Ion channels are protein pores that span cell membranes and open and close in response to stimuli like changes in the transmembrane potential, binding of a ligand, or mechanical stress. When open, ions pass through the pore, and hence across the cell membrane, and when closed, ion-transport is precluded. Hence, these channels are nanodevices that have a current-rectification function. There is intense research effort aimed at understanding the molecular-level mechanism for this function. One approach for elucidating the mechanism is to construct a simple abiotic system that mimics this function and to use the mechanistic details of this mimic as a guide to understand the more complex biological channel. We describe here such an abiotic mimic: a synthetic membrane that contains a single conical gold nanotube. The advantage of this mimic is that the surface charge and chemistry of the nanotube wall can be varied, at will, by judicious choice of electrolyte or by thiol chemisorption. This has allowed us to make conical Au nanotubes that rectify the ion current and, just as importantly, to definitively elucidate the mechanism of this function.
There is considerable interest in developing chemical devices that mimic the function of biological ion channels. We recently described such a device, which consisted of a single conically shaped gold nanotube embedded within a polymeric membrane. This device mimicked one of the key functions of voltage-gated ion channels: the ability to strongly rectify the ionic current flowing through it. The data obtained were interpreted using a simple electrostatic model. While the details are still being debated, it is clear that ion-current-rectification in biological ion channels is more complicated and involves physical movement of an ionically charged portion of the channel in response to a change in the transmembrane potential. We report here artificial ion channels that rectify the ion current flowing through them via this "electromechanical" mechanism. These artificial channels are also based on conical gold nanotubes, but with the critical electromechanical response provided by single-stranded DNA molecules attached to the nanotube walls.
We describe synthetic membranes in which the molecular recognition chemistry used to accomplish selective permeation is DNA hybridization. These membranes contain template-synthesized gold nanotubes with inside diameters of 12 nanometers, and a "transporter" DNA-hairpin molecule is attached to the inside walls of these nanotubes. These DNA-functionalized nanotube membranes selectively recognize and transport the DNA strand that is complementary to the transporter strand, relative to DNA strands that are not complementary to the transporter. Under optimal conditions, single-base mismatch transport selectivity can be obtained.
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