Abstract
AbstractSingle‐molecule junctions exploit the internal structure of molecular orbitals to construct a new class of functional quantum devices. The demonstration of negative differential resistance (NDR) in single‐molecule junctions is direct evidence of quantum mechanical tunneling through a molecular orbital. Here, a pronounced NDR effect is reported with a peak‐to‐valley ratio of 30.1 on a single‐molecule junction of π‐conjugated quinoidal‐fused oligosilole derivatives, Si2 × 2, embedded between the unique electroless gold‐plated heteroepitaxial spherical Au/Pt nanogap electrodes. This NDR feature persists in a consecutive endurance test of 180 current traces. the thermally stable NDR effects in the Si2 × 2 single‐molecule junctions between 9 and 300 K are demonstrated. The density functional theory calculations under electric fields indicate that the NDR effect can be ascribed to the bias‐dependent resonant tunneling transport via the polarized HOMO, which has asymmetrically changed electrode coupling with increased bias voltages. The results confirm a promising electrical platform for constructing functional quantum devices at the single‐molecule level.
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