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Dendrimers in Nanoscale Confinement: The Interplay between Conformational Change and Nanopore Entrance

Ficici, E; Andricioaei, I; Howorka, S; (2015) Dendrimers in Nanoscale Confinement: The Interplay between Conformational Change and Nanopore Entrance. [Letter]. Nano Letters , 15 (7) pp. 4822-4828. 10.1021/acs.nanolett.5b01960. Green open access

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Abstract

Hyperbranched dendrimers are nanocarriers for drugs, imaging agents, and catalysts. Their nanoscale confinement is of fundamental interest and occurs when dendrimers with bioactive payload block or pass biological nanochannels or when catalysts are entrapped in inorganic nanoporous support scaffolds. The molecular process of confinement and its effect on dendrimer conformations are, however, poorly understood. Here, we use single-molecule nanopore measurements and molecular dynamics simulations to establish an atomically detailed model of pore dendrimer interactions. We discover and explain that electrophoretic migration of polycationic PAMAM dendrimers into confined space is not dictated by the diameter of the branched molecules but by their size and generation-dependent compressibility. Differences in structural flexibility also rationalize the apparent anomaly that the experimental nanopore current read-out depends in nonlinear fashion on dendrimer size. Nanoscale confinement is inferred to reduce the protonation of the polycationic structures. Our model can likely be expanded to other dendrimers and be applied to improve the analysis of biophysical experiments, rationally design functional materials such as nanoporous filtration devices or nanoscale drug carriers that effectively pass biological pores.

Type: Article
Title: Dendrimers in Nanoscale Confinement: The Interplay between Conformational Change and Nanopore Entrance
Location: United States
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/acs.nanolett.5b01960
Publisher version: http://dx.doi.org/10.1021/acs.nanolett.5b01960
Language: English
Additional information: This document is the Accepted Manuscript version of a Published Work that appeared in final form in Nano Letters, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://dx/doi/org/10.1021/acs.nanolett.5b01960
Keywords: dendrimer, ionization, molecular dynamics, nanopore, single-molecule, transport
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/1470550
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