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Title: Preparation of nanocrystals and nanocomposites of nanocrystal-conjugated polymer, and their photophysical properties in confined geometries

Abstract

Semiconductors nanocrystals (NCs), also called quantum dots (QDs), have attracted tremendous interest over the past decade in the fields of physics, chemistry, and engineering. Due to the quantum-confined nature of QDs, the variation of particle size provides continuous and predictable changes in fluorescence emission. On the other hand, conjugated polymers (CPs) have been extensively studied for two decades due to their semiconductor-like optical and electronic properties. The electron and energy transfer between NCs and CPs occur in solar cells and light emitting diodes (LEDs), respectively. Placing CPs in direct contact with a NC (i.e., preparing NC-CP nanocomposites) carries advantage over cases where NC aggregation dominates. Such NC-CP nanocomposites possess a well-defined interface that significantly promotes the charge or energy transfer between these two components. However, very few studies have centered on such direct integration. We prepared NCs and NC-CP nanocomposites based on heck coupling and investigated the energy and charge transfer between semiconductor NCs (i.e., CdSe QDs), CPs (i.e., poly(3-hexyl thiophene) (P3HT)) in the nanocomposites in confined geometries. Two novel strategies were used to confine NC and/or NC-CP nanocomposites: (a) directly immobilizing nanohybrids, QDs and nanorods in nanoscopic porous alumina membrane (PAM) , and (b) confining the QDs and CPsmore » in sphere-on-flat geometry to induce self-assembly. While investigating the confinement effect, gradient concentric ring patterns of high regularity form spontaneously simply by allowing a droplet of solution containing either conjugated polymer or semiconductor nanocrystal in a consecutive stick-slip mothion in a confined geometry. Such constrained evaporation can be utilized as a simple, cheap, and robust strategy for self-assembling various materials with easily tailored optical and electronic properties into spatially ordered, two-dimensional patterns. These self-organized patterns of functional nanoscale materials over large areas offer a tremendous potential for applications in optoelectronic devices, LEDs, solar cells, and biosensors. Meanwhile, spherical nanocrystals (i.e. CdSe/ZnS core/shell QDs) were placed in a hexagonal array of highly ordered cylindrical nanopores of PAMs by a simple dip-coating method and vacuum suction process, respectively. The fluorescence of CdSe/ZnS QD was retained after being filled inside PAMs and the filling contents were obtained via transmission UV-vis measurements.« less

Authors:
 [1]
  1. Iowa State Univ., Ames, IA (United States)
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1342577
Report Number(s):
IS-T 3181
DOE Contract Number:
AC02-07CH11358
Resource Type:
Thesis/Dissertation
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Xu, Jun. Preparation of nanocrystals and nanocomposites of nanocrystal-conjugated polymer, and their photophysical properties in confined geometries. United States: N. p., 2007. Web. doi:10.2172/1342577.
Xu, Jun. Preparation of nanocrystals and nanocomposites of nanocrystal-conjugated polymer, and their photophysical properties in confined geometries. United States. doi:10.2172/1342577.
Xu, Jun. Mon . "Preparation of nanocrystals and nanocomposites of nanocrystal-conjugated polymer, and their photophysical properties in confined geometries". United States. doi:10.2172/1342577. https://www.osti.gov/servlets/purl/1342577.
@article{osti_1342577,
title = {Preparation of nanocrystals and nanocomposites of nanocrystal-conjugated polymer, and their photophysical properties in confined geometries},
author = {Xu, Jun},
abstractNote = {Semiconductors nanocrystals (NCs), also called quantum dots (QDs), have attracted tremendous interest over the past decade in the fields of physics, chemistry, and engineering. Due to the quantum-confined nature of QDs, the variation of particle size provides continuous and predictable changes in fluorescence emission. On the other hand, conjugated polymers (CPs) have been extensively studied for two decades due to their semiconductor-like optical and electronic properties. The electron and energy transfer between NCs and CPs occur in solar cells and light emitting diodes (LEDs), respectively. Placing CPs in direct contact with a NC (i.e., preparing NC-CP nanocomposites) carries advantage over cases where NC aggregation dominates. Such NC-CP nanocomposites possess a well-defined interface that significantly promotes the charge or energy transfer between these two components. However, very few studies have centered on such direct integration. We prepared NCs and NC-CP nanocomposites based on heck coupling and investigated the energy and charge transfer between semiconductor NCs (i.e., CdSe QDs), CPs (i.e., poly(3-hexyl thiophene) (P3HT)) in the nanocomposites in confined geometries. Two novel strategies were used to confine NC and/or NC-CP nanocomposites: (a) directly immobilizing nanohybrids, QDs and nanorods in nanoscopic porous alumina membrane (PAM) , and (b) confining the QDs and CPs in sphere-on-flat geometry to induce self-assembly. While investigating the confinement effect, gradient concentric ring patterns of high regularity form spontaneously simply by allowing a droplet of solution containing either conjugated polymer or semiconductor nanocrystal in a consecutive stick-slip mothion in a confined geometry. Such constrained evaporation can be utilized as a simple, cheap, and robust strategy for self-assembling various materials with easily tailored optical and electronic properties into spatially ordered, two-dimensional patterns. These self-organized patterns of functional nanoscale materials over large areas offer a tremendous potential for applications in optoelectronic devices, LEDs, solar cells, and biosensors. Meanwhile, spherical nanocrystals (i.e. CdSe/ZnS core/shell QDs) were placed in a hexagonal array of highly ordered cylindrical nanopores of PAMs by a simple dip-coating method and vacuum suction process, respectively. The fluorescence of CdSe/ZnS QD was retained after being filled inside PAMs and the filling contents were obtained via transmission UV-vis measurements.},
doi = {10.2172/1342577},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Mon Jan 01 00:00:00 EST 2007},
month = {Mon Jan 01 00:00:00 EST 2007}
}

Thesis/Dissertation:
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  • The dielectric response function of electronic systems in restricted geometries is studied as well as some of the consequences, using the self-consistent field method. These consequences include: 1) existence of multiple branches of longitudinal slender acoustic plasma oscillations (SAP) in thin wires; 2) a new superconductivity mechanism in thin wires via the exchange of SAPs by the electrons forming the Cooper pairs, and 3) reduction of the static screening offered by the valence electrons in a thin semiconductor film with respect to the bulk case. The SAP modes are collective modes shown to exist only in thin wires and neithermore » in a bulk system nor in a thin film. They have linear dispersion relations with phase velocities smaller than the Fermi velocity of the system and are not Landau-damped. Numerical examples of these SAP modes in metallic and semiconductor wires are presented, showing that they sould be more easily observable in semiconductor structures. The SAP-induced mechanism of superconductivity is shown to possibly give higher critical temperature T/sub c/ than the phonon mechanism in thin wires. The author presents a semi-rigorous calculation of T/sub c/ and shows that by increasing the frequency of the SAP modes and having a small effective electron mass one would be able to increase T/sub c/. He also shows that the dielectric function of a thin semiconductor slab is wavenumber dependent even at long wavelengths and is not a constant as in the bulk case.« less
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  • A novel repair agent for resin-injection repair of advanced high temperature composites was developed and characterized. The repair agent was based on bisphenol E cyanate ester (BECy) and reinforced with alumina nanoparticles. To ensure good dispersion and compatibility with the BECy matrix in nanocomposites, the alumina nanoparticles were functionalized with silanes. The BECy nanocomposites, containing bare and functionalized alumina nanoparticles, were prepared and evaluated for their thermal, mechanical, rheological, and viscoelastic properties. The monomer of BECy has an extremely low viscosity at ambient temperature, which is good for processability. The cured BECy polymer is a highly cross-linked network with excellentmore » thermal mechanical properties, with a high glass transition temperature (T g) of 270 C and decomposition temperature above 350 C. The incorporation of alumina nanoparticles enhances the mechanical and rheological properties of the BECy nanocomposites. Additionally, the alumina nanoparticles are shown to catalyze the cure of BECy. Characterization of the nanocomposites included dynamic mechanical analysis, differential scanning calorimetry, thermogravimetric analysis, rheological and rheokinetic evaluation, and transmission electron microscopy. The experimental results show that the BECy nanocomposite is a good candidate as repair agent for resin-injection repair applications.« less
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