Van der Waals heterojunctions of two-dimensional transition-metal dichalcogenides are intensely investigated for multiple optoelectronics applications. Strong and adjustable interactions between layers can influence the charge and energy flow that govern material performance. We report ab initio quantum molecular dynamics investigation of the influence of the bilayer twist angle on charge transfer and recombination in MoS 2 /WS 2 heterojunctions, including high-symmetry 0° and 60° configurations, and low symmetry 9.43° and 50.57° structures with Moiré patterns. The twist angle modulates interlayer coupling, as evidenced by changes in the interlayer distance, electron-vibrational interactions, and spectral shifts in the out-of-plane vibrational frequencies. Occurring on a femtosecond timescale, the hole transfer depends weakly on the twist angle and is ultrafast due to high density of acceptor states and large nonadiabatic coupling. In contrast, the electron–hole recombination takes nanoseconds and varies by an order of magnitude depending on the twist angle. The recombination is slow because it occurs across a large energy gap. It depends on the twist angle because the nonadiabatic coupling is sensitive to the interlayer distance and overlap of electron and hole wavefunctions. The Moiré pattern systems exhibit weaker interlayer interaction, generating longer-lived charges. Both charge separation and recombination are driven bymore »
Corrugation-driven symmetry breaking in magic-angle twisted bilayer graphene
The discovery of unconventional superconductivity in magic-angle twisted bilayer graphene (tBLG) supported the twist-angle-induced flat band structure predictions made a decade earlier. Numerous physical properties have since been linked to the interlayer twist angle using the flat band prediction as a guideline. However, some key observations like the nematic phase and striped charge order behind the superconductivity are missing in this initial model. Here we show that a thermodynamically stable large out-of-plane displacement, or corrugation of the bilayer, induced by the interlayer twist, demonstrates partially filled states of the flat band structure, accompanied by a broken symmetry, in the magic-angle regime and the presence of symmetry breaking associated with the superconductivity in tBLG. The distinction between low and high corrugation can also explain the observed evolution of the vibrational spectra of tBLG as a function of twist angle. Our observation that large out-of-plane deformation modes enable partial filling of states near the Fermi energy may lead to a strategy for offsetting the effects of disorder in the local twist angle, which suppresses unconventional superconductivity and correlated insulator behavior in magic-angle tBLG.
- Publication Date:
- NSF-PAR ID:
- 10372827
- Journal Name:
- Communications Physics
- Volume:
- 5
- Issue:
- 1
- ISSN:
- 2399-3650
- Publisher:
- Nature Publishing Group
- Sponsoring Org:
- National Science Foundation
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Abstract Magic-angle twisted bilayer graphene (MATBG) exhibits a panoply of many-body phenomena that are intimately tied to the appearance of narrow and well-isolated electronic bands. The microscopic ingredients that are responsible for the complex experimental phenomenology include electron–electron (phonon) interactions and nontrivial Bloch wavefunctions associated with the narrow bands. Inspired by recent experiments, we focus on two independent quantities that are considerably modified by Coulomb interaction-driven band renormalization, namely the density of states and the minimal spatial extent associated with the Wannier functions. First, we show that a filling-dependent enhancement of the density of states, caused by band flattening, in combination with phonon-mediated attraction due to electron-phonon umklapp processes, increases the tendency towards superconducting pairing in a range of angles around magic-angle. Second, we demonstrate that the minimal spatial extent associated with the Wannier functions, which contributes towards increasing the superconducting phase stiffness, also develops a nontrivial enhancement due to the interaction-induced renormalization of the Bloch wavefunctions. While our modeling of superconductivity (SC) assumes a weak electron-phonon coupling and does not consider many of the likely relevant correlation effects, it explains simply the experimentally observed robustness of SC in the wide range of angles that occurs in the relevant rangemore »
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Moiré superlattices in two-dimensional van der Waals heterostructures provide an efficient way to engineer electron band properties. The recent discovery of exotic quantum phases and their interplay in twisted bilayer graphene (tBLG) has made this moiré system one of the most renowned condensed matter platforms. So far studies of tBLG have been mostly focused on the lowest two flat moiré bands at the first magic angle θ m1 ∼ 1.1°, leaving high-order moiré bands and magic angles largely unexplored. Here we report an observation of multiple well-isolated flat moiré bands in tBLG close to the second magic angle θ m2 ∼ 0.5°, which cannot be explained without considering electron–election interactions. With high magnetic field magnetotransport measurements we further reveal an energetically unbound Hofstadter butterfly spectrum in which continuously extended quantized Landau level gaps cross all trivial band gaps. The connected Hofstadter butterfly strongly evidences the topologically nontrivial textures of the multiple moiré bands. Overall, our work provides a perspective for understanding the quantum phases in tBLG and the fractal Hofstadter spectra of multiple topological bands.
