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Zeitschrift Fur Kristallographie | 2007

The Samson phase, β-Mg2Al3, revisited

M. Feuerbacher; Carsten Thomas; Julien P. A. Makongo; Stefan Hoffmann; Wilder Carrillo-Cabrera; Raul Cardoso; Yuri Grin; Guido Kreiner; Jean-Marc Joubert; Thomas Schenk; J. Gastaldi; Henri Nguyen-Thi; N. Mangelinck-Noël; B. Billia; P. Donnadieu; Aleksandra Czyrska-Filemonowicz; Anna Zielińska-Lipiec; Beata Dubiel; Thomas Weber; Philippe Schaub; Günter Krauss; Volker Gramlich; Jeppe Christensen; Sven Lidin; Daniel C. Fredrickson; Marek Mihalkovic; Wieslawa Sikora; Janusz Malinowski; Stephan Brühne; Thomas Proffen

Co-Authors: Michael Feuerbacher, Carsten Thomas, Julien P. A. Makongo, Stefan Hoffmann, Wilder Carrillo-Cabrera, Raul Cardoso, Yuri Grin, Guido Kreiner, Jean-Marc Joubert, Thomas Schenk, Joseph Gastaldi, Henri Nguyen-Thi, Nathalie Mangelinck-Noël, Bernard Billia, Patricia Donnadieu, Aleksandra Czyrska-Filemonowicz, Anna Zielinska-Lipiec, Beata Dubiel, Thomas Weber, Philippe Schaub, Günter Krauss, Volker Gramlich, Jeppe Christensen, Sven Lidin, Daniel Fredrickson, Marek Mihalkovic, Wieslawa Sikora, Janusz Malinowski, Stefan Brühne, Thomas Proffen, Wolf Assmus, Marc de Boissieu, Francoise Bley, Jean-Luis Chemin, Jürgen Schreuer Abstract. The Al−Mg phase diagram has been reinvestigated in the vicinity of the stability range of the Samson phase, β-Mg2Al3 (cF1168). For the composition Mg 38.5 Al 61.5, this cubic phase, space group Fd-3m (no 227), a = 28.242(1) Å, V = 22526(2) Å3, undergoes at 214 °C a first-order phase transition to rhombohedral β′-Mg2Al3(hR293), a = 19.968(1) Å, c = 48.9114(8) Å, V = 16889(2) Å3, (i.e. 22519 Å3 for the equivalent cubic unit cell) space group R3m (no 160), a subgroup of index four of Fd-3m. The structure of the β-phase has been redetermined at ambient temperature as well as in situ at 400 °C. It essentially agrees with Samsons model, even in most of the many partially occupied and split positions. The structure of β′-Mg2Al3is closely related to that of the β-phase. Its atomic sites can be derived from those of the β-phase by group-theoretical considerations. The main difference between the two structures is that all atomic sites are fully occupied in case of the β′-phase. The reciprocal space, Bragg as well as diffuse scattering, has been explored as function of temperature and the β- to β′-phase transition was studied in detail. The microstructures of both phases have been analyzed by electron microscopy and X-ray topography showing them highly defective. Finally, the thermal expansion coefficients and elastic parameters have been determined. Their values are somewhere in between those of Al and Mg.


Science and Technology of Advanced Materials | 2014

Focus on complex metallic phases - Preface

An Pang Tsai; Juri Grin; Marc de Boissieu

1 Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai 980-8577, Japan Max-Planck-Institut for Chemical Physics of Solids, 01187 Dresden, Germany 3 Sciences de l’Ingéniérie, des Matériaux et des Procédés, Grenoble INP, CNRS, 28402 cedex, France E-mail: aptsai@tagen.tohoku. ac.jp The discovery of quasicrystal in 1982 has facilitated a revolution in crystallography and led to a paradigm shift in our understanding of the structure of ordered solids. The importance of the discovery was demonstrated by the fact that Professor Shechtman was awarded the 2011 Nobel Prize in Chemistry. More than 30 years since the discovery, the field has stimulated an enormous scientific activity ranging from pure mathematics to practical materials. The study of quasicrystal has spread to a new field, which covers complex metallic phases and/or quasicrystal approximants. In fact, it was only very recently that a better understanding of structure of quasicrystal has been attained and some applications in the field of complex metallic alloys have been tackled. The purpose of this issue is to present the current development in the basic and application-driven research on complex metallic phases, including the quasicrystals and their approximants. The issue contains 12 papers altogether, covering the new challenge of materials design for quasicrystals in several directions, such as structural materials, catalysts, thermoelectric materials and thermal rectification, new developments for related intermetallic compounds and the latest development on physical properties and surfaces. The papers are all written by excellent scientists in the field. Some of them are review articles, which will help readers understand the background of quasicrystals and the rest are original papers, which will show the state of the art of the field. We hope this issue will be helpful for scientists who want to learn the basic of quasicrystals or who want to know the recent progress on complex metallic phases in terms of materials science. Last but not the least, we are grateful to all authors for their contribution on this issue. Finally, we would like to thank Drs T Tanaka, T Hatano and T Yoshida at the editorial office of STAM for their generous help in progressing the review process.


Structural Chemistry | 2012

Atomic structure of quasicrystals

Marc de Boissieu

The 2011 Nobel Prize in chemistry has been awarded to Dan Shechtman for his discovery of quasicrystals. The discovery has indeed been a breakthrough in crystallography and solid state physics and chemistry. After a brief introduction to the subject, we review some of the recent advances in the understanding of the atomic structure of icosahedral quasicrystals and in particular for the binary Cd–Yb type quasicrystal. Thanks to a combined analysis of periodic approximant, high quality synchrotron data, and the superspace approach, a detailed insight in the crystal chemistry of this binary quasicrystal has been achieved.


Chemical Society Reviews | 2012

Phonons, phasons and atomic dynamics in quasicrystals

Marc de Boissieu

We review some of the results obtained for the study of phason, phonon and atomic dynamics in quasicrystals. In the framework of the hydrodynamic theory long-wavelength phason modes are characteristic of quasicrystal and are diffusive modes. Quenched-in phason mode gives rise to a characteristic diffuse scattering, observed in all the ‘stable’ icosahedral quasicrystals studied so far. In the AlPdMn icosahedral phase, above T = 500 °C, equilibrium phason modes are shown to be diffusive modes in agreement with the hydrodynamic theory. The lattice dynamics has been studied by inelastic neutron or X-ray scattering. Well defined acoustic modes are only observed for wavevectors smaller than 0.3 A−1. Above this value, the mode rapidly broadens as a result of mixing with higher energy modes. We show that the results can be interpreted using the concept of pseudo-Brillouin zone boundary and can qualitatively explain the differences observed in the response function of the ZnSc 1/1 approximant and its quasicrystalline counterpart. The observations are qualitatively and quantitatively reproduced using oscillating pair potentials, which open the route for a detailed analysis of the lattice dynamics at the atomic scale. An exceptional dynamical flexibility is also evidenced in the 1/1 approximant. A brief discussion on the implication of those results on the stabilizing mechanisms of quasicrystals is given at the end of the paper.


Ferroelectrics | 2004

Ab Initio Structure Solution of Icosahedral Cd-Yb Quasicrystals by a Density Modification Method

Hiroyuki Takakura; Akiji Yamamoto; Marc de Boissieu; An Pang Tsai

The six-dimensional (6D) low density elimination method has been applied to solve an icosahedral Cd-Yb quasicrystal. It shows that i-Cd-Yb is composed of similar atomic clusters that exist in the cubic approximant crystals, but the inner most shell is highly disordered. A construction of the 6D cluster model of i-Cd-Yb is outlined.


Nature Communications | 2017

Direct measurement of individual phonon lifetimes in the clathrate compound Ba 7.81 Ge 40.67 Au 5.33

Pierre-François Lory; Stéphane Pailhès; Valentina M. Giordano; H. Euchner; Hong Duong Nguyen; Reiner Ramlau; Horst Borrmann; Marcus Schmidt; Michael Baitinger; M. Ikeda; Petr Tomeš; Marek Mihalkovic; Céline Allio; Mark R. Johnson; Helmut Schober; Y. Sidis; F. Bourdarot; Louis Pierre Regnault; Jacques Ollivier; S. Paschen; Yuri Grin; Marc de Boissieu

Engineering lattice thermal conductivity requires to control the heat carried by atomic vibration waves, the phonons. The key parameter for quantifying it is the phonon lifetime, limiting the travelling distance, whose determination is however at the limits of instrumental capabilities. Here, we show the achievement of a direct quantitative measurement of phonon lifetimes in a single crystal of the clathrate Ba7.81Ge40.67Au5.33, renowned for its puzzling ‘glass-like’ thermal conductivity. Surprisingly, thermal transport is dominated by acoustic phonons with long lifetimes, travelling over distances of 10 to 100 nm as their wave-vector goes from 0.3 to 0.1 Å−1. Considering only low-energy acoustic phonons, and their observed lifetime, leads to a calculated thermal conductivity very close to the experimental one. Our results challenge the current picture of thermal transport in clathrates, underlining the inability of state-of-the-art simulations to reproduce the experimental data, thus representing a crucial experimental input for theoretical developments.Phonon lifetime is a fundamental parameter of thermal transport however its determination is challenging. Using inelastic neutron scattering and the neutron resonant spin-echo technique, Lory et al. determine the acoustic phonon lifetime in a single crystal of clathrate Ba7.81Ge40.67Au5.33.


Archive | 1999

Experimental Determination of the Structure of Quasicrystals

M. Boudard; Marc de Boissieu

The atomic structure of the matter can be studied by means of diffraction techniques, such as electron, x-ray, and neutron diffraction (Baruchel et al. 1993, Janot 1994). Indeed, the diffraction pattern of a given system depends directly on its structure. In a very schematic way Fig.4.1 shows general results expected for a gas, liquid, amorphous solid, and crystals. Each pattern of the distribution of intensities is characteristic of the different systems, and thus information on the structure can be obtained from the analysis of these diffraction spectra. In the case of periodic crystals, the structure determination is now a routine task, even for complex structures, owing to the application of direct methods.


Journal of Physics: Condensed Matter | 2013

Short- and long-range ordering during the phase transition of the Zn6Sc 1/1 cubic approximant

T. Yamada; Holger Euchner; Cesar Pay Gómez; Hiroyuki Takakura; Ryuji Tamura; Marc de Boissieu

Using in situ x-ray scattering and synchrotron radiation, we have experimentally elucidated the mechanism of the cubic to monoclinic phase transition in the Zn6Sc 1/1 approximant to an icosahedral quasicrystal. The high-temperature cubic phase is described as a bcc packing of a large Tsai-type icosahedral cluster whose center is occupied by an orientationally disordered Zn4 tetrahedron. A clear monoclinic distortion has been found to take place within 2 K around Tc = 157 K, in excellent agreement with the observed anomalies in the electrical resistivity and heat capacity. Also, a rapid variation of the super-structure reflection intensity is observed. The low-temperature monoclinic phase, as determined by single-crystal x-ray diffraction at 40 K, has been confirmed to consist of ordered Zn4 tetrahedra, oriented in an anti-parallel way along the [[Formula: see text]] direction. Above Tc, a diffuse scattering signal is observed at the position of the super-structure reflections, which evidences that a short-range ordering of the Zn4 tetrahedra takes place. In a way similar to a second-order phase transition, the correlation length describing this short-range ordering increases rapidly when the temperature diminishes and almost diverges when the temperature is close to Tc, going from 200 Å at 220 K to reach the very large value of 1200 Å at 161 K. Finally, using single-crystal x-ray diffraction, the atomic structure of the low-temperature monoclinic super-structure (space group C2/c) could be solved. The ordering of the Zn4 tetrahedra is accompanied by a strong distortion of the surrounding shells.


IUCrJ | 2016

Atomic structure and phason modes of the Sc–Zn icosahedral quasicrystal

T. Yamada; Hiroyuki Takakura; H. Euchner; Cesar Pay Gómez; Alexei Bosak; Pierre Fertey; Marc de Boissieu

The detailed atomic structure of the binary icosahedral ScZn7.33 quasicrystal has been investigated by means of high-resolution synchrotron single-crystal X-ray diffraction and absolute scale measurements of diffuse scattering.


Zeitschrift Fur Kristallographie | 2005

Diffuse scattering and phason modes in the i-AlPdMn quasicrystalline phase

Marc de Boissieu; S. Francoual

Abstract We review results obtained in the study of the diffuse scattering in the i-AlPdMn quasicrystal. Most of the diffuse scattering is the result of long wavelength phason modes. The shape and intensity distribution of the diffuse scattering is well reproduced using the generalised elasticity theory and two phason elastic constants. The temperature dependence of the diffuse scattering indicates a softening of the phason elastic constant as the temperature is lowered. Using coherent X-rays and photo-correlation X-ray spectroscopy, it is shown that phason modes are collective diffusive modes, in agreement with the hydrodynamic theory of long wavelength fluctuations in quasicrystals.

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M. Boudard

Centre national de la recherche scientifique

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Fabio Comin

European Synchrotron Radiation Facility

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Joël Chevrier

Joseph Fourier University

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