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On the Mechanism for the Extremely Efficient Sensitization of Yb3+ Luminescence in CsPbCl3 Nanocrystals
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Theoretical Chemistry and Biology.
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Theoretical Chemistry and Biology.ORCID iD: 0000-0002-3282-0711
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Theoretical Chemistry and Biology.ORCID iD: 0000-0002-1780-7746
Harbin Inst Technol, Sch Chem Engn & Technol, Harbin 150001, Heilongjiang, Peoples R China.
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2019 (English)In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 10, no 3, p. 487-492Article in journal (Refereed) Published
Abstract [en]

Rare earth ion (RE3+)-doped inorganic CsPbX3 (X = Cl or Cl/Br) nanocrystals have been presented as promising materials for applications in solar-energy conversion technology. An extremely efficient sensitization of Yb3+ luminescence in CsPbCl3 nanoparticles (NCs) was very recently demonstrated where quantum cutting is responsible for the performance of photoluminescence quantum yields over 100% (T. J. Milstein, et al. Nano Letters 2018, 18, 3792). In the present work, based on the cubic phase of inorganic perovskite, we seek to obtain atom-level insight into the basic mechanisms behind these observations in order to boost the further development of RE3+-doped CsPbX3 NCs for optoelectronics. In our calculations of cubic crystal structure, we do not find any energy level formed in the middle of the band gap, which disfavors a mechanism of stepwise energy transfer from the perovskite host to two Yb3+ ions. Our work indicates that the configuration with "right-angle" Yb3+-V-Pb-Yb3+ couple is most likely to form in Yb3+-doped CsPbCl3. Associated with this "right-angle" couple, the "right-angle" Pb atom with trapped excited states would localize the photogenerated electrons and act as the energy donor in a quantum cutting process, which achieves simultaneous sensitization of two neighboring Yb3+ ions.

Place, publisher, year, edition, pages
2019. Vol. 10, no 3, p. 487-492
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Nano Technology
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URN: urn:nbn:se:kth:diva-246213DOI: 10.1021/acs.jpclett.8b03406ISI: 000458704800026PubMedID: 30642182Scopus ID: 2-s2.0-85061130625OAI: oai:DiVA.org:kth-246213DiVA, id: diva2:1296689
Note

QC 20190318

Available from: 2019-03-16 Created: 2019-03-16 Last updated: 2020-03-09Bibliographically approved

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Li, XiyuDuan, SaiLiu, HaichunLuo, YiÅgren, Hans

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