Photophysical Dynamics in Semiconducting Graphene Quantum Dots Integrated with 2D MoS for Optical Enhancement in the Near UV.

The hybrid structure of zero-dimensional (0D) graphene quantum dots (GQDs) and semiconducting two-dimensional (2D) MoS has been investigated, which exhibit outstanding properties for optoelectronic devices surpassing the limitations of MoS photodetectors where the GQDs extend the optical absorption into the near-UV regime. The GQDs and MoS films are characterized by Raman and photoluminescence (PL) spectroscopies, along with atomic force microscopy. After outlining the fabrication of our 0D-2D heterostructure photodetectors comprising GQDs with bulk MoS sheets, their photoresponse to the incoming radiation was measured. The hybrid GQD/MoS heterostructure photodetector exhibits a high photoresponsivity of more than 1200 A W at 0.64 mW/cm at room temperature . The -dependent optoelectronic measurements revealed a peak of ∼544 A W at 245 K, examined from 5.4 K up to 305 K with an incoming white light power density of 3.2 mW/cm. A tunable laser revealed the photocurrent to be maximal at lower wavelengths in the near ultraviolet (UV) over the 400-1100 nm spectral range, where the of the hybrid GQDs/MoS was ∼775 A W, while a value of 2.33 × 10 Jones was computed for the detectivity * at 400 nm. The external quantum efficiency was measured to be ∼99.8% at 650 nm, which increased to 241% when the wavelength of the incoming laser was reduced to 400 nm. Time-resolved measurements of the photocurrent for the hybrid devices resulted in a rise time τ and a fall time τ of ∼7 and ∼25 ms, respectively, at room , which are 10× lower compared to previous reports. From our promising results, we conclude that the GQDs exhibit a sizable band gap upon optical excitation, where photocarriers are injected into the MoS films, endowing the hybrids with long carrier lifetimes to enable efficient light absorption beyond the visible and into the near-UV regime. The GQD-MoS structure is thus an enabling platform for high-performance photodetectors, optoelectronic circuits, and quantum devices.