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Register a new userControlled Electrochemical Intercalation of Graphene/h-BN van der Waals Heterostructures
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Added by
Shu Yang Frank Zhao
Publication date
2017
fields
Physics
and research's language is
English
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Electrochemical intercalation is a powerful method for tuning the electronic properties of layered solids. In this work, we report an electro-chemical strategy to controllably intercalate lithium ions into a series of van der Waals (vdW) heterostructures built by sandwiching graphene between hexagonal boron nitride (h-BN). We demonstrate that encapsulating graphene with h-BN eliminates parasitic surface side reactions while simultaneously creating a new hetero-interface that permits intercalation between the atomically thin layers. To monitor the electrochemical process, we employ the Hall effect to precisely monitor the intercalation reaction. We also simultaneously probe the spectroscopic and electrical transport properties of the resulting intercalation compounds at different stages of intercalation. We achieve the highest carrier density $> 5 times 10^{13} cm^{-2}$ with mobility $> 10^3 cm^2/(Vs)$ in the most heavily intercalated samples, where Shubnikov-de Haas quantum oscillations are observed at low temperatures. These results set the stage for further studies that employ intercalation in modifying properties of vdW heterostructures.
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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.
Vertically stacked van der Waals heterostructures constitute a promising platform for providing tailored band alignment with enhanced excitonic systems. Here we report observations of neutral and charged interlayer excitons in trilayer WSe2-MoSe2-WSe2 van der Waals heterostructures and their dynamics. The addition of a WSe2 layer in the trilayer leads to significantly higher photoluminescence quantum yields and tunable spectral resonance compared to its bilayer heterostructures at cryogenic temperatures. The observed enhancement in the photoluminescence quantum yield is due to significantly larger electron-hole overlap and higher light absorbance in the trilayer heterostructure, supported via first-principle pseudopotential calculations based on spin-polarized density functional theory. We further uncover the temperature- and power-dependence, as well as time-resolved photoluminescence of the trilayer heterostructure interlayer neutral excitons and trions. Our study elucidates the prospects of manipulating light emission from interlayer excitons and designing atomic heterostructures from first-principles for optoelectronics.
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.
Graphene constitutes one of the key elements in many functional van der Waals heterostructures. However, it has negligible optical visibility due to its monolayer nature. Here we study the visibility of graphene in various van der Waals heterostructures and include the effects of the source spectrum, oblique incidence and the spectral sensitivity of the detector to obtain a realistic model. A visibility experiment is performed at different wavelengths, resulting in a very good agreement with our calculations. This allows us to reliably predict the conditions for better visibility of graphene in van der Waals heterostructures. The framework and the codes provided in this work can be extended to study the visibility of any 2D material within an arbitrary van der Waals heterostructure.
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.
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