TY - JOUR
T1 - High Molecular Conductance and Inverted Conductance Decay over 3 nm in Aminium-Terminated Carbon-Bridged Oligophenylene-Vinylenes
AU - Rieger, Luisa K. I.
AU - Leitherer, Susanne
AU - Bro-Jo̷rgensen, William
AU - Solomon, Gemma C.
AU - Winter, Rainer F.
PY - 2025
Y1 - 2025
N2 - With the progressing miniaturization of electronic device components to improve circuit density while retaining or even reducing spatial requirements, single molecules employed as electric components define the lower limit of accessible structural width. To circumvent the typical exponential conductance decay for increasing length in molecule-based wires, topological states, which describe the occurrence of discontinuities of a bulk material’s electronic structure confined to its surface, can be realized for molecules by the introduction of unpaired spins at the molecular termini. The resulting high conductance and reversed conductance decay are typically only observed for shorter molecules, as the terminal spins must be within the electronic coupling range to produce the desired effects. We expand the realm of long and exceptionally conductive molecular wires by employing highly conjugated, planarized carbon-bridged oligo(phenylene-vinylene)s as conduits between readily oxidizable diarylamine termini. This yields molecular wires of already decent conductance values and small conductance decay in the neutral state. Upon the introduction of topological states, the conductance can be increased by a factor of up to 1800 for a 3 nm long molecule, and the conductance decay becomes inverted, together with an excellent signal intensity at concentrations as low as 0.01 mM.
AB - With the progressing miniaturization of electronic device components to improve circuit density while retaining or even reducing spatial requirements, single molecules employed as electric components define the lower limit of accessible structural width. To circumvent the typical exponential conductance decay for increasing length in molecule-based wires, topological states, which describe the occurrence of discontinuities of a bulk material’s electronic structure confined to its surface, can be realized for molecules by the introduction of unpaired spins at the molecular termini. The resulting high conductance and reversed conductance decay are typically only observed for shorter molecules, as the terminal spins must be within the electronic coupling range to produce the desired effects. We expand the realm of long and exceptionally conductive molecular wires by employing highly conjugated, planarized carbon-bridged oligo(phenylene-vinylene)s as conduits between readily oxidizable diarylamine termini. This yields molecular wires of already decent conductance values and small conductance decay in the neutral state. Upon the introduction of topological states, the conductance can be increased by a factor of up to 1800 for a 3 nm long molecule, and the conductance decay becomes inverted, together with an excellent signal intensity at concentrations as low as 0.01 mM.
U2 - 10.1021/jacs.4c13901
DO - 10.1021/jacs.4c13901
M3 - Journal article
C2 - 39704545
VL - 147
SP - 957
EP - 964
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 1
ER -