A computational framework for guiding the MOCVD-growth of wafer-scale 2D materials
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Abstract
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 WSe2 model 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.
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Research context
OpenAlex topics: 2D Materials and Applications · Graphene research and applications · Thermal properties of materials
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (58)
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1. Lee, C., Wei, X., Kysar, J. W. & Hone, J. Measurement of the elastic properties and intrinsic strength of monolayer graphene. Sci. (80-.) 321, 385–388 (2008).10.1126/science.1157996 ↗
2. Balandin, A. A. Thermal properties of graphene and nanostructured carbon materials. Nat. Mater. 10, 569–581 (2011).10.1038/nmat3064 ↗
3. Geim, A. K. Graphene: status and prospects. Sci. (80-.) 324, 1530 LP–1531534 (2009).10.1126/science.1158877 ↗
4. Sun, Z., Martinez, A. & Wang, F. Optical modulators with 2D layered materials. Nat. Photonics 10, 227–238 (2016).10.1038/nphoton.2016.15 ↗
5. Mannoor, M. S. et al. Graphene-based wireless bacteria detection on tooth enamel. Nat. Commun. 3, 763 (2012).10.1038/ncomms1767 ↗
6. Lv, R. et al. Ultrasensitive gas detection of large-area boron-doped graphene. Proc. Natl Acad. Sci. USA. 112, 14527–14532 (2015).10.1073/pnas.1505993112 ↗
7. Kim, S. K. et al. Directional dependent piezoelectric effect in CVD grown monolayer MoS2 for flexible piezoelectric nanogenerators. Nano Energy 22, 483–489 (2016).10.1016/j.nanoen.2016.02.046 ↗
8. Wu, W. et al. Piezoelectricity of single-atomic-layer MoS2 for energy conversion and piezotronics. Nature 514, 470–474 (2014).10.1038/nature13792 ↗
9. Bolotsky, A. et al. Two-dimensional materials in biosensing and healthcare: from in vitro diagnostics to optogenetics and beyond. ACS Nano 13, 9781–9810 (2019).10.1021/acsnano.9b03632 ↗
10. Fiori, G. et al. Electronics based on two-dimensional materials. Nat. Nanotechnol. 9, 768–779 (2014).10.1038/nnano.2014.207 ↗
11. Jariwala, D., Sangwan, V. K., Lauhon, L. J., Marks, T. J. & Hersam, M. C. Emerging device applications for semiconducting two-dimensional transition metal dichalcogenides. ACS Nano 8, 1102–1120 (2014).10.1021/nn500064s ↗
12. Voiry, D. et al. The role of electronic coupling between substrate and 2D MoS2 nanosheets in electrocatalytic production of hydrogen. Nat. Mater. 15, 1003–1009 (2016).10.1038/nmat4660 ↗
13. Zhang, J. et al. Discovering superior basal plane active two-dimensional catalysts for hydrogen evolution. Mater. Today 25, 28–34 (2019).10.1016/j.mattod.2019.02.014 ↗
14. Wang, Z. L. Nanobelts, nanowires, and nanodiskettes of semiconducting oxides—from materials to nanodevices. Adv. Mater. 15, 432–436 (2003).10.1002/adma.200390100 ↗
15. Li, H., Wu, J., Yin, Z. & Zhang, H. Preparation and applications of mechanically exfoliated single-layer and multilayer MoS2 and WSe2 nanosheets. Acc. Chem. Res. 47, 1067–1075 (2014).10.1021/ar4002312 ↗
16. Nicolosi, V., Chhowalla, M., Kanatzidis, M. G., Strano, M. S. & Coleman, J. N. Liquid exfoliation of layered materials. Sci. (80-.) 340, 1226419 (2013).10.1126/science.1226419 ↗
17. Huang, J. et al. Large-area synthesis of monolayer WSe2 on a SiO2/Si substrate and its device applications. Nanoscale 7, 4193–4198 (2015).10.1039/C4NR07045C ↗
18. Zhou, H. et al. Large area growth and electrical properties of p-type WSe2 atomic layers. Nano Lett. 15, 709–713 (2015).10.1021/nl504256y ↗
19. Chen, L. et al. Step-edge-guided nucleation and growth of aligned WSe2 on Sapphire via a layer-over-layer growth mode. ACS Nano 9, 8368–8375 (2015).10.1021/acsnano.5b03043 ↗
20. Vishwanath, S. et al. Comprehensive structural and optical characterization of MBE grown MoSe2 on graphite, CaF2 and graphene. 2D Mater. 2, 24007 (2015).10.1088/2053-1583/2/2/024007 ↗
21. Mortelmans, W. et al. Epitaxial registry and crystallinity of MoS2 via molecular beam and metalorganic vapor phase van der Waals epitaxy. Appl. Phys. Lett. 117, 33101 (2020).10.1063/5.0013391 ↗
22. Nakano, M., Wang, Y., Kashiwabara, Y., Matsuoka, H. & Iwasa, Y. Layer-by-layer epitaxial growth of scalable WSe2 on sapphire by molecular beam epitaxy. Nano Lett. 17, 5595–5599 (2017).10.1021/acs.nanolett.7b02420 ↗
23. Liu, H. J. et al. Molecular-beam epitaxy of monolayer and bilayer WSe2: a scanning tunneling microscopy/spectroscopy study and deduction of exciton binding energy. 2D Mater. 2, 34004 (2015).10.1088/2053-1583/2/3/034004 ↗
24. Zhang, Y. et al. Direct observation of the transition from indirect to direct bandgap in atomically thin epitaxial MoSe2. Nat. Nanotechnol. 9, 111–115 (2014).10.1038/nnano.2013.277 ↗
25. Zhang, X. et al. Diffusion-controlled epitaxy of large area coalesced WSe2 monolayers on sapphire. Nano Lett. 18, 1049–1056 (2018).10.1021/acs.nanolett.7b04521 ↗
26. Lin, Y. C. et al. Realizing large-scale, electronic-grade two-dimensional semiconductors. ACS Nano 12, 965–975 (2018).10.1021/acsnano.7b07059 ↗
27. Eichfeld, S. M. et al. Highly scalable, atomically Thin WSe2 grown via metal–organic chemical vapor deposition. ACS Nano 9, 2080–2087 (2015).10.1021/nn5073286 ↗
28. Kang, K. et al. High-mobility three-atom-thick semiconducting films with wafer-scale homogeneity. Nature 520, 656–660 (2015).10.1038/nature14417 ↗
29. Kranthi Kumar, V., Dhar, S., Choudhury, T. H., Shivashankar, S. A. & Raghavan, S. A predictive approach to CVD of crystalline layers of TMDs: the case of MoS2. Nanoscale 7, 7802–7810 (2015).10.1039/C4NR07080A ↗
30. Kim, T. et al. Wafer-scale production of highly uniform two-dimensional MoS2 by metal-organic chemical vapor deposition. Nanotechnology 28, 18LT01 (2017).10.1088/1361-6528/aa6958 ↗
31. Kalanyan, B. et al. Rapid wafer-scale growth of polycrystalline 2H-MoS2 by pulsed metal-organic chemical vapor deposition. Chem. Mater. 29, 6279–6288 (2017).10.1021/acs.chemmater.7b01367 ↗
32. Shi, Y. et al. van der waals epitaxy of MoS2 layers using graphene as growth templates. Nano Lett. 12, 2784–2791 (2012).10.1021/nl204562j ↗
33. Bianco, G. V. et al. Direct epitaxial CVD synthesis of tungsten disulfide on epitaxial and CVD graphene. RSC Adv. 5, 98700–98708 (2015).10.1039/C5RA19698A ↗
34. Zhang, F. et al. Controlled synthesis of 2D transition metal dichalcogenides: from vertical to planar MoS2. 2D Mater. 4, 025029 (2017).10.1088/2053-1583/aa5b01 ↗
35. Vilá, R. A. et al. Bottom-up synthesis of vertically oriented two-dimensional materials. 2D Mater. 3, 041003 (2016).10.1088/2053-1583/3/4/041003 ↗
36. Artyukhov, V. I., Liu, Y. & Yakobson, B. I. Equilibrium at the edge and atomistic mechanisms of graphene growth. Proc. Natl Acad. Sci. USA. 109, 15136–15140 (2012).10.1073/pnas.1207519109 ↗
37. Liu, Y., Bhowmick, S. & Yakobson, B. I. BN White Graphene with “Colorful” edges: the energies and morphology. Nano Lett. 11, 3113–3116 (2011).10.1021/nl2011142 ↗
38. Paul, S., Torsi, R., Robinson, J. A. & Momeni, K. Effect of the substrate on MoS2 monolayer morphology: an integrated computational and experimental study. ACS Appl. Mater. Interfaces 14, 18835–18844 (2022).10.1021/acsami.2c03471 ↗
39. Paul, S., Momeni, K. & Levitas, V. I. Shear-induced diamondization of multilayer graphene structures: a computational study. Carbon 167, 140–147 (2020).10.1016/j.carbon.2020.05.038 ↗
40. Paul, S. & Momeni, K. Mechanochemistry of stable diamane and atomically thin diamond films synthesis from Bi- and multilayer graphene: a computational study. J. Phys. Chem. C. 123, 15751–15760 (2019).10.1021/acs.jpcc.9b02149 ↗
41. Momeni, K., Attariani, H. & Lesar, R. A. R. A. Structural transformation in monolayer materials: A 2D to 1D transformation. Phys. Chem. Chem. Phys. 18, 19873–19879 (2016).10.1039/C6CP04007A ↗
42. Meca, E., Lowengrub, J., Kim, H., Mattevi, C. & Shenoy, V. B. Epitaxial graphene growth and shape dynamics on copper: phase-field modeling and experiments. Nano Lett. 13, 5692–5697 (2013).10.1021/nl4033928 ↗
43. Guo, Z., Price, C., Shenoy, V. B. & Lowengrub, J. Modeling the vertical growth of van der Waals stacked 2D materials using the diffuse domain method. Model. Simul. Mater. Sci. Eng. 28, 25002 (2020).10.1088/1361-651X/ab5e9a ↗
44. Ye, H. et al. Toward a mechanistic understanding of vertical growth of van der waals stacked 2D materials: a multiscale model and experiments. ACS Nano 11, 12780–12788 (2017).10.1021/acsnano.7b07604 ↗
45. Momeni, K., Ji, Y. & Chen, L.-Q. Computational synthesis of 2D materials grown by chemical vapor deposition. J. Mater. Res. 37, 114–123 (2022).10.1557/s43578-021-00384-2 ↗
46. Ji, Y., Momeni, K. & Chen, L.-Q. A multiscale insight into the growth of h-BN: effect of the enclosure. 2D Mater. 8, 035033 (2021).10.1088/2053-1583/abfcaa ↗
47. Momeni, K. et al. Multiscale computational understanding and growth of 2D materials: a review. npj Comput. Mater. 6, 22 (2020).10.1038/s41524-020-0280-2 ↗
48. Briggs, N. et al. A roadmap for electronic grade 2D materials. 2D Mater. 6, 022001 (2019).10.1088/2053-1583/aaf836 ↗
49. Momeni, K., Ji, Y., Zhang, K., Robinson, J. A. & Chen, L.-Q. Multiscale framework for simulation-guided growth of 2D materials. npj 2D Mater. Appl 2, 27 (2018).10.1038/s41699-018-0072-4 ↗
50. Baugher, B. W. H., Churchill, H. O. H., Yang, Y. & Jarillo-Herrero, P. Optoelectronic devices based on electrically tunable p–n diodes in a monolayer dichalcogenide. Nat. Nanotechnol. 9, 262–267 (2014).10.1038/nnano.2014.25 ↗
51. Kim, H. et al. Synthetic WSe2 monolayers with high photoluminescence quantum yield. Sci. Adv. 5, eaau4728 (2019).10.1126/sciadv.aau4728 ↗
52. Mak, K. F., Lee, C., Hone, J., Shan, J. & Heinz, T. F. Atomically thin MoS2: a new direct-gap semiconductor. Phys. Rev. Lett. 105, 136805 (2010).10.1103/PhysRevLett.105.136805 ↗
53. Fang, H. et al. High-performance single layered WSe2 p-FETs with chemically doped contacts. Nano Lett. 12, 3788–3792 (2012).10.1021/nl301702r ↗
54. Nayir, N. et al. Modeling for structural engineering and synthesis of two-dimensional WSe2 using a newly developed ReaxFF reactive force field. J. Phys. Chem. C. 124, 28285–28297 (2020).10.1021/acs.jpcc.0c09155 ↗
55. Yue, R. et al. Nucleation and growth of WSe2: enabling large grain transition metal dichalcogenides. 2D Mater. 4, 45019 (2017).10.1088/2053-1583/aa8ab5 ↗
56. Fuller, E. N., Ensley, K. & Giddings, J. C. Diffusion of halogenated hydrocarbons in helium. The effect of structure on collision cross sections. J. Phys. Chem. 73, 3679–3685 (1969).10.1021/j100845a020 ↗
57. Fuller, E. N., Schettler, P. D. & Giddings, J. C. A new method for prediction of binary gas-phase diffusion coefficients. Ind. Eng. Chem. 58, 18–27 (1966).10.1021/ie50677a007 ↗
58. Schlichting, H. & Gersten, K. Boundary-Layer Theory (Springer, 2017).10.1007/978-3-662-52919-5 ↗