Unraveling electronic structure of GeS through ARPES and its correlation with anisotropic optical and transport behavior

Abstract: Two-dimensional (2D) van der Waals (vdW) materials with lower symmetry (triclinic, monoclinic or orthorhombic) exhibit intrinsic anisotropic in-plane structure desirable for future optoelectronic surface operating devices. Herein, we report one such material, 2D $p$-type semiconductor germanium sulfide (GeS), a group IV monochalcogenide with puckered orthorhombic morphology, in which in-plane optical and transport properties can be correlated with its electronic structure. We systematically investigate the electronic band structure of the bulk GeS with micro-focused angle-resolved photoemission spectroscopy ($\mu$-ARPES) and correspond the charge transport properties using the field-effect transistor (FET) device architecture, and optical anisotropy $via$ angle-resolved polarization dependent Raman spectroscopy (ARPRS) on a micron-sized rectangle-shaped exfoliated bulk flake. The experimental valence band dispersion along the two high symmetry directions indicate highly anisotropic in-plane behavior of the charge carrier that agrees well with the density functional theory (DFT) calculations. In addition, we demonstrate the variation of the in-plane hole mobility (ratio $\sim$ 3.4) from the electrical conductivity with gate-sweep in a GeS-on-SiO$_2$ FET. Moreover, we use the angle-resolved fluctuation of the Raman intensity of the characteristic phonon modes to precisely determine the armchair and zigzag edges of the particular flake. The unique structural motif of GeS with correlated electronic and optical properties are of great interest both for the physical understanding of the all-optical switch and their applications in memory devices.