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1. Phase transitions within crystals that are aperiodic by construction

Author

Céline Mariette, Philippe Rabiller, Laurent Guérin, Claude Ecolivet, Ilya Frantsuzov, Bo Wang, Shane M. Nichols, Philippe Bourges, Alexei Bosak, Yu-Sheng Chen, Mark D. Hollingsworth, Bertrand Toudic, Institut de Physique de Rennes (IPR), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), European Synchroton Radiation Facility [Grenoble] (ESRF), Kansas State University, LLB - Nouvelles frontières dans les matériaux quantiques (NFMQ), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), University of Chicago, ChemMatCARS beamline, ANR-SIMI4-ODACE-2011, and ANR-11-BS04-0004,ODACE,Ordre et désordre dans les édifices cristallins apériodiques.(2011)

Subjects
[PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci]
Abstract

International audience; Aperiodic crystals possess long-range order without translational symmetry. They constitute a state of matter that has forced a profound paradigm shift in solid-state physics. A common feature of aperiodic crystals is that they recover periodicity in higher dimensional spaces, the so-called crystallographic superspaces. Much work has been dedicated to the structural order within these superspaces and also to their specific dynamics. This paper focuses on the phase transitions within crystallographic superspaces. Aperiodic crystals are divided into three families: incommensurately modulated crystals, composite crystals, and quasicrystals. Incommensurately modulated crystals have been studied heavily and appear now to be relatively well understood, since they possess a periodic high-symmetry phase. The other two members of the family are aperiodic by construction. In this paper, we present a comprehensive and systematic study of a prototype composite host-guest family of n-alkane/urea inclusion compounds [$n−$ C$_n$H$_{2n+2}$/CO(NH$_2$)$_2$]. For these materials, which exhibit a rich sequence of phases, the phase transitions are described in terms of group/subgroup symmetry breaking within crystallographic superspaces. Such phase transitions may decrease, increase, or maintain the dimension of the crystallographic superspace. These results highlight the multiplicity of specific structural solutions thataperiodicity offers.

Published
2022
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4. Dynamical limits by downsizing for the photo-induced switching in a molecular material revealed by time-resolved X-ray diffraction

Author

Yang F, Jacek Kubicki, Cristian Enachescu, A. Volte, Céline Mariette, Elzbieta Trzop, Matteo Levantino, Eric Collet, Marie-Laure Boillot, Marco Cammarata, Maciej Lorenc, Hervé Cailleau, Corraze B, Roman Bertoni, X. Dong, Michael Wulff, Laurentiu Stoleriu, Institut de Physique de Rennes (IPR), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Université de Rennes 1 (UR1), and Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], Materials science, X-ray crystallography, Molecular materials, Molecular physics
Abstract

Cooperative molecular switching at the solid state is exemplified by spin crossover phenomenon in crystals of transition metal complexes. Time-resolved studies with temporal resolutions that separate molecular level dynamics from macroscopic changes, afford clear distinction between the time scales of the different degrees of freedom involved. In this work we use 100 ps X-ray diffraction to follow simultaneously the molecular spin state and the structure of the lattice during the photoinduced low spin to high spin transition in microcrystals of [FeIII(3-MeO-SalEen)2]PF6. We show the existence of a delay between the crystalline volume increase driven by the propagation of collective volumic strain waves, and the cooperative macroscopic switching of molecular state. Such behaviour is different from the expectation that phase transformation only requires atomic displacements in the unit cell, that can occur simultaneously with propagation of a volumic strain. Model simulations and discussions of the physical picture explain the phenomenon with thermally activated kinetics governed by local energy barriers separating the molecular states.

Published
2021

5. Out-of-equilibrium lattice response to photo-induced charge-transfer in a MnFe Prussian blue analogue

Author

Elzbieta Trzop, Matteo Levantino, Kenta Imoto, Marco Cammarata, Claude Ecolivet, Marie Yoshikiyo, Céline Mariette, Eric Collet, Hiroko Tokoro, Giovanni Azzolina, Shin-ichi Ohkoshi, Roman Bertoni, Mathias Sander, Institut de Physique de Rennes (IPR), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), European Synchrotron Radiation Facility (ESRF), Université de Tsukuba = University of Tsukuba, The University of Tokyo (UTokyo), JSPS Ministry of Education, Culture, Sports, Science and Technology, Japan (MEXT) Japan Society for the Promotion of Science [20H00369], JSPS KAKENHI Ministry of Education, Culture, Sports, Science and Technology, Japan (MEXT) Japan Society for the Promotion of Science Grants-in-Aid for Scientific Research (KAKENHI) [16H06521], Agence Nationale de la Recherche French National Research Agency (ANR) European Commission [ANR-19-CE30-0004, ANR-19-CE07-0027, ANR-19-CE29-0018], University Rennes 1, Fondation Rennes 1, ANR-19-CE30-0004,ELECTROPHONE,Transitions de phase ELECTROnique de matériaux moleculaires controllées par PHONONIQUE non-linéaire(2019), ANR-19-CE07-0027,SMAC,Composés avancés multifonctionnels commutables(2019), ANR-19-CE29-0018,multicross,Trajectoires multiples vers les états excités(2019), and Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], Prussian blue, education.field_of_study, Phase transition, Materials science, Condensed matter physics, Population, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Antibonding molecular orbital, 01 natural sciences, Thermal expansion, 0104 chemical sciences, chemistry.chemical_compound, Lattice (module), chemistry, Excited state, Lattice plane, Materials Chemistry, 0210 nano-technology, education
Abstract

International audience; Photo-induced structural dynamics in molecular materials often involve two main components; local molecular distortions induced by the self-trapping of electronic excited state and incoherent lattice dynamics due to energy dissipation. The latter component frequently hinders clear manifestation at macroscopic scale of local self-trapped entities and their coupling to the lattice. The studied photoactive MnFe Prussian blue analogue exhibits no thermal expansion, which allows observing long-range lattice dynamics induced by the structural trapping of photo-induced charge-transfer (CT) states. The self-trapping of the photo-induced (MnFeII)-Fe-III -> (MnFeIII)-Fe-II is responsible for the emergence of various physical properties. At equilibrium, the lattice volume expansion and the ferroelastic Jahn-Teller distortion associated with the charge-transfer-based phase transition, evolve in a coupled way. Here, we use time resolved X-ray diffraction to investigate the anisotropic out-of-equilibrium lattice dynamics triggered by the self-trapping of photo-induced (MnFeII)-Fe-III -> (MnFeIII)-Fe-II CT. The observed dynamics evidence a decoupling of both types of lattice deformations in the time domain, with an impulsive lattice response driven by the local Jahn-Teller reorganization and a displacive volume expansion controlled by the long-lived photo-induced CT small-polarons, due to the population of antibonding orbitals centered on Mn-N bonds in the (a,b) lattice plane.

Published
2021
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6. Single Laser Shot Photoinduced Phase Transition of Rubidium Manganese Hexacyanoferrate Investigated by X‐ray Diffraction

Author

Giovanni Azzolina, Eric Collet, Céline Mariette, Marco Cammarata, Elzbieta Trzop, Mathias Sander, Matteo Levantino, Kosuke Nakagawa, Hiroko Tokoro, Shin‐ichi Ohkoshi, Roman Bertoni, Institut de Physique de Rennes (IPR), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), European Synchrotron Radiation Facility (ESRF), Department of Chemistry, The University of Tokyo (UTokyo), Division of Materials Science [Tsukuba], Université de Tsukuba = University of Tsukuba, LIA IM-LED, Conseil National de la Recherche Scientifique, 15H05697, Japan Society for the Promotion of Science, ANR-16-CE30-0018, ANR, Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), and ANR-16-CE30-0018,ELASTICA,Cooperativité Elastique Photo-Induite dans des Matériaux Bistables avec Changement de Volume(2016)

Subjects
[PHYS]Physics [physics], Thermal equilibrium, Diffraction, Phase transition, 010405 organic chemistry, Analytical chemistry, chemistry.chemical_element, Atmospheric temperature range, 010402 general chemistry, 01 natural sciences, 0104 chemical sciences, Rubidium, Inorganic Chemistry, Tetragonal crystal system, chemistry, Phase (matter), X-ray crystallography, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], [CHIM.CRIS]Chemical Sciences/Cristallography, [CHIM.COOR]Chemical Sciences/Coordination chemistry, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat]
Abstract

International audience; We study by X-ray diffraction the phase transition of microcrystals of rubidium manganese hexacyanoferrate, for which combined electron transfer and structural reorganization are responsible for a change of magnetic properties. The Rb0.94Mn[Fe(CN)6]0.98•2.5H2O system undergoes a phase transition between the tetragonal phase Fe II (S=0)-CN-Mn III (S=2) and the cubic Fe III (S=1/2)-CN-Mn II (S=5/2) phases. The thermal equilibrium phase transition shows a broad regime of bistability, responsible for the appearance of a thermal hysteresis in the  185-300 K temperature range. We used a deposited film to study by X-ray diffraction the switching from the tetragonal phase to the cubic phase, induced inside the thermal hysteresis by a single laser shot of tunable power. Compared to previous measurements using local probes, our results show that the ns laser pulse induces a stable long-range ordered cubic phase when conversion is partial or complete.

Published
2019
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7. Strain wave pathway to semiconductor-to-metal transition revealed by time-resolved X-ray powder diffraction

Author

Simon Ebner, Majed Chergui, Hervé Cailleau, Paul Beaud, Henrik T. Lemke, Eric Collet, Gerhard Ingold, Alexei Bosak, Andrej Babic, Dmitry Ozerov, S. Vetter, Laurent Cario, Roman Bertoni, Laurent Guérin, Pavle Juranić, Michael Wulff, Giulia F. Mancini, Vincent Esposito, T. Zmofing, Alexander Roland Oggenfuss, Aldo Mozzanica, Shin-ichi Ohkoshi, Yunpei Deng, Maciej Lorenc, Ivan Usov, Serhane Zerdane, Matteo Levantino, Akos Schreiber, Marco Cammarata, Roman Mankowsky, Elzbieta Trzop, Rolf Follath, P. Böhler, Céline Mariette, S. Redford, C. Svetina, Olivier Hernandez, Leonardo Sala, A. Volte, X. Dong, L. Patthey, Hiroko Tokoro, V. Ta Phuoc, B. Lépine, A. Keller, Etienne Janod, Institut de Physique de Rennes (IPR), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Institut des Matériaux Jean Rouxel (IMN), Université de Nantes - UFR des Sciences et des Techniques (UN UFR ST), Université de Nantes (UN)-Université de Nantes (UN)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Ecole Polytechnique de l'Université de Nantes (EPUN), Université de Nantes (UN)-Université de Nantes (UN), GREMAN (matériaux, microélectronique, acoustique et nanotechnologies) (GREMAN - UMR 7347), Institut National des Sciences Appliquées - Centre Val de Loire (INSA CVL), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université de Tours (UT)-Centre National de la Recherche Scientifique (CNRS), The University of Tokyo (UTokyo), Université de Tsukuba = University of Tsukuba, SwissFEL, Paul Scherrer Institut, SLAC National Accelerator Laboratory (SLAC), Stanford University, Ecole Polytechnique Fédérale de Lausanne (EPFL), European Synchrotron Radiation Facility (ESRF), IM‐LED LIA, Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Nantes (UN)-Université de Nantes (UN)-Ecole Polytechnique de l'Université de Nantes (EPUN), Université de Nantes (UN)-Université de Nantes (UN)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Tours (UT)-Institut National des Sciences Appliquées - Centre Val de Loire (INSA CVL), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), ANR-16-CE30-0018,ELASTICA,Cooperativité Elastique Photo-Induite dans des Matériaux Bistables avec Changement de Volume(2016), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université de Tours-Centre National de la Recherche Scientifique (CNRS)

Subjects
Diffraction, Phase transition, Materials science, Electronic properties and materials, Bistability, Science, FOS: Physical sciences, General Physics and Astronomy, Physics::Optics, Applied Physics (physics.app-ph), 02 engineering and technology, 01 natural sciences, General Biochemistry, Genetics and Molecular Biology, Article, Condensed Matter::Materials Science, 0103 physical sciences, Physics::Atomic and Molecular Clusters, [CHIM]Chemical Sciences, 010306 general physics, [PHYS]Physics [physics], Condensed Matter - Materials Science, Multidisciplinary, Condensed matter physics, Materials Science (cond-mat.mtrl-sci), Physics - Applied Physics, General Chemistry, Acoustic wave, 021001 nanoscience & nanotechnology, 3. Good health, Phase transitions and critical phenomena, Picosecond, Femtosecond, 0210 nano-technology, Ultrashort pulse, Powder diffraction
Abstract

Thanks to the remarkable developments of ultrafast science, one of today's challenges is to modify material state by controlling with a light pulse the coherent motions that connect two different phases. Here we show how strain waves, launched by electronic and structural precursor phenomena, determine a macroscopic transformation pathway for the semiconducting-to-metal transition with large volume change in bistable Ti$_3$O$_5$ nanocrystals. Femtosecond powder X-ray diffraction allowed us to quantify the structural deformations associated with the photoinduced phase transition on relevant time scales. We monitored the early intra-cell distortions around absorbing metal dimers, but also long range crystalline deformations dynamically governed by acoustic waves launched at the laser-exposed Ti$_3$O$_5$ surface. We rationalize these observations with a simplified elastic model, demonstrating that a macroscopic transformation occurs concomitantly with the propagating acoustic wavefront on the picosecond timescale, several decades earlier than the subsequent thermal processes governed by heat diffusion., 30 pages (including supplementary text), 5 main figures, 9 supplementary figures; corrected author list

Published
2020
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8. Symmetry breakings in a metal organic framework with a confined guest

Author

Eric Collet, Abdou Boucekkine, Aziz Ghoufi, José Antonio Real, Bertrand Toudic, Elzbieta Trzop, Guillaume Maurin, M. Carmen Muñoz, Jean-Yves Mevellec, Céline Mariette, Institut de Physique de Rennes (IPR), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), Institut des Matériaux Jean Rouxel (IMN), Université de Nantes - UFR des Sciences et des Techniques (UN UFR ST), Université de Nantes (UN)-Université de Nantes (UN)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Ecole Polytechnique de l'Université de Nantes (EPUN), Université de Nantes (UN)-Université de Nantes (UN), Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Departamento de Física Aplicada [Universitat Politècnica de València], Universitat Politècnica de València (UPV), Instituto de Ciencia Molecular (ICMol), Universitat de València (UV), The authors thank Dmitry Chernyshov (SNBL beamline, ESRF) for his support duringthe synchrotron experiment. The authors acknowledge Jumana Shikh Almakara andSimon Le Mehaute for fruitful discussions. Thanks to the Spanish Ministerio de Economiay Competitividad (MINECO), FEDER (CTQ2016-78341-P), Unidad de ExcelenciaMara de Maeztu (MDM-2015-0538), and the Generalitat Valenciana through PROMETEO/2016/147., Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Université de Nantes (UN)-Université de Nantes (UN)-Ecole Polytechnique de l'Université de Nantes (EPUN), Université de Nantes (UN)-Université de Nantes (UN)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), and Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], Physics, Phase transition, Space group, 02 engineering and technology, 021001 nanoscience & nanotechnology, 01 natural sciences, Magnetic susceptibility, Crystallography, symbols.namesake, 0103 physical sciences, symbols, [CHIM]Chemical Sciences, Molecule, Density functional theory, Symmetry breaking, 010306 general physics, 0210 nano-technology, Raman spectroscopy, Single crystal
Abstract

The MOF $[{\text{Fe(tvp)}}_{2}{(\text{NCS})}_{2}]\ifmmode\cdot\else\textperiodcentered\fi{}2\text{BzCHO}$ is demonstrated to undergo a complex sequence of phase transitions and spin-crossover behavior of its constitutive ${\text{Fe}}^{\text{II}}$ ions upon adsorption of benzaldehyde guest molecules. Our study, combining Raman and synchrotron x-ray diffraction measurements on a single crystal, reveals that the conversion from the pure high-spin to the pure low-spin phases implies a rich sequence of intermediate phases, with symmetry breaking forming at least three different space groups. These different symmetries involve spin-state ordering, ligand ordering, and guest ordering, interpreted by combining magnetic susceptibility, Raman measurements, density functional theory, and force field molecular dynamics calculations.

Published
2020
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9. Hot carriers generation and resistive switching induced by electric and light pulses in the Mott insulator GaTa4Se8 (Conference Presentation)

Author

Roman Bertoni, Marina Servol, Laurent Cario, Hervé Cailleau, Marco Cammarata, Benoit Corraze, Danylo Babich, Etienne Janod, Maciej Lorenc, Céline Mariette, and Julien Tranchant

Subjects
Materials science, business.industry, Mott insulator, Physics::Optics, Laser, law.invention, Pulse (physics), Crystal, Wavelength, law, Electric field, Femtosecond, Optoelectronics, Condensed Matter::Strongly Correlated Electrons, Strongly correlated material, business
Abstract

Mott insulators are a class of strongly correlated materials with emergent properties important for modern electronics applications. The key property for application is the Electric Mott insulator to metal Transitions (EMT) whose proposed mechanism is related to the creation of hot electrons by electric field triggering an electronic avalanche after a time delay. This model suggests that the direct creation of hot carriers thanks to a laser pulse should drastically affect the EMT. We have tested this idea by performing pump-pump-probe experiments on single crystals of the Mott insulator GaTa4Se8, whereby electric and laser pulses simultaneously excite the crystal while electric probe monitors its conductivity. Our results show that the concomitant application of femtosecond laser pulse reduced the time delay of EMT by a factor up to. Measurements performed with different laser wavelengths and fluences support moreover that the EMT is driven by a hot carriers generation mechanism.

Published
2020
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10. High spatial resolution studies of phase transitions within organic aperiodic crystals

Author

Laurent Guérin, Céline Mariette, Alexei Bosak, Mariana Verezhak, Christophe Odin, Bertrand Toudic, Philippe Bourges, Claude Ecolivet, Philippe Rabiller, Institut de Physique de Rennes (IPR), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Paul Scherrer Institute (PSI), European Synchrotron Radiation Facility (ESRF), LLB - Nouvelles frontières dans les matériaux quantiques (NFMQ), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), SNSFSwiss National Science Foundation (SNSF) [200021L_169753], European UnionEuropean Union (EU) [701647], Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay

Subjects
[PHYS]Physics [physics], Phase transition, Materials science, Nonadecane, Condensed matter physics, Quasicrystal, Physics::Optics, 02 engineering and technology, 021001 nanoscience & nanotechnology, 01 natural sciences, Landau theory, Mosaicity, Symmetry (physics), 3. Good health, chemistry.chemical_compound, chemistry, Aperiodic graph, Condensed Matter::Superconductivity, 0103 physical sciences, 010306 general physics, 0210 nano-technology, Translational symmetry
Abstract

International audience; The understanding of the symmetry breakings within crystals that are aperiodic by construction is actually very limited. Quasicrystals and incommensurate composite crystals may potentially allow such studies. We focus on the phase transitions of the aperiodic n-nonadecane/urea which recovers a translational symmetry within a four-dimensional space at room temperature. High-resolution neutron and synchrotron studies are reported as a function of the temperature on this organic crystal which presents an exceptional mosaicity. They reveal the richness of such approach, showing the appearance of very long wavelength supplementary intermodulations. This work generalizes the Landau theory to incommensurate composite crystals.

Published
2020
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11. De la simple hélice aux nanostructures tubulaires

Author

Erwan Paineau, Pascale Launois, Mohamed-Salah Amara, Stéphan Rouzière, Denis Petermann, Mathieu Kociak, and Céline Mariette

Subjects
General Medicine
Abstract

Le meme formalisme est utilise pour expliquer la diffraction par l’ADN et par les nanotubes de carbone ou leurs analogues d’oxydes metalliques, les nanotubes d’imogolite.La diffraction permet a la fois de determiner la structure et l’organisation des nanotubes. De la diffraction electronique a celle des rayons X, nous discutons des proprietes individuelles et d’ensemble de ces nanostructures.

Published
2015
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12. Self-Compression in Urea Inclusion Compounds

Author

Laurent Guérin, Shane Nichols, Bo Wang, Céline Mariette, Bertrand Toudic, Ilya Frantsuzov, Philippe Rabiller, and Mark D. Hollingsworth

Subjects
chemistry.chemical_compound, Materials science, chemistry, Compression (functional analysis), Urea, Inclusion (mineral), Composite material, Inclusion compound
Published
2018
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13. Comment on 'The true structural periodicities and superspace group descriptions of the prototypical incommensurate composite materials: Alkane/urea inclusion compounds' by Couzi M. et al

Author

T.J.B.M. Janssen, Philippe Rabiller, Laurent Guérin, Mark D. Hollingsworth, Claude Ecolivet, Ilya Frantsuzov, Céline Mariette, Bertrand Toudic, Groupe matière condensée et matériaux (GMCM), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Service de Chirurgie Générale et Digestive[Lille], Université de Lille, Droit et Santé-Centre Hospitalier Régional Universitaire [Lille] (CHRU Lille), Institut de Physique de Rennes (IPR), Department of Chemistry, Kansas State University, Centre National de la Recherche Scientifique (CNRS)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES), Université de Rennes 1 (UR1), and Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Alkane, chemistry.chemical_classification, Materials science, General Physics and Astronomy, 02 engineering and technology, 021001 nanoscience & nanotechnology, Superspace, 01 natural sciences, chemistry.chemical_compound, Crystallography, chemistry, Group (periodic table), 0103 physical sciences, Urea, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Inclusion (mineral), 010306 general physics, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2017
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14. Formation of local spin-state concentration waves during the relaxation from photoinduced state in a spin-crossover polymer

Author

Daopeng Zhang, Serhane Zerdane, José Antonio Real, Pierre Fertey, Eric Collet, Francisco Javier Valverde-Muñoz, Elzbieta Trzop, Céline Mariette, Institut de Physique de Rennes (IPR), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Instituto de Ciencia Molecular (ICMol), Universitat de València (UV), CTQ2013-46275-P, Ministerio de Ciencia e Innovación, PROMETEO/2016/147, Generalitat Valenciana, 21671121, Natural Science Foundation of China, MDM-2015-0538, Unidad de Excelencia, ANR-13-BS04-0002, National Research Agency, ANR-13-BS04-0002,FEMTOMAT,Etude femtoseconde rayons X et optique de la dynamique ultrarapide de photocommutation de matériaux moléculaires magnétiques(2013), Université de Rennes 1 (UR1), and Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Phase transition, Symmetry breaking 2, Spin states, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Spin crossover, Phase (matter), Materials Chemistry, Organic chemistry, Symmetry breaking, Thermal equilibrium, Aperiodicity, Chemistry, Scattering, Metals and Alloys, 021001 nanoscience & nanotechnology, Atomic and Molecular Physics, and Optics, Photo-crystallography, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, [CHIM.POLY]Chemical Sciences/Polymers, Chemical physics, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Relaxation (physics), Condensed Matter::Strongly Correlated Electrons, 0210 nano-technology
Abstract

The complex relaxation from the photoinduced high-spin phase (PIHS) to the low-spin phase of the bimetallic two-dimensional coordination spin-crossover polymer [Fe[(Hg(SCN)3)2](4,4′-bipy)2]nis reported. During the thermal relaxation, commensurate and incommensurate spin-state concentration waves (SSCWs) form. However, contrary to the steps forming at thermal equilibrium, associated with long-range SSCW order, the SSCWs forming during the relaxation from the PIHS phase correspond to short-range order, revealed by diffuse X-ray scattering. This is interpreted as resulting from the competition between the two types of SSCW order and another structural symmetry breaking, due to ligand ordering, occurring at low temperature and precluding long-range SSCW order.

Published
2017
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15. Front Cover: Single Laser Shot Photoinduced Phase Transition of Rubidium Manganese Hexacyanoferrate Investigated by X‐ray Diffraction (Eur. J. Inorg. Chem. 27/2019)

Author

Matteo Levantino, Céline Mariette, Marco Cammarata, Giovanni Azzolina, Hiroko Tokoro, Elzbieta Trzop, Shin-ichi Ohkoshi, Kosuke Nakagawa, Mathias Sander, Eric Collet, and Roman Bertoni

Subjects
Inorganic Chemistry, Phase transition, Front cover, chemistry, law, Shot (pellet), X-ray crystallography, Analytical chemistry, chemistry.chemical_element, Manganese, Laser, law.invention, Rubidium
Published
2019
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16. Crystallography and dynamics in superspace

Author

Philippe Rabiller, Laurent Guérin, Bertrand Toudic, Céline Mariette, Institut de Physique de Rennes (IPR), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), and Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Physics, Phase transition, QC1-999, Quasicrystal, 02 engineering and technology, 021001 nanoscience & nanotechnology, Superspace, 01 natural sciences, Crystallography, Aperiodic graph, Lattice (order), 0103 physical sciences, Physical space, State of matter, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], 010306 general physics, 0210 nano-technology, Translational symmetry, ComputingMilieux_MISCELLANEOUS
Abstract

The discovery in materials of long range order without lattice periodicity has generated a very broad field of research with the introduction of totally new concepts. The common feature of this new state of matter is the translational symmetry recovered by adding supplementary dimensions to the physical space, defining a crystallographic superspace. Along these supplementary directions, specific low excitations, so-called phasons, are predicted and observed. These quasi-periodic crystals may present phase transitions as function of external parameters, which have then to be described as symmetry breakings within these crystallographic superspaces. Three different families of quasi-periodic crystals are usually considered: incommensurate modulated crystals, aperiodic composites and quasicrystals. Their crystallography and dynamics are discussed.

Published
2017
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17. Frustrated pretransitional phenomena in aperiodic composites

Author

Bo Wang, Laurent Guérin, Ilya Frantsuzov, Bertrand Toudic, Mark D. Hollingsworth, Philippe Rabiller, Céline Mariette, Institut de Physique de Rennes (IPR), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Department of Chemistry, Kansas State University, CHE-0809845, National Science Foundation, 11-BS04-0004, Agence Nationale de la Recherche, Argonne National Laboratory, U.S. Department of Energy, DE-AC02-06CH11357, Basic Energy Sciences, ANR-11-BS04-0004,ODACE,Ordre et désordre dans les édifices cristallins apériodiques.(2011), Université de Rennes 1 (UR1), and Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Diffraction, Physics, [PHYS]Physics [physics], Phase transition, Condensed matter physics, Scattering, Dimension (graph theory), 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Superspace, 01 natural sciences, 0104 chemical sciences, phase transition - aperiodic composites - critical phenomena - synchrotron diffraction, Brillouin zone, Phase (matter), Symmetry breaking, 0210 nano-technology
Abstract

This paper reports on symmetry breaking in the aperiodic inclusion compound $n\text{-octadecane/urea}$ and its isotopomer $n\text{-octadecane/urea-}{d}_{4}$. The high-symmetry phase is described by a hexagonal rank-4 superspace group. Pretransitional phenomena in this crystallographic superspace reveal competing short-range-ordering phenomena within the high-symmetry phase. Very high-resolution diffraction data show that critical scattering appears at inequivalent points within the four-dimensional Brillouin zone, although the first phase transition at ${{T}_{c}}_{1}$ near 158 K implies the condensation at only one of those points. The resulting superspace group remains of dimension 4. Two other phase transitions are reported at ${{T}_{c}}_{2}\phantom{\rule{4pt}{0ex}}=152.8(4)\phantom{\rule{0.28em}{0ex}}\mathrm{K}$ and ${{T}_{c}}_{3}=109(4)\phantom{\rule{0.28em}{0ex}}\mathrm{K}$ in $n\text{-octadecane/urea-}{d}_{4}$. The two low-symmetry phases that arise are described by rank-5 superspace groups.

Published
2016
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19. Multiscale real-time XRD probing of the semiconductor-to-metal ultrafast phase transition in Ti3O5 nanocrystals

Author

Maciej Lorenc, Céline Mariette, Matteo Levantino, A. Volte, Hiroko Tokoro, S.-I. Okhoshi, M. Cammarata, and Henrik T. Lemke

Subjects
Phase transition, Materials science, business.industry, Condensed Matter Physics, Biochemistry, Inorganic Chemistry, Metal, Semiconductor, Nanocrystal, Structural Biology, visual_art, visual_art.visual_art_medium, Optoelectronics, General Materials Science, Physical and Theoretical Chemistry, business, Ultrashort pulse
Published
2018
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20. Long-range modulation of a composite crystal in a five-dimensional superspace

Author

Pierre Fertey, Sylvain Ravy, Thomas Weber, Laurent Guérin, Michael Huard, Bo Wang, Philippe Rabiller, Stefan C. B. Mannsfeld, Shane M. Nichols, Céline Mariette, Mark D. Hollingsworth, and Bertrand Toudic

Subjects
Physics, 02 engineering and technology, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Superspace, 01 natural sciences, Article, Electronic, Optical and Magnetic Materials, Range (mathematics), Modulation, Quantum mechanics, 0103 physical sciences, X-ray crystallography, 010306 general physics, 0210 nano-technology, Composite crystal
Abstract

The intergrowth crystal of n-tetracosane/urea presents a misfit parameter, defined by the ratio γ = ch/cg (chost/cguest), that is very close to a commensurate value (γ ≅ 1/3). High-resolution diffraction studies presented here reveal an aperiodic misfit parameter of γ = 0.3369, which is found to be constant at all temperatures studied. A complex sequence of structural phases is reported. The high temperature phase (phase I) exists in the four-dimensional superspace group P6122(00γ). At Tc1 = 179(1) K, a ferroelastic phase transition increases the dimension of the crystallographic superspace. This orthorhombic phase (phase II) is characterized by the five-dimensional (5D) superspace group C2221(00γ)(10δ) with a modulation vector ao* + cm* = ao* + δ · ch*, in which the supplementary misfit parameter is δ = 0.025(1) in host reciprocal units. This corresponds to the appearance of a modulation of very long period (about 440 ± 16 Å). At Tc2 = 163.0(5) K, a 5D to 5D phase transition leads to the crystallographic superspace group P212121(00γ)(00δ) with a very similar value of δ. This phase transition reveals a significant hysteresis effect.

Published
2015
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21. Neutron Laue and X-ray diffraction study of a new crystallographic superspace phase in n-nonadecane-urea

Author

Céline Mariette, Philippe Rabiller, Marie-Hélène Lemée-Cailleau, Laurent Guérin, Garry J. McIntyre, Bertrand Toudic, Serhane Zerdane, Jean-Claude Ameline, Institut de Physique de Rennes (IPR), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Australian Nuclear Science and Technology Organisation [Australie] (ANSTO), Institut Laue-Langevin (ILL), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), and ILL

Subjects
Nonadecane, 02 engineering and technology, Superspace, 01 natural sciences, Crystal, chemistry.chemical_compound, aperiodic composite crystals, Phase (matter), 0103 physical sciences, Materials Chemistry, Symmetry breaking, 010306 general physics, Translational symmetry, symmetry, Physics, [PHYS]Physics [physics], Metals and Alloys, 021001 nanoscience & nanotechnology, Atomic and Molecular Physics, and Optics, Symmetry (physics), Electronic, Optical and Magnetic Materials, Crystallography, neutron Laue diffraction, chemistry, crystallographic superspace, X-ray crystallography, 0210 nano-technology
Abstract

Aperiodic composite crystals present long-range order without translational symmetry. These materials may be described as the intersection in three dimensions of a crystal which is periodic in a higher-dimensional space. In such materials, symmetry breaking must be described as structural changes within these crystallographic superspaces. The increase in the number of superspace groups with the increase in the dimension of the superspace allows many more structural solutions. This is illustrated inn-nonadecane–urea, revealing a fifth higher-dimensional phase at low temperature.

Published
2015
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22. The creation of modulated monoclinic aperiodic composites in n-alkane/urea compounds

Author

Philippe Rabiller, Bertrand Toudic, Laurent Guérin, Céline Mariette, Yu-Sheng Chen, Mark D. Hollingsworth, Alexander Popov, Alexei Bosak, Institut de Physique de Rennes (IPR), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Argonne National Laboratory [Lemont] (ANL), European Synchrotron Radiation Facility (ESRF), Kansas State University, We thank Shane M. Nichols, Bo Wang, Robert Henning, and Vukica Srager for their help with this work, which was supported by the NSF (CHE-0809845). Portions of this research were carried out at the Advanced Photon Source (beamline 14-BM-C) at Argonne National Laboratory, under DOE Contract No. DE-AC02-06CH11357., Université de Rennes 1 (UR1), and Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Alkane, chemistry.chemical_classification, alkane/urea crystals, [PHYS]Physics [physics], Phase transition, diffraction, aperiodic crystals, Condensed Matter Physics, Superspace, Article, phase transitions, Inorganic Chemistry, chemistry.chemical_compound, Crystallography, chemistry, Group (periodic table), Phase (matter), crystallographic superspace, Urea, Molecule, General Materials Science, Monoclinic crystal system
Abstract

n-Dodecane/urea is a member of the prototype series of n-alkane/urea inclusion compounds. At room temperature, it presents a quasi-one dimensional liquid-like state for the confined guest molecules within the rigid, hexagonal framework of the urea host. At lower temperatures, we report the existence of two other phases. Below Tc=248 K there appears a phase with rank four superspace group P61 22(00γ), the one typically observed at room temperature in n-alkane/urea compounds with longer guest molecules. A misfit parameter, defined by the ratio γ= c h/c g (c host/c guest), is found to be 0.632±0.005. Below Tc1=123 K, a monoclinic modulated phase is created with a constant shift along c of the guest molecules in adjacent channels. The maximal monoclinic space group for this structure is P121 1(α0γ). Analogies and differences with n-heptane/urea, which also presents a monoclinic, modulated low-temperature phase, are discussed.

Published
2015
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23. Imogolite nanotubes: a 2D x-ray scattering study of films of oriented samples

Author

Stéphan Rouzière, Antoine Thill, Erwan-Nicolas Paineau, Mohamed-Salah Amara, Pascale Launois, Céline Mariette, Laboratoire de Physique des Solides (LPS), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interdisciplinaire sur l'Organisation Nanométrique et Supramoléculaire (LIONS), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)

Subjects
Materials science, Mechanical properties of carbon nanotubes, inorganic nanotubes, 02 engineering and technology, Carbon nanotube, 010403 inorganic & nuclear chemistry, 01 natural sciences, Biochemistry, law.invention, Inorganic Chemistry, Optics, Structural Biology, law, [CHIM]Chemical Sciences, General Materials Science, Physical and Theoretical Chemistry, Nanoscopic scale, Condensed matter physics, business.industry, Scattering, 2D scattering, X-ray, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, Optical properties of carbon nanotubes, Reciprocal lattice, 0210 nano-technology, business, Powder diffraction
Abstract

International audience; Inorganic nanotubes represent an emerging class of nanobuilding blocks. Among them, imogolites are alumino-silicate or alumino-germanate nanotubes with well controlled diameter and helicity. As such, they constitute a model platform for the study of molecular interactions and confinement at the nanoscale, complementing the one constituted by carbon nanotubes. We focus here on double-walled alumino-germanate nanotubes, discovered very recently [1]. They are formed of two concentric tubes (figure inset), with respective internal diameters of 1.6 and 3.1nm and up to 1 micron in length [2]. We report the first experimental study, using wide angle x-ray scattering, performed on films of oriented nanotubes (figure). Structural changes of the nanotubes and behavior of the confined water under heating are investigated in-situ. The study of oriented samples gives new information that is not available with powder diffraction. Above all, the contribution to the scattering signal of internal and external tubes can be separated as well as the translational/rotational correlations. The use of wide image plate detectors allows one to access large area of the reciprocal space in a single image. Simulations of the two-dimensionnal scattering diagrams will be presented. A key question, the correlation between internal and external tube, which is of great interest for understanding friction properties at the nanoscale, will be discussed.

Published
2014

24. Critical phenomena in higher dimensional spaces: The hexagonal-to-orthorhombic phase transition in aperiodicn-nonadecane/urea

Author

Claude Ecolivet, P. Bourges, Laurent Guérin, Daniele de Sanctis, Philippe Rabiller, Bertrand Toudic, Alexei Bosak, Mark D. Hollingsworth, Pilar García-Orduña, Céline Mariette, T.J.B.M. Janssen, Institut de Physique de Rennes (IPR), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay, European Synchrotron Radiation Facility (ESRF), Institute for Theoretical Physics, University of Nijmegen, Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)

Subjects
Diffraction, Physics, Phase transition, Nonadecane, Condensed matter physics, Critical phenomena, 02 engineering and technology, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, Electronic, Optical and Magnetic Materials, chemistry.chemical_compound, chemistry, 0103 physical sciences, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Wave vector, Orthorhombic crystal system, 61.44.Fw, 64.60.−i, 61.05.cf, Phason, 010306 general physics, 0210 nano-technology, Intensity (heat transfer)
Abstract

PACS number(s): 61.44.Fw, 64.60.−i, 61.05.cf.-- et al., Upon cooling, the aperiodic inclusion compound n-nonadecane/urea presents a hexagonal-to-orthorhombic group-subgroup phase transition at Tcl that increases the structure's superspace dimensionality from four to five. This paper reports on pretransitional phenomena in such a high-dimensional space, generalizing the critical results previously reported at a lower dimensionality. Very high-resolution diffraction data reveal anomalously large correlation lengths along the aperiodic direction, with all correlation lengths diverging at Tcl. This could be explained by low-frequency phason excitations that soften at Tcl at the critical wave vector, in accordance with an increase in the critical diffuse scattering intensity. © 2013 American Physical Society.

Published
2013
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25. Phase Transitions in Aperiodic Composite Crystals

Author

Philippe Rabiller, Laurent Guérin, Mark D. Hollingsworth, Claude Ecolivet, Céline Mariette, and Bertrand Toudic

Subjects
Diffraction, Alkane, chemistry.chemical_classification, Phase transition, Crystallography, chemistry.chemical_compound, Materials science, chemistry, Aperiodic graph, Composite number, Urea, Molecule, Superspace
Abstract

Aperiodic alkane/urea inclusion compounds (UIC) are prototype composites which exhibit complex sequences of phases that can clearly be described in the (3+d) dimension crystallographic superspace. By simply changing the length of the guest alkane molecules (C n H2n+2) which pile up in the channels of the host urea honeycomb-like framework, it is, for instance, possible to have phase-ordering phase transition from 3 to (3+1) dimension in the case of n-heptane/urea (n=7), or as in the case of n-hexadecane/urea (n=16) or n-nonadecane/urea (n=19), a generalization to higher dimensions of the phase transitions found in modulated structures. Such results are successfully obtained with the help of high resolution diffraction methods.

Published
2013
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26. A molecular 'phase ordering' phase transition leading to a modulated aperiodic composite in n-heptane/urea

Author

Philippe Rabiller, Mickaël Huard, Keith Alquist, Céline Mariette, Shane Nichols, Mark D. Hollingsworth, Bertrand Toudic, Ted Janssen, Claude Ecolivet, Institut de Physique de Rennes (IPR), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Institute for Theoretical Physics, University of Nijmegen, Université de Rennes 1 (UR1), and Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Phase transition, Materials science, Ferroelectricity, Satellites, General Physics and Astronomy, 02 engineering and technology, Crystal structure, 01 natural sciences, Inclusion compound, chemistry.chemical_compound, 0103 physical sciences, Physical and Theoretical Chemistry, 010306 general physics, Heptane, X-ray detectors, 021001 nanoscience & nanotechnology, X-ray diffraction, Radiation detectors, [SDV.BBM.BP]Life Sciences [q-bio]/Biochemistry, Molecular Biology/Biophysics, Crystallography, chemistry, Aperiodic graph, Phase transitions, X-ray crystallography, Image reconstruction, Inclusions, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Mercury (element), 0210 nano-technology, Superstructure (condensed matter)
Abstract

International audience; n-Heptane/urea is an aperiodic inclusion compound in which the ratio of host and guest repeats along the channel axis is very close to unity and is found to have a constant value (0.981) from 280 K to 90 K. Below 280 K, two phase transitions are observed. The first (T(c1) = 145 K) is a ferroelastic phase transition that generates superstructure reflections for the host while leaving the guest with 1D order. The second (T(c2) = 130 K) is a "phase ordering" transition to a four-dimensional structure (P2(1)11(0βγ)) with pronounced host-guest intermodulation and a temperature dependent phase shift between guests in adjacent channels.

Published
2012
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27. Phase transitions and critical phenomena in aperiodic composite crystals

Author

Céline Mariette, Philippe Rabiller, Bertrand Toudic, and Laurent Guérin

Subjects
Inorganic Chemistry, Phase transition, Materials science, Condensed matter physics, Structural Biology, Aperiodic graph, Critical phenomena, Composite number, General Materials Science, Physical and Theoretical Chemistry, Condensed Matter Physics, Biochemistry
Published
2015
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29. Diffuse scattering and phase transitions in aperiodic inclusion compounds

Author

Bertrand Toudic, Céline Mariette, Philippe Rabiller, Laurent Guérin, and Mark D. Hollingsworth

Subjects
Inorganic Chemistry, Phase transition, Materials science, Diffuse scattering, Structural Biology, Aperiodic graph, General Materials Science, Physical and Theoretical Chemistry, Inclusion (mineral), Condensed Matter Physics, Biochemistry, Molecular physics
Abstract

Small molecules, such as urea, thiourea, perhydrotriphenylene can be co-crystallised with long-chain hydrocarbon molecules to form inclusion compounds. The guest chains are confined to narrow, approximately cylindrical, channels created by the host small-molecule lattice. The stoichiometry and the conformations of the chains included inside the channels are function of internal interactions such as intra-chain interaction, but also of overall co-operative properties of the resulting three dimensionally ordered single crystal. These intergrowth compounds may form incommensurate composite crystals. A prototype example of such uniaxial intergrowth aperiodic crystals is n-alkane (CnH2n+2)/urea (CO(NH2)2). In these supra-molecular systems, urea molecules are connected by H-bonds and form helical ribbons, which repeat every six urea molecules to form a series of linear, hexagonal tunnels that can accommodate linear alkanes. Because the channels (~0.53 nm) are larger than the hydrocarbon chains, guests are held loosely and can undergo substantial motions. A significant amount of diffuse scattering of the first and second kinds can be depicted in scattering experiments, static or dynamic. These materials undergo a large variety of continuous or weakly first order structural phase transitions when changing the alkane molecule length and giving place to large pre-transitional effects. The talk will give an overview of the diffuse scattering in these compounds and will focus on connection with aperiodicity.

Published
2014
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33. Phonons in an aperiodic alkane/urea composite crystal studied by inelastic x-ray scattering

Author

Bertrand Toudic, Laurent Guérin, Claude Ecolivet, Mariana Verezhak, Philippe Rabiller, Céline Mariette, Alexei Bosak, J. Ollivier, Institut de Physique de Rennes (IPR), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interdisciplinaire de Physique [Saint Martin d’Hères] (LIPhy), Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Institut Laue-Langevin (ILL), ILL, European Synchrotron Radiation Facility (ESRF), European Synchrotron Radiation Facility, 701647, Horizon 2020, 200021L_169753, Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung, and Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], Materials science, Nonadecane, Phonon, Scattering, 02 engineering and technology, Inelastic scattering, 021001 nanoscience & nanotechnology, 01 natural sciences, Molecular physics, Transverse mode, chemistry.chemical_compound, chemistry, Aperiodic graph, 0103 physical sciences, State of matter, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], 010306 general physics, 0210 nano-technology, Translational symmetry
Abstract

International audience; Aperiodic composite crystals belong to a new state of matter that possesses long-range order without translational symmetry. We report measurements of low-lying phonon branches in a n-alkane/urea compound that provide a new insight to the urea sub-lattice and the commensurate basal plane dynamics. Focusing on the thoroughly studied n-nonadecane/urea compound makes a comparison with other inelastic scattering results possible, allowing the observation of a new aperiodic elastic signature. Using three techniques, slight but reproducible difference in sound velocities is observed between the transverse mode propagating along the aperiodic direction and polarized in the commensurate basal plane, and the one polarized along the aperiodic direction propagating in the basal plane.

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