PubMed Health⌕ Search

Biomedical subjects

Francesco Stellacci

Publications and source records attributed to Francesco Stellacci.

10 recordsLinked to original sources
PubMed2006

From homoligand- to mixed-ligand- monolayer-protected metal nanoparticles: a scanning tunneling microscopy investigation.

The ligand shell that coats, protects, and imparts a large number of properties to gold nanoparticles is a 2-D self-assembled monolayer wrapped around a 3-D metallic core. Here we present a study of the molecular packing of ligand shells on gold nanoparticles based on the analysis of scanning tunneling microscopy (STM) images. We discuss methods for optimal nanoparticle sample preparation in relation to STM imaging conditions. We show that the packing of a self-assembled monolayer composed solely of octanethiols on gold nanoparticles depends on the particle's diameter with an average headgroup spacing of 5.4 A, which is different from that of similar monolayers formed on flat Au(111) surfaces (5.0 A). In the case of nanoparticles coated with mixtures of ligands-known to phase separate into randomly shaped and ordered domains on flat surfaces-we find that phase separation leads to the formation of concentric, ribbonlike domains of alternating composition. The spacing of these domains depends on the ligand shell composition. We find that, for a given composition, the spacing increases with diameter in a manner characterized by discontinuous transitions at "critical" particle sizes. We discuss possible interpretations for the observed trends in our data.

Journal Article↗
PubMed2005

High resolution printing of DNA feature on poly(methyl methacrylate) substrates using supramolecular nano-stamping.

In recent years, a large number of devices based on organic and biological materials have been developed. To scale-up the production of these systems to industrially acceptable standards, there is a need to develop soft-material stamping approaches with the needed resolution, complexity, and versatility. We have recently developed a DNA-based stamping method (supramolecular nano-stamping, SuNS) that has superior resolution and can print multiple molecules at the same time. A similar technique was independently developed by Crooks and co-workers. Here we show that SuNS can be used to efficiently print DNA features on a polymeric substrate (poly(methyl methacrylate), PMMA) with a 40 nm point resolution and a coverage that exceeds 100 mum2. The stamped PMMA substrate was also used as a master to print on a gold substrate. With PMMA being optically clear and electrically insulating, future applications of SuNS to print DNA micro- and nanoarrays are envisioned.

DNA, Single-Stranded↗
PubMed2005

Supramolecular nanostamping: using DNA as movable type.

Here we present a novel printing technique (that we call supramolecular nanostamping), based on the replication of single-stranded DNA features through a hybridization-contact-dehybridization cycle. On a surface containing features each made of single-stranded DNA molecules of known sequence, the complementary DNA molecules are hybridized, spontaneously assembling onto the original pattern due to sequence-specific interactions. These complementary DNA strands, on the end that is assembled far from the original surface, are 5' modified with chemical groups ("sticky ends") that can form bonds with a target surface that is brought into contact. Heating induces dehybridization between DNA strands, leaving the original pattern on the original surface and the copied pattern on the secondary substrate, and thus stamping (see Figure 1). Molecular recognition provides the unique and disruptive ability of transferring large amounts of information in a single printing cycle, that is the simultaneous stamping of spatial information (i.e., the patterns) and of chemical information (i.e., the features' DNA sequence--their chemical composition). This method combines high resolution (<40 nm) with the advantage of an exponential increase in the number of masters; in fact, any printed substrate can be reused as a master. Patterns fabricated via very different lithographic techniques can be replicated.

DNA↗
PubMed2004

Low-voltage organic transistors with an amorphous molecular gate dielectric.

Organic thin film transistors (TFTs) are of interest for a variety of large-area electronic applications, such as displays, sensors and electronic barcodes. One of the key problems with existing organic TFTs is their large operating voltage, which often exceeds 20 V. This is due to poor capacitive coupling through relatively thick gate dielectric layers: these dielectrics are usually either inorganic oxides or nitrides, or insulating polymers, and are often thicker than 100 nm to minimize gate leakage currents. Here we demonstrate a manufacturing process for TFTs with a 2.5-nm-thick molecular self-assembled monolayer (SAM) gate dielectric and a high-mobility organic semiconductor (pentacene). These TFTs operate with supply voltages of less than 2 V, yet have gate currents that are lower than those of advanced silicon field-effect transistors with SiO2 dielectrics. These results should therefore increase the prospects of using organic TFTs in low-power applications (such as portable devices). Moreover, molecular SAMs may even be of interest for advanced silicon transistors where the continued reduction in dielectric thickness leads to ever greater gate leakage and power dissipation.

Journal Article↗
PubMed2004

Morphology control in self-assembled monolayers written by dip pen nanolithography.

Here, we describe the effect of writing speed in dip pen nanolithography on the morphology (height and density) of self-assembled monolayers of alkanethiols on gold surfaces. The analysis of atomic force microscopy images of written monolayers shows that molecules assemble according to a nucleation and growth mechanism. Slow writing speeds lead to dense monolayers that can be used either to direct the self-assembly of metal nanoparticles or as masks for selective etching of conductive gold nanowires.

Alkanes↗
PubMed2004

Spontaneous assembly of subnanometre-ordered domains in the ligand shell of monolayer-protected nanoparticles.

The properties of materials can be created and improved either by confining their dimensions in the nanoscale or by controlling their nanostructure. We have combined these two concepts, and here we describe a new class of nanostructured nanosized materials that show ordered phase-separated domains at an unprecedented molecular length scale. Scanning tunnelling and transmission electron microscope images of monolayer-protected metal nanoparticles, with ligand shells composed of a mixture of molecules, show that the ligands phase-separate into ordered domains as small as 5 A. Importantly, the domain shape and dimensions can be controlled by varying the ligand composition or the metallic core size. We demonstrate that the formation of ordered domains depends on the curvature of the underlying substrate, and that novel properties result from this nanostructuring. For example, because the size of the domains is much smaller than the typical dimensions of a protein, these materials are extremely effective in avoiding non-specific adsorption of a variety of proteins.

Adsorption↗
PubMed2004

Photoswitchable flexible and shape-persistent dendrimers: comparison of the interplay between a photochromic azobenzene core and dendrimer structure.

Two analogous classes of dendrimers with a single azobenzene moiety at the core have been prepared. Flexible benzyl aryl ether dendrimers 1a-e were obtained in good yields by direct alkylation of diphenolic azobenzene 3 with benzyl aryl ether dendrons [G-n]-Br (n = 0-4). In rigid dendrimers 2a-e, the azobenzene configurational switch was linked to phenylacetylene dendrons through acetylenic linkages to maintain the shape-persistent nature of these dendrimers. A comparison of these two different classes of dendrimers with azobenzene cores reveals a difference in the properties of the photochromic moiety upon dendritic incorporation as well as a significant difference in the photomodulation of dendrimer properties. The E --> Z photoisomerization quantum yield decreased markedly with increasing generation for dendrimers 1a-e but only slightly for dendrimers 2a-e. However, increasing generation did not significantly alter thermal isomerization kinetics or activation barriers. The hydrodynamic volumes of azobenzene-containing dendrimers 2b-e were significantly modulated when the azobenzene unit is subjected to irradiation, while those of dendrimers 1b-e were only slightly affected.

Journal Article↗
PubMed2003

Ultrabright supramolecular beacons based on the self-assembly of two-photon chromophores on metal nanoparticles.

Silver nanoparticles coated with a self-assembled layer of approximately 2500 chromophoric alkylthiol ligands, that exhibit a huge per particle two-photon absorption cross section (2.7 x 10-45 cm4 s photon-1) and a high fluorescence quantum yield (0.33), are reported. Polyfunctionalized variants of these nanoparticles have been produced that show reasonable solubility in water/ethanol mixtures. By virtue of the large number of tethered chromophores, these particles act as strongly two-photon absorbing nanobeacons and may have applications in fluorescence imaging and sensing.

Absorptiometry, Photon↗