Layer Number Dependence of MoS₂ Photoconductivity Using Photocurrent Spectral Atomic Force Microscopic Imaging

Atomically thin MoS₂ is of great interest for electronic and optoelectronic applications because of its unique two-dimensional (2D) quantum confinement; however, the scaling of optoelectronic properties of MoS₂ and its junctions with metals as a function of layer number as well the spatial variation of these properties remain unaddressed. In this work, we use photocurrent spectral atomic force microscopy (PCS-AFM) to image the current (in the dark) and photocurrent (under illumination) generated between a biased PtIr tip and MoS₂ nanosheets with thickness ranging between <i>n</i> = 1 to 20 layers. Dark current measurements in both forward and reverse bias reveal characteristic diode behavior well-described by Fowler–Nordheim tunneling with a monolayer barrier energy of 0.61 eV and an effective barrier scaling linearly with layer number. Under illumination at 600 nm, the photocurrent response shows a marked decrease for layers up to <i>n</i> = 4 but increasing thereafter, which we describe using a model that accounts for the linear barrier increase at low <i>n</i>, but increased light absorption at larger <i>n</i> creating a minimum at <i>n</i> = 4. Comparative 2D Fourier analysis of physical height and photocurrent images shows high spatial frequency spatial variations in substrate/MoS₂ contact that exceed the frequencies imposed by the underlying substrates. These results should aid in the design and understanding of optoelectronic devices based on quantum confined atomically thin MoS<sub>2