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Register a new userBulk Termination of the Quasicrystalline Five-Fold Surface of Al_{70}Pd_{21}Mn_{9}
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The structure of the Al_{70}Pd_{21}Mn_{9} surface has been investigated using high resolution scanning tunnelling microscopy (STM). From two large five-fold terraces on the surface in a short decorated Fibonacci sequence, atomically resolved surface images have been obtained. One of these terraces carries a rare local configuration in a form of a ring. The location of the corresponding sequence of terminations in the bulk model M of icosahedral i-AlPdMn based on the three-dimensional tiling T*(2F) of an F-phase has been estimated using this ring configuration and the requirement from the LEED work of Gierer et al. that the average atomic density of the terminations is 0.136 atoms per A^2. A termination contains two atomic plane layers separated by a vertical distance of 0.48 A. The position of the bulk terminations is fixed within the layers of Bergman polytopes in the model M: they are 4.08 A in the direction of the bulk from a surface of the most dense Bergman layers. From the coding windows of the top planes in terminations in M we conclude that a Penrose (P1) tiling is possible on almost all five-fold terraces. The shortest edge of the tiling P1, is either 4.8 A or 7.8 A. The experimentally derived tiling of the surface with the ring configuration has an edge-length of 8.0 +- 0.3 A and hence matches the minimal edge-length expected from the model.
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The nature of the five-fold surface of Al(70)Pd(21)Mn(9) has been investigated using scanning tunneling microscopy. From high resolution images of the terraces, a tiling of the surface has been constructed using pentagonal prototiles. This tiling matches the bulk model of Boudard et. al. (J. Phys.: Cond. Matter 4, 10149, (1992)), which allows us to elucidate the atomic nature of the surface. Furthermore, it is consistent with a Penrose tiling T^*((P1)r) obtained from the geometric model based on the three-dimensional tiling T^*(2F). The results provide direct confirmation that the five-fold surface of i-Al-Pd-Mn is a termination of the bulk structure.
Scanning tunnelling microscopy has been used to study the formation of a Bi monolayer deposited on the five-fold surface of i-Al70Pd21Mn9. Upon deposition of low sub-monolayer coverages, the nucleation of pentagonal clusters of Bi adatoms of edge length 4.9 A is observed. The clusters have a common orientation leading to a film with five-fold symmetry. By inspection of images where both the underlying surface and the Bi atoms are resolved, the pentagonal clusters are found to nucleate on pseudo-Mackay clusters truncated such that a Mn atom lies centrally in the surface plane. The density of these sites is sufficient to form a quasiperiodic framework, and subsequent adsorption of Bi atoms ultimately leads to the formation of a quasicrystalline monolayer. The initial nucleation site is different to that proposed on the basis of recent density functional theory calculations.
Control of surface functionalization of MXenes holds great potential, and in particular, may lead to tuning of magnetic and electronic order in the recently reported magnetic Cr2TiC2Tx. Here, vacuum annealing experiments of Cr2TiC2Tx are reported with in situ electron energy loss spectroscopy and novel in situ Cr K-edge extended energy loss fine structure analysis, which directly tracks the evolution of the MXene surface coordination environment. These in situ probes are accompanied by benchmarking synchrotron X-ray absorption fine structure measurements and density functional theory calculations. With the etching method used here, the MXene has an initial termination chemistry of Cr2TiC2O1.3F0.8. Annealing to 600 C results in the complete loss of -F, but -O termination is thermally stable up to (at least) 700 C. These findings demonstrate thermal control of -F termination in Cr2TiC2Tx and offer a first step towards termination engineering this MXene for magnetic applications. Moreover, this work demonstrates high energy electron spectroscopy as a powerful approach for surface characterization in 2D materials.
The interfacial behavior of quantum materials leads to emergent phenomena such as two dimensional electron gases, quantum phase transitions, and metastable functional phases. Probes for in situ and real time surface sensitive characterization are critical for active monitoring and control of epitaxial synthesis, and hence the atomic-scale engineering of heterostructures and superlattices. Termination switching, especially as an interfacial process in ternary complex oxides, has been studied using a variety of probes, often ex situ; however, direct observation of this phenomena is lacking. To address this need, we establish in situ and real time reflection high energy electron diffraction and Auger electron spectroscopy for pulsed laser deposition, which provide structural and compositional information of the surface during film deposition. Using this unique capability, we show, for the first time, the direct observation and control of surface termination in complex oxide heterostructures of SrTiO3 and SrRuO3. Density-functional-theory calculations capture the energetics and stability of the observed structures and elucidate their electronic behavior. This demonstration opens up a novel approach to monitor and control the composition of materials at the atomic scale to enable next-generation heterostructures for control over emergent phenomena, as well as electronics, photonics, and energy applications.
We present a comprehensive theoretical investigation of the electron-phonon contribution to the lifetime broadening of the surface states on Cu(111) and Ag(111), in comparison with high-resolution photoemission results. The calculations, including electron and phonon states of the bulk and the surface, resolve the relative importance of the Rayleigh mode, being dominant for the lifetime at small hole binding energies. Including the electron-electron interaction, the theoretical results are in excellent agreement with the measured binding energy and temperature dependent lifetime broadening.
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