Heteroepitaxial chemistry of zinc chalcogenides on InP nanocrystals for defect-free interfaces with atomic uniformity

• DOI: 10.1038/s41467-022-35731-2
• Publication Date: 2023-01-03T16:03:43Z
• Authors: Yeongho Choi; Donghyo Hahm; Wan Ki Bae; Jaehoon Lim
• Keywords: Carboxylate; Indium phosphide

Heteroepitaxy on colloidal semiconductor nanocrystals is an essential strategy for manipulating their optoelectronic functionalities. However, practical synthesis typically leads to scattered and unexpected outcomes due the intervention of multiple reaction pathways associated with complicated side products reactants. Here, heteroepitaxy mechanism zinc chalcogenide initiated indium phosphide (InP) elucidated using precursors, carboxylate trialkylphosphine selenide. The high magnetic receptivity 77Se characteristic longitudinal optical phonon mode ZnSe allowed monitoring sequence epilayer formation at molecular level. investigation revealed sterically hindered acyloxytrialkylphosphonium diacyloxytrialkylphosphorane be main intermediates in surface reaction, which retards metal ion adsorption by a large steric hindrance. transformation adsorbates crystalline was disturbed oxides. Raman scattering disclosed pathway secondary oxidation triggered ligands migrated from carboxylate. surface-initiated protocol proposed fabricate core/shell heterostructured atomic-scale uniformity epilayers. Despite lattice mismatch ZnS InP, we realised uniform interface defect-free (~0.3 nm thickness) InP nanocrystals, as evidenced photoluminescence quantum yield 97.3%.