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Register a new userHighly Efficient Carrier Multiplication in van der Waals layered Materials
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Carrier multiplication (CM), a photo-physical process to generate multiple electron-hole pairs by exploiting excess energy of free carriers, is explored for efficient photovoltaic conversion of photons from the blue solar band, predominantly wasted as heat in standard solar cells. Current state-of-the-art approaches with nanomaterials have demonstrated improved CM but are not satisfactory due to high energy loss and inherent difficulties with carrier extraction. Here, we report ultra-efficient CM in van der Waals (vdW) layered materials that commences at the energy conservation limit and proceeds with nearly 100% conversion efficiency. A small threshold energy, as low as twice the bandgap, was achieved, marking an onset of quantum yield with enhanced carrier generation. Strong Coulomb interactions between electrons confined within vdW layers allow rapid electron-electron scattering to prevail over electron-phonon scattering. Additionally, the presence of electron pockets spread over momentum space could also contribute to the high CM efficiency. Combining with high conductivity and optimal bandgap, these superior CM characteristics identify vdW materials for third-generation solar cell.
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Two-dimensional (2D) materials exhibit a number of improved mechanical, optical, electronic properties compared to their bulk counterparts. The absence of dangling bonds in the cleaved surfaces of these materials allows combining different 2D materials into van der Waals heterostructures to fabricate p-n junctions, photodetectors, 2D-2D ohmic contacts that show unexpected performances. These intriguing results are regularly summarized in comprehensive reviews. A strategy to tailor their properties even further and to observe novel quantum phenomena consists in the fabrication of superlattices whose unit cell is formed either by two dissimilar 2D materials or by a 2D material subjected to a periodical perturbation, each component contributing with different characteristics. Furthermore, in a 2D materials-based superlattice, the interlayer interaction between the layers mediated by van der Waals forces constitutes a key parameter to tune the global properties of the superlattice. The above-mentioned factors reflect the potential to devise countless combinations of van der Waals 2D materials based superlattices. In the present feature article, we explain in detail the state-of-the-art of 2D materials-based superlattices and we describe the different methods to fabricate them, classified as vertical stacking, intercalation with atoms or molecules, moire patterning, strain engineering and lithographic design. We also aim to highlight some of the specific applications for each type of superlattices.
Being used in optoelectronic devices as ultra-thin conductor-insulator junctions, detailed investigations are needed about how exactly h-BN and graphene hybridize. Here, we present a comprehensive ab initio study of hot carrier dynamics governed by electron-phonon scattering at the h-BN/graphene interface, using graphite (bulk), monolayer and bilayer graphene as benchmark materials. In contrast to monolayer graphene, all multilayer structures possess low-energy optical phonon modes that facilitate carrier thermalization. We find that the h-BN/graphene interface represents an exception with comparatively weak coupling between low-energy optical phonons and electrons. As a consequence, the thermalization bottleneck effect, known from graphene, survives hybridization with h-BN but is substantially reduced in all other bilayer and multilayer cases considered. In addition, we show that the quantum confinement in bilayer graphene does not have a significant influence on the thermalization time compared to graphite and that bilayer graphene can hence serve as a minimal model for the bulk counterpart.
Sliding and twisting van der Waals layers with respect to each other gives rise to moire structures with emergent electronic properties. Electrons in these moire structures feel weak potentials that are typically in the tens of millielectronvolt range when the moire structures are smooth at the atomic scale. Here we report a facile technique to achieve deep, deterministic trapping potentials via strain-based moire engineering in van der Waals bilayers. We use elasto-scanning tunneling microscopy to show that uniaxial strain drives a commensurate-incommensurate lattice transition in a multilayer MoSe$_2$ system. In the incommensurate state, the top monolayer is partially detached from the bulk through the spontaneous formation of topological solitons where stress is relieved. Intersecting solitons form a honeycomb-like network resulting from the three-fold symmetry of the adhesion potential between layers. The vertices of the honeycomb network occur in bound pairs with different interlayer stacking arrangements. One vertex of the pair is found to be an efficient trap for electrons, displaying two states that are deeply confined within the semiconductor gap and have a spatial extent of 2 nm. Honeycomb soliton networks thus provide a unique path to engineer an array of identical deeply confined states with a strain-dependent tunable spatial separation, without the necessity of introducing chemical defects into the host materials.
Nonlinear mechanics of solids is an exciting field that encompasses both beautiful mathematics, such as the emergence of instabilities and the formation of complex patterns, as well as multiple applications. Two-dimensional crystals and van der Waals (vdW) heterostructures allow revisiting this field on the atomic level, allowing much finer control over the parameters and offering atomistic interpretation of experimental observations. In this work, we consider the formation of instabilities consisting of radially-oriented wrinkles around mono- and few-layer bubbles in two-dimensional vdW heterostructures. Interestingly, the shape and wavelength of the wrinkles depend not only on the thickness of the two-dimensional crystal forming the bubble, but also on the atomistic structure of the interface between the bubble and the substrate, which can be controlled by their relative orientation. We argue that the periodic nature of these patterns emanates from an energetic balance between the resistance of the top membrane to bending, which favors large wavelength of wrinkles, and the membrane-substrate vdW attraction, which favors small wrinkle amplitude. Employing the classical Winkler foundation model of elasticity theory, we show that the number of radial wrinkles conveys a valuable relationship between the bending rigidity of the top membrane and the strength of the vdW interaction. Armed with this relationship, we use our data to demonstrate a nontrivial dependence of the bending rigidity on the number of layers in the top membrane, which shows two different regimes driven by slippage between the layers, and a high sensitivity of the vdW force to the alignment between the substrate and the membrane.
The van der Waals heterostructures are a fertile frontier for discovering emergent phenomena in condensed matter systems. They are constructed by stacking elements of a large library of two-dimensional materials, which couple together through van der Waals interactions. However, the number of possible combinations within this library is staggering, and fully exploring their potential is a daunting task. Here we introduce van der Waals metamaterials to rapidly prototype and screen their quantum counterparts. These layered metamaterials are designed to reshape the flow of ultrasound to mimic electron motion. In particular, we show how to construct analogues of all stacking configurations of bilayer and trilayer graphene through the use of interlayer membranes that emulate van der Waals interactions. By changing the membranes density and thickness, we reach coupling regimes far beyond that of conventional graphene. We anticipate that van der Waals metamaterials will explore, extend, and inform future electronic devices. Equally, they allow the transfer of useful electronic behavior to acoustic systems, such as flat bands in magic-angle twisted bilayer graphene, which may aid the development of super-resolution ultrasound imagers.
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