Large polarons in lead halide perovskites
Lead halide perovskites show marked defect tolerance responsible for their excellent optoelectronic properties. These properties might be explained by the formation of large polarons, but how they are formed and whether organic cations are essential remain open questions. We provide a direct time do...
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| Veröffentlicht in: | Science advances 2017-08, Vol.3 (8), p.e1701217-e1701217 |
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| creator | Miyata, Kiyoshi Meggiolaro, Daniele Trinh, M Tuan Joshi, Prakriti P Mosconi, Edoardo Jones, Skyler C De Angelis, Filippo Zhu, X-Y |
| description | Lead halide perovskites show marked defect tolerance responsible for their excellent optoelectronic properties. These properties might be explained by the formation of large polarons, but how they are formed and whether organic cations are essential remain open questions. We provide a direct time domain view of large polaron formation in single-crystal lead bromide perovskites CH
NH
PbBr
and CsPbBr
. We found that large polaron forms predominantly from the deformation of the PbBr
frameworks, irrespective of the cation type. The difference lies in the polaron formation time, which, in CH
NH
PbBr
(0.3 ps), is less than half of that in CsPbBr
(0.7 ps). First-principles calculations confirm large polaron formation, identify the Pb-Br-Pb deformation modes as responsible, and explain quantitatively the rate difference between CH
NH
PbBr
and CsPbBr
. The findings reveal the general advantage of the soft [PbX
]
sublattice in charge carrier protection and suggest that there is likely no mechanistic limitations in using all-inorganic or mixed-cation lead halide perovskites to overcome instability problems and to tune the balance between charge carrier protection and mobility. |
| doi_str_mv | 10.1126/sciadv.1701217 |
| format | Article |
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NH
PbBr
and CsPbBr
. We found that large polaron forms predominantly from the deformation of the PbBr
frameworks, irrespective of the cation type. The difference lies in the polaron formation time, which, in CH
NH
PbBr
(0.3 ps), is less than half of that in CsPbBr
(0.7 ps). First-principles calculations confirm large polaron formation, identify the Pb-Br-Pb deformation modes as responsible, and explain quantitatively the rate difference between CH
NH
PbBr
and CsPbBr
. The findings reveal the general advantage of the soft [PbX
]
sublattice in charge carrier protection and suggest that there is likely no mechanistic limitations in using all-inorganic or mixed-cation lead halide perovskites to overcome instability problems and to tune the balance between charge carrier protection and mobility.</description><identifier>ISSN: 2375-2548</identifier><identifier>EISSN: 2375-2548</identifier><identifier>DOI: 10.1126/sciadv.1701217</identifier><identifier>PMID: 28819647</identifier><language>eng</language><publisher>United States: AAAS</publisher><subject>INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY ; Materials Science ; SciAdv r-articles</subject><ispartof>Science advances, 2017-08, Vol.3 (8), p.e1701217-e1701217</ispartof><rights>Copyright © 2017 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC). 2017 The Authors</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c483t-b901e44e235c64f50b637bfb1d65a9e4ca0de42198af764bc4311b735bdf4c1c3</citedby><cites>FETCH-LOGICAL-c483t-b901e44e235c64f50b637bfb1d65a9e4ca0de42198af764bc4311b735bdf4c1c3</cites><orcidid>0000-0003-2061-4504 ; 0000-0001-6748-1337 ; 0000-0002-1609-6882 ; 0000-0002-2090-8484 ; 0000000167481337 ; 0000000216096882 ; 0000000220908484 ; 0000000320614504</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC5553817/pdf/$$EPDF$$P50$$Gpubmedcentral$$Hfree_for_read</linktopdf><linktohtml>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC5553817/$$EHTML$$P50$$Gpubmedcentral$$Hfree_for_read</linktohtml><link.rule.ids>230,314,723,776,780,860,881,27901,27902,53766,53768</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/28819647$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/servlets/purl/1536831$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Miyata, Kiyoshi</creatorcontrib><creatorcontrib>Meggiolaro, Daniele</creatorcontrib><creatorcontrib>Trinh, M Tuan</creatorcontrib><creatorcontrib>Joshi, Prakriti P</creatorcontrib><creatorcontrib>Mosconi, Edoardo</creatorcontrib><creatorcontrib>Jones, Skyler C</creatorcontrib><creatorcontrib>De Angelis, Filippo</creatorcontrib><creatorcontrib>Zhu, X-Y</creatorcontrib><creatorcontrib>Columbia Univ., New York, NY (United States)</creatorcontrib><creatorcontrib>Brookhaven National Laboratory (BNL), Upton, NY (United States)</creatorcontrib><title>Large polarons in lead halide perovskites</title><title>Science advances</title><addtitle>Sci Adv</addtitle><description>Lead halide perovskites show marked defect tolerance responsible for their excellent optoelectronic properties. These properties might be explained by the formation of large polarons, but how they are formed and whether organic cations are essential remain open questions. We provide a direct time domain view of large polaron formation in single-crystal lead bromide perovskites CH
NH
PbBr
and CsPbBr
. We found that large polaron forms predominantly from the deformation of the PbBr
frameworks, irrespective of the cation type. The difference lies in the polaron formation time, which, in CH
NH
PbBr
(0.3 ps), is less than half of that in CsPbBr
(0.7 ps). First-principles calculations confirm large polaron formation, identify the Pb-Br-Pb deformation modes as responsible, and explain quantitatively the rate difference between CH
NH
PbBr
and CsPbBr
. The findings reveal the general advantage of the soft [PbX
]
sublattice in charge carrier protection and suggest that there is likely no mechanistic limitations in using all-inorganic or mixed-cation lead halide perovskites to overcome instability problems and to tune the balance between charge carrier protection and mobility.</description><subject>INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY</subject><subject>Materials Science</subject><subject>SciAdv r-articles</subject><issn>2375-2548</issn><issn>2375-2548</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2017</creationdate><recordtype>article</recordtype><recordid>eNpVUU1PwzAMjRCIobErR1RxgkNH3Hy1FyQ08SVN4gLnKE3dLdA1I-km8e8p6pjGyZb9_Gy_R8gF0ClAJm-jdabaTkFRyEAdkbOMKZFmgufHB_mITGL8oJQCl1JAcUpGWZ5DIbk6IzdzExaYrH1jgm9j4tqkQVMlS9O4qq9j8Nv46TqM5-SkNk3EyS6Oyfvjw9vsOZ2_Pr3M7uep5Tnr0rKggJxjxoSVvBa0lEyVdQmVFKZAbg2tkGdQ5KZWkpeWM4BSMVFWNbdg2ZjcDbzrTbnCymLbBdPodXArE761N07_77RuqRd-q4UQLAfVE1wNBD52TvcadWiX1rct2k6DYDJn0IOud1uC_9pg7PTKRYtNY1r0m6ihYJQrBXnRQ6cD1AYfY8B6fwtQ_euDHnzQOx_6gcvDD_bwP9XZD5klhDU</recordid><startdate>20170801</startdate><enddate>20170801</enddate><creator>Miyata, Kiyoshi</creator><creator>Meggiolaro, Daniele</creator><creator>Trinh, M Tuan</creator><creator>Joshi, Prakriti P</creator><creator>Mosconi, Edoardo</creator><creator>Jones, Skyler C</creator><creator>De Angelis, Filippo</creator><creator>Zhu, X-Y</creator><general>AAAS</general><general>American Association for the Advancement of Science</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><scope>OIOZB</scope><scope>OTOTI</scope><scope>5PM</scope><orcidid>https://orcid.org/0000-0003-2061-4504</orcidid><orcidid>https://orcid.org/0000-0001-6748-1337</orcidid><orcidid>https://orcid.org/0000-0002-1609-6882</orcidid><orcidid>https://orcid.org/0000-0002-2090-8484</orcidid><orcidid>https://orcid.org/0000000167481337</orcidid><orcidid>https://orcid.org/0000000216096882</orcidid><orcidid>https://orcid.org/0000000220908484</orcidid><orcidid>https://orcid.org/0000000320614504</orcidid></search><sort><creationdate>20170801</creationdate><title>Large polarons in lead halide perovskites</title><author>Miyata, Kiyoshi ; Meggiolaro, Daniele ; Trinh, M Tuan ; Joshi, Prakriti P ; Mosconi, Edoardo ; Jones, Skyler C ; De Angelis, Filippo ; Zhu, X-Y</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c483t-b901e44e235c64f50b637bfb1d65a9e4ca0de42198af764bc4311b735bdf4c1c3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2017</creationdate><topic>INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY</topic><topic>Materials Science</topic><topic>SciAdv r-articles</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Miyata, Kiyoshi</creatorcontrib><creatorcontrib>Meggiolaro, Daniele</creatorcontrib><creatorcontrib>Trinh, M Tuan</creatorcontrib><creatorcontrib>Joshi, Prakriti P</creatorcontrib><creatorcontrib>Mosconi, Edoardo</creatorcontrib><creatorcontrib>Jones, Skyler C</creatorcontrib><creatorcontrib>De Angelis, Filippo</creatorcontrib><creatorcontrib>Zhu, X-Y</creatorcontrib><creatorcontrib>Columbia Univ., New York, NY (United States)</creatorcontrib><creatorcontrib>Brookhaven National Laboratory (BNL), Upton, NY (United States)</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><collection>OSTI.GOV - Hybrid</collection><collection>OSTI.GOV</collection><collection>PubMed Central (Full Participant titles)</collection><jtitle>Science advances</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Miyata, Kiyoshi</au><au>Meggiolaro, Daniele</au><au>Trinh, M Tuan</au><au>Joshi, Prakriti P</au><au>Mosconi, Edoardo</au><au>Jones, Skyler C</au><au>De Angelis, Filippo</au><au>Zhu, X-Y</au><aucorp>Columbia Univ., New York, NY (United States)</aucorp><aucorp>Brookhaven National Laboratory (BNL), Upton, NY (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Large polarons in lead halide perovskites</atitle><jtitle>Science advances</jtitle><addtitle>Sci Adv</addtitle><date>2017-08-01</date><risdate>2017</risdate><volume>3</volume><issue>8</issue><spage>e1701217</spage><epage>e1701217</epage><pages>e1701217-e1701217</pages><issn>2375-2548</issn><eissn>2375-2548</eissn><abstract>Lead halide perovskites show marked defect tolerance responsible for their excellent optoelectronic properties. These properties might be explained by the formation of large polarons, but how they are formed and whether organic cations are essential remain open questions. We provide a direct time domain view of large polaron formation in single-crystal lead bromide perovskites CH
NH
PbBr
and CsPbBr
. We found that large polaron forms predominantly from the deformation of the PbBr
frameworks, irrespective of the cation type. The difference lies in the polaron formation time, which, in CH
NH
PbBr
(0.3 ps), is less than half of that in CsPbBr
(0.7 ps). First-principles calculations confirm large polaron formation, identify the Pb-Br-Pb deformation modes as responsible, and explain quantitatively the rate difference between CH
NH
PbBr
and CsPbBr
. The findings reveal the general advantage of the soft [PbX
]
sublattice in charge carrier protection and suggest that there is likely no mechanistic limitations in using all-inorganic or mixed-cation lead halide perovskites to overcome instability problems and to tune the balance between charge carrier protection and mobility.</abstract><cop>United States</cop><pub>AAAS</pub><pmid>28819647</pmid><doi>10.1126/sciadv.1701217</doi><orcidid>https://orcid.org/0000-0003-2061-4504</orcidid><orcidid>https://orcid.org/0000-0001-6748-1337</orcidid><orcidid>https://orcid.org/0000-0002-1609-6882</orcidid><orcidid>https://orcid.org/0000-0002-2090-8484</orcidid><orcidid>https://orcid.org/0000000167481337</orcidid><orcidid>https://orcid.org/0000000216096882</orcidid><orcidid>https://orcid.org/0000000220908484</orcidid><orcidid>https://orcid.org/0000000320614504</orcidid><oa>free_for_read</oa></addata></record> |
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| subjects | INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Materials Science SciAdv r-articles |
| title | Large polarons in lead halide perovskites |
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