Influence of plasmon excitations on atomic-resolution quantitative 4D scanning transmission electron microscopy.

Scanning transmission electron microscopy (STEM) allows to gain quantitative information on the atomic-scale structure and composition of materials, satisfying one of todays major needs in the development of novel nanoscale devices. The aim of this study is to quantify the impact of inelastic, i.e. plasmon excitations (PE), on the angular dependence of STEM intensities and answer the question whether these excitations are responsible for a drastic mismatch between experiments and contemporary image simulations observed at scattering angles below [Formula: see text] 40 mrad. For the two materials silicon and platinum, the angular dependencies of elastic and inelastic scattering are investigated. We utilize energy filtering in two complementary microscopes, which are representative for the systems used for quantitative STEM, to form position-averaged diffraction patterns as well as atomically resolved 4D STEM data sets for different energy ranges. The resulting five-dimensional data are used to elucidate the distinct features in real and momentum space for different energy losses. We find different angular distributions for the elastic and inelastic scattering, resulting in an increased low-angle intensity ([Formula: see text] 10-40 mrad). The ratio of inelastic/elastic scattering increases with rising sample thickness, while the general shape of the angular dependency is maintained. Moreover, the ratio increases with the distance to an atomic column in the low-angle regime. Since PE are usually neglected in image simulations, consequently the experimental intensity is underestimated at these angles, which especially affects bright field or low-angle annular dark field imaging. The high-angle regime, however, is unaffected. In addition, we find negligible impact of inelastic scattering on first-moment imaging in momentum-resolved STEM, which is important for STEM techniques to measure internal electric fields in functional nanostructures. To resolve the discrepancies between experiment and simulation, we present an adopted simulation scheme including PE. This study highlights the necessity to take into account PE to achieve quantitative agreement between simulation and experiment. Besides solving the fundamental question of missing physics in established simulations, this finally allows for the quantitative evaluation of low-angle scattering, which contains valuable information about the material investigated.

The role of surface functionalization of colloidal alumina particles on their controlled interactions with viruses.

Materials that interact in a controlled manner with viruses attract increasing interest in biotechnology, medicine, and environmental technology. Here, we show that virus-material interactions can be guided by intrinsic material surface chemistries, introduced by tailored surface functionalizations. For this purpose, colloidal alumina particles are surface functionalized with amino, carboxyl, phosphate, chloropropyl, and sulfonate groups in different surface concentrations and characterized in terms of elemental composition, electrokinetic, hydrophobic properties, and morphology. The interaction of the functionalized particles with hepatitis A virus and phages MS2 and PhiX174 is assessed by virus titer reduction after incubation with particles, activity of viruses conjugated to particles, and imaged by electron microscopy. Type and surface density of particle functional groups control the virus titer reduction between 0 and 99.999% (5 log values). For instance, high sulfonate surface concentrations (4.7 groups/nm(2)) inhibit attractive virus-material interactions and lead to complete virus recovery. Low sulfonate surface concentrations (1.2 groups/nm(2)), native alumina, and chloropropyl-functionalized particles induce strong virus-particle adsorption. The virus conformation and capsid amino acid composition further influence the virus-material interaction. Fundamental interrelations between material properties, virus properties, and the complex virus-material interaction are discussed and a versatile pool of surface functionalization strategies controlling virus-material interactions is presented.

Protein adsorption on colloidal alumina particles functionalized with amino, carboxyl, sulfonate and phosphate groups.

Colloidal oxide particles in biomedical or biotechnological applications immediately become coated with proteins of the biological medium, a process which is strongly influenced by the surface characteristics of the particles. Fundamental correlations between surface characteristics and the, so far mainly uncontrollable, protein adsorption are still not clear. In this study the surface of colloidal alumina particles (d(50)=179 ± 8 nm) was systematically adjusted with NH(2), COOH, SO(3)H and PO(3)H(2) functional groups to investigate the influence on the adsorption of the three model proteins, bovine serum albumin (BSA), lysozyme (LSZ) and trypsin (TRY). The surface functionalization is characterized and discussed in detail with regard to the morphology, isoelectric point, zeta potential, hydrophilic/hydrophobic properties, functional group density and stability. Protein-particle interaction was then assessed by evaluating the amount of protein adsorbed and the zeta potentials of protein-particle conjugates. Protein adsorption was found to be influenced by the type of functional group as well as the expected electrostatic forces under the given experimental conditions. The level of protein adsorption might, hence, be specifically controlled by the type of surface functionalization. Possible adsorption modes of BSA, LSZ and TRY on the particles are suggested by considering the spatial surface potential distribution of the proteins calculated from the protein database file. The particles presented provide an excellent prerequisite for further investigation of fundamental particle-protein interactions and the design of functionally graded materials for biomedical and biotechnological applications, e.g. as drug carriers or for protein purification.