DOI: 10.1021/jacs.6c15479 ISSN: 0002-7863

Local Symmetry Breaking Facilitates Near-Infrared Circularly Polarized Lanthanide Emission in Perovskite Nanocrystals

Tyler Wang, Fangyuan Liu, Yan Zhou, Joseph A. Adewuyi, Zhengjie Li, Mingwei Ge, Haiyan Tan, Gaël Ung, Cong Su, Mengxia Liu

Abstract

Imparting chiroptical activity of lanthanide transitions provides an attractive route to circularly polarized luminescence. However, obtaining intense emission from their Laporte-forbidden f–f transitions while also generating significant rotatory strength remains a formidable challenge in materials design. This work establishes a platform for efficient near-infrared (NIR) circularly polarized luminescence (CPL), centered on the telecom-relevant C-band around 1550 nm, from lanthanide dopants (Yb3+/Er3+) embedded in chiral perovskite nanocrystal (CsPbX3) hosts. Atomic-scale structural analyses reveal a preferential enrichment of lanthanide concentration near the nanocrystal surfaces, where chiral ligands distort the lattice, lowering the local symmetry. Spectroscopic measurements confirm the highly efficient host-to-dopant energy transfer, facilitating strong CPL, with a luminescence dissymmetry factor (glum) of 0.36 and a CPL brightness (BCPL) of 4.2 × 105 M–1 cm–1 at 1550 nm, representing nearly four orders of magnitude above the previous benchmark. With improved photostability, these results establish lanthanide-doped chiral perovskite nanocrystals as a promising route to telecom-relevant CPL.

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