Bond valences and anharmonicity in vacancy-ordered double perovskite halides
Anharmonic lattice dynamics are intimately linked with optical and electronic properties in perovskite halide semiconductors. Vacancy-ordered double perovskites are a subset of the perovskite halide family containing isolated octahedral units. The absence of polyhedral connectivity engenders the vac...
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| Veröffentlicht in: | Journal of materials chemistry. C, Materials for optical and electronic devices Materials for optical and electronic devices, 2018-11, Vol.6 (44), p.1295-1214 |
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| creator | Maughan, Annalise E Paecklar, Arnold A Neilson, James R |
| description | Anharmonic lattice dynamics are intimately linked with optical and electronic properties in perovskite halide semiconductors. Vacancy-ordered double perovskites are a subset of the perovskite halide family containing isolated octahedral units. The absence of polyhedral connectivity engenders the vacancy-ordered double perovskites with additional degrees of dynamic freedom, which presents an ideal structural framework to study dynamic-property relationships in perovskite halide semiconductors. In the present study, we examine the structure and bonding origins of anharmonicity in the vacancy-ordered double perovskites Cs
2
Sn
1−
x
Te
x
I
6
. While X-ray diffraction indicates that all members adopt the cubic vacancy-ordered double perovskite structure, the local coordination environment probed by X-ray pair distribution function (XPDF) analysis reveals asymmetry of the Cs-I/I-I pair correlation that smoothly decreases with increasing tellurium content. Temperature-dependent neutron total scattering suggests that this asymmetry in the PDF occurs due to anharmonic lattice dynamics arising from octahedral tilting and Cs
+
displacements, as supported by Reverse Monte Carlo simulations of the Cs
2
SnI
6
and Cs
2
TeI
6
end members. We further correlate the trends in asymmetry and anharmonicity with the bond valence sum of the Cs
+
ion, and find that the anharmonicity vanishes when the bonding preferences of the Cs
+
are satisfied by the size of the cuboctahedral void. This study presents a simple and effective approach for understanding the origin of anharmonicity in vacancy-ordered double perovskite materials.
Anharmonicity is observed in vacancy-ordered double perovskites when the A-site cation is not optimally coordinated by the octahedral framework. |
| doi_str_mv | 10.1039/c8tc03527j |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_cross</sourceid><recordid>TN_cdi_crossref_primary_10_1039_C8TC03527J</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2133462282</sourcerecordid><originalsourceid>FETCH-LOGICAL-c344t-43495c88f4100b0935d2c9fa0a7b174727aa6ff66e002bfd972860798877d7363</originalsourceid><addsrcrecordid>eNpFkE1LAzEQhoMoWGov3oVFb8Lq5GOT7FEXPyl4qeeQTbJ06zapyVbovzdaqXOZGeZheHkQOsdwg4HWt0aOBmhFxOoITQhUUIqKsuPDTPgpmqW0glwSc8nrCZrfB2-LLz04b1wqdF60X-q4Dr43_bgrep-vRnuzK0O0Ljpb2LBtB1dsXAxf6aMfXbHUQ29dOkMnnR6Sm_31KXp_fFg0z-X87emluZuXhjI2loyyujJSdgwDtFDTyhJTdxq0aLFgggiteddx7gBI29laEMlB1FIKYQXldIou939DGnuVck5nliZ478yoMBOSMMjQ1R7axPC5dWlUq7CNPudSBFPKOCGSZOp6T5kYUoquU5vYr3XcKQzqx6pq5KL5tfqa4Ys9HJM5cP_W6TdvGHIT</addsrcrecordid><sourcetype>Open Access Repository</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2133462282</pqid></control><display><type>article</type><title>Bond valences and anharmonicity in vacancy-ordered double perovskite halides</title><source>Royal Society Of Chemistry Journals 2008-</source><creator>Maughan, Annalise E ; Paecklar, Arnold A ; Neilson, James R</creator><creatorcontrib>Maughan, Annalise E ; Paecklar, Arnold A ; Neilson, James R ; Colorado State Univ., Fort Collins, CO (United States)</creatorcontrib><description>Anharmonic lattice dynamics are intimately linked with optical and electronic properties in perovskite halide semiconductors. Vacancy-ordered double perovskites are a subset of the perovskite halide family containing isolated octahedral units. The absence of polyhedral connectivity engenders the vacancy-ordered double perovskites with additional degrees of dynamic freedom, which presents an ideal structural framework to study dynamic-property relationships in perovskite halide semiconductors. In the present study, we examine the structure and bonding origins of anharmonicity in the vacancy-ordered double perovskites Cs
2
Sn
1−
x
Te
x
I
6
. While X-ray diffraction indicates that all members adopt the cubic vacancy-ordered double perovskite structure, the local coordination environment probed by X-ray pair distribution function (XPDF) analysis reveals asymmetry of the Cs-I/I-I pair correlation that smoothly decreases with increasing tellurium content. Temperature-dependent neutron total scattering suggests that this asymmetry in the PDF occurs due to anharmonic lattice dynamics arising from octahedral tilting and Cs
+
displacements, as supported by Reverse Monte Carlo simulations of the Cs
2
SnI
6
and Cs
2
TeI
6
end members. We further correlate the trends in asymmetry and anharmonicity with the bond valence sum of the Cs
+
ion, and find that the anharmonicity vanishes when the bonding preferences of the Cs
+
are satisfied by the size of the cuboctahedral void. This study presents a simple and effective approach for understanding the origin of anharmonicity in vacancy-ordered double perovskite materials.
Anharmonicity is observed in vacancy-ordered double perovskites when the A-site cation is not optimally coordinated by the octahedral framework.</description><identifier>ISSN: 2050-7526</identifier><identifier>EISSN: 2050-7534</identifier><identifier>DOI: 10.1039/c8tc03527j</identifier><language>eng</language><publisher>Cambridge: Royal Society of Chemistry</publisher><subject>Anharmonicity ; Asymmetry ; Cesium ions ; Computer simulation ; Displacements (lattice) ; Distribution functions ; Electronic properties ; Halides ; Lattice vacancies ; MATERIALS SCIENCE ; Optical properties ; Perovskite structure ; Perovskites ; Semiconductors ; Tellurium ; Temperature dependence ; X-ray diffraction</subject><ispartof>Journal of materials chemistry. C, Materials for optical and electronic devices, 2018-11, Vol.6 (44), p.1295-1214</ispartof><rights>Copyright Royal Society of Chemistry 2018</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c344t-43495c88f4100b0935d2c9fa0a7b174727aa6ff66e002bfd972860798877d7363</citedby><cites>FETCH-LOGICAL-c344t-43495c88f4100b0935d2c9fa0a7b174727aa6ff66e002bfd972860798877d7363</cites><orcidid>0000-0001-9282-5752 ; 0000-0002-3292-4799 ; 0000-0003-4180-1923 ; 0000000341801923 ; 0000000232924799 ; 0000000192825752</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>230,314,776,780,881,27901,27902</link.rule.ids><backlink>$$Uhttps://www.osti.gov/servlets/purl/1478240$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Maughan, Annalise E</creatorcontrib><creatorcontrib>Paecklar, Arnold A</creatorcontrib><creatorcontrib>Neilson, James R</creatorcontrib><creatorcontrib>Colorado State Univ., Fort Collins, CO (United States)</creatorcontrib><title>Bond valences and anharmonicity in vacancy-ordered double perovskite halides</title><title>Journal of materials chemistry. C, Materials for optical and electronic devices</title><description>Anharmonic lattice dynamics are intimately linked with optical and electronic properties in perovskite halide semiconductors. Vacancy-ordered double perovskites are a subset of the perovskite halide family containing isolated octahedral units. The absence of polyhedral connectivity engenders the vacancy-ordered double perovskites with additional degrees of dynamic freedom, which presents an ideal structural framework to study dynamic-property relationships in perovskite halide semiconductors. In the present study, we examine the structure and bonding origins of anharmonicity in the vacancy-ordered double perovskites Cs
2
Sn
1−
x
Te
x
I
6
. While X-ray diffraction indicates that all members adopt the cubic vacancy-ordered double perovskite structure, the local coordination environment probed by X-ray pair distribution function (XPDF) analysis reveals asymmetry of the Cs-I/I-I pair correlation that smoothly decreases with increasing tellurium content. Temperature-dependent neutron total scattering suggests that this asymmetry in the PDF occurs due to anharmonic lattice dynamics arising from octahedral tilting and Cs
+
displacements, as supported by Reverse Monte Carlo simulations of the Cs
2
SnI
6
and Cs
2
TeI
6
end members. We further correlate the trends in asymmetry and anharmonicity with the bond valence sum of the Cs
+
ion, and find that the anharmonicity vanishes when the bonding preferences of the Cs
+
are satisfied by the size of the cuboctahedral void. This study presents a simple and effective approach for understanding the origin of anharmonicity in vacancy-ordered double perovskite materials.
Anharmonicity is observed in vacancy-ordered double perovskites when the A-site cation is not optimally coordinated by the octahedral framework.</description><subject>Anharmonicity</subject><subject>Asymmetry</subject><subject>Cesium ions</subject><subject>Computer simulation</subject><subject>Displacements (lattice)</subject><subject>Distribution functions</subject><subject>Electronic properties</subject><subject>Halides</subject><subject>Lattice vacancies</subject><subject>MATERIALS SCIENCE</subject><subject>Optical properties</subject><subject>Perovskite structure</subject><subject>Perovskites</subject><subject>Semiconductors</subject><subject>Tellurium</subject><subject>Temperature dependence</subject><subject>X-ray diffraction</subject><issn>2050-7526</issn><issn>2050-7534</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2018</creationdate><recordtype>article</recordtype><recordid>eNpFkE1LAzEQhoMoWGov3oVFb8Lq5GOT7FEXPyl4qeeQTbJ06zapyVbovzdaqXOZGeZheHkQOsdwg4HWt0aOBmhFxOoITQhUUIqKsuPDTPgpmqW0glwSc8nrCZrfB2-LLz04b1wqdF60X-q4Dr43_bgrep-vRnuzK0O0Ljpb2LBtB1dsXAxf6aMfXbHUQ29dOkMnnR6Sm_31KXp_fFg0z-X87emluZuXhjI2loyyujJSdgwDtFDTyhJTdxq0aLFgggiteddx7gBI29laEMlB1FIKYQXldIou939DGnuVck5nliZ478yoMBOSMMjQ1R7axPC5dWlUq7CNPudSBFPKOCGSZOp6T5kYUoquU5vYr3XcKQzqx6pq5KL5tfqa4Ys9HJM5cP_W6TdvGHIT</recordid><startdate>20181115</startdate><enddate>20181115</enddate><creator>Maughan, Annalise E</creator><creator>Paecklar, Arnold A</creator><creator>Neilson, James R</creator><general>Royal Society of Chemistry</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SP</scope><scope>7U5</scope><scope>8FD</scope><scope>L7M</scope><scope>OIOZB</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0001-9282-5752</orcidid><orcidid>https://orcid.org/0000-0002-3292-4799</orcidid><orcidid>https://orcid.org/0000-0003-4180-1923</orcidid><orcidid>https://orcid.org/0000000341801923</orcidid><orcidid>https://orcid.org/0000000232924799</orcidid><orcidid>https://orcid.org/0000000192825752</orcidid></search><sort><creationdate>20181115</creationdate><title>Bond valences and anharmonicity in vacancy-ordered double perovskite halides</title><author>Maughan, Annalise E ; Paecklar, Arnold A ; Neilson, James R</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c344t-43495c88f4100b0935d2c9fa0a7b174727aa6ff66e002bfd972860798877d7363</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2018</creationdate><topic>Anharmonicity</topic><topic>Asymmetry</topic><topic>Cesium ions</topic><topic>Computer simulation</topic><topic>Displacements (lattice)</topic><topic>Distribution functions</topic><topic>Electronic properties</topic><topic>Halides</topic><topic>Lattice vacancies</topic><topic>MATERIALS SCIENCE</topic><topic>Optical properties</topic><topic>Perovskite structure</topic><topic>Perovskites</topic><topic>Semiconductors</topic><topic>Tellurium</topic><topic>Temperature dependence</topic><topic>X-ray diffraction</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Maughan, Annalise E</creatorcontrib><creatorcontrib>Paecklar, Arnold A</creatorcontrib><creatorcontrib>Neilson, James R</creatorcontrib><creatorcontrib>Colorado State Univ., Fort Collins, CO (United States)</creatorcontrib><collection>CrossRef</collection><collection>Electronics & Communications Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>Technology Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>OSTI.GOV - Hybrid</collection><collection>OSTI.GOV</collection><jtitle>Journal of materials chemistry. C, Materials for optical and electronic devices</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Maughan, Annalise E</au><au>Paecklar, Arnold A</au><au>Neilson, James R</au><aucorp>Colorado State Univ., Fort Collins, CO (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Bond valences and anharmonicity in vacancy-ordered double perovskite halides</atitle><jtitle>Journal of materials chemistry. C, Materials for optical and electronic devices</jtitle><date>2018-11-15</date><risdate>2018</risdate><volume>6</volume><issue>44</issue><spage>1295</spage><epage>1214</epage><pages>1295-1214</pages><issn>2050-7526</issn><eissn>2050-7534</eissn><abstract>Anharmonic lattice dynamics are intimately linked with optical and electronic properties in perovskite halide semiconductors. Vacancy-ordered double perovskites are a subset of the perovskite halide family containing isolated octahedral units. The absence of polyhedral connectivity engenders the vacancy-ordered double perovskites with additional degrees of dynamic freedom, which presents an ideal structural framework to study dynamic-property relationships in perovskite halide semiconductors. In the present study, we examine the structure and bonding origins of anharmonicity in the vacancy-ordered double perovskites Cs
2
Sn
1−
x
Te
x
I
6
. While X-ray diffraction indicates that all members adopt the cubic vacancy-ordered double perovskite structure, the local coordination environment probed by X-ray pair distribution function (XPDF) analysis reveals asymmetry of the Cs-I/I-I pair correlation that smoothly decreases with increasing tellurium content. Temperature-dependent neutron total scattering suggests that this asymmetry in the PDF occurs due to anharmonic lattice dynamics arising from octahedral tilting and Cs
+
displacements, as supported by Reverse Monte Carlo simulations of the Cs
2
SnI
6
and Cs
2
TeI
6
end members. We further correlate the trends in asymmetry and anharmonicity with the bond valence sum of the Cs
+
ion, and find that the anharmonicity vanishes when the bonding preferences of the Cs
+
are satisfied by the size of the cuboctahedral void. This study presents a simple and effective approach for understanding the origin of anharmonicity in vacancy-ordered double perovskite materials.
Anharmonicity is observed in vacancy-ordered double perovskites when the A-site cation is not optimally coordinated by the octahedral framework.</abstract><cop>Cambridge</cop><pub>Royal Society of Chemistry</pub><doi>10.1039/c8tc03527j</doi><tpages>1</tpages><orcidid>https://orcid.org/0000-0001-9282-5752</orcidid><orcidid>https://orcid.org/0000-0002-3292-4799</orcidid><orcidid>https://orcid.org/0000-0003-4180-1923</orcidid><orcidid>https://orcid.org/0000000341801923</orcidid><orcidid>https://orcid.org/0000000232924799</orcidid><orcidid>https://orcid.org/0000000192825752</orcidid><oa>free_for_read</oa></addata></record> |
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| source | Royal Society Of Chemistry Journals 2008- |
| subjects | Anharmonicity Asymmetry Cesium ions Computer simulation Displacements (lattice) Distribution functions Electronic properties Halides Lattice vacancies MATERIALS SCIENCE Optical properties Perovskite structure Perovskites Semiconductors Tellurium Temperature dependence X-ray diffraction |
| title | Bond valences and anharmonicity in vacancy-ordered double perovskite halides |
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