U2 - 10.1021/acsnano.8b01689
DO - 10.1021/acsnano.8b01689
M3 - Article
C2 - 29869880
SN - 1936-0851
VL - 12
SP - 5800
EP - 5806
JO - ACS Nano
JF - ACS Nano
IS - 6
ER -