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Title: Thermally reconfigurable monoclinic nematic colloidal fluids

Abstract

Fundamental relationships are believed to exist between the symmetries of building blocks and the condensed matter phases that they form. For example, constituent molecular and colloidal rods and disks impart their uniaxial symmetry onto nematic liquid crystals, such as those used in displays. Low-symmetry organizations could form in mixtures of rods and disks, but entropy tends to phase-separate them at the molecular and colloidal scales, whereas strong elasticity-mediated interactions drive the formation of chains and crystals in nematic colloids. To have a structure with few or no symmetry operations apart from trivial ones has so far been demonstrated to be a property of solids alone, but not of their fully fluid condensed matter counterparts, even though such symmetries have been considered theoretically and observed in magnetic colloids. In this work, we show that dispersing highly anisotropic charged colloidal disks in a nematic host composed of molecular rods provides a platform for observing many low-symmetry phases. Depending on the temperature, concentration and surface charge of the disks, we find nematic, smectic and columnar organizations with symmetries ranging from uniaxial to orthorhombic and monoclinic. With increasing temperature, we observe unusual transitions from less- to more-ordered states and re-entrant phases. Most importantly, wemore » demonstrate the presence of reconfigurable monoclinic colloidal nematic order, as well as the possibility of thermal and magnetic control of low-symmetry self-assembly. Our experimental findings are supported by theoretical modelling of the colloidal interactions between disks in the nematic host and may provide a route towards realizing many low-symmetry condensed matter phases in systems with building blocks of dissimilar shapes and sizes, as well as their technological applications.« less

Authors:
 [1];  [1];  [2];  [3]
  1. Univ. of Colorado, Boulder, CO (United States)
  2. Univ. Paris-Saclay, Orsay (France)
  3. Univ. of Colorado, Boulder, CO (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
Univ. of Colorado, Boulder, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1764614
Grant/Contract Number:  
SC0019293
Resource Type:
Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Name: Nature (London); Journal Volume: 590; Journal Issue: 7845; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; symmetry; colloid; phase behavior; monoclinic order; colloids; liquid crystals; molecular self-assembly; nanoparticles; phase transitions and critical phenomena

Citation Formats

Mundoor, Haridas, Wu, Jin-Sheng, Wensink, Henricus H., and Smalyukh, Ivan I. Thermally reconfigurable monoclinic nematic colloidal fluids. United States: N. p., 2021. Web. doi:10.1038/s41586-021-03249-0.
Mundoor, Haridas, Wu, Jin-Sheng, Wensink, Henricus H., & Smalyukh, Ivan I. Thermally reconfigurable monoclinic nematic colloidal fluids. United States. https://doi.org/10.1038/s41586-021-03249-0
Mundoor, Haridas, Wu, Jin-Sheng, Wensink, Henricus H., and Smalyukh, Ivan I. Wed . "Thermally reconfigurable monoclinic nematic colloidal fluids". United States. https://doi.org/10.1038/s41586-021-03249-0. https://www.osti.gov/servlets/purl/1764614.
@article{osti_1764614,
title = {Thermally reconfigurable monoclinic nematic colloidal fluids},
author = {Mundoor, Haridas and Wu, Jin-Sheng and Wensink, Henricus H. and Smalyukh, Ivan I.},
abstractNote = {Fundamental relationships are believed to exist between the symmetries of building blocks and the condensed matter phases that they form. For example, constituent molecular and colloidal rods and disks impart their uniaxial symmetry onto nematic liquid crystals, such as those used in displays. Low-symmetry organizations could form in mixtures of rods and disks, but entropy tends to phase-separate them at the molecular and colloidal scales, whereas strong elasticity-mediated interactions drive the formation of chains and crystals in nematic colloids. To have a structure with few or no symmetry operations apart from trivial ones has so far been demonstrated to be a property of solids alone, but not of their fully fluid condensed matter counterparts, even though such symmetries have been considered theoretically and observed in magnetic colloids. In this work, we show that dispersing highly anisotropic charged colloidal disks in a nematic host composed of molecular rods provides a platform for observing many low-symmetry phases. Depending on the temperature, concentration and surface charge of the disks, we find nematic, smectic and columnar organizations with symmetries ranging from uniaxial to orthorhombic and monoclinic. With increasing temperature, we observe unusual transitions from less- to more-ordered states and re-entrant phases. Most importantly, we demonstrate the presence of reconfigurable monoclinic colloidal nematic order, as well as the possibility of thermal and magnetic control of low-symmetry self-assembly. Our experimental findings are supported by theoretical modelling of the colloidal interactions between disks in the nematic host and may provide a route towards realizing many low-symmetry condensed matter phases in systems with building blocks of dissimilar shapes and sizes, as well as their technological applications.},
doi = {10.1038/s41586-021-03249-0},
journal = {Nature (London)},
number = 7845,
volume = 590,
place = {United States},
year = {Wed Feb 10 00:00:00 EST 2021},
month = {Wed Feb 10 00:00:00 EST 2021}
}

Works referenced in this record:

Triclinic nematic colloidal crystals from competing elastic and electrostatic interactions
journal, March 2016


Colloidal diamond
journal, September 2020


Two-Dimensional Nematic Colloidal Crystals Self-Assembled by Topological Defects
journal, August 2006


Real-Space Imaging of Nucleation and Growth in Colloidal Crystallization
journal, April 2001


One-Step Hydrothermal Synthesis of Carboxyl-Functionalized Upconversion Phosphors for Bioapplications
journal, September 2012

  • Yang, Jianping; Shen, Dengke; Li, Xiaomin
  • Chemistry - A European Journal, Vol. 18, Issue 43
  • DOI: 10.1002/chem.201202336

Novel Colloidal Interactions in Anisotropic Fluids
journal, March 1997


Biaxial Nematic Phase in a Thermotropic Liquid-Crystalline Side-Chain Polymer
journal, March 2004


Observation of a Biaxial Nematic Phase in Potassium Laurate-1-Decanol-Water Mixtures
journal, September 1980


Determination of the positions and orientations of concentrated rod-like colloids from 3D microscopy data
journal, April 2015


Multimodal nonlinear optical polarizing microscopy of long-range molecular order in liquid crystals
journal, January 2010

  • Lee, Taewoo; Trivedi, Rahul P.; Smalyukh, Ivan I.
  • Optics Letters, Vol. 35, Issue 20
  • DOI: 10.1364/OL.35.003447

Three-dimensional parallel particle manipulation and tracking by integrating holographic optical tweezers and engineered point spread functions
journal, January 2011

  • Conkey, Donald B.; Trivedi, Rahul P.; Pavani, Sri Rama Prasanna
  • Optics Express, Vol. 19, Issue 5
  • DOI: 10.1364/OE.19.003835

New Liquid-Crystal Phase Diagram
journal, July 1975


Coupling of the Orientations of Liquid Crystals to Electrical Double Layers Formed by the Dissociation of Surface-Immobilized Salts
journal, May 2001

  • Shah, Rahul R.; Abbott, Nicholas L.
  • The Journal of Physical Chemistry B, Vol. 105, Issue 21
  • DOI: 10.1021/jp004073g

Principles of Condensed Matter Physics
book, January 1995


Insights into phase transition kinetics from colloid science
journal, April 2002

  • Anderson, Valerie J.; Lekkerkerker, Henk N. W.
  • Nature, Vol. 416, Issue 6883
  • DOI: 10.1038/416811a

Molecular field theory for biaxial nematic liquid crystals composed of molecules with C 2 h point group symmetry
journal, July 2011

  • Luckhurst, Geoffrey R.; Naemura, Shohei; Sluckin, Timothy J.
  • Physical Review E, Vol. 84, Issue 1
  • DOI: 10.1103/PhysRevE.84.011704

Colloidal discs in nematic liquid crystals
journal, April 2004

  • Silvestre, N. M.; Patrício, P.; Tasinkevych, M.
  • Journal of Physics: Condensed Matter, Vol. 16, Issue 19
  • DOI: 10.1088/0953-8984/16/19/005

Macroscopic and molecular symmetries of unconventional nematic phases
journal, October 2006


Spectroscopic characterisation of the monoclinic and orthorhombic forms of paracetamol
journal, October 2002


Electrostatically controlled surface boundary conditions in nematic liquid crystals and colloids
journal, September 2019

  • Mundoor, Haridas; Senyuk, Bohdan; Almansouri, Mahmoud
  • Science Advances, Vol. 5, Issue 9
  • DOI: 10.1126/sciadv.aax4257

Experimental Realization of Biaxial Liquid Crystal Phases in Colloidal Dispersions of Boardlike Particles
journal, December 2009


Ultrasensitive Polarized Up-Conversion of Tm 3+ –Yb 3+ Doped β-NaYF 4 Single Nanorod
journal, April 2013

  • Zhou, Jiajia; Chen, Gengxu; Wu, E.
  • Nano Letters, Vol. 13, Issue 5
  • DOI: 10.1021/nl400807m

Glass Transitions in Quasi-Two-Dimensional Suspensions of Colloidal Ellipsoids
journal, August 2011


A General Method To Coat Colloidal Particles with Silica
journal, August 2003

  • Graf, Christina; Vossen, Dirk L. J.; Imhof, Arnout
  • Langmuir, Vol. 19, Issue 17
  • DOI: 10.1021/la0347859

Surface effects and anchoring in liquid crystals
journal, March 1991


Ferromagnetism in suspensions of magnetic platelets in liquid crystal
journal, December 2013

  • Mertelj, Alenka; Lisjak, Darja; Drofenik, Miha
  • Nature, Vol. 504, Issue 7479
  • DOI: 10.1038/nature12863

Liquid-Crystal Phases Formed in Mixed Suspensions of Rod- and Platelike Colloids
journal, December 2000

  • van der Kooij, F. M.; Lekkerkerker, H. N. W.
  • Langmuir, Vol. 16, Issue 26
  • DOI: 10.1021/la000875r

Liquid crystal phase transitions in mixtures of rodlike and platelike molecules
journal, October 1973

  • Alben, Richard
  • The Journal of Chemical Physics, Vol. 59, Issue 8
  • DOI: 10.1063/1.1680625

Freezing by Heating in a Driven Mesoscopic System
journal, February 2000


Rotational and translational diffusion of anisotropic gold nanoparticles in liquid crystals controlled by varying surface anchoring
journal, December 2013


Evidence for general tilt columnar liquid crystalline phase
journal, January 2009

  • Vaupotič, Nataša; Pociecha, Damian; Čepič, Mojca
  • Soft Matter, Vol. 5, Issue 11
  • DOI: 10.1039/b900722a

Electrically and Optically Tunable Plasmonic Guest–Host Liquid Crystals with Long-Range Ordered Nanoparticles
journal, June 2014

  • Liu, Qingkun; Yuan, Ye; Smalyukh, Ivan I.
  • Nano Letters, Vol. 14, Issue 7
  • DOI: 10.1021/nl501581y

Theory of bent-core liquid-crystal phases and phase transitions
journal, September 2002


Stokes Drag on a Sphere in a Nematic Liquid Crystal
journal, November 2004


Optical trapping of director structures and defects in liquid crystals using laser tweezers
journal, January 2007

  • Smalyukh, Ivan I.; Kaputa, Daniel S.; Kachynski, Aliaksandr V.
  • Optics Express, Vol. 15, Issue 7
  • DOI: 10.1364/OE.15.004359

Biaxial ferromagnetic liquid crystal colloids
journal, September 2016

  • Liu, Qingkun; Ackerman, Paul J.; Lubensky, Tom C.
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 38
  • DOI: 10.1073/pnas.1601235113

Hybrid molecular-colloidal liquid crystals
journal, May 2018


Liquid Crystal Colloids
journal, March 2018


Low–temperature biaxial nematic from rod and disc mesogen mixture
journal, January 2012


Alignment of high-aspect ratio colloidal gold nanoplatelets in nematic liquid crystals
journal, August 2011

  • Evans, Julian S.; Beier, Corinne N.; Smalyukh, Ivan I.
  • Journal of Applied Physics, Vol. 110, Issue 3
  • DOI: 10.1063/1.3620550

Ordered States of a Nematic Liquid
journal, May 1970


Mesostructured Composite Materials with Electrically Tunable Upconverting Properties
journal, August 2015


Evidence for Triclinic Symmetry in Smectic Liquid Crystals of Bent-Shape Molecules
journal, June 2001


Chromonic review
journal, January 2010

  • Lydon, John
  • Journal of Materials Chemistry, Vol. 20, Issue 45
  • DOI: 10.1039/b926374h