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231225s2021 xx |||||o 00| ||eng c |
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|a 10.1021/acs.chemmater.0c04491
|2 doi
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|a pubmed25n1080.xml
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|a (DE-627)NLM324223307
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|a (NLM)33867666
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|a DE-627
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|a eng
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|a Benin, Bogdan M
|e verfasserin
|4 aut
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|a Lone-Pair-Induced Structural Ordering in the Mixed-Valent 0D Metal-Halides Rb23BiIII x SbIII 7-x SbV 2Cl54 (0 ≤ x ≤ 7)
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|c 2021
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|a Text
|b txt
|2 rdacontent
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|a ƒaComputermedien
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|2 rdamedia
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|a ƒa Online-Ressource
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|a Date Revised 21.04.2021
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2021 The Authors. Published by American Chemical Society.
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|a Mixed-valent metal-halides containing ns2 lone pairs may exhibit intense visible absorption, while zero-dimensional (0D) ns2-based metal-chlorides are generally colorless but have demonstrated promising optoelectronic properties suitable for thermometry and radiation detection. Here, we report solvothermally synthesized mixed-valent 0D metal-halides Rb23BiIII x SbIII 7-x SbV 2Cl54 (0 ≤ x ≤ 7). Rb23SbIII 7SbV 2Cl54 crystallizes in an orthorhombic space group (Cmcm) with a unique, layered 0D structure driven by the arrangement of the 5s2 lone pairs of the SbIIICl6 octahedra. This red material is likely the true structure of a previously reported monoclinic "Rb2.67SbCl6" phase, the structure of which was not determined. Partially or fully substituting SbIII with isoelectronic BiIII yields the series Rb23BiIII x SbIII 7-x SbV 2Cl54 (0 < x ≤ 7), which exhibits a similar layered 0D structure but with additional disorder that yields a trigonal crystal system with an enantiomorphic space group (R32). Second harmonic generation of 532 nm light from a 1064 nm laser using Rb23BiIII 7SbV 2Cl54 powder confirms the noncentrosymmetry of this space group. As with the prototypical mixed-valent pnictogen halides, the visible absorption bands of the Rb23BiIII x SbIII 7-x SbV 2Cl54 family are the result of intervalent SbIII-SbV and mixed-valent BiIII-SbV charge transfer bands (CTB), with a blueshift of the absorption edge as BiIII substitution increases. No PL is observed from this family of semiconductors, but a crystal of Rb23BiIII 7SbV 2Cl54 exhibits a high resistivity of 1.0 × 1010 Ω·cm and X-ray photoconductivity with a promising μτ product of 8.0 × 10-5 cm2 s-1 V-1. The unique 0D layered structures of the Rb23BiIII x SbIII 7-x SbV 2Cl54 family highlight the versatility of the ns2 lone pair in semiconducting metal-halides, pointing the way toward new functional 0D metal-halide compounds
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|a Journal Article
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1 |
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|a McCall, Kyle M
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Wörle, Michael
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Borgeaud, Dominique
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Vonderach, Thomas
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Sakhatskyi, Kostiantyn
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Yakunin, Sergii
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Günther, Detlef
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Kovalenko, Maksym V
|e verfasserin
|4 aut
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| 773 |
0 |
8 |
|i Enthalten in
|t Chemistry of materials : a publication of the American Chemical Society
|d 1998
|g 33(2021), 7 vom: 13. Apr., Seite 2408-2419
|w (DE-627)NLM098194763
|x 0897-4756
|7 nnas
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| 773 |
1 |
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|g volume:33
|g year:2021
|g number:7
|g day:13
|g month:04
|g pages:2408-2419
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|u http://dx.doi.org/10.1021/acs.chemmater.0c04491
|3 Volltext
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|d 33
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|h 2408-2419
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