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Control of excitons in multi-layer van der Waals heterostructures

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 Added by Eric Calman
 Publication date 2015
  fields Physics
and research's language is English




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We report an experimental study of excitons in a double quantum well van der Waals heterostructure made of atomically thin layers of Mo* and hexagonal boron nitride (hBN). The emission of neutral and charged excitons is controlled by gate voltage, temperature, and both the helicity and the power of optical excitation.



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In van der Waals (vdW) heterostructures formed by stacking two monolayer semiconductors, lattice mismatch or rotational misalignment introduces an in-plane moire superlattice. While it is widely recognized that a moire superlattice can modulate the electronic band structure and lead to novel transport properties including unconventional superconductivity and insulating behavior driven by correlations, its influence on optical properties has not been investigated experimentally. We present spectroscopic evidence that interlayer excitons are confined by the moire potential in a high-quality MoSe2/WSe2 heterobilayer with small rotational twist. A series of interlayer exciton resonances with either positive or negative circularly polarized emission is observed in photoluminescence, consistent with multiple exciton states confined within the moire potential. The recombination dynamics and temperature dependence of these interlayer exciton resonances are consistent with this interpretation. These results demonstrate the feasibility of engineering artificial excitonic crystals using vdW heterostructures for nanophotonics and quantum information applications.
Stacking monolayers of transition metal dichalcogenides into a heterostructure with a finite twist-angle gives rise to artificial moire superlattices with a tunable periodicity. As a consequence, excitons experience a periodic potential, which can be exploited to tailor optoelectronic properties of these materials. While recent experimental studies have confirmed twist-angle dependent optical spectra, the microscopic origin of moire exciton resonances has not been fully clarified yet. Here, we combine first principle calculations with the excitonic density matrix formalism to study transitions between different moire exciton phases and their impact on optical properties of the twisted MoSe$_2$/WSe$_2$ heterostructure. At angles smaller than 2$^{circ}$ we find flat, moire trapped states for inter- and intralayer excitons. This moire exciton phase drastically changes into completely delocalized states already at 3$^{circ}$. We predict a linear and quadratic twist-angle dependence of excitonic resonances for the moire-trapped and delocalized exciton phase, respectively. Our work provides microscopic insights opening the possibility to tailor moire exciton phases in van der Waals superlattices.
Indirect excitons (IXs) in van der Waals transition-metal dichalcogenide (TMD) heterostructures are characterized by a high binding energy making them stable at room temperature and giving the opportunity for exploring fundamental phenomena in excitonic systems and developing excitonic devices operational at high temperatures. We present the observation of IXs at room temperature in van der Waals TMD heterostructures based on monolayers of MoS$_2$ separated by atomically thin hexagonal boron nitride. The IXs realized in the TMD heterostructure have lifetimes orders of magnitude longer than lifetimes of direct excitons in single-layer TMD, and their energy is gate controlled.
Throughout the years, strongly correlated coherent states of excitons have been the subject of intense theoretical and experimental studies. This topic has recently boomed due to new emerging quantum materials such as van der Waals (vdW) bound atomically thin layers of transition metal dichalcogenides (TMDs). We analyze the collective properties of charged interlayer excitons observed recently in bilayer TMD heterostructures. We predict new strongly correlated phases - crystal and Wigner crystal - that can be selectively realized with TMD bilayers of properly chosen electron-hole effective masses by just varying their interlayer separation distance. Our results open up new avenues for nonlinear coherent control, charge transport and spinoptronics applications with quantum vdW heterostuctures.
Atomically-thin layers of two-dimensional materials can be assembled in vertical stacks held together by relatively weak van der Waals forces, allowing for coupling between monolayer crystals with incommensurate lattices and arbitrary mutual rotation. A profound consequence of using these degrees of freedom is the emergence of an overarching periodicity in the local atomic registry of the constituent crystal structures, known as a moire superlattice. Its presence in graphene/hexagonal boron nitride (hBN) structures led to the observation of electronic minibands, whereas its effect enhanced by interlayer resonant conditions in twisted graphene bilayers culminated in the observation of the superconductor-insulator transition at magic twist angles. Here, we demonstrate that, in semiconducting heterostructures built of incommensurate MoSe2 and WS2 monolayers, excitonic bands can hybridise, resulting in the resonant enhancement of the moire superlattice effects. MoSe2 and WS2 are specifically chosen for the near degeneracy of their conduction band edges to promote the hybridisation of intra- and interlayer excitons, which manifests itself through a pronounced exciton energy shift as a periodic function of the interlayer rotation angle. This occurs as hybridised excitons (hX) are formed by holes residing in MoSe2 bound to a twist-dependent superposition of electron states in the adjacent monolayers. For heterostructures with almost aligned pairs of monolayer crystals, resonant mixing of the electron states leads to pronounced effects of the heterostructures geometrical moire pattern on the hX dispersion and optical spectrum. Our findings underpin novel strategies for band-structure engineering in semiconductor devices based on van der Waals heterostructures.
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