Facile Modification of Silica Substrates Provides a Platform for Direct‐Writing Surface Click Chemistry

Oberhansl, Sabine; Hirtz, Michael; Lagunas, Anna; Eritja, Ramón; Martínez, Elena; Fuchs, Harald; Samitier, J.

doi:10.1002/smll.201101875

Cited by 19 publications

(18 citation statements)

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“…[24] Given that each staple in an origami structure has a unique sequence, it is conceivable that hundreds of strands can be modified as DNA ink and subsequently hybridized with any DNA linked molecules or nanomaterials of interest leading to a complex addressable nanostructure. In addition to thiol groups, it is possible to immobilize the oligonucleotides with other chemistries such as thiol-ene, [25] click chemistry, [26] amino reactive groups [27] and on other surfaces such as silica, silicon nitride and polymeric surfaces.This methodology could be implemented as an additional step in top-down methodologies [2c, 10] or the formation of periodic lattices. [14] Future studies could lead to the integration of this methodology within multiplexed microfluidic [11] and more multipurpose read out systems, [10a] For example, the integration of modular addressability with biological processes can be utilized for the high throughput analysis of biochemical reactions and biomolecular interactions that require control over proximity and special distribution.…”

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DNA‐Origami‐Driven Lithography for Patterning on Gold Surfaces with Sub‐10 nm Resolution

et al. 2017

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The programmability [1] and self-assembly properties of DNA provides means of precise organization of matter at the nanoscale. [2] DNA origami allows the folding of DNA into twodimensional [3] and three-dimensional [4] structures, and has been used to organize biomolecules, [2b, e, 5] nanophotonic [2a, c, f, 6] and electronic [7] components with a resolution of 6 nm / pixel. [8] Two-dimensional DNA origami has been also used as a platform to organize other chemical [9] species that can then be placed on technologically relevant substrates. [2c, 10] Nevertheless, these approaches have only used the DNA nanostructure to hold the chemical species on the surface and, to the best of our knowledge, have never been utilized to immobilize nucleic acids patterns on surfaces with sub-10 nm resolution providing an enable 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 61 62 63 64 65 Submitted to 2 platform for potential applications such as multiplexed biochemical assays. [11] to the creation of metasurfaces [12] with potentially reconfigurable features. Revised ManuscriptHerein we report on the use of a two-dimensional DNA origami as a template to covalently attach DNA with a pre-programmed pattern on a surface (see Scheme 1). The method utilizes the incorporation of modified staple strands in programmed positions of the DNA origami (DNA origami stamp), acting as DNA ink. Once the DNA origami is immobilized on the surface, the modified staples can react with the surface creating a defined DNA pattern (Stamping step). The pattern can then be exposed upon denaturation of the DNA origami stamp (Unmasking step), allowing the non-bound staples to be rinsed off of the surface. As a proof-of-principle of this methodology, we have created a linear pattern of thiolmodified DNA ink on gold surfaces. The formation of the linear pattern was revealed by the successful formation of bead-on-a-string-like structures (here named "chains" for simplicity) composed of gold nanoparticles conjugated with thiol-oligonucleotides (OGNP) that are hybridized to the DNA ink pattern (Development step). The linear pattern provided a direct evidence of the stamping process and was chosen as a simple geometry that can be statistically analysed in our experimental setup. Montecarlo Simulations have been used for better understanding of our statistical results and to determine key elements governing the process that can be used for future optimization of pattern information transfer with DNA origami stamp methodology. Furthermore, we have studied the development of more complex patterns using Montecarlo Simulations.We demonstrate that our approach can be employed to form DNA patterns with sub-10 nm resolution to flat gold surfaces, an unsolved goal to date. This methodology can thus be extended to other surfaces utilizing different covalent strategies. [10b, 13] M...

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DNA‐Origami‐Driven Lithography for Patterning on Gold Surfaces with Sub‐10 nm Resolution

et al. 2017

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“…Substrate Preparation : Substrates (alkyne terminated glass) for the CuAAC patterning were prepared using a procedure similar to what has previously been reported . In brief, glass cover slips (VWR, Germany) were cleaned by sonication subsequently in chloroform, ethanol and DI water for 5 min in each solvent.…”

Section: Methodsmentioning

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“…[ 18,21,22 ] CuAAC shows high potential in solid phase chemistry [ 23 ] and was previously shown in DPN and microchannel cantilever spotting to be compatible with protein binding and cell culture applications. [24][25][26][27] We have used click-chemistry to pattern allergen by PPL for mast cell studies. As a model allergen, we chose dinitrophenol (DNP), which has previously been used in mast cell activation assays.…”

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Click-Chemistry Based Allergen Arrays Generated by Polymer Pen Lithography for Mast Cell Activation Studies

Kumar

Bonicelli

Sekula-Neuner

et al. 2016

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The profiling of allergic responses is a powerful tool in biomedical research and in judging therapeutic outcome in patients suffering from allergy. Novel insights into the signaling cascades and easier readouts can be achieved by shifting activation studies of bulk immune cells to the single cell level on patterned surfaces. The functionality of dinitrophenol (DNP) as a hapten in the induction of allergic reactions has allowed the activation process of single mast cells seeded on patterned surfaces to be studied following treatment with allergen specific Immunoglobulin E antibodies. Here, a click-chemistry approach is applied in combination with polymer pen lithography (PPL) to pattern DNP-azide on alkyne-terminated surfaces to generate arrays of allergen. The large area functionalization offered by PPL allows an easy incorporation of such arrays into microfluidic chips. In such a setup, easy handling of cell suspension, incubation process, and read-out by fluorescence microscopy will allow immune cell activation screening to be easily adapted for diagnostics and biomedical research.

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“…In our previous work we have demonstrated the effectiveness of this strategy for the surface functionalization of model substrates using DPN. 65 However, in order to overcome the requirement for a transition metal catalyst in the DPN ink formulation, we introduced a surface capable of participating in the SPAAC click reaction. While the CuAAC has enabled great advances in surface functionalization in general, and in particular for DPN and mCS, the use of a Cubased catalyst may pose severe limitations for the patterning of some types of biomolecules whose activity may be impaired.…”

Section: Signalsmentioning

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Catalyst-free site-specific surface modifications of nanocrystalline diamond films via microchannel cantilever spotting

et al. 2016

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The properties of nanocrystalline diamond (NCD) films offer great potential for the creation of various sensing and photonic devices. A great challenge in order to materialize such applications lies in achieving the micrometrically resolved functionalization of NCD surfaces. In the present work, we introduce a facile approach to meet this challenge employing the novel strain-promoted alkyne-azide cycloaddition "click" chemistry reaction, a catalyst-free ligation protocol compatible with biomolecules.The ability to achieve well-resolved multicomponent patterns with high reproducibility is demonstrated, paving the way for the fabrication of novel devices based on micropatterned NCD films.

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Facile Modification of Silica Substrates Provides a Platform for Direct‐Writing Surface Click Chemistry

Cited by 19 publications

References 42 publications

DNA‐Origami‐Driven Lithography for Patterning on Gold Surfaces with Sub‐10 nm Resolution

DNA‐Origami‐Driven Lithography for Patterning on Gold Surfaces with Sub‐10 nm Resolution

Click-Chemistry Based Allergen Arrays Generated by Polymer Pen Lithography for Mast Cell Activation Studies

Catalyst-free site-specific surface modifications of nanocrystalline diamond films via microchannel cantilever spotting

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