Chiral two-dimensional MoS2 by molecular functionalization as ultra-sensitive detectors for circularly polarized light

Abstract: Inducing chirality in optically and electronically active materials is interesting for applications in sensing and quantum information transmission. Two-dimensional (2D) transition metal chalcogenides (TMDs) possess excellent electronic and optical properties but are achiral. Here we demonstrate chirality induction in atomically thin layers of 2D MoS2 by functionalization with chiral thiol molecules. Analysis of X-ray absorption near-edge structure and Raman optical activity with circularly polarized excitation suggest chemical and electronic interactions that leads chirality transfer from the molecules to the MoS2. We confirm chirality induction in 2D MoS2 with circular dichroism measurements that show absorption bands at wavelengths of 380-520 nm and 520-600 nm with giant molar ellipticity of 10^8 deg cm2/dmol 2-3 orders of magnitude higher than 3D chiral materials. Phototransistors fabricated from atomically thin chiral MoS2 for detection of circularly polarized light exhibit responsivity of >10^2 A/W and maximum anisotropy g-factor of 1.98 close to the theoretical maximum of 2.0, which indicates that the chiral states of photons are fully distinguishable by the photodetectors. Our results demonstrate that it is possible achieve chirality induction in monolayer MoS2 by molecular functionalization and realise ultra-sensitive detectors for circularly polarized photons.