Polarization-Induced Local Pore-Wall Functionalization for Biosensing: From Micropore to Nanopore

Liu, Jie; Pham, Pascale; Haguet, Vincent; Sauter-Starace, Fabien; Leroy, Loïc; Roget, André; Descamps, Emeline; Bouchet, Aurélie; Buhot, Arnaud; Mailley, Pascal; Livache, Thierry

doi:10.1021/ac2033744

Cited by 24 publications

(37 citation statements)

References 54 publications

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“…Micropores with scalloped inner walls were etched in the membrane conserved at the bottom of each pyramidal opening (Figure 1). The 10 µm-thick pore walls were functionalized with ODN probes using the CLEF technique [55], [56]. In brief, an electrolyte solution containing pyrrole and pyrrole-ODN monomers was filled into a reacting chamber, which was separated in two compartments by the silicon micropore chip.…”

Section: Resultsmentioning

confidence: 99%

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Selective Individual Primary Cell Capture Using Locally Bio-Functionalized Micropores

et al. 2013

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BackgroundSolid-state micropores have been widely employed for 6 decades to recognize and size flowing unlabeled cells. However, the resistive-pulse technique presents limitations when the cells to be differentiated have overlapping dimension ranges such as B and T lymphocytes. An alternative approach would be to specifically capture cells by solid-state micropores. Here, the inner wall of 15-µm pores made in 10 µm-thick silicon membranes was covered with antibodies specific to cell surface proteins of B or T lymphocytes. The selective trapping of individual unlabeled cells in a bio-functionalized micropore makes them recognizable just using optical microscopy.Methodology/Principal FindingsWe locally deposited oligodeoxynucleotide (ODN) and ODN-conjugated antibody probes on the inner wall of the micropores by forming thin films of polypyrrole-ODN copolymers using contactless electro-functionalization. The trapping capabilities of the bio-functionalized micropores were validated using optical microscopy and the resistive-pulse technique by selectively capturing polystyrene microbeads coated with complementary ODN. B or T lymphocytes from a mouse splenocyte suspension were specifically immobilized on micropore walls functionalized with complementary ODN-conjugated antibodies targeting cell surface proteins.Conclusions/SignificanceThe results showed that locally bio-functionalized micropores can isolate target cells from a suspension during their translocation throughout the pore, including among cells of similar dimensions in complex mixtures.

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Section: Resultsmentioning

confidence: 99%

“…Detection sensitivity of flowing targets is thus enhanced by focusing target capture events only inside the micropores, i.e. with no missed detection events on the bulk membranes [55], [56]. Cell surface protein-specific antibodies conjugated with complementary ODNs were then immobilized on the pore walls via hybridization.…”

Section: Introductionmentioning

confidence: 99%

Selective Individual Primary Cell Capture Using Locally Bio-Functionalized Micropores

et al. 2013

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“…Notably, the polarization of MD nanopore takes place both on gold and dielectrics-SiN due to high electric fields, which was previously demonstrated by Bouchet and co-workers. [31][32][33] Additionally, the threshold of driving voltage is found to be ≈0.7-0.8 V, higher than the threshold for redox potential of 0.48 V (see Figure S1, Supporting Information). This suggests, in our nanopore, 1.46-fold of the redox potential is required to drive the bipolar effects for these devices.…”

Section: Doi: 101002/adom201600907mentioning

confidence: 92%

“…In addition to floating metals, bulk dielectrics can become polarized by applying an electric field with high intensity. [31][32][33] For the MM nanopores, the sign of E z at +1 V (applied voltage) is negative, indicating the gold holds a lower potential than the electrolyte near the hot spots, while the positive sign of E z at −1 V results in a higher potential on the gold than on the electrolyte. The converse is true for MD nanopores.…”

Section: Doi: 101002/adom201600907mentioning

confidence: 99%

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Probing Local Potentials inside Metallic Nanopores with SERS and Bipolar Electrochemistry

Chang

Willems

et al. 2017

Advanced Optical Materials

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CommuniCation(1 of 6) 1600907 considerable attention. In addition to being used as electrodes, optical nanostructures for extraordinary light transmission, [8] fluorescence, [9] and surface-enhanced Raman spectroscopy (SERS) [10] have demonstrated additional detection and/or control capabilities. For these optical techniques, metal layers are usually unbiased, so-called floating electrode mode, whereas applying a bias voltage may induce a potential drop over the floating metallic nanopore because of its high resistance. In the field of macroscale fluidics, a sufficient DC voltage difference between the floating metal layer and the solution enables the activation of oxidation and reduction reactions. [11,12] However, on the nanoscale, the study on the local potential and electrochemical effects on floating metallic nanopores remains challenging.Local potential and related electrochemistry on floating metal electrodes has been termed "bipolar electrochemistry" [12,13] In an unbiased state, bipolar electrochemistry requires either highly confined electric fields or extremely high concentration-gradients adjacent to bipolar electrodes [14][15][16] to drive reactions and investigate optical properties. Such investigation techniques include electrochemiluminescence, [17] electrochemical corrosion microscopy, [18] epifluoresence, [19] and surface plasmon resonance spectroscopy, [20] which are ultimately restricted by the diffraction of light. Here, working toward subwavelength detection, we propose the use of SERS to study the local potentials. [21][22][23][24][25] To simultaneously align localized SERS hot spots with fluidic focus for high spatial resolution and high specificity, [26] our technique probes the local potential and characterizes nanoscale bipolar electrochemical effects on metallic nanopores for the first time. Figure 1a depicts a schematic of the experiments on the metallic nanopores. The nanopore chip was mounted into a custom-made flow cell, separating the electrolyte into two reservoirs. Next, a 785 nm laser was tightly focused at the nanopore cavity. The electrical potential was applied to the top side of the membrane as shown in Figure 1a, and the other side was connected to ground. This defines the applied bias direction for positive and negative values in the experiments. A doublesided gold (MM) nanopore is used for the demonstration of bipolar electrochemical SERS. To maximize the plasmonic enhancement effect and subsequent SERS signals at 785 nm, It is essential to understand the local potential distribution of solid-state nanopores in nanofluidic systems. However, applying gate voltage or adding external electrical probes tends to disturb the electric field and/or flow patterns. To solve this problem, an approach is described to monitor the local potential using electrochemical surface enhanced Raman spectroscopy (EC-SERS) in two types of nanocavity pores: doubled-sided gold nanopores (MM nanopores) and single-sided gold nanopores with a dielectric passivation layer on the backside (MD nanopor...

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Bipolar Electrochemistry

Bouffier¹,

Zigah

Šojić

et al. 2021

Encyclopedia of Electrochemistry

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Bipolar electrochemistry is a technique that involves two opposite chemical processes, namely an oxidation and a reduction, occurring simultaneously on the surface of a conducting object, usually without connection to a power supply. The basic phenomenon has already been described and used for many decades but regained a lot of interest in recent years, thanks to several attractive features for developing new applications in various areas ranging from materials science and analytical chemistry to catalysis and even life science. Consequently, bipolar electrochemistry has experienced a substantial growth in the number of users and publications. This is mostly due to several advantages over classic electrochemistry, such as the absence of an ohmic contact, the generation of a directional gradient of electroactivity on the object, and the possibility to address simultaneously thousands of objects, which opens the door for high throughput screening of (electro)chemical properties. Also, some features of this "wireless" electrochemistry allow performing experiments that cannot be achieved with a classic electrochemical setup. Last but not least, only rather low-cost equipment is needed. The objective of the present contribution is to introduce first some fundamental aspects of bipolar electrochemistry, and then to illustrate its different developments, highlighting not only the historic landmark achievements, but also the most recent findings, especially in the context of micro-and nanoscience. The chapter will illustrate the singularities and advantages of this straightforward approach and hopefully convince the reader of the power of this interesting electrochemical concept.

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Polarization-Induced Local Pore-Wall Functionalization for Biosensing: From Micropore to Nanopore

Cited by 24 publications

References 54 publications

Selective Individual Primary Cell Capture Using Locally Bio-Functionalized Micropores

Selective Individual Primary Cell Capture Using Locally Bio-Functionalized Micropores

Probing Local Potentials inside Metallic Nanopores with SERS and Bipolar Electrochemistry

Bipolar Electrochemistry

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