TY - JOUR
T1 - 45% Periodicity Reduction in Nanocomposite Thin Films via Rapid Solvent Removal
AU - Huang, Jingyu
AU - Chen, Xiangfan
AU - Bai, Peter
AU - Hai, Rihan
AU - Sun, Cheng
AU - Xu, Ting
N1 - Funding Information:
This work was funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under Contract DE-AC02-05-CH11231 (Organic−Inorganic Nanocomposites KC3104). Optical studies were funded by the NSF EEC1530734. In situ GISAXS and XR were done at Advanced Photon Source, use of the Advanced Photon Source was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract DE-AC02-06CH1135. Scattering studies at the Advanced Light Source is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract DE-AC02-05CH11231.
Funding Information:
GISAXS and XR were done at Advanced Photon Source use of the Advanced Photon Source was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract DE-AC02-06CH1135. Scattering studies at the Advanced Light Source is supported by the U.S. Department of Energy, Office of Science Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract DE-AC02-05CH11231.
Publisher Copyright:
© 2019 American Chemical Society.
PY - 2019/2/26
Y1 - 2019/2/26
N2 - In comparison to top-down approaches, nanocomposite thin films are more compatible with nanoparticle (NP) chemistry, device integration, and scalable manufacturing. Nanocomposites have long been promised as an ideal option to fabricate metamaterials that harvest the collective properties enabled by ordered 3D NP assemblies. However, most of accessible NP assemblies, governed by their phase diagrams, are not suitable to achieve the targeted properties and require lengthy assembly processes. Here, we investigated the kinetic pathway of NP assembly in lamellar supramolecular nanocomposite thin films during solvent vapor annealing and after solvent removal. By balancing the solvent field, diffusion rate, and thermodynamic driving force during rapid solvent removal (<3 s), we produced well-ordered 3D NP assemblies far away from the equilibrium state. Their degree of ordering depends on the terminal solvent fraction rather than the exact rapid solvent removal rate. The periodicity of these nanocomposites can be readily decoupled from the NP size and reduced to ∼50% of the periodicity in melt. The current study provides a facile approach to access nonequilibrium structures in nanocomposite thin films for the fabrication of functional metamaterial coatings.
AB - In comparison to top-down approaches, nanocomposite thin films are more compatible with nanoparticle (NP) chemistry, device integration, and scalable manufacturing. Nanocomposites have long been promised as an ideal option to fabricate metamaterials that harvest the collective properties enabled by ordered 3D NP assemblies. However, most of accessible NP assemblies, governed by their phase diagrams, are not suitable to achieve the targeted properties and require lengthy assembly processes. Here, we investigated the kinetic pathway of NP assembly in lamellar supramolecular nanocomposite thin films during solvent vapor annealing and after solvent removal. By balancing the solvent field, diffusion rate, and thermodynamic driving force during rapid solvent removal (<3 s), we produced well-ordered 3D NP assemblies far away from the equilibrium state. Their degree of ordering depends on the terminal solvent fraction rather than the exact rapid solvent removal rate. The periodicity of these nanocomposites can be readily decoupled from the NP size and reduced to ∼50% of the periodicity in melt. The current study provides a facile approach to access nonequilibrium structures in nanocomposite thin films for the fabrication of functional metamaterial coatings.
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U2 - 10.1021/acs.macromol.8b02071
DO - 10.1021/acs.macromol.8b02071
M3 - Article
AN - SCOPUS:85061896263
SN - 0024-9297
VL - 52
SP - 1803
EP - 1809
JO - Macromolecules
JF - Macromolecules
IS - 4
ER -