Terahertz Emission from Hybrid Perovskites Driven by Ultrafast Charge Separation and Strong Electron-Phonon Coupling

© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 30(2018), 11 vom: 07. März
1. Verfasser: Guzelturk, Burak (VerfasserIn)
Weitere Verfasser: Belisle, Rebecca A, Smith, Matthew D, Bruening, Karsten, Prasanna, Rohit, Yuan, Yakun, Gopalan, Venkatraman, Tassone, Christopher J, Karunadasa, Hemamala I, McGehee, Michael D, Lindenberg, Aaron M
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2018
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article MAPbI3 THz emission carrier-lattice coupling charge separation hybrid organic-inorganic perovskites ultrafast structural dynamics
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520 |a Unusual photophysical properties of organic-inorganic hybrid perovskites have not only enabled exceptional performance in optoelectronic devices, but also led to debates on the nature of charge carriers in these materials. This study makes the first observation of intense terahertz (THz) emission from the hybrid perovskite methylammonium lead iodide (CH3 NH3 PbI3 ) following photoexcitation, enabling an ultrafast probe of charge separation, hot-carrier transport, and carrier-lattice coupling under 1-sun-equivalent illumination conditions. Using this approach, the initial charge separation/transport in the hybrid perovskites is shown to be driven by diffusion and not by surface fields or intrinsic ferroelectricity. Diffusivities of the hot and band-edge carriers along the surface normal direction are calculated by analyzing the emitted THz transients, with direct implications for hot-carrier device applications. Furthermore, photogenerated carriers are found to drive coherent terahertz-frequency lattice distortions, associated with reorganizations of the lead-iodide octahedra as well as coupled vibrations of the organic and inorganic sublattices. This strong and coherent carrier-lattice coupling is resolved on femtosecond timescales and found to be important both for resonant and far-above-gap photoexcitation. This study indicates that ultrafast lattice distortions play a key role in the initial processes associated with charge transport 
650 4 |a Journal Article 
650 4 |a MAPbI3 
650 4 |a THz emission 
650 4 |a carrier-lattice coupling 
650 4 |a charge separation 
650 4 |a hybrid organic-inorganic perovskites 
650 4 |a ultrafast structural dynamics 
700 1 |a Belisle, Rebecca A  |e verfasserin  |4 aut 
700 1 |a Smith, Matthew D  |e verfasserin  |4 aut 
700 1 |a Bruening, Karsten  |e verfasserin  |4 aut 
700 1 |a Prasanna, Rohit  |e verfasserin  |4 aut 
700 1 |a Yuan, Yakun  |e verfasserin  |4 aut 
700 1 |a Gopalan, Venkatraman  |e verfasserin  |4 aut 
700 1 |a Tassone, Christopher J  |e verfasserin  |4 aut 
700 1 |a Karunadasa, Hemamala I  |e verfasserin  |4 aut 
700 1 |a McGehee, Michael D  |e verfasserin  |4 aut 
700 1 |a Lindenberg, Aaron M  |e verfasserin  |4 aut 
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773 1 8 |g volume:30  |g year:2018  |g number:11  |g day:07  |g month:03 
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