The device's integration of molecular electronics is limited regarding the large-scale fabrication of gap electrodes on a molecular scale. The van der Waals integration (vdWI) of a vertically aligned molecular layer (0D) with 2D or 3D electrodes indicates the possibility of device's integration; however, the active junction area of 0D-2D and 0D-3D vdWIs remains at a microscale size. Here, we introduce the robust fabrication of a vertical 1D-0D-1D vdWI device with the ultra-small junction area of 1 nm2 achieved by cross-stacking top carbon nanotubes (CNTs) on molecularly assembled bottom CNTs. 1D-0D-1D vdWI memories are demonstrated through ferroelectric switching of azobenzene molecules owing to the cis-trans transformation combined with the permanent dipole moment of the end-tail -CF3 group. In this work, our 1D-0D-1D vdWI memory exhibits a retention performance above 2000 s, over 300 cycles with an on/off ratio of approximately 105 and record current density (3.4 × 108 A/cm2), which is 100 times higher than previous study through the smallest junction area achieved in a vdWI. The simple stacking of aligned CNTs (4 × 4) allows integration of memory arrays (16 junctions) with high device operational yield (100%), offering integration guidelines for future molecular electronics.
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