Irreversible nucleation in molecular beam epitaxy: From theory to experiments

Recently, the nucleation rate on top of a terrace during the irreversible growth of a crystal surface by MBE has been determined exactly. In this paper we go beyond the standard model usually employed to study the nucleation process, and we analyze the qualitative and quantitative consequences of two important additional physical ingredients: the nonuniformity of the Ehrlich-Schwoebel barrier at the step-edge, because of the existence of kinks, and the steering effects, due to the interaction between the atoms of the flux and the substrate. We apply our results to typical experiments of second layer nucleation.Comment: 11 pages. Table I corrected and one appendix added. To be published in Phys. Rev. B (scheduled issue: 15 February 2003

Spatio-temporal distribution of nucleation events during crystal growth

We consider irreversible second-layer nucleation that occurs when two adatoms on a terrace meet. We solve the problem analytically in one dimension for zero and infinite step-edge barriers, and numerically for any value of the barriers in one and two dimensions. For large barriers, the spatial distribution of nucleation events strongly differs from $\rho^2$, where $\rho$ is the stationary adatom density in the presence of a constant flux. The probability $Q(t)$ that nucleation occurs at time $t$ after the deposition of the second adatom, decays for short time as a power law [$Q(t)\sim t^{-1/2}$] in $d=1$ and logarithmically [$Q(t)\sim 1/\ln(t/t_0)$] in $d=2$; for long time it decays exponentially. Theories of the nucleation rate $\omega$ based on the assumption that it is proportional to $\rho^2$ are shown to overestimate $\omega$ by a factor proportional to the number of times an adatom diffusing on the terrace visits an already visited lattice site.Comment: 4 pages, 3 figures; accepted for publication on PR

Island nucleation in the presence of step edge barriers: Theory and applications

We develop a theory of nucleation on top of two-dimensional islands bordered by steps with an additional energy barrier $\Delta E_S$ for descending atoms. The theory is based on the concept of the residence time of an adatom on the island,and yields an expression for the nucleation rate which becomes exact in the limit of strong step edge barriers. This expression differs qualitatively and quantitatively from that obtained using the conventional rate equation approach to nucleation [J. Tersoff et al., Phys. Rev. Lett.72, 266 (1994)]. We argue that rate equation theory fails because nucleation is dominated by the rare instances when two atoms are present on the island simultaneously. The theory is applied to two distinct problems: The onset of second layer nucleation in submonolayer growth, and the distribution of the sizes of top terraces of multilayer mounds under conditions of strong step edge barriers. Application to homoepitaxial growth on Pt(111) yields the estimate $\Delta E_S \geq 0.33$ eV for the additional energy barrier at CO-decorated steps.Comment: 13 pages, 3 figure

Simulations of energetic beam deposition: from picoseconds to seconds

We present a new method for simulating crystal growth by energetic beam deposition. The method combines a Kinetic Monte-Carlo simulation for the thermal surface diffusion with a small scale molecular dynamics simulation of every single deposition event. We have implemented the method using the effective medium theory as a model potential for the atomic interactions, and present simulations for Ag/Ag(111) and Pt/Pt(111) for incoming energies up to 35 eV. The method is capable of following the growth of several monolayers at realistic growth rates of 1 monolayer per second, correctly accounting for both energy-induced atomic mobility and thermal surface diffusion. We find that the energy influences island and step densities and can induce layer-by-layer growth. We find an optimal energy for layer-by-layer growth (25 eV for Ag), which correlates with where the net impact-induced downward interlayer transport is at a maximum. A high step density is needed for energy induced layer-by-layer growth, hence the effect dies away at increased temperatures, where thermal surface diffusion reduces the step density. As part of the development of the method, we present molecular dynamics simulations of single atom-surface collisions on flat parts of the surface and near straight steps, we identify microscopic mechanisms by which the energy influences the growth, and we discuss the nature of the energy-induced atomic mobility

The process of irreversible nucleation in multilayer growth. I. Failure of the mean-field approach

The formation of stable dimers on top of terraces during epitaxial growth is investigated in detail. In this paper we focus on mean-field theory, the standard approach to study nucleation. Such theory is shown to be unsuitable for the present problem, because it is equivalent to considering adatoms as independent diffusing particles. This leads to an overestimate of the correct nucleation rate by a factor N, which has a direct physical meaning: in average, a visited lattice site is visited N times by a diffusing adatom. The dependence of N on the size of the terrace and on the strength of step-edge barriers is derived from well known results for random walks. The spatial distribution of nucleation events is shown to be different from the mean-field prediction, for the same physical reason. In the following paper we develop an exact treatment of the problem.Comment: 19 pages, 3 figures. To appear in Phys. Rev.

Primary Human Hepatocytes Repopulate Livers of Mice After In Vitro Culturing and Lentiviral-Mediated Gene Transfer

Cell-based therapies represent a promising alternative to orthotopic liver transplantation. However, therapeutic effects are limited by low cell engraftment rates. We recently introduced a technique creating human hepatocyte spheroids for potential therapeutic application. The aim of this study was to evaluate whether these spheroids are suitable for engraftment in diseased liver tissues. Intrasplenic spheroid transplantation into immunodeficient uPA/SCID/beige mice was performed. Hepatocyte transduction ability prior to transplantation was tested by lentiviral labeling using red-green-blue (RGB) marking. Eight weeks after transplantation, animals were sacrificed and livers were analyzed by immunohistochemistry and immunofluorescence. To investigate human hepatocyte-specific gene expression profiles in mice, quantitative real-time-PCR was applied. Human albumin and alpha-1-antitrypsin concentrations in mouse serum were quantified to assess the levels of human chimerism. Precultured human hepatocytes reestablished their physiological liver tissue architecture and function upon transplantation in mice. Positive immunohistochemical labeling of the proliferating cell nuclear antigen revealed that human hepatocytes retained their in vivo proliferation capacity. Expression profiles of human genes analyzed in chimeric mouse livers resembled levels determined in native human tissue. Extensive vascularization of human cell clusters was detected by demonstration of von Willebrand factor activity. To model gene therapy approaches, lentiviral transduction was performed ex vivo and fluorescent microscopic imaging revealed maintenance of RGB marking in vivo. Altogether, this is the first report demonstrating that cultured and retroviral transduced human hepatocyte spheroids are able to engraft and maintain their regenerative potential in vivo

Inorganic carbon promotes photosynthesis, growth, and maximum biomass of phytoplankton in eutrophic water bodies

1.The traditional perception in limnology has been that phytoplankton biomass in lakes is limited by phosphorus, nitrogen, and light, but not by dissolved inorganic carbon (DIC) because CO2 can be supplied from the atmosphere. We tested the possibility of carbon limitation of photosynthesis, growth, and biomass accumulation of phytoplankton communities across an alkalinity and DIC gradient (0.15–3.26 mM) in nutrient‐rich freshwater. 2.During 47‐day long experiments, we measured phytoplankton biomass, organic carbon, calcium, DIC, pH, and oxygen in indoor, constantly mixed mesocosms with either no removal or a 70% weekly removal of the biomass. Photosynthesis was measured in the morning and in the afternoon at high biomass. 3.Maximum biomass and organic carbon production increased two‐ to four‐fold with DIC, which supported 7% of organic carbon production at low DIC and 53% at high DIC concentration, while atmospheric CO2 uptake supplied the remainder. Weekly biomass removal increased growth rates through improved light conditions leading to enhanced total phytoplankton biomass production at high DIC. Photosynthesis was significantly higher in the morning compared to afternoon due to daily DIC depletion. 4.We conclude that phytoplankton photosynthesis, growth rate, maximum biomass, and organic carbon production can be markedly carbon limited in eutrophic lake waters. Consequently, lakes of high DIC and pH can support a faster primary production by greater DIC use and chemically enhanced atmospheric CO2 uptake.publishedVersio