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Register a new userTuning of impurity-bound interlayer complexes in a van der Waals heterobilayer
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Due to their unique two-dimensional nature, charge carriers in semiconducting transition metal dichalcogenides (TMDs) exhibit strong unscreened Coulomb interactions and sensitivity to defects and impurities. The versatility of van der Waals layer stacking allows spatially separating electrons and holes between different TMD layers with staggered band structure, yielding interlayer few-body excitonic complexes whose nature is still debated. Here we combine quantum Monte Carlo calculations with spectrally and temporally resolved photoluminescence measurements on a top- and bottom-gated MoSe2/WSe2 heterostructure, and identify the emitters as impurity-bound interlayer excitonic complexes. Using independent electrostatic control of doping and out-of-plane electric field, we demonstrate control of the relative populations of neutral and charged complexes, their emission energies on a scale larger than their linewidth, and an increase of their lifetime into the microsecond regime. This work unveils new physics of confined carriers and is key to the development of novel optoelectronics applications.
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Van der Waals heterostructures of 2D materials provide a powerful approach towards engineering various quantum phases of matters. Examples include topological matters such as quantum spin Hall (QSH) insulator, and correlated matters such as exciton superfluid. It can be of great interest to realize these vastly different quantum matters on a common platform, however, their distinct origins tend to restrict them to material systems of incompatible characters. Here we show that heterobilayers of two-dimensional valley semiconductors can be tuned through interlayer bias between an exciton superfluid (ES), a quantum anomalous Hall (QAH) insulator, and a QSH insulator. The tunability between these distinct phases results from the competition of Coulomb interaction with the interlayer quantum tunnelling that has a chiral form in valley semiconductors. Our findings point to exciting opportunities for harnessing both protected topological edge channels and bulk superfluidity in an electrically configurable platform.
Exciton binding energies of hundreds of meV and strong light absorption in the optical frequency range make transition metal dichalcogenides (TMDs) promising for novel optoelectronic nanodevices. In particular, atomically thin TMDs can be stacked to heterostructures enabling the design of new materials with tailored properties. The strong Coulomb interaction gives rise to interlayer excitons, where electrons and holes are spatially separated in different layers. In this work, we reveal the microscopic processes behind the formation, thermalization and decay of these fundamentally interesting and technologically relevant interlayer excitonic states. In particular, we present for the exemplary MoSe$_2$-WSe$_2$ heterostructure the interlayer exciton binding energies and wave functions as well as their time- and energy-resolved dynamics. Finally, we predict the dominant contribution of interlayer excitons to the photoluminescence of these materials.
We report first-principles calculations of the structural and vibrational properties of the synthesized two-dimensional van der Waals heterostructures formed by single-layers dichalcogenides MoSe2 and WSe2. We show that, when combining these systems in a periodic two-dimensional heterostructures, the intrinsic phonon characteristics of the free-standing constituents are to a large extent preserved but, furthermore, exhibit shear and breathing phonon modes that are not present in the individual building blocks. These peculiar modes depend strongly on the weak vdW forces and has a great contibution to the thermal properties of the layered materials. Besides these features, the departure of flexural modes of heterobilayer from the ones of its monolayer parents are also found.
Different atomistic registry between the layers forming the inner and outer nanotubes can form one-dimensional (1D) van der Waals (vdW) moire superlattices. Unlike the two-dimensional (2D) vdW moire superlattices, effects of 1D vdW moire superlattices on electronic and optical properties in 1D moire superlattices are not well understood, and they are often neglected. In this Perspective, we summarize new experimental observations and theoretical perspectives related to interlayer interactions in double-walled carbon nanotubes (DWNTs), a representative 1D vdW moire system. Our discussion will focus on new optical features emerging from the interlayer electronic interactions in DWNTs. Exciting correlated physics and exotic phases of matter are anticipated to exist in 1D vdW moire superlattices, analogous with those discovered in the 2D vdW moire superlattices. We further discuss the future directions in probing and uncovering interesting physical phenomena in 1D moire superlattices.
We develop a theory for interlayer tunneling in van der Waals heterostructures driven under a strong electromagnetic field, using graphene/{it h}-BN/graphene as a paradigmatic example. Our theory predicts that strong anti-resonances appear at bias voltage values equal to an integer multiple of the light frequency. These features are found to originate from photon-assisted resonant tunneling transitions between Floquet sidebands of different graphene layers, and are unique to two-band systems due to the interplay of both intraband and interband tunneling transitions. Our results point to the possibility of tunneling localization in van der Waals heterostructures using strong electromagnetic fields.
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