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Sphalerite-Chalcopyrite Polymorphism in Semimetallic ZnSnSb2
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK), Avdelningen för oorganisk kemi och strukturkemi.
Max-Planck Institute for Solid State Research.
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK), Avdelningen för oorganisk kemi och strukturkemi.
Solid State Physics, IMIT, Royal Institute of Technology, KTH.
Vise andre og tillknytning
2005 (engelsk)Inngår i: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 17, nr 24, s. 6080-6085Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

We have investigated the system ZnSnSb2 in the course of our attempts to modify thermoelectricZn-Sb frameworks. ZnSnSb2 is only accessible when employing Sn as reactive flux in the synthesis.The material shows an order-disorder transition in the temperature interval between 225 and 240 °Cand decomposes peritectically at about 360 °C. The high-temperature form of ZnSnSb2 adopts the Zn/Sndisordered cubic sphalerite-type structure. Electron microscopy investigations reveal that samples quenchedfrom 350 °C already contain domains of the low-temperature form, which has the Zn/Sn ordered tetragonalchalcopyrite structure. The c/a ratio of the tetragonal structure is, within experimental errors, identical tothe ideal value 2. This gives rise to intricate microtwinning in the low-temperature chalcopyrite form ofZnSnSb2 as obtained in samples quenched from 250 °C. First principles electronic structure calculationsdemonstrate that the tetragonal low-temperature form of ZnSnSb2 has a narrow band gap of about 0.2eV. This is in agreement with the semimetallic behavior of the material found from resistivity measurement.The shape of the electronic density of states for ZnSnSb2 is similar to thermoelectric binary Zn-Sbframeworks. However, the thermopower of ZnSnSb2 is rather low with room-temperature values rangingfrom 10 to 30 íV/K.

sted, utgiver, år, opplag, sider
Washington, DC, 2005. Vol. 17, nr 24, s. 6080-6085
HSV kategori
Forskningsprogram
oorganisk kemi
Identifikatorer
URN: urn:nbn:se:su:diva-42921DOI: 10.1021/cm0516053OAI: oai:DiVA.org:su-42921DiVA, id: diva2:352224
Tilgjengelig fra: 2010-09-21 Laget: 2010-09-20 Sist oppdatert: 2022-02-24bibliografisk kontrollert
Inngår i avhandling
1. Thermoelectric Properties of Antimony Based Networks
Åpne denne publikasjonen i ny fane eller vindu >>Thermoelectric Properties of Antimony Based Networks
2010 (engelsk)Doktoravhandling, med artikler (Annet vitenskapelig)
Abstract [en]

With the retreating sources of carbon based fuels, thermoelectric materials can play an important role in the future of environmentally friendly power generators. Sb based framework have in some cases shown some promising properties as thermoelectric materials. The physical properties may be modified with doping or incorporation of new elements. Zn4Sb3 and Cd4Sb3 are structurally related with a Sb-based network and Zn/Cd occupying the rest of the positions. Both structures undergo order-disorder αβ transition of the Zn/Cd positions, at 254 K and ~355 K respectively. The previously ordered interstitial atoms become distributed in the structure and the two high temperature phases are isostructural (R-3c). Cd4Sb3 was synthesized from melt-quench, flux synthesis with Sn, Bi and In. The syntheses made with In resulted in interstitial-free β-Cd4Sb3 with the composition Cd11.7In1.5Sb10. This compound exhibits no phase transitions until decomposition. ZnSnSb2 and InSb both exhibit the cubic sphalerite structure. ZnSnSb2 is metallic and InSb narrow band-gap semiconductor. Attempts were made to fine-tune the electrical properties by probing the mutual solid solubility range. The formula [ZnSnSb2]x[2(InSb)]1-xSn4 and 0<X<1 with 0.1 increments for the whole composition range was used. Resistivity changes from semiconducting to metallic conduction between x=0.9 and x=0.8. In the attempt to dope Zn4Sb3 by In a novel metastable compound with the composition Zn9Sb6In2 was found. Another novel phase was discovered with the composition Zn5Sb4In2-δ (δ=0.15).  The two phases have the same Sb-framework with a CuAl2 structure. Zn and In arrangements fill the square antiprisms formed by the stacking of 32434 nets in anti configuration. The filling of the antiprisms in the two phases are different, in Zn9Sb6In2 the antiprisms have two filling arrangements, an In or Zn3 triangles. In Zn5Sb4In2-δ the antiprisms are filled with an In and a Zn that occupies a split position to form a hetero-atomic dimers.

sted, utgiver, år, opplag, sider
Stockholm: Department of Materials and Environmental Chemistry, Stockholm University, 2010. s. 65
Emneord
thermoelectric, narrow gap semiconductors, zinc antimonides, cadmium antimonides, chalcopyrites, sphalerites
HSV kategori
Forskningsprogram
materialkemi
Identifikatorer
urn:nbn:se:su:diva-42981 (URN)978-91-7447-143-4 (ISBN)
Disputas
2010-10-22, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 13:00 (engelsk)
Opponent
Veileder
Tilgjengelig fra: 2010-09-30 Laget: 2010-09-22 Sist oppdatert: 2022-02-24bibliografisk kontrollert

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