BACKGROUND Materials by design is an appealing idea that is very hard to realize in practice. Combining the best of different ingredients in one ultimate material is a task for which we currently have no general solution. However, we do have some successful examples to draw upon: Composite materials and III-V heterostructures have revolutionized many aspects of our lives. Still, we need a general strategy to solve the problem of mixing and matching crystals with different properties, creating combinations with predetermined attributes and functionalities. ADVANCES Two-dimensional (2D) materials offer a platform that allows creation of heterostructures with a variety of properties. One-atom-thick crystals now comprise a large family of these materials, collectively covering a very broad range of properties. The first material to be included was graphene, a zero-overlap semimetal. The family of 2D crystals has grown to includes metals (e.g., NbSe 2 ), semiconductors (e.g., MoS 2 ), and insulators [e.g., hexagonal boron nitride (hBN)]. Many of these materials are stable at ambient conditions, and we have come up with strategies for handling those that are not. Surprisingly, the properties of such 2D materials are often very different from those of their 3D counterparts. Furthermore, even the study of familiar phenomena (like superconductivity or ferromagnetism) in the 2D case, where there is no long-range order, raises many thought-provoking questions. A plethora of opportunities appear when we start to combine several 2D crystals in one vertical stack. Held together by van der Waals forces (the same forces that hold layered materials together), such heterostructures allow a far greater number of combinations than any traditional growth method. As the family of 2D crystals is expanding day by day, so too is the complexity of the heterostructures that could be created with atomic precision. When stacking different crystals together, the synergetic effects become very important. In the first-order approximation, charge redistribution might occur between the neighboring (and even more distant) crystals in the stack. Neighboring crystals can also induce structural changes in each other. Furthermore, such changes can be controlled by adjusting the relative orientation between the individual elements. Such heterostructures have already led to the observation of numerous exciting physical phenomena. Thus, spectrum reconstruction in graphene interacting with hBN allowed several groups to study the Hofstadter butterfly effect and topological currents in such a system. The possibility of positioning crystals in very close (but controlled) proximity to one another allows for the study of tunneling and drag effects. The use of semiconducting monolayers leads to the creation of optically active heterostructures. The extended range of functionalities of such heterostructures yields a range of possible applications. Now the highest-mobility graphene transistors are achieved by encapsulating graphene with hBN. Photovoltaic and light-emitting devices have been demonstrated by combining optically active semiconducting layers and graphene as transparent electrodes. OUTLOOK Currently, most 2D heterostructures are composed by direct stacking of individual monolayer flakes of different materials. Although this method allows ultimate flexibility, it is slow and cumbersome. Thus, techniques involving transfer of large-area crystals grown by chemical vapor deposition (CVD), direct growth of heterostructures by CVD or physical epitaxy, or one-step growth in solution are being developed. Currently, we are at the same level as we were with graphene 10 years ago: plenty of interesting science and unclear prospects for mass production. Given the fast progress of graphene technology over the past few years, we can expect similar advances in the production of the heterostructures, making the science and applications more achievable.

2D materials and van der Waals heterostructures

Two-dimensional layered materials (2DLMs) have been a central focus of materials research since the discovery of graphene just over a decade ago. Each layer in 2DLMs consists of a covalently bonded, dangling-bond-free lattice and is weakly bound to neighbouring layers by van der Waals interactions. This makes it feasible to isolate, mix and match highly disparate atomic layers to create a wide range of van der Waals heterostructures (vdWHs) without the constraints of lattice matching and processing compatibility. Exploiting the novel properties in these vdWHs with diverse layering of metals, semiconductors or insulators, new designs of electronic devices emerge, including tunnelling transistors, barristors and flexible electronics, as well as optoelectronic devices, including photodetectors, photovoltaics and light-emitting devices with unprecedented characteristics or unique functionalities. We review the recent progress and challenges, and offer our perspective on the exploration of 2DLM-based vdWHs for future application in electronics and optoelectronics. With a dangling-bond-free surface, two dimensional layered materials (2DLMs) can enable the creation of diverse van der Waals heterostructures (vdWHs) without the conventional constraint of lattice matching or process compatibility. This Review discusses the recent advances in exploring 2DLM vdWHs for future electronics and optoelectronics.

Van der Waals heterostructures and devices

Semiconductor technology is currently based on the manipulation of electronic charge; however, electrons have additional degrees of freedom, such as spin and valley, that can be used to encode and process information. Over the past several decades, there has been significant progress in manipulating electron spin for semiconductor spintronic devices, motivated by potential spin-based information processing and storage applications. However, experimental progress towards manipulating the valley degree of freedom for potential valleytronic devices has been limited until very recently. We review the latest advances in valleytronics, which have largely been enabled by the isolation of 2D materials (such as graphene and semiconducting transition metal dichalcogenides) that host an easily accessible electronic valley degree of freedom, allowing for dynamic control. The energy extrema of an electronic band are referred to as valleys. In 2D materials, two distinguishable valleys can be used to encode information and explore other valleytronic applications.

Valleytronics in 2D materials

The advent of graphene and related 2D materials has recently led to a new technology: heterostructures based on these atomically thin crystals. The paradigm proved itself extremely versatile and led to rapid demonstration of tunnelling diodes with negative differential resistance, tunnelling transistors, photovoltaic devices and so on. Here, we take the complexity and functionality of such van der Waals heterostructures to the next level by introducing quantum wells (QWs) engineered with one atomic plane precision. We describe light-emitting diodes (LEDs) made by stacking metallic graphene, insulating hexagonal boron nitride and various semiconducting monolayers into complex but carefully designed sequences. Our first devices already exhibit an extrinsic quantum efficiency of nearly 10% and the emission can be tuned over a wide range of frequencies by appropriately choosing and combining 2D semiconductors (monolayers of transition metal dichalcogenides). By preparing the heterostructures on elastic and transparent substrates, we show that they can also provide the basis for flexible and semi-transparent electronics. The range of functionalities for the demonstrated heterostructures is expected to grow further on increasing the number of available 2D crystals and improving their electronic quality.

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Light-emitting diodes by band-structure engineering in van der Waals heterostructures

The advent of graphene and related 2D materials has recently led to a new technology: heterostructures based on these atomically thin crystals. The paradigm proved itself extremely versatile and led to rapid demonstration of tunnelling diodes with negative differential resistance, tunnelling transistors5, photovoltaic devices, etc. Here we take the complexity and functionality of such van der Waals heterostructures to the next level by introducing quantum wells (QWs) engineered with one atomic plane precision. We describe light emitting diodes (LEDs) made by stacking up metallic graphene, insulating hexagonal boron nitride (hBN) and various semiconducting monolayers into complex but carefully designed sequences. Our first devices already exhibit extrinsic quantum efficiency of nearly 10% and the emission can be tuned over a wide range of frequencies by appropriately choosing and combining 2D semiconductors (monolayers of transition metal dichalcogenides). By preparing the heterostructures on elastic and transparent substrates, we show that they can also provide the basis for flexible and semi-transparent electronics. The range of functionalities for the demonstrated heterostructures is expected to grow further with increasing the number of available 2D crystals and improving their electronic quality.

/pdf/light-emitting-diodes-by-bandstructure-engineering-in-van-1u78i9kl4v.pdf

Light-emitting diodes by bandstructure engineering in van der Waals heterostructures

In order to fully exploit the potential of transition metal dichalcogenide monolayers (TMD-MLs), the well-controlled creation of atomically sharp lateral heterojunctions within these materials is highly desirable. A promising approach to create such heterojunctions is the local modulation of the electronic structure of an intrinsic TMD-ML via dielectric screening induced by its surrounding materials. For the realization of this non-invasive approach, an in-depth understanding of such dielectric effects is required. We report on the modulations of excitonic transitions in TMD-MLs through the effect of dielectric environments including low-k and high-k dielectric materials. We present absolute tuning ranges as large as 37 meV for the optical band gaps of WSe2 and MoSe2 MLs and relative tuning ranges on the order of 30% for the binding energies of neutral excitons in WSe2 MLs. The findings suggest the possibility to reduce the electronic band gap of WSe2 MLs by 120 meV, paving the way towards dielectrically defined lateral heterojunctions.

Engineering of Neutral Excitons and Exciton Complexes in Transition Metal Dichalcogenide Monolayers through External Dielectric Screening

Long-ranged coherent qubit coupling is a missing function block for scaling up spin qubit based quantum computing solutions. Spin-coherent conveyor-mode electron-shuttling could enable spin quantum-chips with scalable and sparse qubit-architecture. Its key feature is the operation by only few easily tuneable input terminals and compatibility with industrial gate-fabrication. Single electron shuttling in conveyor-mode in a 420 nm long quantum bus has been demonstrated previously. Here we investigate the spin coherence during conveyor-mode shuttling by separation and rejoining an Einstein-Podolsky-Rosen (EPR) spin-pair. Compared to previous work we boost the shuttle velocity by a factor of 10000. We observe a rising spin-qubit dephasing time with the longer shuttle distances due to motional narrowing and estimate the spin-shuttle infidelity due to dephasing to be 0.7 % for a total shuttle distance of nominal 560 nm. Shuttling several loops up to an accumulated distance of 3.36 $\mu$m, spin-entanglement of the EPR pair is still detectable, giving good perspective for our approach of a shuttle-based scalable quantum computing architecture in silicon.

J. S. Tu

Papers

Engineering of Neutral Excitons and Exciton Complexes in Transition Metal Dichalcogenide Monolayers through External Dielectric Screening

Spin-EPR-pair separation by conveyor-mode single electron shuttling in Si/SiGe