Strong optoelectronic response in the binary van der Waals heterostructures of graphene and transition metal dichalcogenides (TMDCs) is an emerging route towards high-sensitivity light sensing. While the high sensitivity is an effect of photogating of graphene due to inter-layer transfer of photo-excited carriers, the impact of intrinisic defects, such as traps and mid-gap states in the chalcogen layer remain largely unexplored. Here we employ graphene/hBN (hexagonal boron nitride)/MoS 2 (molybdenum disulphide) trilayer heterostructures to explore the photogating mechanism, where the hBN layer acts as interfacial barrier to tune the charge transfer timescale. We find two new features in the photoresponse: First, an unexpected positive component in photoconductance upon illumination at short times that preceeds the conventional negative photoconductance due to charge transfer, and second, a strong negative photoresponse at infrared wavelengths (up to 1720 nm) well-below the band gap of single layer MoS 2 . Detailed time and gate voltage-dependence of the photoconductance indicates optically-driven charging of trap states as possible origin of these observations. The responsivity of the trilayer structure in the infrared regime was found to be extremely large (> 10 8 A/W at 1550 nm using 20 mV source drain bias at 180 K temperature and ≈ − 30 V back gate voltage). Our experiment demonstrates that interface engineering in the optically sensitive van der Waals heterostructures may cast crucial insight onto both inter-and intra-layer charge reorganization processes in graphene/TMDC heterostructures.
The fundamental origin of low-frequency noise in graphene field effect transistors (GFETs) has been widely explored but a generic engineering strategy towards low noise GFETs is lacking.
The transfer of charge carriers across the optically excited hetero-interface of graphene and semiconducting transition metal dichalcogenides (TMDCs) is the key to convert light to electricity, although the intermediate steps from the creation of excitons in TMDC to the collection of free carriers in the graphene layer are not fully understood. Here, we investigate photo-induced charge transport across graphene–MoS2 and graphene–WSe2 hetero-interfaces using time-dependent photoresistance relaxation with varying temperature, wavelength, and gate voltage. In both types of heterostructures, we observe an unprecedented resonance in the inter-layer charge transfer rate as the Fermi energy ( E F) of the graphene layer is tuned externally with a global back gate. We attribute this to a resonant quantum tunneling from the excitonic state of the TMDC to E F of the graphene layer and outline a new method to estimate the excitonic binding energies ( E b) in the TMDCs, which are found to be 400 meV and 460 meV in MoS2 and WSe2 layers, respectively. The gate tunability of the inter-layer charge transfer timescales may allow precise engineering and readout of the optically excited electronic states at graphene–TMDC interfaces.
Binary van der Waals heterostructures of graphene (Gr) and transition metal dichalcogenide (TMDC) have evolved as a promising candidate for photodetection with very high responsivity due to the separation of photo‐excited electron–hole pairs across the interface. The spectral range of optoelectronic response in such hybrids has so far been limited by the optical bandgap of the light absorbing TMDC layer. Here, the bidirectionality of interlayer charge transfer is utilized for detecting sub‐band gap photons in Gr‐TMDC heterostructures. A Gr/MoSe2 heterostructure sequentially driven by visible and near infra‐red (NIR) photons is employed, to demonstrate that NIR induced back transfer of charge allows fast and repeatable detection of the low energy photons (less than the optical band gap of the TMDC layer). This mechanism provides photoresponsivity as high as ≈3000 A W−1 close to the communication wavelength. The experiment provides a new strategy for achieving highly efficient photodetection over a broad range of energies beyond the spectral bandgap with the 2D semiconductor family.
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