Leitend verbunden: Eine zentrale Tetrathiafulvalen(TTF)‐Einheit vermittelt im abgebildeten Dichinon‐Tetrathiafulvalen effektiv die elektronische Kopplung zwischen den Chinonfunktionen in der Peripherie. Es erfolgt schrittweise Einelektronenreduktion; die Potentialdifferenz zwischen den Reduktionsschritten zeigt, dass die Reduktion der zweiten Chinoneinheit durch das Vorliegen einer Radikalanionspezies auf der anderen Seite der TTF‐Brücke beeinflusst wird.

Intramolecular electron-transfer phenomena in the radical anions derived from the partial reduction of diradicals (E,E)-p-divinylbenzene-beta,beta'-ylene bis(4-tetradecachlorotriphenylmethyl) diradical (1) and (E,E)-m-divinylbenzene-beta,beta'-ylene bis(4-tetradecachlorotriphenylmethyl) diradical (2) have been studied by optical and ESR spectroscopy. The synthetic methodology used allows for complete control of the geometry of diradicals 1 and 2, which have para and meta topologies, respectively, as well as of their E/Z isomerism. This fact is used to show the influence of the different topologies on the ease of electron transfer, which is larger for the para than for the meta isomer, in which a small or negligible electronic coupling is observed. A related monoradical compound (E)-bis(pentachlorophenyl)[4-(4-bromophenyl-beta-styryl)-2,3,5,6-tetrachlorophenyl]-methyl radical (3), which has only one such redox site, has also been obtained and studied for comparison purposes.

Dotierte Drähte: Die Organisation der π‐Einheiten von amidfunktionalisiertem Tetrathiafulvalen in einem Gel durch Wasserstoffbrücken führt zur Bildung von Nanofasern. Dotieren mit Iod erzeugt ein leitfähiges Material, das durch Tempern in Nanodrähte mit metallartiger Leitfähigkeit übergeht (siehe Rasterkraftmikroskopiebild).

The synthesis and study of structural and electronic properties of mono-ferrocenyl π-conjugated complexes 5a-d, whose electronic characteristics have been systematically varied by introducing an electron-donating or electron-withdrawing substituent either at the 1-position or at the 4-position of the 2-aza-1,3-butadiene moiety linked to the ferrocenyl unit, are presented. The structural and electronic properties of the homobimetallic complex 5f, with two ferrocene units linked through the asymmetric and oxidizable 2-aza-1,3-butadiene bridge, is also reported. The crystal structures of complexes 5b, 5d, and 5f show a large degree of conjugation in this family of compounds. Complexes 5 show a rich electrochemical behavior due both to the oxidation of ferrocenyl units and the 2-aza-1,3-butadiene bridge, as revealed by cyclic voltammetry. Radical cations 5 +· were prepared from 5 by coulomet-

A new quasi‐2D molecular conductorbased on BEDT‐TTF with an assembly of the trihalide anions I2Br–, IBr2–, and BrICl– is presented here. This set of anions promotes the formation of α′‐ and α‴‐type conducting layers (see Figure, top) along with a low‐temperature α‴→β″ transition seen for the first time in BEDT‐TTF salts.