Understanding the transition from nonplanar to planar clusters is crucial for the controllable synthesis of transition metal dichalcogenide (TMDC) monolayers. Using PtSe2 as a model, we investigate how the chemical environment influences the nucleation and growth stages of monolayer PtSe2 through structure searching and first-principles calculations. We established a comprehensive database of platinum selenide clusters (PtxSey, x = 1-10), analyzing 2095 unique clusters and identifying 191 stable isomers and 63 structures with the lowest formation energy on the convex hull. Our findings reveal a chemical environment-dependent phase transition from 3D structures to the planar T-phase of PtxSey clusters, representing an evolutionary route for PtSe2 growth. Clusters such as PtSe6, Pt2Se9, Pt3Se10, and Pt7Se10 in Pt-rich environments, as well as Pt2Se15 and Pt10Se32 in Se-rich environments, have been found to exhibit high stability. Additionally, the impact of varying chemical potentials of Pt and Se on the stability of these clusters is explored. PtSe4 and PtSe6 are found to be highly stable under most experimentally achievable chemical potential conditions and may serve as dominant precursors during PtSe2 growth. This work advances our understanding of the nucleation processes of PtSe2 and other T-phase TMDC materials.

This study investigates the scope of application of a recently designed inversion methodology that is capable of obtaining structural information about disordered systems through the analysis of their conductivity response signals. Here we demonstrate that inversion tools of this type are capable of sensing the presence of disorderly distributed defects and impurities even in the case where the scattering properties of the device are only weakly affected. This is done by inverting the DC conductivity response of monolayered MoS2films containing a minute amount of AuCl3coordinated complexes. Remarkably, we have successfully extracted detailed information about the concentration of AuCl3by decoding its signatures on the transport features of simulated devices. In addition to the case of theoretically generated Hamiltonians, we have also carried out a full inversion procedure from experimentally measured signals of similar structures. Based on experimental input signals of MoS2with naturally occurring vacancies, we were able to quantify the vacancy concentration contained in the samples, which indicates that the inversion methodology has experimental applicability as long as the input signal is able to resolve the characteristic contributions of the type of disorder in question. Being able to handle more complex, realistic scenarios unlocks the method\'s applicability for designing and engineering even more elaborate materials.

A fully quantum, numerically accurate methodology is presented for the simulation of the exciton dynamics and time-resolved fluorescence of cavity-tuned two-dimensional (2D) materials at finite temperatures. This approach was specifically applied to a monolayer WSe2 system. Our methodology enabled us to identify the dynamical and spectroscopic signatures of polaronic and polaritonic effects and to elucidate their characteristic timescales across a range of exciton-cavity couplings. The approach employed can be extended to simulation of various cavity-tuned 2D materials, specifically for exploring finite temperature nonlinear spectroscopic signals.

One of the primary factors hindering the development of 2D material-based devices is the difficulty of overcoming fabrication processes, which pose a challenge in achieving low-resistance contacts. Widely used metal deposition methods lead to unfavorable Fermi level pinning effect (FLP), which prevents control over the Schottky barrier height at the metal/2D material junction. We propose to harness the FLP effect to lower contact resistance in field-effect transistors (FETs) by using an additional 2D interlayer at the conducting channel and metallic contact interface (under-contact interlayer). To do so, we developed a new approach using the gold-assisted transfer method, which enables the fabrication of heterostructures consisting of TMDs monolayers with complex shapes, prepatterned using e-beam lithography, with lateral dimensions even down to 100 nm. We designed and demonstrated tungsten disulfide (WS2) monolayer-based devices in which the molybdenum disulfide (MoS2) monolayer is placed only in the contact area of the FET, creating an Au/MoS2/WS2 junction, which effectively reduces contact resistance by over 60% and improves the Ion/Ioff ratio 10 times in comparison to WS2-based devices without MoS2 under-contact interlayer. The enhancement in the device operation arises from the FLP effect occurring only at the interface between the metal and the first layer of the MoS2/WS2 heterostructure. This results in favorable band alignment, which enhances the current flow through the junction. To ensure the reproducibility of our devices, we systematically analyzed 160 FET devices fabricated with under-contact interlayer and without it. Statistical analysis shows a consistent improvement in the operation of the device and reveals the impact of contact resistance on key FET performance indicators.

Due to their unique properties, two-dimensional transition metal dichalcogenides (2D TMDCs) are considered for diverse applications in microelectronics, sensing, catalysis, to name a few. A common challenge in 2D TMDC research is the film\'s inherent instability i.e. spontaneous oxidation upon ambient exposure. The present study systematically explores the effect aging on the film composition and photoluminescent properties of monolayer WS2, synthetically grown by metal-organic chemical vapor deposition. The aging rate is investigated for different oxygen- (i.e. O2gas concentration and humidity) and light-controlled environments. Simple mitigation strategies that do not involve capping the 2D TMDC layer are discussed, and their effectiveness demonstrated by benchmarking the evolution in photoluminescence response against ambient exposed monolayer WS2. These results highlight the need to store 2D TMDCs in controlled environments to preserve the film quality and how future studies can account for the aging effect.

Semiconducting transition metal dichalcogenides (TMDs) are promising for high-specific-power photovoltaics due to their desirable band gaps, high absorption coefficients, and ideally dangling-bond-free surfaces. Despite their potential, the majority of TMD solar cells to date are fabricated in a nonscalable fashion, with exfoliated materials, due to the lack of high-quality, large-area, multilayer TMDs. Here, we present the scalable, thickness-tunable synthesis of multilayer WSe2 films by selenizing prepatterned tungsten with either solid-source selenium at 900 °C or H2Se precursors at 650 °C. Both methods yield photovoltaic-grade, wafer-scale WSe2 films with a layered van der Waals structure and superior characteristics, including charge carrier lifetimes up to 144 ns, over 14× higher than those of any other large-area TMD films previously demonstrated. Simulations show that such carrier lifetimes correspond to ∼22% power conversion efficiency and ∼64 W g-1 specific power in a packaged solar cell, or ∼3 W g-1 in a fully packaged solar module. The results of this study could facilitate the mass production of high-efficiency multilayer WSe2 solar cells at low cost.

A significantly enhanced THz radiation generation from femtosecond photoexcited MoS2 layers due to Nb-doping is reported here. Different microscopic mechanisms involved in the THz photocurrent generation vary in their relative contributions in the two cases of photoexcitation, i.e., above and below the electronic bandgap of the layers. For a moderate Nb-doping level of just ∼0.05%, we have observed a multifold enhancement in the THz emission for the case of the above bandgap excitation, which is, though, nearly 1.5 times for the case of the below bandgap excitation of the monolayer MoS2. Alongside the difference in THz generation efficiency, the THz pulse polarity is also reversed at the above bandgap excitation of the Nb-doped layers, consequent to the reversed surface depletion field. Except for a slightly smaller difference in the THz enhancement factor, all the observations are reproducible in the bilayers as well to imply a weaker inversion symmetry and reduced screening of the surface depletion field due to Nb-doping. Furthermore, we employed pristine MoS2 and Nb-doped MoS2 monolayers to fabricate piezoelectric nanogenerator devices. Like enhancement in the ultrafast THz emission, the piezoelectric performance of the nanogenerator, fabricated with the Nb-doped MoS2 monolayer is also increased by a similar factor.

The remarkable electronic properties of monolayer MoTe2 make it a very adaptable material for use in optoelectronic and nano-electronic applications. MoTe2 growth often exhibits intrinsic defects, which significantly influence the material\'s characteristics. In this work, we conducted a thorough investigation of the electronic characteristics of intrinsic defects, including point defects, in monolayer MoTe2 using first-principles calculations based on density functional theory (DFT). Our findings indicate that the presence of point defects leads to the formation of n-type properties as the Fermi level situates above the conduction band. Our first-principles density functional theory calculation revealed an appearance of donor level in the band gap close to the conduction band in MoTe2. Our study signifies that the formation energy of a vacancy in a Te atom is lower than that of both a vacancy in a Mo atom and two vacancies in Te atom. This suggests that during the synthesis process, it is more probable for Te atom vacancies to be created. A defect in the pristine monolayer of MoTe2 leads to a slight decrease in the band gap, causing a transition from a direct band gap semiconductor to an indirect band gap semiconductor. The results of our study indicate that the presence of vacancy defects may modify the electronic properties of monolayer MoTe2, suggesting its potential as a new platform for electronic applications. Hence, our analysis offers significant theoretical backing for defect engineering in MoTe2 monolayers and other 2D materials, a critical aspect in the advancement of nanoscale devices with the desired functionality.
The study explores the electronic properties of monolayer MoTe2, revealing intrinsic defects that can enhance its potential for electronic applications and providing theoretical support for defect engineering in 2D materials.

With their fascinating properties, emerging two-dimensional (2D) materials offer innovative ways to prepare high-performance infrared (IR) detectors. However, the current performance of 2D IR photodetectors is still below the requirements for practical application owing to the severe interfacial recombination, sharply raised contact resistance, and deteriorated metal conductivity at nanoscale. Here, we introduce a vertical barrier heterojunction with a structure of PtSe2/GaAs that combines the excellent optoelectronic properties of transition metal sulfides with topological semi-metals, which allows for an adjustable bandgap and high carrier mobility. The heterojunction was fabricated using the wet transfer method. The heterostructures show significant rectification behaviors and photovoltaic effects, which allow it to operate as a self-driven photodetector at zero bias. The photoresponse parameters at 850 nm with zero bias voltage are 67.2 mA W-1, 6.7 × 1012 Jones, 9.8%, 3.8 × 105, 164 μs, and 198 μs for the responsivity, specific detectivity, external quantum efficiency, Ilight/Idark ratio, rise time, and fall time, respectively. Moreover, the heterojunction is highly sensitive to a wide spectral band from ultraviolet to near-infrared (360-1550 nm). At the same time, this heterostructure demonstrates significant potential for applications in IR polarized light detection and room-temperature high-resolution IR imaging. The excellent properties of the heterojunction make it well-suited for high-performance, self-powered IR detection.

Achieving robust electrical contacts is crucial for realizing the promise of monolayer 2D semiconductors such as semiconducting transition metal dichalcogenides (s-TMDs) in electronics. Despite recent breakthroughs, a gap remains between the experimental and theoretical understanding of metal-s-TMDs contacts. This study explores bismuth semimetal contacts to monolayer MoSe2, using a platform that minimizes experimental sources of uncertainty; we combine contact-front and contact-end measurements to measure key parameters like specific resistivity (ρc) and transfer length (Lt). We find that the resistivity of MoSe2 under the contacts is enhanced due to charge transfer that can be modeled using a self-consistent approach. In contrast, ab initio calculations of the interlayer charge transfer rate are inconsistent with the measured value of ρc, highlighting the need for new theoretical approaches.