Engineering Interfacial Charge Transfer in CsPbBr3 Perovskite Nanocrystals by Heterovalent Doping

Handle URI:
http://hdl.handle.net/10754/622783
Title:
Engineering Interfacial Charge Transfer in CsPbBr3 Perovskite Nanocrystals by Heterovalent Doping
Authors:
Begum, Raihana; Parida, Manas R.; Abdelhady, Ahmed L.; Banavoth, Murali ( 0000-0002-7806-2274 ) ; AlYami, Noktan; Ahmed, Ghada H. ( 0000-0003-1709-8692 ) ; Hedhili, Mohamed N. ( 0000-0002-3624-036X ) ; Bakr, Osman M. ( 0000-0002-3428-1002 ) ; Mohammed, Omar F. ( 0000-0001-8500-1130 )
Abstract:
Since compelling device efficiencies of perovskite solar cells have been achieved, investigative efforts have turned to understand other key challenges in these systems, such as engineering interfacial energy-level alignment and charge transfer (CT). However, these types of studies on perovskite thin-film devices are impeded by the morphological and compositional heterogeneity of the films and their ill-defined surfaces. Here, we use well-defined ligand-protected perovskite nanocrystals (NCs) as model systems to elucidate the role of heterovalent doping on charge-carrier dynamics and energy level alignment at the interface of perovskite NCs with molecular acceptors. More specifically, we develop an in situ doping approach for colloidal CsPbBr3 perovskite NCs with heterovalent Bi3+ ions by hot injection to precisely tune their band structure and excited-state dynamics. This synthetic method allowed us to map the impact of doping on CT from the NCs to different molecular acceptors. Using time-resolved spectroscopy with broadband capability, we clearly demonstrate that CT at the interface of NCs can be tuned and promoted by metal ion doping. We found that doping increases the energy difference between states of the molecular acceptor and the donor moieties, subsequently facilitating the interfacial CT process. This work highlights the key variable components not only for promoting interfacial CT in perovskites, but also for establishing a higher degree of precision and control over the surface and the interface of perovskite molecular acceptors.
KAUST Department:
Imaging and Characterization Core Lab; Physical Sciences and Engineering (PSE) Division
Citation:
Begum R, Parida MR, Abdelhady AL, Murali B, Alyami NM, et al. (2017) Engineering Interfacial Charge Transfer in CsPbBr3 Perovskite Nanocrystals by Heterovalent Doping. Journal of the American Chemical Society 139: 731–737. Available: http://dx.doi.org/10.1021/jacs.6b09575.
Publisher:
American Chemical Society (ACS)
Journal:
Journal of the American Chemical Society
Issue Date:
17-Dec-2016
DOI:
10.1021/jacs.6b09575
Type:
Article
ISSN:
0002-7863; 1520-5126
Sponsors:
This work was supported by King Abdullah University of Science and Technology (KAUST). Also, part of this work was supported by a Saudi Arabia Basic Industries Corporation (SABIC) Grant RGC/3/2470-01.
Additional Links:
http://pubs.acs.org/doi/full/10.1021/jacs.6b09575
Appears in Collections:
Articles; Advanced Nanofabrication, Imaging and Characterization Core Lab; Physical Sciences and Engineering (PSE) Division

Full metadata record

DC FieldValue Language
dc.contributor.authorBegum, Raihanaen
dc.contributor.authorParida, Manas R.en
dc.contributor.authorAbdelhady, Ahmed L.en
dc.contributor.authorBanavoth, Muralien
dc.contributor.authorAlYami, Noktanen
dc.contributor.authorAhmed, Ghada H.en
dc.contributor.authorHedhili, Mohamed N.en
dc.contributor.authorBakr, Osman M.en
dc.contributor.authorMohammed, Omar F.en
dc.date.accessioned2017-01-29T13:51:39Z-
dc.date.available2017-01-29T13:51:39Z-
dc.date.issued2016-12-17en
dc.identifier.citationBegum R, Parida MR, Abdelhady AL, Murali B, Alyami NM, et al. (2017) Engineering Interfacial Charge Transfer in CsPbBr3 Perovskite Nanocrystals by Heterovalent Doping. Journal of the American Chemical Society 139: 731–737. Available: http://dx.doi.org/10.1021/jacs.6b09575.en
dc.identifier.issn0002-7863en
dc.identifier.issn1520-5126en
dc.identifier.doi10.1021/jacs.6b09575en
dc.identifier.urihttp://hdl.handle.net/10754/622783-
dc.description.abstractSince compelling device efficiencies of perovskite solar cells have been achieved, investigative efforts have turned to understand other key challenges in these systems, such as engineering interfacial energy-level alignment and charge transfer (CT). However, these types of studies on perovskite thin-film devices are impeded by the morphological and compositional heterogeneity of the films and their ill-defined surfaces. Here, we use well-defined ligand-protected perovskite nanocrystals (NCs) as model systems to elucidate the role of heterovalent doping on charge-carrier dynamics and energy level alignment at the interface of perovskite NCs with molecular acceptors. More specifically, we develop an in situ doping approach for colloidal CsPbBr3 perovskite NCs with heterovalent Bi3+ ions by hot injection to precisely tune their band structure and excited-state dynamics. This synthetic method allowed us to map the impact of doping on CT from the NCs to different molecular acceptors. Using time-resolved spectroscopy with broadband capability, we clearly demonstrate that CT at the interface of NCs can be tuned and promoted by metal ion doping. We found that doping increases the energy difference between states of the molecular acceptor and the donor moieties, subsequently facilitating the interfacial CT process. This work highlights the key variable components not only for promoting interfacial CT in perovskites, but also for establishing a higher degree of precision and control over the surface and the interface of perovskite molecular acceptors.en
dc.description.sponsorshipThis work was supported by King Abdullah University of Science and Technology (KAUST). Also, part of this work was supported by a Saudi Arabia Basic Industries Corporation (SABIC) Grant RGC/3/2470-01.en
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.urlhttp://pubs.acs.org/doi/full/10.1021/jacs.6b09575en
dc.titleEngineering Interfacial Charge Transfer in CsPbBr3 Perovskite Nanocrystals by Heterovalent Dopingen
dc.typeArticleen
dc.contributor.departmentImaging and Characterization Core Laben
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.identifier.journalJournal of the American Chemical Societyen
kaust.authorBegum, Raihanaen
kaust.authorParida, Manas R.en
kaust.authorAbdelhady, Ahmed L.en
kaust.authorBanavoth, Muralien
kaust.authorAlYami, Noktanen
kaust.authorAhmed, Ghada H.en
kaust.authorHedhili, Mohamed N.en
kaust.authorBakr, Osman M.en
kaust.authorMohammed, Omar F.en
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