Reconstructing bulk crystal-like structures via solution assembly of 2D nanosheets
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Abstract
Abstract Solution-processed electronics based on two-dimensional materials rely on the deposition of high-quality nanosheet networks to produce high-performance devices, but creating devices with performance approaching the intrinsic limits of the 2D material requires structures that resemble bulk crystal conditions. This Perspective compares two assembly techniques that have achieved this by decoupling in-plane packing and out-of-plane stacking: spin coating and liquid-interface deposition. By outlining their respective strengths and limitations, we provide an overview on selecting appropriate deposition strategies to advance high-performance large-area electronics.
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Research context
OpenAlex topics: 2D Materials and Applications · Solar-Powered Water Purification Methods · Nanowire Synthesis and Applications
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References (62)
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1. Hu, G. et al. Functional inks and printing of two-dimensional materials. Chem. Soc. Rev. 47, 3265–3300 (2018).10.1039/C8CS00084K ↗
2. Torrisi, F. & Carey, T. Graphene, related two-dimensional crystals and hybrid systems for printed and wearable electronics. Nano Today 23, 73–96 (2018).10.1016/j.nantod.2018.10.009 ↗
3. Kelly, A. G. et al. All-printed thin-film transistors from networks of liquid-exfoliated nanosheets. Science 356, 69–73 (2017).10.1126/science.aal4062 ↗
4. Conti, S. et al. Low-voltage 2D materials-based printed field-effect transistors for integrated digital and analog electronics on paper. Nat. Commun. 11, 3566 (2020).10.1038/s41467-020-17297-z ↗
5. Park, S.-H. et al. High areal capacity battery electrodes enabled by segregated nanotube networks. Nat. Energy 4, 560–567 (2019).10.1038/s41560-019-0398-y ↗
6. Kim, S. J. et al. High mass loading, binder-free MXene anodes for high areal capacity Li-ion batteries. Electrochim. Acta 163, 246–251 (2015).10.1016/j.electacta.2015.02.132 ↗
7. Tang, B. et al. Wafer-scale solution-processed 2D material analog resistive memory array for memory-based computing. Nat. Commun. 13, 3037 (2022).10.1038/s41467-022-30519-w ↗
8. Sangwan, V. K. et al. Visualizing Thermally Activated Memristive Switching in Percolating Networks of Solution-Processed 2D Semiconductors. Adv. Funct. Mater. 31, 2107385 (2021).10.1002/adfm.202107385 ↗
9. Kelly, A. G., Finn, D., Harvey, A., Hallam, T. & Coleman, J. N. All-printed capacitors from graphene-BN-graphene nanosheet heterostructures. Appl. Phys. Lett. 109, 023107 (2016).10.1063/1.4958858 ↗
10. Nalawade, Y. et al. All-Printed Dielectric Capacitors from High-Permittivity, Liquid-Exfoliated BiOCl Nanosheets. ACS Appl. Electron. Mater. 2, 3233–3241 (2020).10.1021/acsaelm.0c00561 ↗
11. Zhu, J. et al. Layer-by-Layer Assembled 2D Montmorillonite Dielectrics for Solution-Processed Electronics. Adv. Mater. 28, 63–68 (2016).10.1002/adma.201504501 ↗
12. Shahzad, F. et al. Electromagnetic interference shielding with 2D transition metal carbides (MXenes). Science 353, 1137–1140 (2016).10.1126/science.aag2421 ↗
13. Kelly, A. G. et al. Highly Conductive Networks of Silver Nanosheets. Small 18, 2105996 (2022).10.1002/smll.202105996 ↗
14. Bonaccorso, F., Bartolotta, A., Coleman, J. N. & Backes, C. 2D-Crystal-Based Functional Inks. Adv. Mater. 28, 6136–6166 (2016).10.1002/adma.201506410 ↗
15. Lin, Z. et al. Solution-processable 2D semiconductors for high-performance large-area electronics. Nature 562, 254 (2018).10.1038/s41586-018-0574-4 ↗
16. Li, J. et al. Printable two-dimensional superconducting monolayers. Nat. Mater. 1–7 (2020) doi:Intra-%20and%20inter-nanocrystal%20charge%20transport%20in%20nanocrystal%20films.
17. Biccai, S. et al. Exfoliation of 2D materials by high shear mixing. 2D Mater. 6, 015008 (2018).10.1088/2053-1583/aae7e3 ↗
18. Secor, E. B., Ahn, B. Y., Gao, T. Z., Lewis, J. A. & Hersam, M. C. Rapid and Versatile Photonic Annealing of Graphene Inks for Flexible Printed Electronics. Adv. Mater. 27, 6683–6688 (2015).10.1002/adma.201502866 ↗
19. Torrisi, F. et al. Inkjet-Printed Graphene Electronics. ACS Nano 6, 2992–3006 (2012).10.1021/nn2044609 ↗
20. Finn, D. J. et al. Inkjet deposition of liquid-exfoliated graphene and MoS2 nanosheets for printed device applications. J. Mater. Chem. C. 2, 925–932 (2014).10.1039/C3TC31993H ↗
21. Li, J. et al. Efficient Inkjet Printing of Graphene. Adv. Mater. 25, 3985–3992 (2013).10.1002/adma.201300361 ↗
22. Kelly, A. G., O’Suilleabhain, D., Gabbett, C. & Coleman, J. N. The electrical conductivity of solution-processed nanosheet networks. Nat. Rev. Mater. 1–18 https://doi.org/10.1038/s41578-021-00386-w (2021).10.1038/s41578-021-00386-w ↗
23. Carey, T. et al. High-Mobility Flexible Transistors with Low-Temperature Solution-Processed Tungsten Dichalcogenides. ACS Nano https://doi.org/10.1021/acsnano.2c11319 (2023) .10.1021/acsnano.2c11319 ↗
24. Zhou, J. et al. Layered Intercalation Materials. Adv. Mater. 33, 2004557 (2021).10.1002/adma.202004557 ↗
25. Zhao, M., Casiraghi, C. & Parvez, K. Electrochemical exfoliation of 2D materials beyond graphene. Chem. Soc. Rev. 53, 3036–3064 (2024).10.1039/D3CS00815K ↗
26. Yang, R. et al. Synthesis of atomically thin sheets by the intercalation-based exfoliation of layered materials. Nat. Synth. 2, 101–118 (2023).10.1038/s44160-022-00232-z ↗
27. Yang, R. et al. Intercalation in 2D materials and in situ studies. Nat. Rev. Chem. 8, 410–432 (2024).10.1038/s41570-024-00605-2 ↗
28. Hinrichsen, E. L., Feder, J. & Jøssang, T. Random packing of disks in two dimensions. Phys. Rev. A 41, 4199–4209 (1990).10.1103/PhysRevA.41.4199 ↗
29. Cheng, F. et al. Two-dimensional tessellation by molecular tiles constructed from halogen–halogen and halogen–metal networks. Nat. Commun. 9, 4871 (2018).10.1038/s41467-018-07323-6 ↗
30. Neilson, J., Avery, M. P. & Derby, B. Tiled Monolayer Films of 2D Molybdenum Disulfide Nanoflakes Assembled at Liquid/Liquid Interfaces. ACS Appl. Mater. Interfaces 12, 25125–25134 (2020).10.1021/acsami.0c03794 ↗
31. Sakai, N. & Sasaki, T. Highly Organized Monolayer Arrangement of 2D Materials and Its Applications. Acc. Mater. Res. 5, 752–760 (2024).10.1021/accountsmr.4c00072 ↗
32. Quickenden, T. I. & Tan, G. K. Random packing in two dimensions and the structure of monolayers. J. Colloid Interface Sci. 48, 382–393 (1974).10.1016/0021-9797(74)90181-7 ↗
33. Donev, A., Torquato, S., Stillinger, F. H. & Connelly, R. Jamming in hard sphere and disk packings. J. Appl. Phys. 95, 989–999 (2004).10.1063/1.1633647 ↗
34. He, J. et al. Solution-processed wafer-scale indium selenide semiconductor thin films with high mobilities. Nat Electron https://doi.org/10.1038/s41928-025-01338-w (2025) .10.1038/s41928-025-01338-w ↗
35. Carey, T. et al. Inkjet Printed Circuits with 2D Semiconductor Inks for High-Performance Electronics. Adv. Electron. Mater. 7, 2100112 (2021).10.1002/aelm.202100112 ↗
36. Kelly, Adam G. et al. High-viscosity constraints in the solution-processing of carbon nanomaterials using Cyrene. Carbon 121453 (2026).10.1016/j.carbon.2026.121453 ↗
37. Sakai, N. & Sasaki, T. Guidelines for Arranging 2D Nanosheets into Neatly Tiled Monolayer Films by a Spin-Coating Process. Langmuir 38, 12399–12407 (2022).10.1021/acs.langmuir.2c02211 ↗
38. Dai, Y., He, Q., Huang, Y., Duan, X. & Lin, Z. Solution-Processable and Printable Two-Dimensional Transition Metal Dichalcogenide Inks. Chem. Rev. 124, 5795–5845 (2024).10.1021/acs.chemrev.3c00791 ↗
39. Xue, J. et al. Solution-processable assembly of 2D semiconductor thin films and superlattices with photoluminescent monolayer inks. Chem S2451929424000202 (2024) doi:9.10.1016/j.chempr.2024.01.016 ↗
40. Matsuba, K. et al. Neat monolayer tiling of molecularly thin two-dimensional materials in 1 min. Sci. Adv. 3, e1700414 (2017).10.1126/sciadv.1700414 ↗
41. Yan, Z. et al. Highly stretchable van der Waals thin films for adaptable and breathable electronic membranes. Science 375, 852–859 (2022).10.1126/science.abl8941 ↗
42. Woltornist, S. J., Oyer, A. J., Carrillo, J.-M. Y., Dobrynin, A. V. & Adamson, D. H. Conductive Thin Films of Pristine Graphene by Solvent Interface Trapping. ACS Nano 7, 7062–7066 (2013).10.1021/nn402371c ↗
43. Biswas, S. & Drzal, L. T. A Novel Approach to Create a Highly Ordered Monolayer Film of Graphene Nanosheets at the Liquid−Liquid Interface. Nano Lett. 9, 167–172 (2009).10.1021/nl802724f ↗
44. Zheng, Q. et al. Transparent Conductive Films Consisting of Ultralarge Graphene Sheets Produced by Langmuir–Blodgett Assembly. ACS Nano 5, 6039–6051 (2011).10.1021/nn2018683 ↗
45. Lvov, Y., Ariga, K., Ichinose, I. & Kunitake, T. Formation of Ultrathin Multilayer and Hydrated Gel from Montmorillonite and Linear Polycations. Langmuir 12, 3038–3044 (1996).10.1021/la951002d ↗
46. Li, X. et al. Highly conducting graphene sheets and Langmuir–Blodgett films. Nat. Nanotech 3, 538–542 (2008).10.1038/nnano.2008.210 ↗
47. Yu, X., Prévot, M. S., Guijarro, N. & Sivula, K. Self-assembled 2D WSe2 thin films for photoelectrochemical hydrogen production. Nat. Commun. 6, 7596 (2015).10.1038/ncomms8596 ↗
48. Cote, L. J., Kim, J., Zhang, Z., Sun, C. & Huang, J. Tunable assembly of graphene oxide surfactant sheets: wrinkles, overlaps and impacts on thin film properties. Soft Matter 6, 6096–6101 (2010).10.1039/c0sm00667j ↗
49. Cassidy, O. et al. Layer-by-layer assembly yields thin graphene films with near theoretical conductivity. npj 2D Mater. Appl 9, 1–11 (2025).10.1038/s41699-025-00525-9 ↗
50. Shi, Y., Osada, M., Ebina, Y. & Sasaki, T. Single Droplet Assembly for Two-Dimensional Nanosheet Tiling. ACS Nano 14, 15216–15226 (2020).10.1021/acsnano.0c05434 ↗
51. Shi, Y. et al. Ultrafast 2D Nanosheet Assembly via Spontaneous Spreading Phenomenon. Small 2403915 https://doi.org/10.1002/smll.202403915 (2024).10.1002/smll.202403915 ↗
52. Gabbett, C. et al. Understanding how junction resistances impact the conduction mechanism in nano-networks. Nat. Commun. 15, 4517 (2024).10.1038/s41467-024-48614-5 ↗
53. Gabbett, C. et al. Quantitative analysis of printed nanostructured networks using high-resolution 3D FIB-SEM nanotomography. Nat. Commun. 15, 278 (2024).10.1038/s41467-023-44450-1 ↗
54. Neilson, J. et al. Production of Ultrathin and High-Quality Nanosheet Networks via Layer-by-Layer Assembly at Liquid–Liquid Interfaces. ACS Nano 18, 32589–32601 (2024).10.1021/acsnano.4c09745 ↗
55. Carey, T. et al. Electronic properties and circuit applications of networks of electrochemically exfoliated 2D nanosheets. Nat. Commun. 16, 9038 (2025).10.1038/s41467-025-64100-y ↗
56. Tang, B. et al. Solution-processable 2D materials for monolithic 3D memory-sensing-computing platforms: opportunities and challenges. npj 2D Mater. Appl 8, 74 (2024).10.1038/s41699-024-00508-2 ↗
57. Wells, R. A., Johnson, H., Lhermitte, C. R., Kinge, S. & Sivula, K. Roll-to-Roll Deposition of Semiconducting 2D Nanoflake Films of Transition Metal Dichalcogenides for Optoelectronic Applications. ACS Appl. Nano Mater. 2, 7705–7712 (2019).10.1021/acsanm.9b01774 ↗
58. Neilson, J., Cataldi, P. & Derby, B. Graphene-Based Transparent Flexible Strain Gauges with Tunable Sensitivity and Strain Range. ACS Appl. Nano Mater. 6, 21763–21774 (2023).10.1021/acsanm.3c03967 ↗
59. Prat, D. et al. CHEM21 selection guide of classical- and less classical-solvents. Green. Chem. 18, 288–296 (2016).10.1039/C5GC01008J ↗
60. Ly, T. H. et al. Misorientation-angle-dependent electrical transport across molybdenum disulfide grain boundaries. Nat. Commun. 7, 10426 (2016).10.1038/ncomms10426 ↗
61. Kelly, A. G. Junction engineering in solution-processed nanosheet networks. npj 2D Mater. Appl 10, 10 (2025).10.1038/s41699-025-00647-0 ↗
62. Pham, P. V. et al. 2D Heterostructures for Ubiquitous Electronics and Optoelectronics: Principles, Opportunities, and Challenges. Chem. Rev. 122, 6514–6613 (2022).10.1021/acs.chemrev.1c00735 ↗