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Two-dimensional (2D) semiconducting monolayers such as transition metal dichalcogenides (TMDs) are promising channel materials to extend Moore's Law in advanced electronics. Synthetic TMD layers from chemical vapor deposition (CVD) are scalable for fabrication but notorious for their high defect densities. Therefore, innovative endeavors on growth reaction to enhance their quality are urgently needed. Here, we report that the hydroxide W species, an extremely pure vapor phase metal precursor form, is very efficient for sulfurization, leading to about one order of magnitude lower defect density compared to those from conventional CVD methods. The field-effect transistor (FET) devices based on the proposed growth reach a peak electron mobility ~200 cm2/Vs (~800 cm2/Vs) at room temperature (15 K), comparable to those from exfoliated flakes. The FET device with a channel length of 100 nm displays a high on-state current of ~400 µA/µm, encouraging the industrialization of 2D materials. Chemical vapor deposition enables the scalable production of 2D semiconductors, but the grown materials are usually affected by high defect densities. Here, the authors report a hydroxide vapour phase deposition method to synthesize wafer-scale monolayer WS2 with reduced defect density and electrical properties comparable to those of exfoliated flakes. [ABSTRACT FROM AUTHOR]

Van der Waals heterostructures consisting of 2D semiconductors and conjugated molecules are of increasing interest because of the prospect of a synergistic enhancement of (opto)electronic properties. In particular, perylenetetracarboxylic dianhydride (PTCDA) on monolayer (ML)‐MoS2 has been identified as promising candidate and a staggered type‐II energy level alignment and excited state interfacial charge transfer have been proposed. In contrast, it is here found with inverse and direct angle resolved photoelectron spectroscopy that PTCDA/ML‐MoS2 supported by insulating sapphire exhibits a straddling type‐I level alignment, with PTCDA having the wider energy gap. Photoluminescence (PL) and sub‐picosecond transient absorption measurements reveal that resonance energy transfer, i.e., electron–hole pair (exciton) transfer, from PTCDA to ML‐MoS2 occurs on a sub‐picosecond time scale. This gives rise to an enhanced PL yield from ML‐MoS2 in the heterostructure and an according overall modulation of the photoresponse. These results underpin the importance of a precise knowledge of the interfacial electronic structure in order to understand excited state dynamics and to devise reliable design strategies for optimized optoelectronic functionality in van der Waals heterostructures. [ABSTRACT FROM AUTHOR]

In article number 2100215, Soohyung Park, Sylke Blumstengel, Norbert Koch, and co‐workers demonstrate a key mechanism for opto‐electronic properties enhancement of an organic/inorganic van der Waals semiconductor heterostructure in the 2D limit. A straddling type‐I energy level alignment enables sub‐picosecond resonance energy transfer from organic molecules to a 2D inorganic semiconductor monolayer, with enhanced luminescence yield from the inorganic component. [ABSTRACT FROM AUTHOR]

In article number 2100215, Soohyung Park, Sylke Blumstengel, Norbert Koch, and co-workers demonstrate a key mechanism for opto-electronic properties enhancement of an organic/inorganic van der Waals semiconductor heterostructure in the 2D limit. A straddling type-I energy level alignment enables sub-picosecond resonance energy transfer from organic molecules to a 2D inorganic semiconductor monolayer, with enhanced luminescence yield from the inorganic component. Van der Waals Heterostructures: Type-I Energy Level Alignment at the PTCDA - Monolayer MoS2 Interface Promotes Resonance Energy Transfer and Luminescence Enhancement (Adv. Sci. 12/2021). [Extracted from the article]

Tuning the Fermi level (EF) in two-dimensional transition metal dichalcogenide (TMDC) semiconductors is crucial for optimizing their application in (opto-)electronic devices. Doping by molecular electron acceptors and donors has been suggested as a promising method to achieve EF-adjustment. Here, we demonstrate that the charge transfer (CT) mechanism between TMDC and molecular dopant depends critically on the electrical nature of the substrate as well as its electronic coupling with the TMDC. Using angle-resolved ultraviolet and X-ray photoelectron spectroscopy, we reveal three fundamentally different, substrate-dependent CT mechanisms between the molecular electron acceptor 1,3,4,5,7,8-hexafluoro-tetracyano-naphthoquinodimethane (F6TCNNQ) and a MoS2 monolayer. Our results demonstrate that any substrate that acts as charge reservoir for dopant molecules can prohibit factual doping of a TMDC monolayer. On the other hand, the three different CT mechanisms can be exploited for the design of advanced heterostructures, exhibiting tailored electronic properties in (opto-)electronic devices based on two-dimensional semiconductors. Doping of 2D semiconductors by electron acceptor or donor molecules has been suggested as a method to optimize their properties for electronic devices. Here, the authors identify three distinct charge transfer mechanisms that depend on the substrate and yield different doping efficiencies. [ABSTRACT FROM AUTHOR]