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Title: Temperature response of soft ionizable polymer nanoparticles

Abstract

The temperature response of luminescent ionizable polymers confined into far from equilibrium nanoparticles without chemical links was studied using molecular dynamics simulations. These nanoparticles, often referred to as polydots, are emerging as a promising tool for nanomedicine. Incorporating ionizable groups into these polymers enables biofunctionality; however, they also affect the delicate balance of interactions that hold these nanoparticles together. Here polydots formed by a model polymer dialkyl p-phenylene ethynylene with varying number of carboxylate groups along the polymer backbone were probed. We find that increasing temperature affects neutral and charged polydots differently, where neutral polydots exhibit a transition above which their structure becomes dynamic and they unravel. The dependence of the transition temperature on the surface to volume ratio of these polydots is much stronger than what has previously been observed in polymeric thin films. In conclusion, charged polydots become dynamic enabling migration of the ionizable groups toward the particle interface, while retaining the overall particle shape.

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2]
  1. Clemson Univ., Clemson, SC (United States)
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1473954
Report Number(s):
[SAND-2018-9940J]
[Journal ID: ISSN 0021-9606; 667772]
Grant/Contract Number:  
[AC04-94AL85000]
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
[ Journal Volume: 149; Journal Issue: 8]; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Wijesinghe, Sidath, Perahia, Dvora, and Grest, Gary S. Temperature response of soft ionizable polymer nanoparticles. United States: N. p., 2018. Web. doi:10.1063/1.5043226.
Wijesinghe, Sidath, Perahia, Dvora, & Grest, Gary S. Temperature response of soft ionizable polymer nanoparticles. United States. doi:10.1063/1.5043226.
Wijesinghe, Sidath, Perahia, Dvora, and Grest, Gary S. Mon . "Temperature response of soft ionizable polymer nanoparticles". United States. doi:10.1063/1.5043226. https://www.osti.gov/servlets/purl/1473954.
@article{osti_1473954,
title = {Temperature response of soft ionizable polymer nanoparticles},
author = {Wijesinghe, Sidath and Perahia, Dvora and Grest, Gary S.},
abstractNote = {The temperature response of luminescent ionizable polymers confined into far from equilibrium nanoparticles without chemical links was studied using molecular dynamics simulations. These nanoparticles, often referred to as polydots, are emerging as a promising tool for nanomedicine. Incorporating ionizable groups into these polymers enables biofunctionality; however, they also affect the delicate balance of interactions that hold these nanoparticles together. Here polydots formed by a model polymer dialkyl p-phenylene ethynylene with varying number of carboxylate groups along the polymer backbone were probed. We find that increasing temperature affects neutral and charged polydots differently, where neutral polydots exhibit a transition above which their structure becomes dynamic and they unravel. The dependence of the transition temperature on the surface to volume ratio of these polydots is much stronger than what has previously been observed in polymeric thin films. In conclusion, charged polydots become dynamic enabling migration of the ionizable groups toward the particle interface, while retaining the overall particle shape.},
doi = {10.1063/1.5043226},
journal = {Journal of Chemical Physics},
number = [8],
volume = [149],
place = {United States},
year = {2018},
month = {8}
}

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