Impermeable Atomic Membranes from Graphene Sheets

Abstract

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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