Doping is the cornerstone of semiconductor technology, enabling the success of modern digital electronics. 2D transition metal dichalcogenides (TMDCs) are promising material platforms for future electronics applications where its wafer-scale synthesis and controllable doping will be a required prerequisite to drive the next technological revolution. [1-6] Successful realization of wafer-scale, electronic grade, intrinsic 2D TMDCs via common deposition methods is rapidly progressing, however, advances in scalable doping still remain in the "proof-of-concept" stage, delaying the largescale fabrication of logic circuits based on extrinsic 2D semiconductors. [7-12] Moreover, integration of 2D TMDCs with Si complementary metal-oxide-semiconductor at the back-end-of-line (BEOL) is being actively explored for diffusion barriers, liners, and thin-film-transistors to improve the overall integrated circuit performance. [13-16] However, BEOL production lines are Reliable, controlled doping of 2D transition metal dichalcogenides will enable the realization of next-generation electronic, logic-memory, and magnetic devices based on these materials. However, to date, accurate control over dopant concentration and scalability of the process remains a challenge. Here, a systematic study of scalable in situ doping of fully coalesced 2D WSe 2 films with Re atoms via metal-organic chemical vapor deposition is reported. Dopant concentrations are uniformly distributed over the substrate surface, with precisely controlled concentrations down to <0.001% Re achieved by tuning the precursor partial pressure. Moreover, the impact of doping on morphological, chemical, optical, and electronic properties of WSe 2 is elucidated with detailed experimental and theoretical examinations, confirming that the substitutional doping of Re at the W site leads to n-type behavior of WSe 2. Transport characteristics of fabricated back-gated fieldeffect-transistors are directly correlated to the dopant concentration, with degrading device performances for doping concentrations exceeding 1% of Re. The study demonstrates a viable approach to introducing true dopantlevel impurities with high precision, which can be scaled up to batch production for applications beyond digital electronics.
Scalable substitutional doping of 2D transition metal dichalcogenides is a prerequisite to developing next-generation logic and memory devices based on 2D materials. To date, doping efforts are still nascent. Here, scalable growth and vanadium (V) doping of 2D WSe 2 at front-end-of-line and backend-of-line compatible temperatures of 800 and 400 °C, respectively, is reported. A combination of experimental and theoretical studies confirm that vanadium atoms substitutionally replace tungsten in WSe 2 , which results in p-type doping via the introduction of discrete defect levels that lie close to the valence band maxima. The p-type nature of the V dopants is further verified by constructed field-effect transistors, where hole conduction becomes dominant with increasing vanadium concentration. Hence, this study presents a method to precisely control the density of intentionally introduced impurities, which is indispensable in the production of electronic-grade wafer-scale extrinsic 2D semiconductors.
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