Epitaxy: Programmable Atom Equivalents

The programmability of DNA makes it an attractive structure-directing ligand for the assembly of nanoparticle (NP) superlattices in a manner that mimics many aspects of atomic crystallization. However, the synthesis of multilayer single crystals of defined size remains a challenge. Though previous studies considered lattice mismatch as the major limiting factor for multilayer assembly, thin film growth depends on many interlinked variables. Here, a more comprehensive approach is taken to study fundamental elements, such as the growth temperature and the thermodynamics of interfacial energetics, to achieve epitaxial growth of NP thin films. Both surface morphology and internal thin film structure are examined to provide an understanding of particle attachment and reorganization during growth. Under equilibrium conditions, single crystalline, multilayer thin films can be synthesized over 500 × 500 μm² areas on lithographically patterned templates, whereas deposition under kinetic conditions leads to the rapid growth of glassy films. Importantly, these superlattices follow the same patterns of crystal growth demonstrated in atomic thin film deposition, allowing these processes to be understood in the context of well-studied atomic epitaxy and enabling a nanoscale model to study fundamental crystallization processes. Through understanding the role of epitaxy as a driving force for NP assembly, we are able to realize 3D architectures of arbitrary domain geometry and size.United States. Air Force Office of Scientific Research (AFOSR FA9550-11-1-0275)United States. Air Force Office of Scientific Research (FA9550-12-1-0280)United States. Department of Defense (N00014-15-1-0043)United States. Department of Energy (Grant DE-SC0000989-0002)National Science Foundation (U.S.) (Award DMR-1121262

Structural, magnetic and superconducting properties of pulsed-laser-deposition-grown La1.85Sr0.15CuO4/La2/3Ca1/3MnO3\rm{La_{1.85}Sr_{0.15}CuO_{4}/La_{2/3}Ca_{1/3}MnO_{3}} superlattices on (001)\rm{(001)}-oriented LaSrAlO4\rm{LaSrAlO_{4}} substrates

Epitaxial La1.85Sr0.15CuO4/La2/3Ca1/3MnO3 superlattices on (001)-oriented LaSrAlO4 substrates have been grown with pulsed laser deposition technique. Their structural, magnetic and superconducting properties have been determined with in-situ reflection high energy electron diffraction, x-ray diffraction, specular neutron reflectometry, scanning transmission electron microscopy, electric transport, and magnetization measurements. We find that despite the large mismatch between the in-plane lattice parameters of LSCO and LCMO these superlattices can be grown epitaxially and with a high crystalline quality. While the first LSCO layer remains clamped to the LSAO substrate, a sizeable strain relaxation occurs already in the first LCMO layer. The following LSCO and LCMO layers adopt a nearly balanced state in which the tensile and compressive strain effects yield alternating in-plane lattice parameters with an almost constant average value. No major defects are observed in the LSCO layers, while a significant number of vertical antiphase boundaries are found in the LCMO layers. The LSCO layers remain superconducting with a relatively high superconducting onset temperature of about 36 K. The macroscopic superconducting response is also evident in the magnetization data due to a weak diamagnetic signal below 10 K for H || ab and a sizeable paramagnetic shift for H || c that can be explained in terms of a vortex-pinning-induced flux compression. The LCMO layers maintain a strongly ferromagnetic state with a Curie temperature of about 190 K and a large low-temperature saturation moment of about 3.5(1) muB. These results suggest that the LSCO/LCMO superlattices can be used to study the interaction between the antagonistic ferromagnetic and superconducting orders and, in combination with previous studies on YBCO/LCMO superlattices, may allow one to identify the relevant mechanisms.Comment: 13 pages, 11 figure

Nonlinear evolution of surface morphology in InAs/AlAs superlattices via surface diffusion

Continuum simulations of self-organized lateral compositional modulation growth in InAs/AlAs short-period superlattices on InP substrate are presented. Results of the simulations correspond quantitatively to the results of synchrotron x-ray diffraction experiments. The time evolution of the compositional modulation during epitaxial growth can be explained only including a nonlinear dependence of the elastic energy of the growing epitaxial layer on its thickness. From the fit of the experimental data to the growth simulations we have determined the parameters of this nonlinear dependence. It was found that the modulation amplitude don't depend on the values of the surface diffusion constants of particular elements.Comment: 4 pages, 3 figures, published in Phys. Rev. Lett. http://link.aps.org/abstract/PRL/v96/e13610

Contribution of Ex-Situ and In-Situ X-ray Grazing Incidence Scattering Techniques to the Understanding of Quantum Dot Self-Assembly:A Review

Quantum dots are under intense research, given their amazing properties which favor their use in electronics, optoelectronics, energy, medicine and other important applications. For many of these technological applications, quantum dots are used in their ordered self-assembled form, called superlattice. Understanding the mechanism of formation of the superlattices is crucial to designing quantum dots devices with desired properties. Here we review some of the most important findings about the formation of such superlattices that have been derived using grazing incidence scattering techniques (grazing incidence small and wide angle X-ray scattering (GISAXS/GIWAXS)). Acquisition of these structural information is essential to developing some of the most important underlying theories in the field

Influence of Annealing on the Interface Structure and Strain Relief in Si/Ge Heterostructures on (100) Si

Research work on the general problem of the nature and thermal stability of the Si/Ge semiconductor interface is reviewed. We report on our recent studies of the interface structure in [(Si)m(Ge)n]p superlattices and (Ge)n layers buried in Si as revealed by Raman scattering, extended X-ray absorption fine structure, and X-ray techniques. Strain relaxation and interdiffusion in the superlattices caused by annealing have been investigated, and it is found that considerable strain-enhanced intermixing together with partial relaxation of Ge-Ge bonds occurs even for very short anneal times at 700°C. Further annealing leads to diffusion at a much slower rate and to the eventual formation of an alloy layer. The Ge-Ge bond lengths in as-grown samples are that expected for a fully strained Ge layer. Similar studies of the (Ge)n layers reveal that two-dimensional pseudomorphic growth proceeds up to n = 5, probably mediated by a Si-Ge interface interdiffusion over one or two monolayers of approximately 20%. A n = 12 layer gave evidence of strain relaxation by the introduction of dislocations and clustering. Interdiffusion proceeds rapidly on annealing at 750°C

Resonant Elastic Soft X-Ray Scattering

Resonant (elastic) soft x-ray scattering (RSXS) offers a unique element, site, and valence specific probe to study spatial modulations of charge, spin, and orbital degrees of freedom in solids on the nanoscopic length scale. It cannot only be used to investigate single crystalline materials. This method also enables to examine electronic ordering phenomena in thin films and to zoom into electronic properties emerging at buried interfaces in artificial heterostructures. During the last 20 years, this technique, which combines x-ray scattering with x-ray absorption spectroscopy, has developed into a powerful probe to study electronic ordering phenomena in complex materials and furthermore delivers important information on the electronic structure of condensed matter. This review provides an introduction to the technique, covers the progress in experimental equipment, and gives a survey on recent RSXS studies of ordering in correlated electron systems and at interfaces