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Unravelling the multilayer growth of the fullerene C60 in real time.

ABSTRACT: Molecular semiconductors are increasingly used in devices, but understanding of elementary nanoscopic processes in molecular film growth is in its infancy. Here we use real-time in situ specular and diffuse X-ray scattering in combination with kinetic Monte Carlo simulations to study C60 nucleation and multilayer growth. We determine a self-consistent set of energy parameters describing both intra- and interlayer diffusion processes in C60 growth. This approach yields an effective Ehrlich-Schwoebel barrier of EES=110?meV, diffusion barrier of ED=540?meV and binding energy of EB=130?meV. Analysing the particle-resolved dynamics, we find that the lateral diffusion is similar to colloids, but characterized by an atom-like Schwoebel barrier. Our results contribute to a fundamental understanding of molecular growth processes in a system, which forms an important intermediate case between atoms and colloids.

SUBMITTER: Bommel S

PROVIDER: S-EPMC4272254 | biostudies-literature | 2014 Nov

REPOSITORIES: biostudies-literature

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Unravelling the multilayer growth of the fullerene C60 in real time.

Bommel S S Kleppmann N N Weber C C Spranger H H Schäfer P P Novak J J Roth S V SV Schreiber F F Klapp S H L SH Kowarik S S

Nature communications 20141105

Molecular semiconductors are increasingly used in devices, but understanding of elementary nanoscopic processes in molecular film growth is in its infancy. Here we use real-time in situ specular and diffuse X-ray scattering in combination with kinetic Monte Carlo simulations to study C60 nucleation and multilayer growth. We determine a self-consistent set of energy parameters describing both intra- and interlayer diffusion processes in C60 growth. This approach yields an effective Ehrlich-Schwoe ...[more]

PMID: 25369851

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Project description:A new class of water-soluble C60 transfecting agents has been prepared using Hirsch-Bingel chemistry and assessed for their ability to act as gene-delivery vectors in vitro. In an effort to elucidate the relationship between the hydrophobicity of the fullerene core, the hydrophilicity of the water-solubilizing groups, and the overall charge state of the C60 vectors in gene delivery and expression, several different C60 derivatives were synthesized to yield either positively charged, negatively charged, or neutral chemical functionalities under physiological conditions. These fullerene derivatives were then tested for their ability to transfect cells grown in culture with DNA carrying the green fluorescent protein (GFP) reporter gene. Statistically significant expression of GFP was observed for all forms of the C60 derivatives when used as DNA vectors and compared to the ability of naked DNA alone to transfect cells. However, efficient in vitro transfection was only achieved with the two positively charged C60 derivatives, namely, an octa-amino derivatized C60 and a dodeca-amino derivatized C60 vector. All C60 vectors showed an increase in toxicity in a dose-dependent manner. Increased levels of cellular toxicity were observed for positively charged C60 vectors relative to the negatively charged and neutral vectors. Structural analyses using dynamic light scattering and optical microscopy offered further insights into possible correlations between the various derivatized C60 compounds, the C60 vector/DNA complexes, their physical attributes (aggregation, charge) and their transfection efficiencies. Recently, similar Gd@C60-based compounds have demonstrated potential as advanced contrast agents for magnetic resonance imaging (MRI). Thus, the successful demonstration of intracellular DNA uptake, intracellular transport, and gene expression from DNA using C60 vectors suggests the possibility of developing analogous Gd@C60-based vectors to serve simultaneously as both therapeutic and diagnostic agents.

Dataset Information

Unravelling the multilayer growth of the fullerene C60 in real time.

Publications

Unravelling the multilayer growth of the fullerene C60 in real time.

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