Mixed Ligand Passivation as the Origin of Near-Unity Emission Quantum Yields in CsPbBr3 Nanocrystals

Ding, Yang; Zhang, Zhuoming; Toso, Stefano; Gushchina, Irina; Trepalin, Vadim; Shi, Kejia; Peng, Jeffrey W.; Kuno, Masaru

doi:10.1021/jacs.2c13527

Mixed Ligand Passivation as the Origin of Near-Unity Emission Quantum Yields in CsPbBr₃ Nanocrystals

Journal Article · Mon Mar 06 23:00:00 EST 2023 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.2c13527· OSTI ID:2338293

Ding, Yang ^[1]; Zhang, Zhuoming ^[2]; ^[3]; ^[2]; Trepalin, Vadim ^[2]; Shi, Kejia ^[2]; ^[2]; ^[2]

University of Notre Dame, IN (United States); University of Notre Dame
University of Notre Dame, IN (United States)
University of Notre Dame, IN (United States); Instituto Italiano di Tecnologia, Genova (Italy)

Key features of syntheses, involving the quaternary ammonium passivation of CsPbBr₃ nanocrystals (NCs), include stable, reproducible and large (often near-unity) emission quantum yields (QYs). The archetypical example involves didodecyl dimethyl ammonium (DDDMA⁺) passivated CsPbBr₃ NCs where robust QYs stem from interactions between DDDMA⁺ and NC surfaces. Despite widespread adoption of this synthesis, specific ligand-NC surface interactions responsible for large DDDMA⁺-passivated NC QYs have not been fully established. Multidimensional nuclear magnetic resonance experiments now reveal a new DDDMA⁺-NC surface interaction, beyond established “tightly-bound” DDDMA⁺ interactions, which strongly affects observed emission QYs. Depending upon the existence of this new DDDMA⁺ coordination, NC QYs vary broadly between 60% and 85%. More importantly, these measurements reveal surface passivation through unexpected didodecyl ammonium (DDA⁺) that works in concert with DDDMA⁺, to produce near unity (i.e. >90%) QYs.

View Accepted Manuscript (DOE)

Research Organization:: University of Notre Dame, IN (United States)

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

Grant/Contract Number:: SC0014334

OSTI ID:: 2338293

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 11 Vol. 145; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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