eprintid: 1470550
rev_number: 29
eprint_status: archive
userid: 608
dir: disk0/01/47/05/50
datestamp: 2015-11-05 14:00:50
lastmod: 2021-10-04 00:52:34
status_changed: 2015-11-05 14:00:50
type: article
metadata_visibility: show
creators_name: Ficici, E
creators_name: Andricioaei, I
creators_name: Howorka, S
title: Dendrimers in Nanoscale Confinement: The Interplay between Conformational Change and Nanopore Entrance
ispublished: pub
divisions: UCL
divisions: B04
divisions: C06
divisions: F56
keywords: dendrimer, ionization, molecular dynamics, nanopore, single-molecule, transport
note: 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
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.
date: 2015-07-08
date_type: published
official_url: http://dx.doi.org/10.1021/acs.nanolett.5b01960
oa_status: green
full_text_type: other
language: eng
primo: open
primo_central: open_green
article_type: letter
article_type_text: Journal Article
verified: verified_manual
elements_id: 1038588
doi: 10.1021/acs.nanolett.5b01960
language_elements: eng
lyricists_name: Howorka, Stefan
lyricists_id: SHOWO39
actors_name: Howorka, Stefan
actors_id: SHOWO39
actors_role: owner
full_text_status: public
publication: Nano Letters
volume: 15
number: 7
pagerange: 4822-4828
event_location: United States
issn: 1530-6992
citation:        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 <https://doi.org/10.1021/acs.nanolett.5b01960>.       Green open access   
 
document_url: https://discovery.ucl.ac.uk/id/eprint/1470550/1/Ficici%20Nano%20Letters%202015.pdf