Assembly of multi-flavored two-dimensional colloidal crystals

Mahynski, Nathan A.; Zerze, Hasan; Hatch, Harold W.; Shen, Vincent K.; Mittal, Jeetain

doi:10.1039/c7sm01005b

Cited by 20 publications

(23 citation statements)

References 64 publications

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“…This sequence of phases is accompanied by a change in the relative stoichiometry from one to zero. These results are consistent with previous computational studies (25,26).…”

Section: Physicssupporting

confidence: 94%

Two-step crystallization and solid–solid transitions in binary colloidal mixtures

Fang

Hagan

Rogers

2020

Proc. Natl. Acad. Sci. U.S.A.

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Crystallization is fundamental to materials science and is central to a variety of applications, ranging from the fabrication of silicon wafers for microelectronics to the determination of protein structures. The basic picture is that a crystal nucleates from a homogeneous fluid by a spontaneous fluctuation that kicks the system over a single free-energy barrier. However, it is becoming apparent that nucleation is often more complicated than this simple picture and, instead, can proceed via multiple transformations of metastable structures along the pathway to the thermodynamic minimum. In this article, we observe, characterize, and model crystallization pathways using DNA-coated colloids. We use optical microscopy to investigate the crystallization of a binary colloidal mixture with single-particle resolution. We observe classical one-step pathways and nonclassical two-step pathways that proceed via a solid–solid transformation of a crystal intermediate. We also use enhanced sampling to compute the free-energy landscapes corresponding to our experiments and show that both one- and two-step pathways are driven by thermodynamics alone. Specifically, the two-step solid–solid transition is governed by a competition between two different crystal phases with free energies that depend on the crystal size. These results extend our understanding of available pathways to crystallization, by showing that size-dependent thermodynamic forces can produce pathways with multiple crystal phases that interconvert without free-energy barriers and could provide approaches to controlling the self-assembly of materials made from colloids.

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“…This sequence of phases is accompanied by a change in the relative stoichiometry from one to zero. These results are consistent with previous computational studies (25,26).…”

Section: Physicssupporting

confidence: 94%

Two-step crystallization and solid–solid transitions in binary colloidal mixtures

Fang

Hagan

Rogers

2020

Proc. Natl. Acad. Sci. U.S.A.

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“…Specifically, we have applied this methodology to probe the self-assembly of monodisperse colloidal monolayers formed from systems inspired by the multi-flavoring motif used in DFP assembly; this scheme enables all pairwise interactions in the system to become independent of one another, qualitatively ranging from being attractive to repulsive. In the limit of strong binding, the ground state ( T * → 0) serves as a reasonable approximation of the thermodynamically stable state 55 . Multi-flavored binary mixtures of colloids dominated by enthalpic interactions are known to exhibit a wide variety of morphologies, both experimentally and theoretically 18,55 ; however, the full impact of stoichiometry on the thermodynamics of their self-assembly is not yet understood.…”

Section: Resultsmentioning

confidence: 99%

“…In the limit of strong binding, the ground state ( T * → 0) serves as a reasonable approximation of the thermodynamically stable state 55 . Multi-flavored binary mixtures of colloids dominated by enthalpic interactions are known to exhibit a wide variety of morphologies, both experimentally and theoretically 18,55 ; however, the full impact of stoichiometry on the thermodynamics of their self-assembly is not yet understood. Here we employ a simplified model (cf.…”

Section: Resultsmentioning

confidence: 99%

Using symmetry to elucidate the importance of stoichiometry in colloidal crystal assembly

et al. 2019

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We demonstrate a method based on symmetry to predict the structure of self-assembling, multicomponent colloidal mixtures. This method allows us to feasibly enumerate candidate structures from all symmetry groups and is many orders of magnitude more computationally efficient than combinatorial enumeration of these candidates. In turn, this permits us to compute ground-state phase diagrams for multicomponent systems. While tuning the interparticle potentials to produce potentially complex interactions represents the conventional route to designing exotic lattices, we use this scheme to demonstrate that simple potentials can also give rise to such structures which are thermodynamically stable at moderate to low temperatures. Furthermore, for a model two-dimensional colloidal system, we illustrate that lattices forming a complete set of 2-, 3-, 4-, and 6-fold rotational symmetries can be rationally designed from certain systems by tuning the mixture composition alone, demonstrating that stoichiometric control can be a tool as powerful as directly tuning the interparticle potentials themselves.

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“…Previous investigation into the self-assembly of two-dimensional multiflavored nanoscale colloids revealed that their morphologies could be rationalized on the basis of energetic arguments. 40 However, three-dimensional micron-scale systems remain largely unexplored systematically. Furthermore, many studies of binary DFP systems focus on cases where size disparity between the system components is used in addition to interparticle interactions to drive the assembly towards desired structures.…”

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confidence: 99%

Assembly of three-dimensional binary superlattices from multi-flavored particles

et al. 2018

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Binary superlattices constructed from nano- or micron-sized colloidal particles have a wide variety of applications, including the design of advanced materials. Self-assembly of such crystals from their constituent colloids can be achieved in practice by, among other means, the functionalization of colloid surfaces with single-stranded DNA sequences. However, when driven by DNA, this assembly is traditionally premised on the pairwise interaction between a single DNA sequence and its complement, and often relies on particle size asymmetry to entropically control the crystalline arrangement of its constituents. The recently proposed "multi-flavoring" motif for DNA functionalization, wherein multiple distinct strands of DNA are grafted in different ratios to different colloids, can be used to experimentally realize a binary mixture in which all pairwise interactions are independently controllable. In this work, we use various computational methods, including molecular dynamics and Wang-Landau Monte Carlo simulations, to study a multi-flavored binary system of micron-sized DNA-functionalized particles modeled implicitly by Fermi-Jagla pairwise interactions. We show how self-assembly of such systems can be controlled in a purely enthalpic manner, and by tuning only the interactions between like particles, demonstrate assembly into various morphologies. Although polymorphism is present over a wide range of pairwise interaction strengths, we show that careful selection of interactions can lead to the generation of pure compositionally ordered crystals. Additionally, we show how the crystal composition changes with the like-pair interaction strengths, and how the solution stoichiometry affects the assembled structures.

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Assembly of multi-flavored two-dimensional colloidal crystals

Cited by 20 publications

References 64 publications

Two-step crystallization and solid–solid transitions in binary colloidal mixtures

Two-step crystallization and solid–solid transitions in binary colloidal mixtures

Using symmetry to elucidate the importance of stoichiometry in colloidal crystal assembly

Assembly of three-dimensional binary superlattices from multi-flavored particles

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