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Register a new userA non-invasive sub-surface electrical probe to encapsulated layers in van der Waals heterostructures
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Van der Waals heterostructures formed by stacking different atomically thin layered materials have emerged as the sought-after device platform for electronic and optoelectronic applications. Determining the spatial extent of all the encapsulated components in such vertical stacks is key to optimal fabrication methods and improved device performance. Here we employ electrostatic force microscopy as a fast and non-invasive microscopic probe that provides compelling images of two dimensional layers buried over 30 nm below the sample surface. We demonstrate the versatility of the technique by studying heterojunctions comprising graphene, hexagonal boron nitride and transition metal dichalcogenides. Work function of each constituent layer acts as a unique fingerprint during imaging, thereby providing important insights into the charge environment, disorder, structural imperfections and doping profile. The technique holds great potential for gaining a comprehensive understanding of the quality, flatness as well as local electrical properties of buried layers in a large class of nanoscale materials and vertical heterostructures.
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Van der Waals materials can be easily combined in lateral and vertical heterostructures, providing an outstanding platform to engineer elusive quantum states of matter. However, a critical problem in material science is to establish tangible links between real materials properties and terms that can be cooked up on the model Hamiltonian level to realize different exotic phenomena. Our review aims to do precisely this: we first discuss, in a way accessible to the materials community, what ingredients need to be included in the hybrid quantum materials recipe, and second, we elaborate on the specific materials that would possess the necessary qualities. We will review the well-established procedures for realizing 2D topological superconductors, quantum spin-liquids and flat bands systems, emphasizing the connection between well-known model Hamiltonians and real compounds. We will use the most recent experimental results to illustrate the power of the designer approach.
The development of van der Waals (vdW) crystals and their heterostructures has created a fascinating platform for exploring optoelectronic properties in the two-dimensional (2D) limit. With the recent discovery of 2D magnets, the control of the spin degree of freedom can be integrated to realize 2D spin-optoelectronics with spontaneous time-reversal symmetry breaking. Here, we report spin photovoltaic effects in vdW heterostructures of atomically thin magnet chromium triiodide (CrI3) sandwiched by graphene contacts. In the absence of a magnetic field, the photocurrent displays a distinct dependence on light helicity, which can be tuned by varying the magnetic states and photon energy. Circular polarization-resolved absorption measurements reveal that these observations originate from magnetic-order-coupled and thus helicity-dependent charge-transfer exciton states. The photocurrent displays multiple plateaus as the magnetic field is swept, which are associated with different spin configurations enabled by the layered antiferromagnetism and spin-flip transitions in CrI3. Remarkably, giant photo-magnetocurrent is observed, which tends to infinity for a small applied bias. Our results pave the way to explore emergent photo-spintronics by engineering magnetic vdW heterostructures.
Vertically stacked van der Waals heterostructures are a lucrative platform for exploring the rich electronic and optoelectronic phenomena in two-dimensional materials. Their performance will be strongly affected by impurities and defects at the interfaces. Here we present the first systematic study of interfaces in van der Waals heterostructure using cross sectional scanning transmission electron microscope (STEM) imaging. By measuring interlayer separations and comparing these to density functional theory (DFT) calculations we find that pristine interfaces exist between hBN and MoS2 or WS2 for stacks prepared by mechanical exfoliation in air. However, for two technologically important transition metal dichalcogenide (TMDC) systems, MoSe2 and WSe2, our measurement of interlayer separations provide the first evidence for impurity species being trapped at buried interfaces with hBN: interfaces which are flat at the nanometer length scale. While decreasing the thickness of encapsulated WSe2 from bulk to monolayer we see a systematic increase in the interlayer separation. We attribute these differences to the thinnest TMDC flakes being flexible and hence able to deform mechanically around a sparse population of protruding interfacial impurities. We show that the air sensitive two dimensional (2D) crystal NbSe2 can be fabricated into heterostructures with pristine interfaces by processing in an inert-gas environment. Finally we find that adopting glove-box transfer significantly improves the quality of interfaces for WSe2 compared to processing in air.
The properties of van der Waals (vdW) heterostructures are drastically altered by a tunable moire superlattice arising from periodic variations of atomic alignment between the layers. Exciton diffusion represents an important channel of energy transport in semiconducting transition metal dichalcogenides (TMDs). While early studies performed on TMD heterobilayers have suggested that carriers and excitons exhibit long diffusion lengths, a rich variety of scenarios can exist. In a moire crystal with a large supercell size and deep potential, interlayer excitons may be completely localized. As the moire period reduces at a larger twist angle, excitons can tunnel between supercells and diffuse over a longer lifetime. The diffusion length should be the longest in commensurate heterostructures where the moire superlattice is completely absent. In this study, we experimentally demonstrate that the moire potential impedes interlayer exciton diffusion by comparing a number of WSe2/MoSe2 heterostructures prepared with chemical vapor deposition and mechanical stacking with accurately controlled twist angles. Our results provide critical guidance to developing twistronic devices that explore the moire superlattice to engineer material properties.
Van-der-Waals heterostructures show many intriguing phenomena including ultrafast charge separation following strong excitonic absorption in the visible spectral range. However, despite the enormous potential for future applications in the field of optoelectronics, the underlying microscopic mechanism remains controversial. Here we use time- and angle-resolved photoemission spectroscopy combined with microscopic many-particle theory to reveal the relevant microscopic charge transfer channels in epitaxial WS$_2$/graphene heterostructures. We find that the timescale for efficient ultrafast charge separation in the material is determined by direct tunneling at those points in the Brillouin zone where WS$_2$ and graphene bands cross, while the lifetime of the charge separated transient state is set by defect-assisted tunneling through localized sulphur vacanices. The subtle interplay of intrinsic and defect-related charge transfer channels revealed in the present work can be exploited for the design of highly efficient light harvesting and detecting devices.
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