skip to main content


Title: Multiscale framework for simulation-guided growth of 2D materials
Abstract

Chemical vapor deposition (CVD) is a powerful technique for synthesizing monolayer materials such as transition metal dichalcogenides. It has advantages over exfoliation techniques, including higher purity and the ability to control the chemistry of the products. However, controllable and reproducible synthesis of 2D materials using CVD is a challenge because of the complex growth process and its sensitivity to subtle changes in growth conditions, making it difficult to extend conclusions obtained in one CVD chamber to another. Here, we developed a multiscale model linking CVD control parameters to the morphology, size, and distribution of synthesized 2D materials. Its capabilities are experimentally validated via the systematic growth of MoS2. In particular, we coupled the reactor-scale governing heat and mass transport equations with the mesoscale phase-field equations for the growth morphology considering the variation of edge energies with the precursor concentration within the growth chamber. The predicted spatial distributions of 2D islands are statistically analyzed, and experiments are then performed to validate the predicted island morphology and distributions. It is shown that the model can be employed to predict and control the morphology and characteristics of synthesized 2D materials.

 
more » « less
NSF-PAR ID:
10154427
Author(s) / Creator(s):
; ; ; ;
Publisher / Repository:
Nature Publishing Group
Date Published:
Journal Name:
npj 2D Materials and Applications
Volume:
2
Issue:
1
ISSN:
2397-7132
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Reproducible wafer-scale growth of two-dimensional (2D) materials using the Chemical Vapor Deposition (CVD) process with precise control over their properties is challenging due to a lack of understanding of the growth mechanisms spanning over several length scales and sensitivity of the synthesis to subtle changes in growth conditions. A multiscale computational framework coupling Computational Fluid Dynamics (CFD), Phase-Field (PF), and reactive Molecular Dynamics (MD) was developed – called the CPM model – and experimentally verified. Correlation between theoretical predictions and thorough experimental measurements for a Metal-Organic CVD (MOCVD)-grown WSe2model material revealed the full power of this computational approach. Large-area uniform 2D materials are synthesized via MOCVD, guided by computational analyses. The developed computational framework provides the foundation for guiding the synthesis of wafer-scale 2D materials with precise control over the coverage, morphology, and properties, a critical capability for fabricating electronic, optoelectronic, and quantum computing devices.

     
    more » « less
  2. Abstract

    The exotic properties of 2D materials made them ideal candidates for applications in quantum computing, flexible electronics, and energy technologies. A major barrier to their adaptation for industrial applications is their controllable and reproducible growth at a large scale. A significant effort has been devoted to the chemical vapor deposition (CVD) growth of wafer-scale highly crystalline monolayer materials through exhaustive trial-and-error experimentations. However, major challenges remain as the final morphology and growth quality of the 2D materials may significantly change upon subtle variation in growth conditions. Here, we introduced a multiscale/multiphysics model based on coupling continuum fluid mechanics and phase-field models for CVD growth of 2D materials. It connects the macroscale experimentally controllable parameters, such as inlet velocity and temperature, and mesoscale growth parameters such as surface diffusion and deposition rates, to morphology of the as-grown 2D materials. We considered WSe2as our model material and established a relationship between the macroscale growth parameters and the growth coverage. Our model can guide the CVD growth of monolayer materials and paves the way to their synthesis-by-design.

    Graphic abstract 
    more » « less
  3. Abstract

    The large‐area synthesis of high‐quality MoS2plays an important role in realizing industrial applications of optoelectronics, nanoelectronics, and flexible devices. However, current techniques for chemical vapor deposition (CVD)‐grown MoS2require a high synthetic temperature and a transfer process, which limits its utilization in device fabrications. Here, the direct synthesis of high‐quality monolayer MoS2with the domain size up to 120 µm by metal‐organic CVD (MOCVD) at a temperature of 320 °C is reported. Owing to the low‐substrate temperature, the MOCVD‐grown MoS2exhibits low impurity doping and nearly unstrained properties on the growth substrate, demonstrating enhanced electronic performance with high electron mobility of 68.3 cm2V−1s−1at room temperature. In addition, by tuning the precursor ratio, a better understanding of the MoS2growth process via a geometric model of the MoS2flake shape, is developed, which can provide further guidance for the synthesis of 2D materials.

     
    more » « less
  4. Abstract

    Two‐dimensional coordination polymers (2DCPs) have been predicted to exhibit exotic properties such as superconductivity, topological insulating behavior, catalytic activity, and superior ion transport for energy applications; experimentally, these materials have fallen short of their expectation due to the lack of synthesis protocols that yield continuous, large crystallite domains, and highly ordered thin films with controllable physical and chemical properties. Herein, the fabrication of large‐area, highly ordered 2DCP thin films with large crystallite domains using chemical vapor deposition (CVD) approaches is described. It is demonstrated that defects and the packing motifs of 2DCP thin films may be controlled by adjusting the vapor–vapor and vapor–solid interactions of the metal and organic linker precursors during the CVD fabrication process. Such control allows for the fabrication of defects‐controlled 2DCP thin films that show either semiconducting or metallic behavior. The findings provide the first demonstration of tuning the electrical properties of sub 100 nm‐thick continuous 2DCP thin films by controlling their electronic landscape through defect engineering. As such, it is determined that large‐area, highly ordered 2DCP thin films may undergo a semiconducting to metallic transition that is correlated to changes in morphology, crystalline domain sizes, crystallite orientation, defect interactions, and electronic structure.

     
    more » « less
  5. Abstract

    2D materials‐based device performance is significantly affected by film non‐uniformity, especially for large area devices. Here, it investigates the dependence of large area 2D MoS2phototransistor performance on film morphology through correlative mapping. Monolayer MoS2films are quazi‐epitaxially synthesized on C‐plane sapphire (Al2O3) substrates by chemical vapor deposition, and the growth time and molybdenum trioxide MoO3precursor volume are varied to obtain variations in film morphology. Raman, photoluminescence, transmittance, and photocurrent maps are generated and compared with each other to obtain a holistic understanding of large area 2D optoelectronic device performance. For example, it shows that the photoluminescence peak shift and intensity can be used to investigate strain and other defects across multiple film morphologies, giving insight into their effects on the photogenerated current in these devices. It also combines photocurrent and absorption maps to generate large area high‐resolution external quantum efficiency and internal quantum efficiency maps for the devices. This study demonstrates the benefit of correlative mapping in the understanding and advancement of large area 2D material‐based electronic and optoelectronic devices.

     
    more » « less