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The nonzero interlayer Schottky barrier leads to a compromise between photodetectivity and photoresponsivity in photodiodes based on vdW heterojunctions. Seeking for the appropriate vdW heterojunction with Ohmic contact and a high tunneling barrier is of great significance to realize highperformance photodiodes. We built borophene/C4N4 (B/C4N4) vdW heterojunctions with a reduced interlayer Schottky barrier, by combining density functional theory and non-equilibrium Green’s function. The adsorption of Li-ions can further tune its Schottky contact into n-type Ohmic contact. The electronic properties of the Li-ion-adsorbed B/C4N4 vdW heterojunction, including the separation of hole–electron pairs, the work function, as well as the effective mass of carrier, can be modulated by changing the adsorption site of Li-ions. B/C4N4/Li shows the most excellent absorbing capability of the infrared illumination and the strongest negative rectification, due to the highest interlayer tunneling barrier. The bottom surface of the C4N4 sublayer is the optimal adsorption site of Li-ions, for the potential application of B/C4N4 vdW heterojunctions in tunneling photodiodes. Our work unveils the great significance of Li-ion adsorption in modulating the interlayer Schottky and tunneling barriers in vdW heterojunctions, thus improving their device performance.

journal of materials chemistry. c

Elimination of interlayer Schottky barrier in borophene/C4N4 vdW heterojunctions via Li-ion adsorption for tunneling photodiodes