Abstract
The layered transition metal dichalcogenides (TMDs) exhibit the intriguing physical properties and potential application in novel electronic devices. However, controllable growth of multilayer TMDs remains challenging. Herein, large-scale and high-quality multilayer prototype TMDs of W(Mo)Se2 were synthesized via chemical vapor deposition. For Raman and PL measurements, 2H and 3R multilayer WSe2 crystals displayed significant layer-dependent peak position and intensity feature. Besides, different from the oscillatory relationship of SHG intensity for odd-even layer numbers in 2H-stacked multilayer WSe2, the second harmonic generation intensity of 3R-stacked ones parabolically increased with the thickness due to the absence of inversion symmetry. For device application, photodetectors based on WSe2 with increasing thickness exhibited p-type (bilayer), ambipolar (trilayer), and n-type (4 layers) semiconductor behaviors, respectively. Furthermore, photodetectors based on the as-synthesized 3R-stacked WSe2 flakes displayed an excellent responsivity (R) of 7.8×103 mA/W, high specific detectivity (Da*) of 1.7×1014 Jones, outstanding external quantum efficiency (EQE) of 8.6×102 %, and fast response time (τRise=57 ms and τFall=53 ms) under 532 nm illumination with bias voltage of Vds=5 V. Similar results have also been achieved in multilayer MoSe2 crystals. All these findings indicate great potential of 3R-stacked TMDs in two-dimensional optoelectronic applications.