Design Principles for Trap-Free CsPbX3 Nanocrystals: Enumerating and Eliminating Surface Halide Vacancies with Softer Lewis Bases

Nenon, David P.; Pressler, Kimo; Kang, Jun; Koscher, Brent A.; Olshansky, Jacob H.; Osowiecki, Wojciech T.; Koc, Matthew A.; Wang, Lin-Wang; Alivisatos, A. Paul

doi:10.1021/jacs.8b11035

Title: Design Principles for Trap-Free CsPbX₃ Nanocrystals: Enumerating and Eliminating Surface Halide Vacancies with Softer Lewis Bases

Journal Article · Sun Dec 02 00:00:00 EST 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.8b11035· OSTI ID:1542345

^[1]; Pressler, Kimo ^[2]; Kang, Jun ^[3];

^[1];

^[1]; Wang, Lin-Wang ^[3];

^[4]

Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States). Kavli Energy NanoScience Inst.; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

We introduce a general surface passivation mechanism for cesium lead halide perovskite materials (CsPbX₃, X = Cl, Br, I) that is supported by a combined experimental and theoretical study of the nanocrystal surface chemistry. A variety of spectroscopic methods are employed together with ab initio calculations to identify surface halide vacancies as the predominant source of charge trapping. The number of surface traps per nanocrystal is quantified by ¹H NMR spectroscopy, and that number is consistent with a simple trapping model in which surface halide vacancies create deleterious under-coordinated lead atoms. These halide vacancies exhibit trapping behavior that differs among CsPbCl₃, CsPbBr₃, and CsPbI₃. Ab initio calculations suggest that introduction of anionic X-type ligands can produce trap-free band gaps by altering the energetics of lead-based defect levels. General rules for selecting effective passivating ligand pairs are introduced by considering established principles of coordination chemistry. Introducing softer, anionic, X-type Lewis bases that target under-coordinated lead atoms results in absolute quantum yields approaching unity and monoexponential luminescence decay kinetics, thereby indicating full trap passivation. This work provides a systematic framework for preparing highly luminescent CsPbX₃ nanocrystals with variable compositions and dimensionalities, thereby improving the fundamental understanding of these materials and informing future synthetic and post-synthetic efforts toward trap-free CsPbX₃ nanocrystals.

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Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1542345

Journal Information:: Journal of the American Chemical Society, Vol. 140, Issue 50; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 334 works

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