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Retuerto, M.; Yin, Z.; Emge, T.J.; Stephens, P.W.; Li, M.R.; Sarkar, T.; Croft, M.C.; Ignatov, A.; Yuan, Z.; Zhang, S.J.; Jin, C.; Paria Sena, R.; Hadermann, J.; Kotliar, G.; Greenblatt, M.; |
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Title |
Hole doping and structural transformation in CsTl1-xHgxCl3 |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
Inorganic chemistry |
Abbreviated Journal |
Inorg Chem |
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Volume |
54 |
Issue |
54 |
Pages |
1066-1075 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
CsTlCl3 and CsTlF3 perovskites have been theoretically predicted to be superconductors when properly hole-doped. Both compounds have been previously prepared as pure compounds: CsTlCl3 in a tetragonal (I4/m) and a cubic (Fm3̅m) perovskite polymorph and CsTlF3 as a cubic perovskite (Fm3̅m). In this work, substitution of Tl in CsTlCl3 with Hg is reported, in an attempt to hole-dope the system and induce superconductivity. The whole series CsTl1xHgxCl3 (x = 0.0, 0.1, 0.2, 0.4, 0.6, and 0.8) was prepared. CsTl0.9Hg0.1Cl3 is tetragonal as the more stable phase of CsTlCl3. However, CsTl0.8Hg0.2Cl3 is already cubic with the space group Fm3̅m and with two different positions for Tl+ and Tl3+. For x = 0.4 and 0.5, solid solutions could not be formed. For x ≥ 0.6, the samples are primitive cubic perovskites with one crystallographic position for Tl+, Tl3+, and Hg2+. All of the samples formed are insulating, and there is no signature of superconductivity. X-ray absorption spectroscopy indicates that all of the samples have a mixed-valence state of Tl+ and Tl3+. Raman spectroscopy shows the presence of the active TlClTl stretching mode over the whole series and the intensity of the TlClHg mode increases with increasing Hg content. First-principle calculations confirmed that the phases are insulators in their ground state and that Hg is not a good dopant in the search for superconductivity in this system. |
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Place of Publication |
Easton, Pa |
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Wos |
000348887400048 |
Publication Date |
2014-12-09 |
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ISSN |
0020-1669;1520-510X; |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.857 |
Times cited |
5 |
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Approved |
Most recent IF: 4.857; 2015 IF: 4.762 |
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Call Number |
c:irua:124420 |
Serial |
1476 |
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Author |
Retuerto, M.; Emge, T.; Hadermann, J.; Stephens, P.W.; Li, M.R.; Yin, Z.P.; Croft, M.; Ignatov, A.; Zhang, S.J.; Yuan, Z.; Jin, C.; Simonson, J.W.; Aronson, M.C.; Pan, A.; Basov, D.N.; Kotliar, G.; Greenblatt, M.; |
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Title |
Synthesis and properties of charge-ordered thallium halide perovskites, CsTl0.5+Tl0.53+X3 (X = F or Cl) : theoretical precursors for superconductivity? |
Type |
A1 Journal article |
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Year |
2013 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
25 |
Issue |
20 |
Pages |
4071-4079 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Recently, CsTlCl3 and CsTlF3 perovskites were theoretically predicted to be potential superconductors if they were optimally doped. The syntheses of these two compounds together with a complete characterization of the samples are reported. CsTlCl3 was obtained as orange crystals in two different polymorphs: a tetragonal phase (I4/m) and a cubic phase (Fm (3) over barm). CsTlF3 was formed as a light brown powder, and also as a double cubic perovskite (Fm (3) over barm). In all three CsTlX3 phases, Tl+ and Tl3+ were located in two different crystallographic positions that accommodate their different bond lengths. In CsTlCl3, some Tl vacancies were found in the Tl+ position. The charge ordering between Tl+ and Tl3+ was confirmed by X-ray absorption and Raman spectroscopy. The Raman spectroscopy of CsTlCl3 at high pressure (58 GPa) did not indicate any phase transition to a possible single Tl2+ state. However, the highly insulating material became less resistive with an increasing high pressure, while it underwent a change in its optical properties, from transparent to deeply opaque red, indicative of a decrease in the magnitude of the band gap. The theoretical design and experimental validation of the existence of CsTlF3 and CsTlCl3 cubic perovskites are the necessary first steps in confirming the theoretical prediction of superconductivity in these materials. |
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Place of Publication |
Washington, D.C. |
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Wos |
000326209200017 |
Publication Date |
2013-09-18 |
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ISSN |
0897-4756;1520-5002; |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
28 |
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Notes |
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Approved |
Most recent IF: 9.466; 2013 IF: 8.535 |
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Call Number |
UA @ lucian @ c:irua:112248 |
Serial |
3434 |
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