Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites
Femtosecond resolution electron scattering techniques are applied to resolve the first atomic-scale steps following absorption of a photon in the prototypical hybrid perovskite methylammonium lead iodide. Following above-gap photoexcitation, we directly resolve the transfer of energy from hot carrie...
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| Veröffentlicht in: | Science advances 2017-07, Vol.3 (7), p.e1602388-e1602388 |
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| creator | Wu, Xiaoxi Tan, Liang Z Shen, Xiaozhe Hu, Te Miyata, Kiyoshi Trinh, M Tuan Li, Renkai Coffee, Ryan Liu, Shi Egger, David A Makasyuk, Igor Zheng, Qiang Fry, Alan Robinson, Joseph S Smith, Matthew D Guzelturk, Burak Karunadasa, Hemamala I Wang, Xijie Zhu, Xiaoyang Kronik, Leeor Rappe, Andrew M Lindenberg, Aaron M |
| description | Femtosecond resolution electron scattering techniques are applied to resolve the first atomic-scale steps following absorption of a photon in the prototypical hybrid perovskite methylammonium lead iodide. Following above-gap photoexcitation, we directly resolve the transfer of energy from hot carriers to the lattice by recording changes in the mean square atomic displacements on 10-ps time scales. Measurements of the time-dependent pair distribution function show an unexpected broadening of the iodine-iodine correlation function while preserving the Pb-I distance. This indicates the formation of a rotationally disordered halide octahedral structure developing on picosecond time scales. This work shows the important role of light-induced structural deformations within the inorganic sublattice in elucidating the unique optoelectronic functionality exhibited by hybrid perovskites and provides new understanding of hot carrier-lattice interactions, which fundamentally determine solar cell efficiencies. |
| doi_str_mv | 10.1126/sciadv.1602388 |
| format | Article |
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Following above-gap photoexcitation, we directly resolve the transfer of energy from hot carriers to the lattice by recording changes in the mean square atomic displacements on 10-ps time scales. Measurements of the time-dependent pair distribution function show an unexpected broadening of the iodine-iodine correlation function while preserving the Pb-I distance. This indicates the formation of a rotationally disordered halide octahedral structure developing on picosecond time scales. This work shows the important role of light-induced structural deformations within the inorganic sublattice in elucidating the unique optoelectronic functionality exhibited by hybrid perovskites and provides new understanding of hot carrier-lattice interactions, which fundamentally determine solar cell efficiencies.</description><identifier>ISSN: 2375-2548</identifier><identifier>EISSN: 2375-2548</identifier><identifier>DOI: 10.1126/sciadv.1602388</identifier><identifier>PMID: 28782016</identifier><language>eng</language><publisher>United States: AAAS</publisher><subject>INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY ; MATERIALS SCIENCE ; Physical Sciences ; SciAdv r-articles ; Solar Energy</subject><ispartof>Science advances, 2017-07, Vol.3 (7), p.e1602388-e1602388</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. 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Tan, Liang Z ; Shen, Xiaozhe ; Hu, Te ; Miyata, Kiyoshi ; Trinh, M Tuan ; Li, Renkai ; Coffee, Ryan ; Liu, Shi ; Egger, David A ; Makasyuk, Igor ; Zheng, Qiang ; Fry, Alan ; Robinson, Joseph S ; Smith, Matthew D ; Guzelturk, Burak ; Karunadasa, Hemamala I ; Wang, Xijie ; Zhu, Xiaoyang ; Kronik, Leeor ; Rappe, Andrew M ; Lindenberg, Aaron M</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c483t-7ae5ef01801ca38751d25ab47799d159656b5b4bd0bd72d68a38bf11e7e36553</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>Physical Sciences</topic><topic>SciAdv r-articles</topic><topic>Solar Energy</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Wu, Xiaoxi</creatorcontrib><creatorcontrib>Tan, Liang Z</creatorcontrib><creatorcontrib>Shen, Xiaozhe</creatorcontrib><creatorcontrib>Hu, Te</creatorcontrib><creatorcontrib>Miyata, Kiyoshi</creatorcontrib><creatorcontrib>Trinh, M Tuan</creatorcontrib><creatorcontrib>Li, Renkai</creatorcontrib><creatorcontrib>Coffee, Ryan</creatorcontrib><creatorcontrib>Liu, Shi</creatorcontrib><creatorcontrib>Egger, David A</creatorcontrib><creatorcontrib>Makasyuk, Igor</creatorcontrib><creatorcontrib>Zheng, Qiang</creatorcontrib><creatorcontrib>Fry, Alan</creatorcontrib><creatorcontrib>Robinson, Joseph S</creatorcontrib><creatorcontrib>Smith, Matthew D</creatorcontrib><creatorcontrib>Guzelturk, Burak</creatorcontrib><creatorcontrib>Karunadasa, Hemamala I</creatorcontrib><creatorcontrib>Wang, Xijie</creatorcontrib><creatorcontrib>Zhu, Xiaoyang</creatorcontrib><creatorcontrib>Kronik, Leeor</creatorcontrib><creatorcontrib>Rappe, Andrew M</creatorcontrib><creatorcontrib>Lindenberg, Aaron M</creatorcontrib><creatorcontrib>SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (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>Wu, Xiaoxi</au><au>Tan, Liang Z</au><au>Shen, Xiaozhe</au><au>Hu, Te</au><au>Miyata, Kiyoshi</au><au>Trinh, M Tuan</au><au>Li, Renkai</au><au>Coffee, Ryan</au><au>Liu, Shi</au><au>Egger, David A</au><au>Makasyuk, Igor</au><au>Zheng, Qiang</au><au>Fry, Alan</au><au>Robinson, Joseph S</au><au>Smith, Matthew D</au><au>Guzelturk, Burak</au><au>Karunadasa, Hemamala I</au><au>Wang, Xijie</au><au>Zhu, Xiaoyang</au><au>Kronik, Leeor</au><au>Rappe, Andrew M</au><au>Lindenberg, Aaron M</au><aucorp>SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites</atitle><jtitle>Science advances</jtitle><addtitle>Sci Adv</addtitle><date>2017-07-01</date><risdate>2017</risdate><volume>3</volume><issue>7</issue><spage>e1602388</spage><epage>e1602388</epage><pages>e1602388-e1602388</pages><issn>2375-2548</issn><eissn>2375-2548</eissn><abstract>Femtosecond resolution electron scattering techniques are applied to resolve the first atomic-scale steps following absorption of a photon in the prototypical hybrid perovskite methylammonium lead iodide. Following above-gap photoexcitation, we directly resolve the transfer of energy from hot carriers to the lattice by recording changes in the mean square atomic displacements on 10-ps time scales. Measurements of the time-dependent pair distribution function show an unexpected broadening of the iodine-iodine correlation function while preserving the Pb-I distance. This indicates the formation of a rotationally disordered halide octahedral structure developing on picosecond time scales. This work shows the important role of light-induced structural deformations within the inorganic sublattice in elucidating the unique optoelectronic functionality exhibited by hybrid perovskites and provides new understanding of hot carrier-lattice interactions, which fundamentally determine solar cell efficiencies.</abstract><cop>United States</cop><pub>AAAS</pub><pmid>28782016</pmid><doi>10.1126/sciadv.1602388</doi><orcidid>https://orcid.org/0000-0002-2619-8823</orcidid><orcidid>https://orcid.org/0000-0002-2090-8484</orcidid><orcidid>https://orcid.org/0000-0003-3233-7161</orcidid><orcidid>https://orcid.org/0000-0001-6748-1337</orcidid><orcidid>https://orcid.org/0000000220908484</orcidid><orcidid>https://orcid.org/0000000332337161</orcidid><orcidid>https://orcid.org/0000000226198823</orcidid><orcidid>https://orcid.org/0000000167481337</orcidid><oa>free_for_read</oa></addata></record> |
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| subjects | INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY MATERIALS SCIENCE Physical Sciences SciAdv r-articles Solar Energy |
| title | Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites |
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