Mechanistic Exploration of Dodecanethiol-Treated Colloidal CsPbBr3 Nanocrystals with Photoluminescence Quantum Yields Reaching Near 100%

Uddin, Md Aslam; Mobley, Justin K.; Masud, Abdullah A.; Liu, Tuo; Calabro, Rosemary L.; Kim, Doo-Young; Richards, Christopher I.; Graham, Kenneth R.

doi:10.1021/acs.jpcc.9b05612

Mechanistic Exploration of Dodecanethiol-Treated Colloidal CsPbBr₃ Nanocrystals with Photoluminescence Quantum Yields Reaching Near 100%

Journal Article · Fri Jun 21 00:00:00 EDT 2019 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.9b05612· OSTI ID:1594889

Uddin, Md Aslam ^[1]; ^[2]; Masud, Abdullah A. ^[2]; Liu, Tuo ^[2]; Calabro, Rosemary L. ^[2]; ^[2]; ^[2]; ^[2]

Univ. of Kentucky, Lexington, KY (United States); University of Kentucky Research Foundation
Univ. of Kentucky, Lexington, KY (United States)

Metal halide perovskite nanocrystals (NCs) are attractive materials for optoelectronics. However, further improvements in stability, reproducibility, and photoluminescence quantum yield (Φ_PL) are essential for enabling future applications. Inadequate surface passivation is a major cause of instability, irreproducibility, and less than unity Φ_PL. Herein, we probe the influence of multiple ligand binding groups on the colloidal stability and Φ_PL of CsPbBr₃ nanocrystals (NCs). Here, we find that post-synthetic treatment with dodecanethiol reproducibly yields highly stable NCs with near-unity Φ_PL for a range of synthetic conditions and initial Φ_PL of the as-synthesized NCs. A mechanistic investigation shows that thiol addition leads to thioether formation via the thiol–ene reaction with octadecene, oleic acid, and oleylamine. Both thiolates and thioethers are suspected to bind to undercoordinated Pb atoms on the NC surfaces, and this surface binding can be rapidly accelerated through exposure to blue or UV light. Furthermore, we show that metallic Pb nanoparticles appear in many batches of synthesized CsPbBr₃ NCs and that dodecanethiol addition eliminates these metallic Pb particles.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Kentucky, Lexington, KY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); Kentucky Science & Engineering Foundation, Lexington, KY (United States)

Grant/Contract Number:: SC0018208

OSTI ID:: 1594889

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 29 Vol. 123; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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