journal article·2025-05-07Open access

Rapid assembly of highly ordered DNA origami lattices at mica surfaces

Bhanu Kiran Pothineni, Jörg Barner, Guido Grundmeier, David Contreras, Mario Castro, Adrian Keller

Discover Nano· Volume 20· Issue 1

Abstract

Abstract The surface-assisted assembly of DNA origami lattices is a potent method for creating molecular lithography masks. Lattice quality and assembly kinetics are controlled by various environmental parameters, including the employed surface, the assembly temperature, and the ionic composition of the buffer, with optimized parameter combinations resulting in highly ordered lattices that can span surface areas of several cm2. Established assembly protocols, however, employ assembly times ranging from hours to days. Here, the assembly of highly ordered hexagonal DNA origami lattices at mica surfaces is observed within few minutes using high-speed atomic force microscopy (HS-AFM). A moderate increase in the DNA origami concentration enables this rapid assembly. While forming a regular lattice takes 10 min at a DNA origami concentration of 4 nM, this time is shortened to about 2 min at a concentration of 6 nM. Increasing the DNA origami concentration any further does not result in shorter assembly times, presumably because DNA origami arrival at the mica surface is diffusion-limited. Over short length scales up to 1 µm, lattice order is independent of the DNA origami concentration. However, at larger length scales of a few microns, a DNA origami concentration of 10 nM yields slightly better order than lower and higher concentrations. Therefore, 10 nM can be considered the optimum concentration for the rapid assembly of highly ordered DNA origami lattices. These results thus represent an important step toward the industrial-scale application of DNA origami-based lithography masks.
Source: crossref · Quality: baseline

Research context

OpenAlex topics: Advanced biosensing and bioanalysis techniques · RNA Interference and Gene Delivery · Nanopore and Nanochannel Transport Studies

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (49)

Show source-provided references
1. Elemans JAAW, Lei S, de Feyter S. Molecular and supramolecular networks on surfaces: from two-dimensional crystal engineering to reactivity. Angew Chem Int Ed Engl. 2009;48:7298–332. https://doi.org/10.1002/anie.200806339.10.1002/anie.200806339 ↗
2. Kudernac T, Lei S, Elemans JAAW, de Feyter S. Two-dimensional supramolecular self-assembly: nanoporous networks on surfaces. Chem Soc Rev. 2009;38:402–21. https://doi.org/10.1039/B708902N.10.1039/B708902N ↗
3. Peng X, Zhao F, Peng Y, Li J, Zeng Q. Dynamic surface-assisted assembly behaviours mediated by external stimuli. Soft Matter. 2020;16:54–63. https://doi.org/10.1039/C9SM01847F.10.1039/C9SM01847F ↗
4. Verstraete L, de Feyter S. 2D self-assembled molecular networks and on-surface reactivity under nanoscale lateral confinement. Chem Soc Rev. 2021;50:5884–97. https://doi.org/10.1039/D0CS01338B.10.1039/D0CS01338B ↗
5. Vigier-Carrière C, Boulmedais F, Schaaf P, Jierry L. Surface-Assisted self-assembly strategies leading to supramolecular hydrogels. Angew Chem Int Ed Engl. 2018;57:1448–56. https://doi.org/10.1002/anie.201708629.10.1002/anie.201708629 ↗
6. Yang B, Adams DJ, Marlow M, Zelzer M. Surface-mediated supramolecular self-assembly of protein, peptide, and nucleoside derivatives: from surface design to the underlying mechanism and tailored functions. Langmuir. 2018;34:15109–25. https://doi.org/10.1021/acs.langmuir.8b01165.10.1021/acs.langmuir.8b01165 ↗
7. Kundu B, Eltohamy M, Yadavalli VK, Kundu SC, Kim H-W. Biomimetic designing of functional silk nanotopography using self-assembly. ACS Appl Mater Interfaces. 2016;8:28458–67. https://doi.org/10.1021/acsami.6b07872.10.1021/acsami.6b07872 ↗
8. Xu T, Liang C, Ji S, Ding D, Kong D, Wang L, Yang Z. Surface-induced hydrogelation for fluorescence and naked-eye detections of enzyme activity in blood. Anal Chem. 2016;88:7318–23. https://doi.org/10.1021/acs.analchem.6b01660.10.1021/acs.analchem.6b01660 ↗
9. Li J, Liu C, Han X, Tian M, Jiang B, Li W, Ou C, Dou N, Han Z, Ji T, et al. Supramolecular electronics: monolayer assembly of nonamphiphilic molecules via water surface-assisted molecular deposition. ACS Appl Mater Interfaces. 2024;16:48438–47. https://doi.org/10.1021/acsami.4c05552.10.1021/acsami.4c05552 ↗
10. Hu T, Minoia A, Velpula G, Ryskulova K, van Hecke K, Lazzaroni R, Mali KS, Hoogenboom R, de Feyter S. From one-dimensional disordered racemate to ordered racemic conglomerates through metal-coordination-driven self-assembly at the liquid-solid interface. Chem Eur J. 2024;30:e202302545. https://doi.org/10.1002/chem.202302545.10.1002/chem.202302545 ↗
11. Abb S, Harnau L, Gutzler R, Rauschenbach S, Kern K. Two-dimensional honeycomb network through sequence-controlled self-assembly of oligopeptides. Nat Commun. 2016;7:10335. https://doi.org/10.1038/ncomms10335.10.1038/ncomms10335 ↗
12. Pyles H, Zhang S, Yoreo JJ. Controlling protein assembly on inorganic crystals through designed protein interfaces. Nature. 2019;571:251–6. https://doi.org/10.1038/s41586-019-1361-6.10.1038/s41586-019-1361-6 ↗
13. Sun X, Hyeon Ko S, Zhang C, Ribbe AE, Mao C. Surface-mediated DNA self-assembly. J Am Chem Soc. 2009;131:13248–9. https://doi.org/10.1021/ja906475w.10.1021/ja906475w ↗
14. Li X, Wang J, Baptist AV, Wu W, Heuer-Jungemann A, Zhang T. Crystalline assemblies of DNA nanostructures and their functional properties. Angew Chem Int Ed Engl. 2025;64:e202416948. https://doi.org/10.1002/anie.202416948.10.1002/anie.202416948 ↗
15. Parikka JM, Sokołowska K, Markešević N, Toppari JJ. Constructing large 2D lattices out of DNA-tiles. Molecules. 2021;26:1502. https://doi.org/10.3390/molecules26061502.10.3390/molecules26061502 ↗
16. Julin S, Keller A, Linko V. Dynamics of DNA origami lattices. Bioconjug Chem. 2023;34:18–29. https://doi.org/10.1021/acs.bioconjchem.2c00359.10.1021/acs.bioconjchem.2c00359 ↗
17. Xin Y, Martinez Rivadeneira S, Grundmeier G, Castro M, Keller A. Self-assembly of highly ordered DNA origami lattices at solid-liquid interfaces by controlling cation binding and exchange. Nano Res. 2020;13:3142–50. https://doi.org/10.1007/s12274-020-2985-4.10.1007/s12274-020-2985-4 ↗
18. Tapio K, Kielar C, Parikka JM, Keller A, Järvinen H, Fahmy K, Toppari JJ. Large-scale formation of DNA origami lattices on silicon. Chem Mater. 2023;35:1961–71. https://doi.org/10.1021/acs.chemmater.2c03190.10.1021/acs.chemmater.2c03190 ↗
19. Tekin C, Caroprese V, Bastings MMC. Dynamic Surface interactions enable the self-assembly of perfect supramolecular crystals. ACS Appl Mater Interfaces. 2024;16:59040–8. https://doi.org/10.1021/acsami.4c11813.10.1021/acsami.4c11813 ↗
20. Aghebat Rafat A, Pirzer T, Scheible MB, Kostina A, Simmel FC. Surface-assisted large-scale ordering of DNA origami tiles. Angew Chem Int Ed Engl. 2014;53:7665–8. https://doi.org/10.1002/anie.201403965.10.1002/anie.201403965 ↗
21. Liu L, Mao D, Li Z, Zheng M, He K, Mao C. Surface-assisted self-assembly of 2D, DNA Binary Crystals. Nanoscale. 2023;15:9941–5. https://doi.org/10.1039/D3NR01187A.10.1039/D3NR01187A ↗
22. Hamada S, Murata S. Substrate-assisted assembly of interconnected single-duplex DNA nanostructures. Angew Chem Int Ed Engl. 2009;48:6820–3. https://doi.org/10.1002/anie.200902662.10.1002/anie.200902662 ↗
23. Xin Y, Ji X, Grundmeier G, Keller A. Dynamics of lattice defects in mixed DNA origami monolayers. Nanoscale. 2020;12:9733–43. https://doi.org/10.1039/d0nr01252a.10.1039/d0nr01252a ↗
24. Xin Y, Shen B, Kostiainen MA, Grundmeier G, Castro M, Linko V, Keller A. Scaling Up DNA origami lattice assembly. Chem Eur J. 2021;27:8564–71. https://doi.org/10.1002/chem.202100784.10.1002/chem.202100784 ↗
25. Kielar C, Ramakrishnan S, Fricke S, Grundmeier G, Keller A. Dynamics of DNA origami lattice formation at solid-liquid interfaces. ACS Appl Mater Interfaces. 2018;10:44844–53. https://doi.org/10.1021/acsami.8b16047.10.1021/acsami.8b16047 ↗
26. Liu L, Li Y, Wang Y, Zheng J, Mao C. Regulating DNA Self-assembly by DNA-surface interactions. ChemBioChem. 2017;18:2404–7. https://doi.org/10.1002/cbic.201700545.10.1002/cbic.201700545 ↗
27. Nievergelt AP, Kammer C, Brillard C, Kurisinkal E, Bastings MMC, Karimi A, Fantner GE. Large-range HS-AFM imaging of DNA self-assembly through in situ data-driven control. Small Meth. 2019;3:1900031. https://doi.org/10.1002/smtd.201900031.10.1002/smtd.201900031 ↗
28. Woo S, Rothemund PWK. Self-assembly of two-dimensional DNA origami lattices using cation-controlled surface diffusion. Nat Commun. 2014;5:4889. https://doi.org/10.1038/ncomms5889.10.1038/ncomms5889 ↗
29. Julin S, Linko V, Kostiainen MA. Reconfigurable pH-responsive DNA origami lattices. ACS Nano. 2023;17:11014–22. https://doi.org/10.1021/acsnano.3c03438.10.1021/acsnano.3c03438 ↗
30. Kempter S, Khmelinskaia A, Strauss MT, Schwille P, Jungmann R, Liedl T, Bae W. Single particle tracking and super-resolution imaging of membrane-assisted stop-and-Go diffusion and lattice assembly of DNA origami. ACS Nano. 2019;13:996–1002. https://doi.org/10.1021/acsnano.8b04631.10.1021/acsnano.8b04631 ↗
31. Kocabey S, Kempter S, List J, Xing Y, Bae W, Schiffels D, Shih WM, Simmel FC, Liedl T. Membrane-assisted growth of DNA origami nanostructure arrays. ACS Nano. 2015;9:3530–9. https://doi.org/10.1021/acsnano.5b00161.10.1021/acsnano.5b00161 ↗
32. Suzuki Y, Endo M, Sugiyama H. Lipid-bilayer-assisted two-dimensional self-assembly of DNA origami nanostructures. Nat Commun. 2015;6:8052. https://doi.org/10.1038/ncomms9052.10.1038/ncomms9052 ↗
33. Suzuki Y, Sugiyama H, Endo M. Complexing DNA origami frameworks through sequential self-assembly based on directed docking. Angew Chem Int Ed Engl. 2018;57:7061–5. https://doi.org/10.1002/anie.201801983.10.1002/anie.201801983 ↗
34. Sato Y, Endo M, Morita M, Takinoue M, Sugiyama H, Murata S, Nomura SM, Suzuki Y. Environment-dependent self-assembly of DNA origami lattices on phase-separated lipid membranes. Adv Mater Interfaces. 2018;17:1800437. https://doi.org/10.1002/admi.201800437.10.1002/admi.201800437 ↗
35. Avakyan N, Conway JW, Sleiman HF. Long-range ordering of blunt-ended DNA tiles on supported lipid bilayers. J Am Chem Soc. 2017;139:12027–34. https://doi.org/10.1021/jacs.7b06572.10.1021/jacs.7b06572 ↗
36. Gavrilović S, Brüggenthies GA, Weck JM, Heuer-Jungemann A, Schwille P. Protein-assisted large-scale assembly and differential patterning of DNA origami lattices. Small. 2024;20:e2309680. https://doi.org/10.1002/smll.202309680.10.1002/smll.202309680 ↗
37. Pothineni BK, Grundmeier G, Keller A. Cation-dependent assembly of hexagonal DNA origami lattices on SiO2 surfaces. Nanoscale. 2023;15:12894–906. https://doi.org/10.1039/D3NR02926C.10.1039/D3NR02926C ↗
38. Mao D, Liu L, Zhang C, Liu H, Mao C. Molecular lithography on silicon wafers guided by porous, extended arrays of small DNA tiles. Langmuir. 2023;39:11782–7. https://doi.org/10.1021/acs.langmuir.3c01422.10.1021/acs.langmuir.3c01422 ↗
39. Pothineni BK, Theile-Rasche C, Müller H, Grundmeier G, Los Arcos T. DNA origami adsorption and lattice formation on different siox surfaces. Chem Eur J. 2025;31:e202404108. https://doi.org/10.1002/chem.202404108.10.1002/chem.202404108 ↗
40. Yan H, Park SH, Finkelstein G, Reif JH, LaBean TH. DNA-templated self-assembly of protein arrays and highly conductive nanowires. Science. 2003;301:1882–4. https://doi.org/10.1126/science.1089389.10.1126/science.1089389 ↗
41. Liu W, Zhong H, Wang R, Seeman NC. Crystalline two-dimensional DNA-origami arrays. Angew Chem Int Ed Engl. 2011;50:264–7. https://doi.org/10.1002/anie.201005911.10.1002/anie.201005911 ↗
42. Rothemund PWK. Folding DNA to create nanoscale shapes and patterns. Nature. 2006;440:297–302. https://doi.org/10.1038/nature04586.10.1038/nature04586 ↗
43. Ramakrishnan S, Subramaniam S, Stewart AF, Grundmeier G, Keller A. Regular nanoscale protein patterns via directed adsorption through self-assembled DNA origami masks. ACS Appl Mater Interfaces. 2016;8:31239–47. https://doi.org/10.1021/acsami.6b10535.10.1021/acsami.6b10535 ↗
44. Liu L, Zheng M, Li Z, Li Q, Mao C. Patterning nanoparticles with DNA molds. ACS Appl Mater Interfaces. 2019;11:13853–8. https://doi.org/10.1021/acsami.8b22691.10.1021/acsami.8b22691 ↗
45. Yang S, Liu W, Zhang Y, Wang R. Bottom-up fabrication of large-scale gold nanorod arrays by surface diffusion-mediated DNA origami assembly. ACS Appl Mater Interfaces. 2021;13:50516–23. https://doi.org/10.1021/acsami.1c13173.10.1021/acsami.1c13173 ↗
46. Nečas D, Klapetek P. Gwyddion: an open-source software for SPM data analysis. Open Phys. 2012;10:99. https://doi.org/10.2478/s11534-011-0096-2.10.2478/s11534-011-0096-2 ↗
47. Revellame ED, Fortela D, Sharp W, Hernandez R, Zappi ME. Adsorption kinetic modeling using pseudo-first order and pseudo-second order rate laws: a review. Clean Engin Technol. 2020;1:100032. https://doi.org/10.1016/j.clet.2020.100032.10.1016/j.clet.2020.100032 ↗
48. Kielar C, Zhu S, Grundmeier G, Keller A. Quantitative assessment of tip effects in single-molecule high-speed atomic force microscopy using DNA origami substrates. Angew Chem Int Ed Engl. 2020;59:14336–41. https://doi.org/10.1002/anie.202005884.10.1002/anie.202005884 ↗
49. Nievergelt AP, Banterle N, Andany SH, Gönczy P, Fantner GE. High-speed photothermal off-resonance atomic force microscopy reveals assembly routes of centriolar scaffold protein SAS-6. Nat Nanotechnol. 2018;13:696–701. https://doi.org/10.1038/s41565-018-0149-4.10.1038/s41565-018-0149-4 ↗