Abstract
The design and assembly of monodisperse colloidal particles not only advances the development of functional materials, but also provides colloidal model systems for understanding phase behaviors of molecules. This communication describes the gram-scale synthesis of highly uniform colloidal cuboids with tunable dimension and shape biaxiality and their molecular mesogen-like assembly into various mesophasic structures in pristine purity. The synthesis relies on the nanoemulsion-guided generation of ammonium sulfate crystals that template the subsequent silica coating. The shape of the cuboidal particles can be tuned from square platelike, to biaxial boardlike, and to rodlike by independently controlling the length, width and thickness of the particles. We demonstrated the assembly of the cuboidal colloids into highly pure mesoscopic liquid crystal phases, including smectic A, biaxial smectic A, crystal B, discotic, and columnar phases, as well as established a correlation between mesophasic formation and colloidal biaxiality in experiments.
Highlights
The design and assembly of monodisperse colloidal particles advances the development of functional materials, and provides colloidal model systems for understanding phase behaviors of molecules
The assembly of such colloids leads to the coexistence of multiple phases and genetic defects, which hinders a deep understanding of their liquid crystals (LCs) behaviors and the discovery of potential applications of resulting materials[35]. This communication presents the gram-scale synthesis of highly monodisperse colloidal cuboids with tunable dimension and shape biaxiality and their molecular mesogen-like assembly into various mesophasic structures in pristine purity. This synthetic method relies on the nanoemulsion-guided formation of well-defined ammonium sulfate ((NH4)2SO4) crystals that template the subsequent hydrolysis of tetraethoxysilane (TEOS) to produce uniform cuboids in a one-pot reaction with iron (III) cation (Fe3+), PVP, and sodium citrate (SC) as structuredirecting agents
An aqueous solution containing ethanol, iron (III) sulfate (Fe2(SO4)3), and SC was first emulsified in n-pentanol dissolved with PVP to generate nanosized water-inoil emulsions (Fig. 1a and see Methods for experimental details) 28,36,37
Summary
The design and assembly of monodisperse colloidal particles advances the development of functional materials, and provides colloidal model systems for understanding phase behaviors of molecules This communication describes the gram-scale synthesis of highly uniform colloidal cuboids with tunable dimension and shape biaxiality and their molecular mesogen-like assembly into various mesophasic structures in pristine purity. The assembly of such colloids leads to the coexistence of multiple phases and genetic defects (rather than single pristine phases), which hinders a deep understanding of their LC behaviors and the discovery of potential applications of resulting materials[35] This communication presents the gram-scale synthesis of highly monodisperse colloidal cuboids with tunable dimension and shape biaxiality and their molecular mesogen-like assembly into various mesophasic structures in pristine purity. It offers a mesoscopic model of LC molecules for understanding molecular assembly
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