Phase-Engineering-Induced Generation and Control of Highly Anisotropic and Robust Excitons in Few-Layer ReS₂

The anisotropic exciton behavior in two-dimensional materials induced by spin–orbit coupling or anisotropic spatial confinement has been exploited in imaging applications. Herein, we propose a new strategy to generate high-energy and robust anisotropic excitons in few-layer ReS₂ nanosheets by phase engineering. This approach overcomes the limitation imposed by the layer thickness, enabling production of visible polarized photoluminescence at room temperature. Ultrasonic chemical exfoliation is implemented to introduce the metallic T phase of ReS₂ into the few-layer semiconducting Td nanosheets. In this configuration, light excitation can readily produce “hot” electrons to tunnel to the Td phase via the metal–​semiconductor interface to enhance the overlap between the wave functions and screened Coulomb interactions. Owing to the strong electron–hole interaction, significant increase in the optical band gap is observed. Highly anisotropic and tightly bound excitons with visible light emission (1.5–2.25 eV) are produced and can be controlled by tailoring the T phase concentration. This novel strategy allows manipulation of polarized optical information and has great potential in optoelectronic devices.