CsPbBr3 nanocrystal films: Deviations from bulk vibrational and optoelectronic properties

Metal‐halide perovskites (MHP) are highly promising semiconductors for light‐emitting and photovoltaic applications. The colloidal synthesis of nanocrystals (NCs) is an effective approach for obtaining nearly defect‐free MHP that can be processed into inks for low‐cost, high‐performance device fabri...

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Detalhes bibliográficos
Principais autores: Motti, SG, Krieg, F, Ramadan, AJ, Patel, JB, Snaith, HJ, Kovalenko, MV, Johnston, MB, Herz, LM
Formato: Journal article
Idioma:English
Publicado em: Wiley 2020
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author Motti, SG
Krieg, F
Ramadan, AJ
Patel, JB
Snaith, HJ
Kovalenko, MV
Johnston, MB
Herz, LM
author_facet Motti, SG
Krieg, F
Ramadan, AJ
Patel, JB
Snaith, HJ
Kovalenko, MV
Johnston, MB
Herz, LM
author_sort Motti, SG
collection OXFORD
description Metal‐halide perovskites (MHP) are highly promising semiconductors for light‐emitting and photovoltaic applications. The colloidal synthesis of nanocrystals (NCs) is an effective approach for obtaining nearly defect‐free MHP that can be processed into inks for low‐cost, high‐performance device fabrication. However, disentangling the effects of surface ligands, morphology, and boundaries on charge‐carrier transport in thin films fabricated with these high‐quality NCs is inherently difficult. To overcome this fundamental challenge, terahertz (THz) spectroscopy is employed to optically probe the photoconductivity of CsPbBr3 NC films. The vibrational and optoelectronic properties of the NCs are compared with those of the corresponding bulk polycrystalline perovskite and significant deviations are found. Charge‐carrier mobilities and recombination rates are demonstrated to vary significantly with the NC size. Such dependences derive from the localized nature of charge carriers within NCs, with local mobilities dominating over interparticle transport. It is further shown that the colloidally synthesized NCs have distinct vibrational properties with respect to the bulk perovskite, exhibiting blue‐shifted optical phonon modes with enhanced THz absorption strength that also manifest as strong modulations in the THz photoconductivity spectra. Such fundamental insights into NC versus bulk properties will guide the optimization of nanocrystalline perovskite thin films for optoelectronic applications.
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spelling oxford-uuid:c1917c0e-fd3a-48df-86f5-a25f7f8ec2b82022-03-27T06:02:25ZCsPbBr3 nanocrystal films: Deviations from bulk vibrational and optoelectronic propertiesJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:c1917c0e-fd3a-48df-86f5-a25f7f8ec2b8EnglishSymplectic ElementsWiley2020Motti, SGKrieg, FRamadan, AJPatel, JBSnaith, HJKovalenko, MVJohnston, MBHerz, LMMetal‐halide perovskites (MHP) are highly promising semiconductors for light‐emitting and photovoltaic applications. The colloidal synthesis of nanocrystals (NCs) is an effective approach for obtaining nearly defect‐free MHP that can be processed into inks for low‐cost, high‐performance device fabrication. However, disentangling the effects of surface ligands, morphology, and boundaries on charge‐carrier transport in thin films fabricated with these high‐quality NCs is inherently difficult. To overcome this fundamental challenge, terahertz (THz) spectroscopy is employed to optically probe the photoconductivity of CsPbBr3 NC films. The vibrational and optoelectronic properties of the NCs are compared with those of the corresponding bulk polycrystalline perovskite and significant deviations are found. Charge‐carrier mobilities and recombination rates are demonstrated to vary significantly with the NC size. Such dependences derive from the localized nature of charge carriers within NCs, with local mobilities dominating over interparticle transport. It is further shown that the colloidally synthesized NCs have distinct vibrational properties with respect to the bulk perovskite, exhibiting blue‐shifted optical phonon modes with enhanced THz absorption strength that also manifest as strong modulations in the THz photoconductivity spectra. Such fundamental insights into NC versus bulk properties will guide the optimization of nanocrystalline perovskite thin films for optoelectronic applications.
spellingShingle Motti, SG
Krieg, F
Ramadan, AJ
Patel, JB
Snaith, HJ
Kovalenko, MV
Johnston, MB
Herz, LM
CsPbBr3 nanocrystal films: Deviations from bulk vibrational and optoelectronic properties
title CsPbBr3 nanocrystal films: Deviations from bulk vibrational and optoelectronic properties
title_full CsPbBr3 nanocrystal films: Deviations from bulk vibrational and optoelectronic properties
title_fullStr CsPbBr3 nanocrystal films: Deviations from bulk vibrational and optoelectronic properties
title_full_unstemmed CsPbBr3 nanocrystal films: Deviations from bulk vibrational and optoelectronic properties
title_short CsPbBr3 nanocrystal films: Deviations from bulk vibrational and optoelectronic properties
title_sort cspbbr3 nanocrystal films deviations from bulk vibrational and optoelectronic properties
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