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Ordering Phenomena in Complex Chalcogenides – the Showcase of A2In12Q19 (A = K, Tl, NH4; Q = Se, Te) and Pseudobinary In2Q3

Kienle, Lorenz and Schlosser, Marc and Manos, Manolis J. and Malliakas, Christos D. and Duppel, Viola and Reiner, Christof and Deiseroth, Hans-Jörg and Kanatzidis, Mercouri G. and Kelm, Klemens and Simon, Arndt (2010) Ordering Phenomena in Complex Chalcogenides – the Showcase of A2In12Q19 (A = K, Tl, NH4; Q = Se, Te) and Pseudobinary In2Q3. European Journal of Inorganic Chemistry, pp. 367-378. Wiley VCH. DOI: 10.1002/ejic.200900721. ISSN 1434-1948.

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Official URL: http://www.wiley-vch.de/publish/en/journals/alphabeticIndex/2005/?jURL=http://www.wiley-vch.de/vch/journals/2005/cover/current.html

Abstract

A group of solids with the general composition A2In12Q19 (A = K, Tl, NH4; Q = Se, Te) is characterized by combined Xray single-crystal and high-resolution transmission-electron microscopy (HRTEM). Similar nanosize domains with variable sizes and complex internal structures are common to all three compounds. Although a partial ordering of domains for the bulk of K2In12Se19 is dominating, the observed ordering patterns in microdomains range from total random orientation to a pattern with a ninefold superstucture (rare precursor phase not stable under HRTEM conditions). In spite of testing various synthesis conditions it was not possible to avoid these unusual structural features for K2In12Se19, which are apparently intrinsic. The formation of significantly larger domains is observed for K2In12Se19–xTex and K2–yTlyIn12Se19 and results in a twofold superstructure that can be observed with X-ray diffraction also on a macroscopic scale. (NH4)- In12Se19 is a special case where an initial weak ordering is observed that is characterized by ring X-ray reflections forming hexagons around certain reciprocal lattice positions. This pattern has apparent similarities to K2In12Se19 but is not stable in the HRTEM. Instead, it disappears rapidly and is finally replaced by a twofold superstructure similar to K2In12Se19–xTex and K2–yTlyIn12Se19. The reason was identified as a combined process of domain broadening and NH3 evaporation. As observed for K2In12Se19 at T 473 K, the superstructure reflections disappear. Surprisingly, the pseudobinary phase In2Q3 (Q: chalcogen) shows strong structural similarities to K2In12Se19 with respect to the internal structure of the nanodomains. Their three-dimensional arrangement, however, and the resulting superstructure are closer related to K2In12Se19–xTex and K2–yTlyIn12Se19.

Document Type:Article
Title:Ordering Phenomena in Complex Chalcogenides – the Showcase of A2In12Q19 (A = K, Tl, NH4; Q = Se, Te) and Pseudobinary In2Q3
Authors:
AuthorsInstitution or Email of Authors
Kienle, Lorenz CAU Kiel, Technische Fakultät, Kaiserstraße 2, 24143 Kiel
Schlosser, MarcUniversity of Siegen, Inorganic Chemistry I, Adolf-Reichwein-Straße 2, 57068 Siegen
Manos, Manolis J.Department of Chemistry, Northwestern University, 2145 Sheridian Rd, Evanstown, IL 60208, USA
Malliakas, Christos D.Department of Chemistry, Northwestern University, 2145 Sheridian Rd, Evanstown, IL 60208, USA
Duppel, ViolaMax Planck Institute for Solid State Research, Heisenbergstraße 1, 70569 Stuttgart
Reiner, ChristofUniversity of Siegen, Inorganic Chemistry I, Adolf-Reichwein-Straße 2, 57068 Siegen
Deiseroth, Hans-JörgUniversity of Siegen, Inorganic Chemistry I, Adolf-Reichwein-Straße 2, 57068 Siegen
Kanatzidis, Mercouri G.Department of Chemistry, Northwestern University, 2145 Sheridian Rd, Evanstown, IL 60208, USA
Kelm, KlemensDLR, Institut für Werkstoff-Forschung, Linder Höhe, 51147 Köln
Simon, ArndtMax Planck Institute for Solid State Research, Heisenbergstraße 1, 70569 Stuttgart
Date:2010
Journal or Publication Title:European Journal of Inorganic Chemistry
Refereed publication:Yes
In SCOPUS:Yes
In ISI Web of Science:Yes
DOI:10.1002/ejic.200900721
Page Range:pp. 367-378
Publisher:Wiley VCH
ISSN:1434-1948
Status:Published
Keywords:Electron microscopy / Real structure / X-ray diffraction / Disordered structure / Diffuse scattering / Chalcogens / Solid-state structures
HGF - Research field:Energy
HGF - Program:Efficient Energy Conversion (old)
HGF - Program Themes:E EV - Energy process technology (old)
DLR - Research area:Energy
DLR - Program:E EV - Energy process technology
DLR - Research theme (Project):E - Thermochemische Prozesse (old)
Location: Köln-Porz
Institutes and Institutions:Institute of Materials Research > Microanalysis
Deposited By: Klemens Kelm
Deposited On:07 Dec 2009 10:10
Last Modified:04 Apr 2013 16:18

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