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 n = 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 n = 4 but increasing thereafter, which we describe using a model that accounts for the linear barrier increase at low n, but increased light absorption at larger n creating a minimum at n = 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 MoS₂.