TY - JOUR
T1 - Precise control of CsPbBr3 perovskite nanocrystal growth at room temperature
T2 - Size tunability and synthetic insights
AU - Brown, Alasdair A.M.
AU - Mathews, Nripan
AU - Vashishtha, Parth
AU - Hooper, Thomas J.N.
AU - Ng, Yan Fong
AU - Nutan, Gautam V.
AU - Fang, Yanan
AU - Giovanni, David
AU - Tey, Ju Nie
AU - Jiang, Liudi
AU - Damodaran, Bahulayan
AU - Sum, Tze Chien
AU - Pu, Suan Hui
AU - Mhaisalkar, Subodh G.
N1 - Publisher Copyright:
© 2021 American Chemical Society
PY - 2021
Y1 - 2021
N2 - Room-temperature perovskite nanocrystal syntheses have previously lacked the size tunability attainable through high-temperature methods. Herein, we outline a scalable approach whereby the nucleation and growth of CsPbBr3 nanocrystals (NCs) can be decoupled and controlled at room temperature by utilizing different ligands. We employed octylphosphonic acid (OPA) ligands to regulate the critical radius and the NC growth rate. The subsequent addition of a bulkier didodecyldimethylammonium bromide ligand quenches the NC growth, defining the reaction duration. Management of these three variables enables precise tuning of the NC diameter between 6.8 and 13.6 nm. The photoluminescence quantum yield of the NCs remains above 80% for all sizes even after thorough antisolvent purification. The use of hydrogen-bonding OPA ligands enhances quantum confinement effects, characterized by strong, well-resolved absorption peaks. Solution and solid-state nuclear magnetic resonance spectra confirmed the effective removal of unbound ligands during purification and the presence of a hydrogen-bonded network of OPA ligands on the surface of the purified NCs. Overall, this approach has the potential to facilitate a broad range of future endeavors from studies of hot carrier dynamics to both optically and electrically driven device applications.
AB - Room-temperature perovskite nanocrystal syntheses have previously lacked the size tunability attainable through high-temperature methods. Herein, we outline a scalable approach whereby the nucleation and growth of CsPbBr3 nanocrystals (NCs) can be decoupled and controlled at room temperature by utilizing different ligands. We employed octylphosphonic acid (OPA) ligands to regulate the critical radius and the NC growth rate. The subsequent addition of a bulkier didodecyldimethylammonium bromide ligand quenches the NC growth, defining the reaction duration. Management of these three variables enables precise tuning of the NC diameter between 6.8 and 13.6 nm. The photoluminescence quantum yield of the NCs remains above 80% for all sizes even after thorough antisolvent purification. The use of hydrogen-bonding OPA ligands enhances quantum confinement effects, characterized by strong, well-resolved absorption peaks. Solution and solid-state nuclear magnetic resonance spectra confirmed the effective removal of unbound ligands during purification and the presence of a hydrogen-bonded network of OPA ligands on the surface of the purified NCs. Overall, this approach has the potential to facilitate a broad range of future endeavors from studies of hot carrier dynamics to both optically and electrically driven device applications.
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U2 - 10.1021/acs.chemmater.0c04569
DO - 10.1021/acs.chemmater.0c04569
M3 - Article
AN - SCOPUS:85105023998
SN - 0897-4756
VL - 33
SP - 2387
EP - 2397
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 7
ER -