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Title: Amphiphile-Induced Phase Transition of Liquid Crystals at Aqueous Interfaces

Abstract

We report that monolayer assemblies of amphiphiles at planar interfaces between thermotropic liquid crystals (LCs) and an aqueous phase can give rise to configurational transitions of the underlying LCs. A common assumption has been that a reconfiguration of the LC phase is caused by an interdigitation of the hydrophobic tails of amphiphiles with the molecules of the LC at the interface. A different mechanism is discovered here, whereby reorientation of the LC systems is shown to occur through lowering of the orientation-dependent surface energy of the LC due to formation of a thin isotropic layer at the aqueous interface. Using a combination of atomistic molecular dynamics simulations and experiments, we demonstrate that a monolayer of specific amphiphiles at an aqueous interface can cause a local nematic-to-isotropic phase transition of the LC by disturbing the antiparallel configuration of the LC molecules. Lastly, these results provide new insights into the interfacial, molecular-level organization of LCs that can be exploited for rational design of biological sensors and responsive systems.

Authors:
 [1];  [1];  [2]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [2]; ORCiD logo [4]
  1. Univ. of Chicago, IL (United States)
  2. Univ. of Wisconsin, Madison, WI (United States)
  3. Univ. of Massachusetts, Amherst, MA (United States)
  4. Univ. of Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE; US Army Research Office (ARO)
OSTI Identifier:
1498497
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 10; Journal Issue: 43; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; aqueous phase; simulations and experiments; thermotropic liquid crystals; thin isotropic layer

Citation Formats

Ramezani-Dakhel, Hadi, Rahimi, Mohammad, Pendery, Joel, Kim, Young-Ki, Thayumanavan, Sankaran, Roux, Benoît, Abbott, Nicholas L., and de Pablo, Juan J. Amphiphile-Induced Phase Transition of Liquid Crystals at Aqueous Interfaces. United States: N. p., 2018. Web. doi:10.1021/acsami.8b09639.
Ramezani-Dakhel, Hadi, Rahimi, Mohammad, Pendery, Joel, Kim, Young-Ki, Thayumanavan, Sankaran, Roux, Benoît, Abbott, Nicholas L., & de Pablo, Juan J. Amphiphile-Induced Phase Transition of Liquid Crystals at Aqueous Interfaces. United States. doi:10.1021/acsami.8b09639.
Ramezani-Dakhel, Hadi, Rahimi, Mohammad, Pendery, Joel, Kim, Young-Ki, Thayumanavan, Sankaran, Roux, Benoît, Abbott, Nicholas L., and de Pablo, Juan J. Thu . "Amphiphile-Induced Phase Transition of Liquid Crystals at Aqueous Interfaces". United States. doi:10.1021/acsami.8b09639. https://www.osti.gov/servlets/purl/1498497.
@article{osti_1498497,
title = {Amphiphile-Induced Phase Transition of Liquid Crystals at Aqueous Interfaces},
author = {Ramezani-Dakhel, Hadi and Rahimi, Mohammad and Pendery, Joel and Kim, Young-Ki and Thayumanavan, Sankaran and Roux, Benoît and Abbott, Nicholas L. and de Pablo, Juan J.},
abstractNote = {We report that monolayer assemblies of amphiphiles at planar interfaces between thermotropic liquid crystals (LCs) and an aqueous phase can give rise to configurational transitions of the underlying LCs. A common assumption has been that a reconfiguration of the LC phase is caused by an interdigitation of the hydrophobic tails of amphiphiles with the molecules of the LC at the interface. A different mechanism is discovered here, whereby reorientation of the LC systems is shown to occur through lowering of the orientation-dependent surface energy of the LC due to formation of a thin isotropic layer at the aqueous interface. Using a combination of atomistic molecular dynamics simulations and experiments, we demonstrate that a monolayer of specific amphiphiles at an aqueous interface can cause a local nematic-to-isotropic phase transition of the LC by disturbing the antiparallel configuration of the LC molecules. Lastly, these results provide new insights into the interfacial, molecular-level organization of LCs that can be exploited for rational design of biological sensors and responsive systems.},
doi = {10.1021/acsami.8b09639},
journal = {ACS Applied Materials and Interfaces},
number = 43,
volume = 10,
place = {United States},
year = {2018},
month = {10}
}

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