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Register a new userEffective chemical potential for non-equilibrium systems and its application to molecular beam epitaxy of Bi2Se3
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First-principles studies often rely on the assumption of equilibrium, which can be a poor approximation, e.g., for growth. Here, an effective chemical potential method for non-equilibrium systems is developed. A salient feature of the theory is that it maintains the equilibrium limits as the correct limit. In application to molecular beam epitaxy, rate equations are solved for the concentrations of small clusters, which serve as feedstock for growth. We find that the effective chemical potential is determined by the most probable, rather than by the lowest-energy, cluster. In the case of Bi2Se3, the chemical potential is found to be highly supersaturated, leading to a high nucleus concentration in agreement with experiment.
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SrxBi2Se3 is a candidate topological superconductor but its superconductivity requires the intercalation of Sr by into the van-der-Waals gaps of Bi2Se3. We report the synthesis of SrxBi2Se3 thin films by molecular beam epitaxy, and we characterize their structural, vibrational and electrical properties. X-ray diffraction and Raman spectroscopy show evidence of substitutional Sr alloying into the structure, while transport measurements allow us to correlate the increasing Sr content with an increased n-type doping, but do not reveal superconductivity down to 1.5K. Our results suggest that Sr predominantly occupies sites within a quintuple layer, simultaneously substituting for Bi and as an interstitial. Our results motivate future density functional studies to further investigate the energetics of Sr substitution into Bi2Se3.
Layered van der Waals (vdW) materials grown by physical vapor deposition techniques are generally assumed to have a weak interaction with the substrate during growth. This leads to films with relatively small domains that are usually triangular and a terraced morphology. In this paper, we demonstrate that Bi2Se3, a prototypical vdW material, will form a nano-column morphology when grown on GaAs(001) substrates. This morphology is explained by a relatively strong film/substrate interaction, long adatom diffusion lengths, and a high reactive selenium flux. This discovery paves the way toward growth of self-assembled vdW structures even in the absence of strain.
We report the growth of self-assembled Bi2Se3 quantum dots (QDs) by molecular beam epitaxy on GaAs substrates using the droplet epitaxy technique. The QD formation occurs after anneal of Bismuth droplets under Selenium flux. Characterization by atomic force microscopy, scanning electron microscopy, X-ray diffraction, high-resolution transmission electron microscopy and X-ray reflectance spectroscopy is presented. The quantum dots are crystalline, with hexagonal shape, and have average dimensions of 12 nm height (12 quintuple layers) and 46 nm width, and a density of $8.5 cdot 10^9 cm^{-2}$. This droplet growth technique provides a means to produce topological insulator QDs in a reproducible and controllable way, providing convenient access to a promising quantum material with singular spin properties.
High-index Bi2Se3(221) film has been grown on In2Se3-buffered GaAs(001), in which a much retarded strain relaxation dynamics is recorded. The slow strain-relaxation process of in epitaxial Bi2Se3(221) can be attributed to the layered structure of Bi2Se3 crystal, where the epifilm grown along [221] is like a pile of weakly-coupled quintuple layer slabs stacked side-by-side on substrate. Finally, we have revealed the strong chemical bonding at the interface of Bi2Se3 and In2Se3 by plotting differential charge contour calculated by first-principle method. This study points to the feasibility of achieving strained TIs for manipulating the properties of topological systems.
Epitaxial layers of the topological insulator Bi2Se3 have been grown by molecular beam epitaxy on laterally lattice-matched InP(111)B substrates. High resolution X-ray diffraction shows a significant improvement of Bi2Se3 crystal quality compared to layers deposited on other substrates. The measured full width at half maximum of the rocking curve is Delta omega=13 arcsec, and the (omega-2theta) scans exhibit clear layer thickness fringes. Atomic force microscope images show triangular twin domains with sizes increasing with layer thickness. The structural quality of the domains is confirmed on the microscopic level by transmission electron microscopy.
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