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Title: Nonadditive Interactions Unlock Small-Particle Mobility in Binary Colloidal Monolayers

Journal Article · · ACS Nano
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]
  1. Univ. of California, Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States); STROBE NSF Science & Technology Center, Berkeley, CA (United States)

We examine the organization and dynamics of binary colloidal monolayers composed of micron-scale silica particles interspersed with smaller-diameter silica particles that serve as minority component impurities. These binary monolayers are prepared at the surface of ionic liquid droplets over a range of size ratios (σ = 0.16–0.66) and are studied with low-dose minimally perturbative scanning electron microscopy (SEM). The high resolution of SEM imaging provides direct tracking of all particle coordinates over time, enabling a complete description of the microscopic state. In these bidisperse size mixtures, particle interactions are nonadditive because interfacial pinning to the droplet surface causes the equators of differently sized particles to lie in separate planes. By varying the size ratio, we control the extent of nonadditivity in order to achieve phase behavior inaccessible to additive 2D systems. Across the range of size ratios, we tune the system from a mobile small-particle phase (σ < 0.24) to an interstitial solid (0.24 < σ < 0.33) and furthermore to a disordered glass (σ > 0.33). These distinct phase regimes are classified through measurements of hexagonal ordering of the large-particle host lattice and the lattice’s capacity for small-particle transport. Altogether, we explain these structural and dynamic trends by considering the combined influence of interparticle interactions and the colloidal packing geometry. Our measurements are reproduced in molecular dynamics simulations of 2D nonadditive disks, suggesting an efficient method for describing confined systems with reduced dimensionality representations.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
2234121
Journal Information:
ACS Nano, Vol. 17, Issue 9; ISSN 1936-0851
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (48)

Quasicrystalline order in self-assembled binary nanoparticle superlattices journal October 2009
Assessing Pair Interaction Potentials of Nanoparticles on Liquid Interfaces journal February 2019
Self-diffusion in two-dimensional binary colloidal hard-sphere fluids journal January 2017
Complex alloy phases for binary hard-disc mixtures journal July 1993
Self-Organization of Bidisperse Colloids in Water Droplets journal October 2005
Transition in Dynamics as Nanoparticles Jam at the Liquid/Liquid Interface journal October 2017
Structural phases in non-additive soft-disk mixtures: Glasses, substitutional order, and random tilings journal December 2011
Structure factors in a two-dimensional binary colloidal hard sphere system journal July 2018
The physics of the colloidal glass transition journal May 2012
Colloidal matter: Packing, geometry, and entropy journal August 2015
Role of Repulsive Forces in Determining the Equilibrium Structure of Simple Liquids journal June 1971
Layering, freezing, and re-entrant melting of hard spheres in soft confinement journal February 2012
Visualizing the Dynamics of Nanoparticles in Liquids by Scanning Electron Microscopy journal May 2016
Geometric frustration in buckled colloidal monolayers journal December 2008
Perspective: The Asakura Oosawa model: A colloid prototype for bulk and interfacial phase behavior journal October 2014
Dynamics of particles and cages in an experimental 2D glass former journal December 2009
Equilibrium Grain Boundary Segregation and Clustering of Impurities in Colloidal Polycrystalline Monolayers journal November 2016
Two-Dimensional Binary and Ternary Nanocrystal Superlattices: The Case of Monolayers and Bilayers journal April 2011
Nonadditivity of nanoparticle interactions journal October 2015
Explicit Analytical Solution for Random Close Packing in d=2 and d=3 journal January 2022
Experimental Observation of Structural Crossover in Binary Mixtures of Colloidal Hard Spheres journal May 2007
Mapping the jamming transition of bidisperse mixtures journal March 2016
Discovery of two-dimensional binary nanoparticle superlattices using global Monte Carlo optimization journal December 2022
Directed self-assembly of a colloidal kagome lattice journal January 2011
Nanoparticle Assembly at Liquid-Liquid Interfaces: From the Nanoscale to Mesoscale journal July 2018
Two-Dimensional Interfacial Colloidal Crystals journal August 1980
Bidisperse Nanospheres Jammed on a Liquid Surface journal August 2020
LAMMPS - a flexible simulation tool for particle-based materials modeling at the atomic, meso, and continuum scales journal February 2022
Quasicrystalline nanocrystal superlattice with partial matching rules journal September 2016
Solid Nanoparticles that Catalyze Biofuel Upgrade Reactions at the Water/Oil Interface journal December 2009
Layer-by-Layer Growth of Binary Colloidal Crystals journal April 2002
Non-additive simple potentials for pre-programmed self-assembly journal January 2015
Methods of Digital Video Microscopy for Colloidal Studies journal April 1996
Partial clustering prevents global crystallization in a binary 2D colloidal glass former journal July 2009
Approaches to self-assembly of colloidal monolayers: A guide for nanotechnologists journal August 2017
Prediction of binary hard-sphere crystal structures journal April 2009
Phase Behavior of Dense Colloidal Binary Monolayers journal November 2012
Anomalous dynamics of interstitial dopants in soft crystals journal November 2016
Imaging and Manipulating Energy Transfer Among Quantum Dots at Individual Dot Resolution journal May 2017
Communication: Radial distribution functions in a two-dimensional binary colloidal hard sphere system journal April 2014
Experimental realization of a model glass former in 2D journal October 2005
Infinite-pressure phase diagram of binary mixtures of (non)additive hard disks journal May 2020
Phase behavior of nonadditive hard-sphere mixtures journal December 1998
Charging-driven coarsening and melting of a colloidal nanoparticle monolayer at an ionic liquid–vacuum interface journal January 2020
Self-Assembly of Colloidal Nanocrystals: From Intricate Structures to Functional Materials journal August 2016
Self-assembly of dodecagonal and octagonal quasicrystals in hard spheres on a plane journal January 2023
Tailoring the Wettability of Colloidal Particles for Pickering Emulsions via Surface Modification and Roughness journal June 2018
Diffusion and interactions of interstitials in hard-sphere interstitial solid solutions journal December 2017