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 by out-of-plane vibrational motions. The simulations rationalize the experimental results on the influence of the bilayer twist angle on the charge separation and recombination. The atomistic insights provide theoretical guidance for design of high-performance optoelectronic devices based on 2D van der Waals heterostructures.
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Moiré metrology of energy landscapes in van der Waals heterostructures
Abstract The emerging field of twistronics, which harnesses the twist angle between two-dimensional materials, represents a promising route for the design of quantum materials, as the twist-angle-induced superlattices offer means to control topology and strong correlations. At the small twist limit, and particularly under strain, as atomic relaxation prevails, the emergent moiré superlattice encodes elusive insights into the local interlayer interaction. Here we introduce moiré metrology as a combined experiment-theory framework to probe the stacking energy landscape of bilayer structures at the 0.1 meV/atom scale, outperforming the gold-standard of quantum chemistry. Through studying the shapes of moiré domains with numerous nano-imaging techniques, and correlating with multi-scale modelling, we assess and refine first-principle models for the interlayer interaction. We document the prowess of moiré metrology for three representative twisted systems: bilayer graphene, double bilayer graphene and H-stacked MoSe 2 /WSe 2 . Moiré metrology establishes sought after experimental benchmarks for interlayer interaction, thus enabling accurate modelling of twisted multilayers.
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- Award ID(s):
- 1922172
- NSF-PAR ID:
- 10297388
- Author(s) / Creator(s):
- ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more »
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 12
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1038/s41467-020-20428-1
