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1.
Nat Commun ; 10(1): 987, 2019 02 25.
Artigo em Inglês | MEDLINE | ID: mdl-30804336

RESUMO

The original version of this Article contained an error in the spelling of the author Matthew Holwill, which was incorrectly given as Mathew Holwill. This has now been corrected in both the PDF and HTML versions of the Article.

2.
Nat Commun ; 10(1): 230, 2019 01 16.
Artigo em Inglês | MEDLINE | ID: mdl-30651554

RESUMO

Despite a rich choice of two-dimensional materials, which exists these days, heterostructures, both vertical (van der Waals) and in-plane, offer an unprecedented control over the properties and functionalities of the resulted structures. Thus, planar heterostructures allow p-n junctions between different two-dimensional semiconductors and graphene nanoribbons with well-defined edges; and vertical heterostructures resulted in the observation of superconductivity in purely carbon-based systems and realisation of vertical tunnelling transistors. Here we demonstrate simultaneous use of in-plane and van der Waals heterostructures to build vertical single electron tunnelling transistors. We grow graphene quantum dots inside the matrix of hexagonal boron nitride, which allows a dramatic reduction of the number of localised states along the perimeter of the quantum dots. The use of hexagonal boron nitride tunnel barriers as contacts to the graphene quantum dots make our transistors reproducible and not dependent on the localised states, opening even larger flexibility when designing future devices.

3.
Langmuir ; 34(15): 4634-4639, 2018 04 17.
Artigo em Inglês | MEDLINE | ID: mdl-29597351

RESUMO

By selective attachment of fluorescent dyes to the core-forming block, we produced patchy micelles of diblock copolymers with fluorophores localized in the micellar cores. From these patchy micelles functionalized with dyes, fluorescent supracolloidal chains in a few micrometers were polymerized by combining the patches in neighboring micelles, indicating that selective modification of the core-forming block delivered the functionality into the supracolloidal chain without altering the polymerization of patchy micelles. Thus, with the same polymerization condition, we were able to produce red-, green-, and blue-emitting supracolloidal chains by varying the fluorescent dyes attached to the core-forming block. In addition, we directly visualized individual supracolloidal chains by fluorescence confocal microscopy as well as by transmission electron microscopy.

4.
Soft Matter ; 13(38): 6756-6760, 2017 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-28937168

RESUMO

Supracolloidal chains of diblock copolymer micelles were functionalized with gold and silver nanoparticles (NPs). Both NPs were independently synthesized in situ in the core of spherical micelles which were then converted to patchy micelles. With these patchy micelles as colloidal monomers, supracolloidal chains were polymerized by combining the patches of neighboring micelles. Since all micelles contained NPs, NPs were incorporated in every repeat unit of chains. In addition, a single gold NP was synthesized in the micellar core in contrast to several silver NPs so that we differentiated the chains with Au NPs from those with Ag NPs by the number of NPs in the repeat unit as well as by plasmonic bands in UV-Vis spectra.

5.
Nanotechnology ; 28(22): 225303, 2017 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-28443831

RESUMO

We report the synthesis of arrayed nanorings with tunable physical dimensions from thin films of polystyrene-block-poly(4-vinylpyridine) (PS-P4VP) micelles. For accurate control of the inner and outer diameters of the nanorings, we added imidazolium-based ionic liquids (ILs) into the micellar solution, which were eventually incorporated into the micellar cores. We observed the structural changes of the micellar cores coated on a substrate due to the presence of ILs. The spin-coated micellar cores were treated with an acidic precursor solution and generated toroid nanostructures, of which size depended on the amount of IL loaded into the micelles. We then treated the transformed micellar films with oxygen plasma to produce arrays of various metal and oxide nanorings on a substrate. The spacings and diameters of nanorings were governed by the molecular weight of the PS-P4VP and the amount of IL used. We also demonstrated that arrayed Pt nanorings enabled the fabrication of reduced graphene oxide anti-nanoring arrays via a catalytic tailoring process.

6.
Chem Commun (Camb) ; 52(60): 9430-3, 2016 Aug 04.
Artigo em Inglês | MEDLINE | ID: mdl-27377162

RESUMO

We report controlled branching and eventual crosslinking in supracolloidal chains by introducing well-defined trifunctional patchy micelles. Uniform micelles having three patches were induced from core-crosslinked micelles of diblock copolymers. Three patches in the micelles served as functional groups for crosslinking as well as branching in supracolloidal polymerization.

7.
Nanoscale ; 8(22): 11472-9, 2016 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-27195519

RESUMO

We fabricated perovskite solar cells with enhanced device efficiency based on vertically oriented TiO2 nanostructures using a nanoporous template of block copolymers (BCPs). The dimension and shape controllability of the nanopores of the BCP template allowed for the construction of one-dimensional (1-D) TiO2 nanorods and two-dimensional (2-D) TiO2 nanowalls. The TiO2 nanorod-based perovskite solar cells showed a more efficient charge separation and a lower charge recombination, leading to better performance compared to TiO2 nanowall-based solar cells. The best solar cells employing 1-D TiO2 nanorods showed an efficiency of 15.5% with VOC = 1.02 V, JSC = 20.0 mA cm(-2) and fill factor = 76.1%. Thus, TiO2 nanostructures fabricated from BCP nanotemplates could be applied to the preparation of electron transport layers for improving the efficiency of perovskite solar cells.

8.
Nanoscale ; 8(20): 10823-31, 2016 May 19.
Artigo em Inglês | MEDLINE | ID: mdl-27168228

RESUMO

Photonic crystals can be represented by periodic nanostructures with alternating refractive indices, which create artificial stop bands with the appearance of colors. In this regard, nanodomains of block copolymers and the corresponding structural colors have been intensively studied in the past. However, the practical application of photonic crystals of block copolymers has been limited to a large degree because of the presence of large defects and grain boundaries in the nanodomains of block copolymers. The present study focuses on the alternative opportunity of short-range ordered nanodomains of block copolymers for fluorescence enhancement, which also has a direct relevance to the development of fluorescence sensors or detectors. The enhancement mechanism was found to be interconnected with the excitation process rather than the alternation of the decay kinetics. In particular, we demonstrate that randomly oriented, but regular grains of lamellae of polystyrene-block-polyisoprene, PS-b-PI, diblock copolymers and their blend with PS homopolymers can behave as Bragg mirrors to induce multiple reflections of the excitation source inside the photonic structures. This process in turn significantly increases the effective absorption of the given fluorophores inside the polymeric photonic structures to amplify the fluorescence signal.

9.
Chem Commun (Camb) ; 52(38): 6475-8, 2016 May 11.
Artigo em Inglês | MEDLINE | ID: mdl-27101089

RESUMO

We demonstrate the fabrication of fluorescent supracolloidal chains functionalized with quantum dots, which were polymerized from patched micelles of diblock copolymers by adjusting the polarity of the solvent. Supracolloidal random and block chains with green- and red-emitting quantum dots were also synthesized.

10.
Nanotechnology ; 26(16): 165302, 2015 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-25824622

RESUMO

Superhydrophobic surfaces are normally fixed on the chosen materials. Here, we report transferrable superhydrophobicity which was enabled by fabricating TiO2 nanorods on a reduced graphene oxide (rGO) film. Superhydrophobic TiO2 nanorods were first synthesized from a nanoporous template of block copolymers (BCPs). The controllability over the dimension and shape of nanopores of the BCP template allowed for the adjustment of TiO2 nanostructures for superhydrophobicity. Since the rGO film provided effective transferring, TiO2 nanorods were conveyed onto a flexible polymer film and a metal substrate. Thus, the surface of the designated substrate was successfully changed to a superhydrophobic surface without alteration of its inherent characteristics.

11.
Macromol Rapid Commun ; 36(11): 1026-46, 2015 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-25761127

RESUMO

Hybrid materials composed of colloidal semiconductor quantum dots and π-conjugated organic molecules and polymers have attracted continuous interest in recent years, because they may find applications in bio-sensing, photodetection, and photovoltaics. Fundamental processes occurring in these nanohybrids are light absorption and emission as well as energy and/or charge transfer between the components. For future applications it is mandatory to understand, control, and optimize the wide parameter space with respect to chemical assembly and the desired photophysical properties. Accordingly, different approaches to tackle this issue are described here. Simple organic dye molecules (Dye)/quantum dot (QD) conjugates are studied with stationary and time-resolved spectroscopy to address the dynamics of energy and ultra-fast charge transfer. Micellar as well as lamellar nanostructures derived from diblock copolymers are employed to fine-tune the energy transfer efficiency of QD donor/dye acceptor couples. Finally, the transport of charges through organic components coupled to the quantum dot surface is discussed with an emphasis on functional devices.


Assuntos
Nanoestruturas/química , Semicondutores , Corantes/química , Transporte de Elétrons , Transferência de Energia , Nanopartículas/química , Nanofios/química , Polímeros/química , Pontos Quânticos/química
12.
Chem Commun (Camb) ; 51(16): 3324-7, 2015 Feb 25.
Artigo em Inglês | MEDLINE | ID: mdl-25536364

RESUMO

Directional attraction with lateral repulsion between colloidal nanoparticles can create their supracolloidal chains. Here, we demonstrate supracolloidal polymers of diblock copolymer micelles, which were polymerized by adjusting the polarity of the solvent. We also synthesized supracolloidal random and block copolymer chains.

13.
Nanotechnology ; 25(45): 455602, 2014 Nov 14.
Artigo em Inglês | MEDLINE | ID: mdl-25333410

RESUMO

We fabricated a single-layered film consisting of spherical micelles of diblock copolymers and one-dimensional Au nanorods that were surface modified with the same polymer as the corona block of the copolymers. When the diameters of micelles were larger than the lengths of the nanorods, spherical micelles arranged in a hexagonal configuration surrounded by nanorods with their long axes perpendicular to the radial direction of the micelles. This arrangement provided selective organization of the Au nanorods and Ag nanoparticles which were selectively synthesized within the cores of the copolymer micelles. Thus, position-selective arrangement of Au nanorods and Ag nanoparticles was demonstrated at the nanometer scale such that a homogenous distribution of two different nanomaterials over a large area without aggregation was achieved.

14.
Nanotechnology ; 25(13): 135609, 2014 Apr 04.
Artigo em Inglês | MEDLINE | ID: mdl-24598198

RESUMO

We report the density- and size-controlled growth of zinc oxide (ZnO) nanorod arrays on arbitrary substrates using reduced graphene oxide (rGO) nanodot arrays. For the controlled growth of the ZnO nanorod arrays, rGO nanodot arrays with tunable density and size were designed using a monolayer of diblock copolymer micelles and oxygen plasma etching. While the diameter and number density of the ZnO nanorods were readily determined by those of the rGO nanodots, the length of the ZnO nanorods was easily controlled by changing the growth time. x-ray diffraction and electron microscopy confirmed that the vertically well-aligned ZnO nanorod arrays were heteroepitaxially grown on the rGO nanodots. Strong, sharp near-band-edge emission peaks with no carbon-related peak were observed in the photoluminescence spectra, implying that the ZnO nanostructures grown on the rGO nanodots were of high optical quality and without carbon contamination. Our approach provides a general and rational route for heteroepitaxial growth of high-quality inorganic materials with tunable number density, size, and spatial arrangement on arbitrary substrates using rGO nanodot arrays.

15.
Micron ; 46: 35-42, 2013 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-23313130

RESUMO

Three-dimensional nanostructures of TiO2 related materials including nanotubes, electron acceptor materials in hybrid polymer solar cells, and working electrodes of dye sensitized solar cells (DSSCs) were visualized by electron tomography as well as TEM micrographs. The regions on the wall of TiO2 nanotubes where the streptavidins were attached were elucidated by electron tomogram analysis. The coverage of TiO2 nanotubes by streptavidin was also investigated. The TiO2 nanostructures in hybrid polymer solar cells made by sol-gel and atomic layer deposition (ALD) methods and the morphologies of pores between TiO2 particles in DSSCs were also observed by reconstructed three-dimensional images made by electron tomography.

16.
ACS Nano ; 6(6): 5051-9, 2012 Jun 26.
Artigo em Inglês | MEDLINE | ID: mdl-22621410

RESUMO

Recently, it has been noticed that surface plasmon resonance of metal nanoparticles can alter the intrinsic properties of nearby fluorophores. Field enhancement and radiative decay engineering are major principles for understanding a number of experimental observations such as enhanced and quenched emission of fluorophores in the vicinity of metal nanoparticles. At the same time, there are apparent similarities between surface-plasmon-coupled fluorescence and fluorescence resonance energy transfer (FRET), as both are near-field through-space interactions. From this perspective, we hypothesize that donor-acceptor interaction in the FRET can be altered by metal nanoparticles. Our approach is based on diblock copolymer micelles, which have been widely applied for nanoscale arrangement of functionalities. By applying self-assembling techniques of copolymer micelles to organize the spatial location of semiconductor quantum dots, fluorescent dyes, and metal nanoparticles, the FRET in hybrid assemblies can be switched off by plasmonic effects.


Assuntos
Transferência Ressonante de Energia de Fluorescência/métodos , Corantes Fluorescentes/química , Nanopartículas/química , Polímeros/química , Pontos Quânticos , Ressonância de Plasmônio de Superfície/métodos , Micelas
17.
Nanotechnology ; 23(12): 125301, 2012 Mar 30.
Artigo em Inglês | MEDLINE | ID: mdl-22398242

RESUMO

Nanostructured graphenes such as nanoribbons, nanomeshes, and nanodots have attracted a great deal of attention in relation to graphene-based semiconductor devices. The block copolymer micellar approach is a promising bottom-up technique for generating large area nanostructures of various materials without using sophisticated electron-beam lithography. Here we demonstrate the fabrication of an array of graphene nanodots with tunable size and inter-distance with the utilization of a monolayer of diblock copolymer micelles. Au nanoparticles were synthesized in the micellar cores and effectively worked as shielding nanostructures in generating graphene nanodots by oxygen plasma etching. We also controlled the radius and inter-distance of graphene nanodots simply through the molecular weight of the copolymers.

18.
Langmuir ; 27(19): 12191-6, 2011 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-21875133

RESUMO

We report the formation of ordered complex nanostructures from single-layered films of mixtures of polystyrene-poly(2-vinylpyridine) (PS-P2VP) and polystyrene-poly(4-vinylpyridine) (PS-P4VP) diblock copolymer micelles by THF (tetrahydrofuran) annealing. We first examined the influence of THF vapor on PS-P2VP and PS-P4VP micelles in their single-layered films. Due to the different solubility of PS-P2VP and PS-P4VP copolymers in THF, a hexagonal array of PS-P2VP micelles was changed into cylindrical nanodomains, but that of PS-P4VP micelles was not changed. The different influence of THF on PS-P2VP and PS-P4VP micelles was combined in single-layered films of mixtures of both micelles. For the purpose, we prepared mixture solutions of independently prepared small PS-P2VP and large PS-P4VP micelles. Then, bimodal self-assemblies of micelles were prepared from the mixtures, for which the hexagonal array of large PS-P4VP micelles was surrounded by small PS-P2VP micelles. When the bimodal self-assembly was annealed by THF vapor, PS-P2VP micelles were transformed into cylindrical nanodomains, but their reorganization was guided by hexagonally arranged PS-P4VP micelles. As a result, we were able to produce ordered complex nanostructures in the form of a hexagonal array of PS-P4VP micelles surrounded by PS-P2VP cylinders, which was further utilized for the synthesis of Au nanoparticles.


Assuntos
Furanos/química , Nanoestruturas/química , Poliestirenos/química , Polivinil/química , Piridinas/química , Membranas Artificiais , Micelas , Tamanho da Partícula , Solubilidade , Solventes/química , Propriedades de Superfície
20.
J Nanosci Nanotechnol ; 10(10): 6819-24, 2010 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-21137804

RESUMO

We controlled the fluorescence resonance energy transfer (FRET) between ZnO nanoparticles and rhodamine B (RB) within multilayered thin films prepared by the layer-by-layer (LbL) assembling method. Positively charged ZnO nanoparticles and RB-labeled poly(allyamine hydrochloride) (RB-PAH) were accurately incorporated into LbL assemblies of polyelectrolytes. The distance between ZnO nanoparticles and RB-PAH was adjusted by varying the number of layers of pure polyelectrolytes, leading to the controlled FRET from ZnO nanoparticles to RB-PAH.

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