Scalable heterojunctions based on two-dimensional transitional metal dichalcogenides are of great importance for their applications in the next generation of electronic and optoelectronic devices. However, reliable techniques for the fabrication of such heterojunctions are still at its infancy. Here we demonstrate a simple technique for the scalable fabrication of lateral heterojunctions via selective chemical doping of TMD thin films. We demonstrate that the resistance of large area MoS 2 and MoSe 2 thin film, prepared via low pressure chalcogenation of molybdenum film, decreases by up to two orders of magnitude upon doping using benzyl viologen (BV) molecule. X-ray photoelectron spectroscopy (XPS) measurements confirms n-doping of the films by BV molecules. Since thin films of MoS 2 and MoSe 2 are typically more resistive than their exfoliated and co-evaporation based CVD counterparts, the decrease in resistance by BV doping represents a significant step in the utilization of these samples in electronic devices. Using selective BV doping, we simultaneously fabricated many lateral heterojunctions in 1 cm 2 MoS 2 and 1 cm 2 MoSe 2 films. The electrical transport measurements performed across the heterojunctions exhibit current rectification behavior due to a band offset created between the doped and undoped regions of the material. Almost 84% of the fabricated devices showed rectification behavior demonstrating the scalability of this technique.
Au‐mediated exfoliation of 2D transition‐metal dichalcogenides (TMDs) has received significant attention due to its ability to produce large‐area monolayer (ML) flakes. This process has been attributed to strong TMD/Au binding energy (BE) as well as the uniform strain between the TMDs and Au. However, large‐area exfoliation of TMDs with other metals that have even stronger theoretical BE than Au/TMD is not successful, leading to question whether the BE plays any role in the exfoliation process. Here, successful demonstration of large‐area ML MoS2 using Cu, Ni, and Ag with various predicted strain, including Pd with almost no strain, but stronger BE than Au/MoS2 is demonstrated. Optical micrographs show MoS2 flakes with 100s of µm in size with a yield of several tens to hundreds of ML flakes per exfoliation. Photoluminescence and Raman spectroscopy confirm the ML nature of the flakes, while electrical transport measurements show mobilities of ≈6 cm2 V−1 s−1 with a current on‐off ratio ≈108 consistent with high‐quality ML MoS2. Given that MoS2 can be exfoliated with metals that have strong BE irrespective of their strain values suggests that BE is the primary mechanism in successful exfoliation of large‐area ML MoS2.
Modulating physical and chemical properties of two-dimensional (2D) transition metal dichalcogenides (TMDCs) by defect engineering induced by oxygen plasma is actively pursued. In this work, exfoliated 2D MoS2 layers treated by medium power oxygen plasma for different times (0, 10, 20, 40, and 60 s) are investigated using Kelvin probe force microscopy and tip-enhanced Raman spectroscopy (TERS) besides micro-Raman and photoluminescence (PL) spectroscopy. Under oxygen plasma, defects (mono- and di-sulfur vacancies) and chemical oxidation are predominant from 0 (native defects) up to 40 s, while etching becomes dominant beyond 40 s for mono- (1L), bi- (2L), and tri- (3L) layer MoS2 with optimal defect density for four- (4L) and more layers. While Raman spectra exhibited lattice distortion (broadening of phonon bands) and surface oxidation by the presence of sub-stoichiometric molytrioxide MoO3 (i.e., MoO3–x or MoSxO2–x), the increased spectral weight of trions and quenching in PL spectra are observed with treatment time. The localized nanodomains (∼20–40 nm) and aggregated vacancies as nanovoids and intermixed MoS2/MoO3–x alloy are identified in near-field Raman spectra. The atomic force microscopy also showed defects aggregation, and Kelvin probe force microscopy revealed the work function (WF) increase from 4.98 to 5.56 eV, corroborating the existence of MoO3–x phase which enables doping and shift Fermi level. We also highlight the unique interaction between the gold substrate and the formed MoO3–x facilitating Mo6+ cation reduction to lower oxidation (i.e., Mo4+), thereby yielding intermediate oxidation states responsible for lower WF (ca. theoretical 6.3 eV for stoichiometric MoO3). Strong correlations among the work function and vibrational and optical responses are established while exploring the oxygen plasma-induced defects and changing the landscape on oxygen doping at the nanoscale with varying MoS2 layers, which are useful for heterogeneous electrocatalysis and applicable to other 2D-TMDCs.
Palladium diselenide (PdSe2) is an emerging 2D material with exotic optical and electrical properties and widely tunable layer dependent band gap in the infrared regime. The ability to further tune the electronic properties of PdSe2 via doping is of fundamental importance for a wide range of electronic and optoelectronic device applications. Here, surface charge transfer doping of chemical vapor deposition grown p‐type PdSe2 thin film using benzyl viologen (BV) molecules is reported. The electrical transport measurements of the PdSe2 device show an increase in resistance by ≈1700 percent from 2.1 MΩ for the pristine sample to 36.2 MΩ upon BV doping, revealing electrons are transferred from BV molecules to PdSe2 resulting in an n‐doping. Raman characterization shows a red‐shift and broadening of A3g characteristic peak for the doped sample, while X‐ray photoelectron spectroscopy shows a negative shift in Pd 3d and Se 3d binding energies confirming n‐doping by BV. Kelvin force probe microscopy measurements show a ≈0.3 eV decrease in work function for doped PdSe2, consistent with the n‐doping by BV molecules. A selective doping of PdSe2 channel is implemented for the fabrication of lateral heterojunction device which shows good current rectifying behavior with a rectification ratio of up to ≈55.
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