Fig. 1: Chemical structures of NDITTF-MF and NDITTF-SHe and their synthetic approaches.

Conductance measurements. We firstly probe the electronic transport properties of the four carboxylic acid methyl ester groups terminated TTF molecule (NDITTF-MF, see Fig. 1) using the scanning tunneling microscope-break junction (STM-BJ) technique (Fig. 2a), which can measure single-molecule conductance at room temperature in ambient environment8,30. Briefly, we repeatably drive a gold STM tip in and out of contact with a gold substrate in 1,2,4-trichlorobenzene (TCB) solution of NDITTF-MF molecule (0.01–0.1 mM). After the Au–Au point contact is broken, the molecule can bridge the two electrodes and form a single-molecule junction. We measure the conductance as a function of the tip-substrate displacement during this process. The inset of Fig. 2b shows sample conductance traces of NDITTF-MF measured at an applied tip bias of 0.5 V. A clear conductance plateau appears at ~10−2 G0 (where G0 = 2e2/h is the quantum of conductance), indicating the formation of single-molecule junctions of NDITTF-MF.