Charge- and size-based separation of macromolecules using ultrathin silicon membranes

Striemer, Christopher C.; Gaborski, Thomas R.; McGrath, James L.; Fauchet, Philippe M.

doi:10.1038/nature05532

Cited by 704 publications

(715 citation statements)

References 18 publications

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“…21,22 In addition to these spectroscopic studies, graphene drumheads offer the opportunity to probe the permeability of gases through atomic vacancies in single layers of atoms 23 and defects patterned in the graphene membrane can act as selective barriers for ultrafiltration. 24,25 The tensioned suspended graphene membranes also provide a platform for STM imaging of both graphene [26][27][28] and graphene-fluid interfaces and offer a unique separation barrier between two distinct phases of matter that is only one atom thick. Helium Atoms across a Graphene Sheet, and Classical Effusion through Single Atom Lattice Vacancies.…”

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confidence: 99%

Impermeable Atomic Membranes from Graphene Sheets

et al. 2008

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We demonstrate that a monolayer graphene membrane is impermeable to standard gases including helium. By applying a pressure difference across the membrane, we measure both the elastic constants and the mass of a single layer of graphene. This pressurized graphene membrane is the world's thinnest balloon and provides a unique separation barrier between 2 distinct regions that is only one atom thick.Membranes are fundamental components of a wide variety of physical, chemical, and biological systems, used in everything from cellular compartmentalization to mechanical pressure sensing. They divide space into two regions, each capable of possessing different physical or chemical properties. A simple example is the stretched surface of a balloon, where a pressure difference across the balloon is balanced by the surface tension in the membrane. Graphene, a single layer of graphite, is the ultimate limit: a chemically stable and electrically conducting membrane one atom in thickness. 1-3 An interesting question is whether such an atomic membrane can be impermeable to atoms, molecules and ions. In this letter, we address this question for gases. We show that these membranes are impermeable and can support pressure differences larger than one atmosphere. We use such pressure differences to tune the mechanical resonance frequency by ∼100 MHz. This allows us to measure the mass and elastic constants of graphene membranes. We demonstrate that atomic layers of graphene have stiffness similar to bulk graphite (E ∼ 1 TPa). These results show that single atomic sheets can be integrated with microfabricated structures to create a new class of atomic scale membrane-based devices.A schematic of the device geometry used heresa graphene-sealed microchambersis shown in Figure 1a. Graphene sheets are suspended over predefined wells in silicon oxide using mechanical exfoliation (see Supporting Information). Each graphene membrane is clamped on all sides by the van der Waals force between the graphene and SiO 2 , creating a ∼(µm) 3 volume of confined gas. The inset of Figure 1a shows an optical image of a single layer graphene sheet forming a sealed square drumhead with a width W ) 4.75 µm on each side. Raman spectroscopy was used to confirm that this graphene sheet was a single layer in thickness. [4][5][6] Chambers with graphene thickness from 1 to ∼75 layers were studied.After initial fabrication, the pressure inside the microchamber, p int , is atmospheric pressure (101 kPa). If the pressure external to the chamber, p ext , is changed, we found that p int will equilibrate to p ext on a time scale that ranges from minutes to days, depending on the gas species and the temperature. On shorter time scales than this equilibration time, a significant pressure difference ∆p ) p int -p ext can exist across the membrane, causing it to stretch like the surface of a balloon (Figure 1b). Examples are shown for ∆p > 0 in Figure 1c and ∆p < 0 in Figure 1d.To create a positive pressure difference, ∆p > 0, as shown in Figure 1c, we place a s...

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Impermeable Atomic Membranes from Graphene Sheets

et al. 2008

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“…Highly porous ultrathin silicon membranes can be obtained by thermally annealing thin silicon films, which results in spontaneous pore formation (25,26). The pore diameter can be controlled with high precision by choosing appropriate annealing conditions.…”

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Versatile ultrathin nanoporous silicon nitride membranes

Vlassiouk

Apel

Dmitriev

et al. 2009

Proc. Natl. Acad. Sci. U.S.A.

152

144

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Single-and multiple-nanopore membranes are both highly interesting for biosensing and separation processes, as well as their ability to mimic biological membranes. The density of pores, their shape, and their surface chemistry are the key factors that determine membrane transport and separation capabilities. Here, we report silicon nitride (SiN) membranes with fully controlled porosity, pore geometry, and pore surface chemistry. An ultrathin freestanding SiN platform is described with conical or doubleconical nanopores of diameters as small as several nanometers, prepared by the track-etching technique. This technique allows the membrane porosity to be tuned from one to billions of pores per square centimeter. We demonstrate the separation capabilities of these membranes by discrimination of dye and protein molecules based on their charge and size. This separation process is based on an electrostatic mechanism and operates in physiological electrolyte conditions. As we have also shown, the separation capabilities can be tuned by chemically modifying the pore walls. Compared with typical membranes with cylindrical pores, the conical and double-conical pores reported here allow for higher fluxes, a critical advantage in separation applications. In addition, the conical pore shape results in a shorter effective length, which gives advantages for single biomolecule detection applications such as nanopore-based DNA analysis.ion track-etching ͉ nanofluidics ͉ filtration ͉ SiN

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“…F ree-standing nano-membranes have been fabricated from various materials, such as Si-based inorganics [1][2][3][4][5][6] , thin metal foils 7,8 and other types of nano-materials [9][10][11][12][13][14] , for use in a wide range of applications including shadow masking 3,4 , molecular separation 5,6,15 , plasmonics 4,7 , energy devices [16][17][18] and bio-inspired microfluidic devices 19,20 . In general, a series of standard semiconductor processes and/or specific materials 7,21 with high mechanical rigidity have been required to maintain the membrane's shape firmly without mechanical fracture or tear against external forces that arise during the handling process.…”

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“…In general, a series of standard semiconductor processes and/or specific materials 7,21 with high mechanical rigidity have been required to maintain the membrane's shape firmly without mechanical fracture or tear against external forces that arise during the handling process. For example, a highly robust SiN x (Young's modulus, E4130 GPa) nano-membrane was formed on top of a rigid silicon support via electron-beam lithography or focused ion-beam milling 3,4,6 . Such a thin SiN x membrane is known to be complicated and expensive to fabricate, and fragile under mechanical contact or moisture at ambient conditions.…”

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Replication of flexible polymer membranes with geometry-controllable nano-apertures via a hierarchical mould-based dewetting

et al. 2014

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Membranes with nano-apertures are versatile templates that possess a wide range of electronic, optical and biomedical applications. However, such membranes have been limited to silicon-based inorganic materials to utilize standard semiconductor processes. Here we report a new type of flexible and free-standing polymeric membrane with nano-apertures by exploiting high-wettability difference and geometrical reinforcement via multiscale, multilevel architecture. In the method, polymeric membranes with various pore sizes (50-800 nm) and shapes (dots, lines) are fabricated by a hierarchical mould-based dewetting of ultravioletcurable resins. In particular, the nano-pores are monolithically integrated on a two-level hierarchical supporting layer, allowing for the rapid (o5 min) and robust formation of multiscale and multilevel nano-apertures over large areas (2 Â 2 cm 2 ).

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Charge- and size-based separation of macromolecules using ultrathin silicon membranes

Cited by 704 publications

References 18 publications

Impermeable Atomic Membranes from Graphene Sheets

Impermeable Atomic Membranes from Graphene Sheets

Versatile ultrathin nanoporous silicon nitride membranes

Replication of flexible polymer membranes with geometry-controllable nano-apertures via a hierarchical mould-based dewetting

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