Abstract Two‐dimensional transition metal dichalcogenides (TMDs)/graphene van der Waals (vdW) heterostructures integrate the superior light–solid interaction in TMDs and charge mobility in graphene, and therefore are promising for surface‐enhanced Raman spectroscopy (SERS). Herein, a novel TMD (MoS2and WS2) nanodome/graphene vdW heterostructure SERS substrate, on which an extraordinary SERS sensitivity is achieved, is reported. Using fluorescent Rhodamine 6G (R6G) as probe molecules, the SERS sensitivity is in the range of 10−11to 10−12mon the TMD nanodomes/graphene vdW heterostructure substrates using 532 nm Raman excitation, which is comparable to the best sensitivity reported so far using plasmonic metal nanostructures/graphene SERS substrates, and is more than three orders of magnitude higher than that on single‐layer TMD and graphene substrates. Density functional theory simulation reveals enhanced electric dipole moments and dipole–dipole interaction at the TMD/graphene vdW interface, yielding an effective means to facilitate an external electrostatic perturbation on the graphene surface and charge transfer. This not only promotes chemical enhancement on SERS, but also enables electromagnetic enhancement of SERS through the excitation of localized surface plasmonic resonance on the TMD nanodomes. This TMD nanodome/graphene vdW heterostructure is therefore promising for commercial applications in high‐performance optoelectronics and sensing. 
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                            Enhanced Photoresponse in Intermingled WS 2 and MoS 2 Nanodiscs on Graphene Heterostructure Nanohybrids
                        
                    
    
            Abstract Nanohybrids based on van der Waals (vdW) heterostructures of two dimensional (2D) atomic materials have recently emerged as a unique scheme for designing high‐performance quantum sensors. This work explores vdW nanohybrids for photodetection, which consist of graphene decorated with intermingled transition‐metal dichalcogenide (TMDC) nanodiscs (TMDC‐NDs) obtained using wafer‐size, layer‐by‐layer growth. The obtained TMDC‐NDs/graphene nanohybrids take advantage of strong quantum confinement in graphene for high charge mobility and hence high photoconductive gain, and localized surface plasmonic resonance (LSPR) enabled on the TMDC‐NDs for enhanced light absorption. Since the LSPR depends on the nanostructure's size and density, intermingled TMDC‐NDs of different kinds of TMDCs, such as WS2(W) and MoS2(M), have been found to allow small‐size, high‐concentration TMDC‐NDs to be achieved for high photoresponse. Remarkably, high photoresponsivity up to 31 A/W (550 nm wavelength and 20 µW cm−2light intensity) has been obtained on the WMW‐NDs/graphene nanohybrids photodetectors made using three consecutive coatings of WS2(1st and 3rd coating) and MoS2(2nd coating), which is considerably higher by a factor of ≈4 than that of the counterparts MoS2‐ND/graphene or WS2‐NDs/graphene devices. This result provides a facile approach to control the size and concentration of the TMDC‐NDs for high‐performance, low‐cost optoelectronic device applications. 
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                            - PAR ID:
- 10641362
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials Interfaces
- Volume:
- 12
- Issue:
- 13
- ISSN:
- 2196-7350
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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