Beschreibung:
<jats:title>Abstract</jats:title><jats:p>The design and synthesis of a new molecular tweezer (<jats:bold>T‐tmp</jats:bold>) with electron‐rich pincers are reported. The stable monocationic radicals and self‐assembled dimeric radicals of this molecular tweezer platform were prepared by chemical oxidative titration. With the aid of DFT calculations, it was found that the dimeric radicals with <jats:italic>syn</jats:italic>‐<jats:italic>syn</jats:italic>‐<jats:italic>syn</jats:italic> conformer has the most stable structure, with the hole primarily delocalized between parallel stacked pyrenyl groups.</jats:p>