Van der Waals (vdW) heterostructures consisting of two dimensional materials offer a platform to obtain material by design and are very attractive owing to novel electronic states. Research on 2D van der Waals heterostructures (vdWH) has so far been focused on fabricating individually stacked atomically thin unary or binary crystals. Such systems include graphene (Gr), hexagonal boron nitride (h-BN) and member of the transition metal dichalcogenides family. Here we present our experimental study of the opto-electronic properties of a naturally occurring vdWH, known as Franckeite, which is a complex layered crystal composed of lead, tin, antimony, iron and sulfur. We present here that thin film franckeite (60 nm < d < 100 nm) behave as narrow band gap semiconductor demonstrating a wide band photoresponse. We have observed the band-edge transition at ~ 1500 nm (~830 meV) and high external quantum efficiency (EQE~3%) at room temperature. Laser power resolved and temperature resolved photocurrent measurements reveal that the photo-carrier generation and recombination are dominated by continuously distributed trap states within the band gap. To understand wavelength resolved photocurrent, we also calculated the optical absorption properties via density functional theory. Finally, we have shown that the device has fast photoresponse with rise time as fast as ~ 1 ms. Our study provides a fundamental understanding of the optoelectronic behavior in a complex naturally occurring vdWH and can open up the possibilities of producing new type of nanoscale optoelectronic devices with tailored properties.

have contributed equally to this work.Scalable fabrication of high quality photodetectors derived from synthetically grown monolayer transition metal dichalcogenides is highly desired and important for wide range of nanophotonics applications. We present here scalable fabrication of monolayer MoS 2 photodetectors on sapphire substrates through an efficient process, which includes growing large scale monolayer MoS 2 via chemical vapor deposition (CVD), and multi-step optical lithography for device patterning and high quality metal electrodes fabrication. In every measured device, we observed the following universal features: (i) negligible dark current (I dark 10f A); (ii) sharp peaks in photocurrent at ∼1.9eV and ∼2.1eV attributable to the optical transitions due to band edge excitons; (iii) a rapid onset of photocurrent above ∼2.5eV peaked at ∼2.9eV due to an excitonic absorption originating from the van Hove singularity of MoS 2 . We observe low ( 300%) device-to-device variation of photoresponsivity. Furthermore, we observe very fast rise time ∼0.5 ms, which is three orders of magnitude faster than other reported CVD grown 1L-MoS 2 based photodetectors. The combination of scalable device fabrication, ultra-high sensitivity and high speed offer a great potential for applications in photonics.Atomically thin monolayer two-dimensional (2D) transition-metal dichalcogenides (TMDs) are attractive materials for next-generation nanoscale optoelectronic applications and have gained tremendous interest in wide range of fields.1-4 TMDs demonstrate several extraordinary properties that make TMDs very attractive for optical, electrical and opto-electronic applications. First, 2D confinement, direct band-gap nature 5 , large surfaceto-volume ratio 6 , and weak screening of charge carriers enhance the light-matter interactions 5,7-10 in these materials that lead to extraordinarily high absorption. Second, strong light-matter interaction creates electron-hole (e-h) pairs and forms two-body bound states, known as excitons (a hydrogenic entity made of an e-h pair).

Atomically thin two-dimensional (2D) transition metal dichalcogenides (TMDCs) are attractive materials for next generation nanoscale optoelectronic applications. Understanding nanoscale optical behavior of the edges and grain boundaries of synthetically grown TMDCs is vital for optimizing their optoelectronic properties. Elucidating the nanoscale optical properties of 2D materials through farfield optical microscopy requires a diffraction-limited optical beam diameter sub-micron in size. Here we present our experimental work on spatial photoluminescence (PL) scanning of large size ( 50 m) monolayer MoS 2 grown by chemical vapor deposition (CVD) using a diffraction limited blue laser beam spot (wavelength 405 nm) with a beam diameter as small as ∼200 nm allowing us to probe nanoscale excitonic phenomena which was not observed before. We have found several important features: (i) there exists a sub-micron width strip (~500 nm) along the edges that fluoresces ~1000% brighter than the region far inside; (ii) there is another brighter wide region consisting of parallel fluorescing lines ending at the corners of the zig-zag peripheral edges; (iii) there is a giant blue shifted A-excitonic peak, as large as ∼120 meV, in the PL spectra from the edges. Using density functional theory calculations, we attribute this giant blue shift to the adsorption of oxygen dimers at the edges, which reduces the excitonic binding energy. Our results not only shed light on defectinduced excitonic properties, but also offer an attractive route to tailor optical properties at the TMDC edges through defect engineering. 2 INTRODUCTIONS