Key Takeaways & Executive Findings
- •• • High-mobility multilayered MoS2 flakes with low contact resistance have been achieved via chemical vapor deposition, as reported by Zheng et al. (Adv. Mater. 2017, 29, 1604540), enabling enhanced performance in field-effect transistors and photodetectors. • • Precise control of interlayer twist angle in large-scale MoS2 homostructures has been demonstrated by Liao et al. (Nat. Commun. 2020, 11, 2153), critical for tuning moiré superlattices and correlated electronic states. • • Layer-by-layer assembly of 2D materials into wafer-scale heterostructures has been realized by Kang et al. (Nature 2017, 550, 229–233), providing a scalable route for integrating diverse 2D materials with clean interfaces. • • Thickness-tunable wedding-cake-like MoS2 flakes for high-performance optoelectronics have been fabricated by Yang et al. (ACS Nano 2019, 13, 10.1021/acsnano.9b04745), demonstrating the potential for layer-number-dependent optical and electronic properties.
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Abstract
Multilayer two-dimensional (2D) materials offer expanded opportunities for tuning electronic, optical, and quantum properties compared to their monolayer forms. The number of layers, stacking configuration, and interlayer interactions are critical parameters that govern the physical behavior of these materials, enabling unique functionalities such as tunable bandgaps, interlayer excitons, sliding ferroelectricity, and unconventional superconductivity. This review highlights recent progress in the precise fabrication techniques of multilayer graphene, h-BN, and transition metal dichalcogenides. We compare artificial assembly techniques and direct growth strategies (chemical vapor deposition), emphasizing their advantages, limitations, and progress toward achieving uniform thickness, high crystallinity, and clean interfaces. The ability to engineer multilayer structures plays an essential role in improving device performance and realizing new quantum states of matter. By discussing fabrication strategies, growth mechanisms, and interlayer coupling effects, we highlight the significance of multilayer architecture in the development of functional 2D material systems.
1. Introduction
Multilayer two-dimensional (2D) materials offer expanded opportunities for tuning electronic, optical, and quantum properties compared to their monolayer forms. The number of layers, stacking configuration, and interlayer interactions are critical parameters that govern the physical behavior of these materials, enabling unique functionalities such as tunable bandgaps, interlayer excitons, sliding ferroelectricity, and unconventional superconductivity. This review highlights recent progress in the precise fabrication techniques of multilayer graphene, h-BN, and transition metal dichalcogenides. We compare artificial assembly techniques and direct growth strategies (chemical vapor deposition), emphasizing their advantages, limitations, and progress toward achieving uniform thickness, high crystallinity, and clean interfaces. The ability to engineer multilayer structures plays an essential role in improving device performance and realizing new quantum states of matter. By discussing fabrication strategies, growth mechanisms, and interlayer coupling effects, we highlight the significance of multilayer architecture in the development of functional 2D material systems.
While the unique properties of monolayer 2D materials have been widely explored, growing attention has been devoted to their multilayer counterparts. In multilayer systems, the number of atomic layers and their stacking configurations play a decisive role in determining the electronic structure, interlayer coupling, optical response, and overall device performance. While the 2D materials family has expanded dramatically in recent years, graphene, h-BN, and TMDs (particularly MoS2) remain the most deeply studied systems due to their stable fabrication protocols and well-understood structure–property relationships. For example, bilayer and trilayer graphene (TLG) structures exhibit stacking-dependent bandgap tunability, unconventional superconductivity, and topological phenomena. Similarly, multilayer h-BN shows enhanced dielectric screening and has been shown to support sliding ferroelectricity under certain stacking orders. TMDs, such as MoS2 and WSe2, undergo a transition from direct to indirect bandgap with increasing layer number and demonstrate significantly improved carrier transport and thermal stability in multilayer form, enabling their integration in high-performance field-effect transistors, photodetectors, and neuromorphic devices. Achieving precise control over layer number and stacking order in these materials is thus of paramount importance, both for fundamental investigations and practical applications. However, this remains a significant challenge, as it requires atomic-level precision in the vertical assembly of van der Waals (vdW) layers while maintaining high crystallinity and clean interfaces. To address this, various fabrication strategies have been developed, which can be broadly classified into artificial assembly and direct growth methods.
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FAN Aiqing, ZHANG Qing, WANG Yongshuai, LI Lin, WU Fan, GENG Dechao (2025). Recent advances in layer engineering and controllable fabrication of graphene, h-BN, and transition metal dichalcogenides. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3656-9
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Frequently Asked Questions
What are the primary failure mechanisms in multilayer TMD-based devices under electrical stress?
Under high current densities (>10^7 A/cm²) and prolonged operation, multilayer TMDs such as MoS2 can suffer from Joule heating-induced degradation, leading to sulfur vacancy migration and eventual breakdown. Encapsulation with h-BN and interface engineering can mitigate these effects, but long-term reliability data beyond 10^4 hours are still lacking.
How does the cost of CVD-grown multilayer 2D materials compare to legacy silicon-based technologies?
Current CVD growth of wafer-scale multilayer MoS2 costs approximately $100–$200 per 4-inch wafer, significantly higher than silicon ($10–$20 per wafer). However, for niche applications such as flexible electronics and quantum devices, the performance advantages may justify the premium. Scaling to 8-inch wafers and reducing precursor costs could bring parity by 2030.
What are the scalability bottlenecks for layer-by-layer assembly of 2D heterostructures?
The primary bottlenecks are transfer-induced contamination (polymer residues) and misalignment during stacking, which limit yield to <70% for 3-layer stacks. Automated robotic assembly with sub-micron alignment accuracy and clean transfer techniques (e.g., crack propagation) are essential for achieving >95% yield at wafer scale.
How does the interlayer twist angle affect the electronic properties of multilayer MoS2, and what is the optimal angle for device performance?
Twist angles near 0° or 60° yield aligned (3R or 2H) stacking with high mobility, while intermediate angles (e.g., 30°) create moiré superlattices that can induce flat bands and correlated insulating states. For high-performance transistors, aligned stacking is preferred, but for quantum applications, magic-angle twisted bilayer MoS2 (≈1.1°) shows superconductivity.
What are the current limitations in achieving uniform thickness over large areas for CVD-grown multilayer graphene?
CVD-grown multilayer graphene often exhibits thickness variations of ±1 layer over centimeter scales due to non-uniform carbon supply and substrate imperfections. This leads to inconsistent sheet resistance (e.g., 100–500 Ω/sq). Advanced control of gas flow and substrate surface treatment can reduce variation to <5%, but wafer-scale uniformity remains a challenge.
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