Designer phospholipid capping ligands for soft metal halide nanocrystals

Viktoriia Morad, Andriy Stelmakh, Mariia Svyrydenko, Leon G. Feld, Simon C. Boehme, Marcel Aebli, Joel Affolter, Christoph J. Kaul, Nadine J. Schrenker, Sara Bals, Yesim Sahin, Dmitry N. Dirin, Ihor Cherniukh, Gabriele Raino, Andrij Baumketner and Maksym V. Kovalenko ()
Additional contact information
Viktoriia Morad: Institute of Inorganic Chemistry, ETH Zürich
Andriy Stelmakh: Institute of Inorganic Chemistry, ETH Zürich
Mariia Svyrydenko: Institute of Inorganic Chemistry, ETH Zürich
Leon G. Feld: Institute of Inorganic Chemistry, ETH Zürich
Simon C. Boehme: Institute of Inorganic Chemistry, ETH Zürich
Marcel Aebli: Institute of Inorganic Chemistry, ETH Zürich
Joel Affolter: Institute of Inorganic Chemistry, ETH Zürich
Christoph J. Kaul: Institute of Inorganic Chemistry, ETH Zürich
Nadine J. Schrenker: University of Antwerp
Sara Bals: University of Antwerp
Yesim Sahin: Institute of Inorganic Chemistry, ETH Zürich
Dmitry N. Dirin: Institute of Inorganic Chemistry, ETH Zürich
Ihor Cherniukh: Institute of Inorganic Chemistry, ETH Zürich
Gabriele Raino: Institute of Inorganic Chemistry, ETH Zürich
Andrij Baumketner: National Academy of Sciences of Ukraine
Maksym V. Kovalenko: Institute of Inorganic Chemistry, ETH Zürich

Nature, 2024, vol. 626, issue 7999, 542-548

Abstract: Abstract The success of colloidal semiconductor nanocrystals (NCs) in science and optoelectronics is inextricable from their surfaces. The functionalization of lead halide perovskite NCs1–5 poses a formidable challenge because of their structural lability, unlike the well-established covalent ligand capping of conventional semiconductor NCs6,7. We posited that the vast and facile molecular engineering of phospholipids as zwitterionic surfactants can deliver highly customized surface chemistries for metal halide NCs. Molecular dynamics simulations implied that ligand–NC surface affinity is primarily governed by the structure of the zwitterionic head group, particularly by the geometric fitness of the anionic and cationic moieties into the surface lattice sites, as corroborated by the nuclear magnetic resonance and Fourier-transform infrared spectroscopy data. Lattice-matched primary-ammonium phospholipids enhance the structural and colloidal integrity of hybrid organic–inorganic lead halide perovskites (FAPbBr3 and MAPbBr3 (FA, formamidinium; MA, methylammonium)) and lead-free metal halide NCs. The molecular structure of the organic ligand tail governs the long-term colloidal stability and compatibility with solvents of diverse polarity, from hydrocarbons to acetone and alcohols. These NCs exhibit photoluminescence quantum yield of more than 96% in solution and solids and minimal photoluminescence intermittency at the single particle level with an average ON fraction as high as 94%, as well as bright and high-purity (about 95%) single-photon emission.

Date: 2024
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DOI: 10.1038/s41586-023-06932-6

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