Self‐assembly continuously gains attention as an excellent method to create novel nanoscale structures with a wide range of applications in photonics, optoelectronics, biomedical engineering, and heat transfer applications. However, self‐assembly is governed by a diversity of complex interparticle forces that cause fabricating defectless large scale (>1 cm) colloidal crystals, or opals, to be a daunting challenge. Despite numerous efforts to find an optimal method that offers the perfect colloidal crystal by minimizing defects, it has been difficult to provide physical interpretations that govern the development of defects such as grain boundaries. This study reports the control over grain domains and intentional defect characteristics that develop during evaporative vertical deposition. The degree of particle crystallinity and evaporation conditions is shown to govern the grain domain characteristics, such as shapes and sizes. In particular, the grains fabricated with 300 and 600 nm sphere diameters can be tuned into single‐column structures exceeding ≈1 mm by elevating heating temperature up to 93 °C. The understanding of self‐assembly physics presented in this work will enable the fabrication of novel self‐assembled structures with high periodicity and offer fundamental groundworks for developing large‐scale crack‐free structures.
- Award ID(s):
- 1810485
- NSF-PAR ID:
- 10282421
- Date Published:
- Journal Name:
- Chemical Society Reviews
- Volume:
- 50
- Issue:
- 10
- ISSN:
- 0306-0012
- Page Range / eLocation ID:
- 5898 to 5951
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
Abstract -
Abstract Liquid crystals offer a dynamic platform for developing advanced photonics and soft actuation systems due to their unique and facile tunability and reconfigurability. Achieving precise spatial patterning of the liquid crystal alignment is critical to developing electro‐optical devices, programmable origami, directed colloidal assembly, and controlling active matter. Here, a simple method is demonstrated to achieve continuous 3D control of the directions of liquid crystal mesogens using a two‐step photo‐exposure process. In the first step, polarized light sets the orientation in the plane of confining substrates; the second step uses unpolarized light of a prescribed dose to set the out‐of‐plane orientation. The method enables smoothly varying orientational patterns with sub‐micrometer precision. As a demonstration, the setup is used to create gradient‐index lenses with parabolic refractive index profiles that remain stable without external electric fields. The lenses' focal length and sensitivity to light polarization are characterized through experimental and numerical methods. The findings pave the way for developing next‐generation photonic devices and actuated materials, with potential applications in molecular self‐assembly, re‐configurable optics, and responsive matter.
-
Abstract Metamolecules and crystals consisting of nanoscale building blocks offer rich models to study colloidal chemistry, materials science, and photonics. Herein we demonstrate the self‐assembly of colloidal Ag nanoparticles into quasi‐one‐dimensional metamolecules with an intriguing self‐healing ability in a linearly polarized optical field. By investigating the spatial stability of the metamolecules, we found that the origin of self‐healing is the inhomogeneous interparticle electrodynamic interactions enhanced by the formation of unusual nanoparticle dimers, which minimize the free energy of the whole structure. The equilibrium configuration and self‐healing behavior can be further tuned by modifying the electrical double layers surrounding the nanoparticles. Our results reveal a unique route to build self‐healing colloidal structures assembled from simple metal nanoparticles. This approach could potentially lead to reconfigurable plasmonic devices for photonic and sensing applications.
-
Abstract Metamolecules and crystals consisting of nanoscale building blocks offer rich models to study colloidal chemistry, materials science, and photonics. Herein we demonstrate the self‐assembly of colloidal Ag nanoparticles into quasi‐one‐dimensional metamolecules with an intriguing self‐healing ability in a linearly polarized optical field. By investigating the spatial stability of the metamolecules, we found that the origin of self‐healing is the inhomogeneous interparticle electrodynamic interactions enhanced by the formation of unusual nanoparticle dimers, which minimize the free energy of the whole structure. The equilibrium configuration and self‐healing behavior can be further tuned by modifying the electrical double layers surrounding the nanoparticles. Our results reveal a unique route to build self‐healing colloidal structures assembled from simple metal nanoparticles. This approach could potentially lead to reconfigurable plasmonic devices for photonic and sensing applications.
-
Abstract The unique optical properties of transition metal dichalcogenide (TMD) monolayers have attracted significant attention for both photonics applications and fundamental studies of low-dimensional systems. TMD monolayers of high optical quality, however, have been limited to micron-sized flakes produced by low-throughput and labour-intensive processes, whereas large-area films are often affected by surface defects and large inhomogeneity. Here we report a rapid and reliable method to synthesize macroscopic-scale TMD monolayers of uniform, high optical quality. Using 1-dodecanol encapsulation combined with gold-tape-assisted exfoliation, we obtain monolayers with lateral size > 1 mm, exhibiting exciton energy, linewidth, and quantum yield uniform over the whole area and close to those of high-quality micron-sized flakes. We tentatively associate the role of the two molecular encapsulating layers as isolating the TMD from the substrate and passivating the chalcogen vacancies, respectively. We demonstrate the utility of our encapsulated monolayers by scalable integration with an array of photonic crystal cavities, creating polariton arrays with enhanced light-matter coupling strength. This work provides a pathway to achieving high-quality two-dimensional materials over large areas, enabling research and technology development beyond individual micron-sized devices.