J. Tao

Coordination-dependent surface atomic contraction in nanocrystals revealed by coherent diffraction

Surface atoms have fewer interatomic bonds than those in the bulk that they often relax and reconstruct on extended two-dimensional surfaces. Far less is known about the surface structures of nanocrystals. Here, we show that coherent diffraction patterns recorded from individual nanocrystals are very sensitive to the atomic structure of nanocrystal surfaces. Nanocrystals of Au of 3-5 nm in diameter were studied by examining diffraction intensity oscillations around the Bragg peaks. Both results obtained from modelling the experimental data and molecular dynamics simulations strongly suggest inhomogeneous relaxations, involving large out-of-plane bond length contractions for the edge atoms (approximately 0.2 A); a significant contraction (approximately 0.13 A) for {100} surface atoms; and a much smaller contraction (approximately 0.05 A) for atoms in the middle of the {111} facets. These results denote a coordination/facet dependence that markedly differentiates the structural dynamics of nanocrystals from bulk crystalline surfaces.

Lamellar phase separation and dynamic competition in La0.23Ca0.77MnO3.

We report the coexistence of lamellar charge-ordered (CO) and charge-disordered (CD) domains, and their dynamical behavior, in La0.23Ca0.77MnO3. Using high-resolution transmission electron microscopy (TEM), we show that below T(CD) approximately 170 K a CD-monoclinic phase forms within the established CO-orthorhombic matrix. The CD phase has a sheetlike morphology, perpendicular to the q vector of the CO superlattice (a axis of the Pnma structure). For temperatures between 64 and 130 K, both the TEM and resistivity experiments show a dynamic competition between the two phases: at constant T, the CD phase slowly advances over the CO one. This slow dynamics appears to be linked to the magnetic transitions occurring in this compound, suggesting important magnetoelastic effects.

Quantitative structural analysis of individual nanotubes by electron diffraction

A general method for quantitative structure analysis of individual, cylindrical, carbon nanotubes is described here. The method is based on electron diffraction of individual nanotubes and analysis using a combination of helical diffraction theory and diffraction geometry of the underlying lattice. Experimental recording of nanotube diffraction is achieved using a nanometer-sized electron beam. Procedures are developed for 1) the measurement of chiral angles in both single- and multi-wall nanotubes and 2) structure determination based on Bessel function fitting of layer line intensity oscillations. The accuracy of the method is demonstrated for the structure determination of a single- and double-wall carbon nanotubes and partial structural analysis of a multiwall carbon nanotube. The results show that the single-, double- and incommensurate multi-wall tubes are well described by the cylindrical tube model. However, a large Debye-Waller factor in the radial direction is obtained. The method developed here is general and can be applied to other cylindrical nanotubes.