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Predictive supracolloidal helices from patchy particles.

Guo R, Mao J, Xie XM, Yan LT - Sci Rep (2014)

Bottom Line: Here, inspired by biological helices, we show that the rational design of patchy arrangement and interaction can drive patchy particles to self-assemble into biomolecular mimetic supracolloidal helices.We further derive a facile design rule for encoding the target supracolloidal helices, thus opening the doors to the predictive science of these supracolloidal architectures.It is also found that kinetics and reaction pathway during the formation of supracolloidal helices offer a unique way to study supramolecular polymerization, and that well-controlled supracolloidal helices can exhibit tailorable circular dichroism effects at visible wavelengths.

View Article: PubMed Central - PubMed

Affiliation: Key Laboratory of Advanced Materials (MOE), Department of Chemical Engineering, Tsinghua University, Beijing 100084, P. R. China.

ABSTRACT
A priori prediction of supracolloidal architectures from nanoparticle and colloidal assembly is a challenging goal in materials chemistry and physics. Despite intense research in this area, much less has been known about the predictive science of supracolloidal helices from designed building blocks. Therefore, developing conceptually new rules to construct supracolloidal architectures with predictive helicity is becoming an important and urgent task of great scientific interest. Here, inspired by biological helices, we show that the rational design of patchy arrangement and interaction can drive patchy particles to self-assemble into biomolecular mimetic supracolloidal helices. We further derive a facile design rule for encoding the target supracolloidal helices, thus opening the doors to the predictive science of these supracolloidal architectures. It is also found that kinetics and reaction pathway during the formation of supracolloidal helices offer a unique way to study supramolecular polymerization, and that well-controlled supracolloidal helices can exhibit tailorable circular dichroism effects at visible wavelengths.

No MeSH data available.


Related in: MedlinePlus

Reaction pathways of helical self-assembly.The mechanisms, all of which we have observed in simulations, include addition of individual particles, addition of fragments, cyclization of fragments, break of incomplete rings, fracture and reconfiguration of disordered clusters, and addition and reconfiguration of helices. Details of the structure evolution are shown in Figs. S10–S12.
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f4: Reaction pathways of helical self-assembly.The mechanisms, all of which we have observed in simulations, include addition of individual particles, addition of fragments, cyclization of fragments, break of incomplete rings, fracture and reconfiguration of disordered clusters, and addition and reconfiguration of helices. Details of the structure evolution are shown in Figs. S10–S12.

Mentions: To understand the kinetic mechanisms, we turn to the detailed analysis of the change in the concentrations of different species in the course of self-assembly. Based on patchy interactions directed by their types, four representative species are concerned: individual patchy particle (IP), colloidal cluster linked by self-complementary patches (SP), colloidal cluster linked by a pair of complementary patches (PP), and the elementary colloidal cluster of perfect helix (EC) (Fig. 3b). Fig. 3b shows that the concentration of IP is extremely reduced at the initial stage owing to the formation of SP and PP. The complementary patches in SP and PP link each other spontaneously while the formation of EC with long-ranged patchy addition is relatively slow. Thus, the reactions of SP and PP dominate the kinetics in the first regime, resulting in the characteristic of reaction-controlled step-growth polymerization. In the second regime, the reaction of EC however becomes the major effect, where sophisticated dynamical interconversion between clusters, which is elaborated in Fig. 4 and Fig. S9, induces obvious fluctuation in the kinetic plot. The distribution of colloidal clusters also becomes wider in the second regime, as demonstrated by Fig. 3c.


Predictive supracolloidal helices from patchy particles.

Guo R, Mao J, Xie XM, Yan LT - Sci Rep (2014)

Reaction pathways of helical self-assembly.The mechanisms, all of which we have observed in simulations, include addition of individual particles, addition of fragments, cyclization of fragments, break of incomplete rings, fracture and reconfiguration of disordered clusters, and addition and reconfiguration of helices. Details of the structure evolution are shown in Figs. S10–S12.
© Copyright Policy - open-access
Related In: Results  -  Collection

License
Show All Figures
getmorefigures.php?uid=PMC4228328&req=5

f4: Reaction pathways of helical self-assembly.The mechanisms, all of which we have observed in simulations, include addition of individual particles, addition of fragments, cyclization of fragments, break of incomplete rings, fracture and reconfiguration of disordered clusters, and addition and reconfiguration of helices. Details of the structure evolution are shown in Figs. S10–S12.
Mentions: To understand the kinetic mechanisms, we turn to the detailed analysis of the change in the concentrations of different species in the course of self-assembly. Based on patchy interactions directed by their types, four representative species are concerned: individual patchy particle (IP), colloidal cluster linked by self-complementary patches (SP), colloidal cluster linked by a pair of complementary patches (PP), and the elementary colloidal cluster of perfect helix (EC) (Fig. 3b). Fig. 3b shows that the concentration of IP is extremely reduced at the initial stage owing to the formation of SP and PP. The complementary patches in SP and PP link each other spontaneously while the formation of EC with long-ranged patchy addition is relatively slow. Thus, the reactions of SP and PP dominate the kinetics in the first regime, resulting in the characteristic of reaction-controlled step-growth polymerization. In the second regime, the reaction of EC however becomes the major effect, where sophisticated dynamical interconversion between clusters, which is elaborated in Fig. 4 and Fig. S9, induces obvious fluctuation in the kinetic plot. The distribution of colloidal clusters also becomes wider in the second regime, as demonstrated by Fig. 3c.

Bottom Line: Here, inspired by biological helices, we show that the rational design of patchy arrangement and interaction can drive patchy particles to self-assemble into biomolecular mimetic supracolloidal helices.We further derive a facile design rule for encoding the target supracolloidal helices, thus opening the doors to the predictive science of these supracolloidal architectures.It is also found that kinetics and reaction pathway during the formation of supracolloidal helices offer a unique way to study supramolecular polymerization, and that well-controlled supracolloidal helices can exhibit tailorable circular dichroism effects at visible wavelengths.

View Article: PubMed Central - PubMed

Affiliation: Key Laboratory of Advanced Materials (MOE), Department of Chemical Engineering, Tsinghua University, Beijing 100084, P. R. China.

ABSTRACT
A priori prediction of supracolloidal architectures from nanoparticle and colloidal assembly is a challenging goal in materials chemistry and physics. Despite intense research in this area, much less has been known about the predictive science of supracolloidal helices from designed building blocks. Therefore, developing conceptually new rules to construct supracolloidal architectures with predictive helicity is becoming an important and urgent task of great scientific interest. Here, inspired by biological helices, we show that the rational design of patchy arrangement and interaction can drive patchy particles to self-assemble into biomolecular mimetic supracolloidal helices. We further derive a facile design rule for encoding the target supracolloidal helices, thus opening the doors to the predictive science of these supracolloidal architectures. It is also found that kinetics and reaction pathway during the formation of supracolloidal helices offer a unique way to study supramolecular polymerization, and that well-controlled supracolloidal helices can exhibit tailorable circular dichroism effects at visible wavelengths.

No MeSH data available.


Related in: MedlinePlus