14 research outputs found
Demonstration of the key substrate dependent charge transfer mechanisms between monolayer MoS2 and molecular dopants
Electronic band dispersion determination in azimuthally disordered transition metal dichalcogenide monolayers
The Schottky Mott Rule Expanded for Two Dimensional Semiconductors Influence of Substrate Dielectric Screening
A comprehensive understanding of the energy level alignment mechanisms between two dimensional 2D semiconductors and electrodes is currently lacking, but it is a prerequisite for tailoring the interface electronic properties to the requirements of device applications. Here, we use angle resolved direct and inverse photoelectron spectroscopy to unravel the key factors that determine the level alignment at interfaces between a monolayer of the prototypical 2D semiconductor MoS2 and conductor, semiconductor, and insulator substrates. For substrate work function amp; 934;sub values below 4.5 eV we find that Fermi level pinning occurs, involving electron transfer to native MoS2 gap states below the conduction band. For amp; 934;sub above 4.5 eV, vacuum level alignment prevails but the charge injection barriers do not strictly follow the changes of amp; 934;sub as expected from the Schottky Mott rule. Notably, even the trends of the injection barriers for holes and electrons are different. This is caused by the band gap renormalization of monolayer MoS2 by dielectric screening, which depends on the dielectric constant amp; 949;r of the substrate. Based on these observations, we introduce an expanded Schottky Mott rule that accounts for band gap renormalization by amp; 949;r dependent screening and show that it can accurately predict charge injection barriers for monolayer MoS2. It is proposed that the formalism of the expanded Schottky Mott rule should be universally applicable for 2D semiconductors, provided that material specific experimental benchmark data are availabl
The epitaxy of 2D materials growth
Two dimensional (2D) materials consist of one to a few atomic layers, where the intra-layer atoms are chemically bonded and the atomic layers are weakly bonded. The high bonding anisotropicity in 2D materials make their growth on a substrate substantially different from the conventional thin film growth. Here, we proposed a general theoretical framework for the epitaxial growth of a 2D material on an arbitrary substrate. Our extensive density functional theory (DFT) calculations show that the propagating edge of a 2D material tends to align along a high symmetry direction of the substrate and, as a conclusion, the interplay between the symmetries of the 2D material and the substrate plays a critical role in the epitaxial growth of the 2D material. Based on our results, we have outlined that orientational uniformity of 2D material islands on a substrate can be realized only if the symmetry group of the substrate is a subgroup of that of the 2D material. Our predictions are in perfect agreement with most experimental observations on 2D materials' growth on various substrates known up to now. We believe that this general guideline will lead to the large-scale synthesis of wafer-scale single crystals of various 2D materials in the near future. Advances in our ability to manipulate genetics leads to deeper understanding of biological systems. In this perspective, the authors argue that synthetic genomics facilitates complex modifications that open up new areas of research
Type-I Energy Level Alignment at the PTCDAâMonolayer MoS2 Interface Promotes Resonance Energy Transfer and Luminescence Enhancement
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., electronâhole 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.Peer Reviewe
Direct determination of monolayer MoS2 and WSe2 exciton binding energies on insulating and metallic substrates
Understanding the excitonic nature of exited states in two dimensional 2D transition metal dichalcogenides TMDCs is of key importance to make use of their optical and charge transport properties in optoelectronic applications. We contribute to this by the direct experimental determination of the exciton binding energy Eb,exc of monolayer MoS2 and WSe2 on two fundamentally different substrates, i.e., the insulator sapphire and the metal gold. By combining angle resolved direct and inverse photoelectron spectroscopy we measure the transport single particle band gap Et , and by reflectance measurements the optical excitonic band gap Eexc . The difference of these two energies is Eb,exc. The values of Et and Eb,exc are 2.11 eV and 240 meV for MoS2 on sapphire, and 1.89 eV and 240 meV for WSe2 on sapphire. On Au Eb,exc is decreased to 90 meV and 140 meV for MoS2 and WSe2, respectively. The significant Eb,exc reduction is primarily due to a reduction of Et resulting from enhanced screening by the metal, while Eexc is barely decreased for the metal support. Energy level diagrams determined at the K point of the 2D TMDCs Brillouin zone show that MoS2 has more p type character on Au as compared to sapphire, while WSe2 appears close to intrinsic on both. These results demonstrate that the impact of the dielectric environment of 2D TMDCs is more pronounced for individual charge carriers than for a correlated electron hole pair, i.e., the exciton. A proper dielectric surrounding design for such 2D semiconductors can therefore be used to facilitate superior optoelectronic device function
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Mixed-dimensional MXene-hydrogel heterostructures for electronic skin sensors with ultrabroad working range.
Skin-mountable microelectronics are garnering substantial interest for various promising applications including human-machine interfaces, biointegrated devices, and personalized medicine. However, it remains a critical challenge to develop e-skins to mimic the human somatosensory system in full working range. Here, we present a multifunctional e-skin system with a heterostructured configuration that couples vinyl-hybrid-silica nanoparticle (VSNP)-modified polyacrylamide (PAM) hydrogel with two-dimensional (2D) MXene through nano-bridging layers of polypyrrole nanowires (PpyNWs) at the interfaces, featuring high toughness and low hysteresis, in tandem with controlled crack generation and distribution. The multidimensional configurations endow the e-skin with an extraordinary working range (2800%), ultrafast responsiveness (90 ms) and resilience (240 ms), good linearity (800%), tunable sensing mechanisms, and excellent reproducibility. In parallel, this e-skin platform is capable of detecting, quantifying, and remotely monitoring stretching motions in multiple dimensions, tactile pressure, proximity sensing, and variations in temperature and light, establishing a promising platform for next-generation smart flexible electronics
Recommended from our members
Mixed-dimensional MXene-hydrogel heterostructures for electronic skin sensors with ultrabroad working range.
Skin-mountable microelectronics are garnering substantial interest for various promising applications including human-machine interfaces, biointegrated devices, and personalized medicine. However, it remains a critical challenge to develop e-skins to mimic the human somatosensory system in full working range. Here, we present a multifunctional e-skin system with a heterostructured configuration that couples vinyl-hybrid-silica nanoparticle (VSNP)-modified polyacrylamide (PAM) hydrogel with two-dimensional (2D) MXene through nano-bridging layers of polypyrrole nanowires (PpyNWs) at the interfaces, featuring high toughness and low hysteresis, in tandem with controlled crack generation and distribution. The multidimensional configurations endow the e-skin with an extraordinary working range (2800%), ultrafast responsiveness (90 ms) and resilience (240 ms), good linearity (800%), tunable sensing mechanisms, and excellent reproducibility. In parallel, this e-skin platform is capable of detecting, quantifying, and remotely monitoring stretching motions in multiple dimensions, tactile pressure, proximity sensing, and variations in temperature and light, establishing a promising platform for next-generation smart flexible electronics
Temperature Dependent Electronic Ground State Charge Transfer in van der Waals Heterostructures
Electronic charge rearrangement between components of a heterostructure is the fundamental principle to reach the electronic ground state. It is acknowledged that the density of state distribution of the components governs the amount of charge transfer, but a notable dependence on temperature is not yet considered, particularly for weakly interacting systems. Here, it is experimentally observed that the amount of ground state charge transfer in a van der Waals heterostructure formed by monolayer MoS2 sandwiched between graphite and a molecular electron acceptor layer increases by a factor of 3 when going from 7 K to room temperature. State of the art electronic structure calculations of the full heterostructure that accounts for nuclear thermal fluctuations reveal intracomponent electron phonon coupling and intercomponent electronic coupling as the key factors determining the amount of charge transfer. This conclusion is rationalized by a model applicable to multicomponent van der Waals heterostructure