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Ultraefficient Singlet Oxygen Generation from Manganese-Doped Cesium Lead Chloride Perovskite Quantum Dots
Harbin Inst Technol, MIIT Key Lab Crit Mat Technol New Energy Convers, Sch Chem & Chem Engn, Harbin 150001, Peoples R China.;Harbin Inst Technol, Minist Educ, State Key Lab Urban Water Resource & Environm, Harbin 150001, Peoples R China.;Harbin Inst Technol, Minist Educ, Key Lab Microsyst & Microstruct, Harbin 150001, Peoples R China..ORCID iD: 0000-0001-8754-9909
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Theoretical Chemistry and Biology.
Harbin Inst Technol, MIIT Key Lab Crit Mat Technol New Energy Convers, Sch Chem & Chem Engn, Harbin 150001, Peoples R China.;Harbin Inst Technol, Minist Educ, State Key Lab Urban Water Resource & Environm, Harbin 150001, Peoples R China.;Harbin Inst Technol, Minist Educ, Key Lab Microsyst & Microstruct, Harbin 150001, Peoples R China..
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Theoretical Chemistry and Biology.ORCID iD: 0000-0002-1780-7746
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2020 (English)In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 14, no 10, p. 12596-12604Article in journal (Refereed) Published
Abstract [en]

Lead halide perovskites hold promise for photo-voltaics, lasers, and light-emitting diode (LED) applications, being known as light-harvesting or -emitting materials. Here we show that colloidal lead halide CsPbCl3 perovskite quantum dots (PQDs), when incorporating divalent manganese (Mn2+) ions, are able to produce spin-paired singlet oxygen molecules with over-unit quantum yield (similar to 1.08) in air conditions. Our mechanistic studies and atomic-level density functional theory calculations endorse an energy-migration-mediated quantum cutting process favoring multiple singlet oxygen generation (MSOG), in which one exciton-activated bulk Mn2+ ion (similar to 2.0 eV) inside the nanocrystal migrates its energy among the Mn2+ sublattice to two surface Mn2+ defect states (similar to 1.0 eV), followed by nonradiative energy transfers to two surrounding oxygen molecules. Moreover, superhydrophobicization of MSOG PQDs through silica-mediated polystyrene encapsulation prevents them from disintegrating in aqueous medium, enabling photodegradation of methyl orange at a rate even higher than that of the canonical titanium oxide photocatalyst. The observation of ultraefficient singlet oxygen generation in PQDs has implications for fields ranging from photodynamic therapy to photocatalytic applications.

Place, publisher, year, edition, pages
American Chemical Society (ACS) , 2020. Vol. 14, no 10, p. 12596-12604
Keywords [en]
perovskite quantum dots, singlet oxygen, pliotocatalysts, Mn2+ doping, quantum cutting
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-288450DOI: 10.1021/acsnano.0c04181ISI: 000586793400018PubMedID: 32790335Scopus ID: 2-s2.0-85094982929OAI: oai:DiVA.org:kth-288450DiVA, id: diva2:1524449
Note

QC 20210201

Available from: 2021-02-01 Created: 2021-02-01 Last updated: 2022-06-25Bibliographically approved

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Li, XiyuLiu, HaichunÅgren, Hans

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