Chiral Perovskite Nanoplatelets with Tunable Circularly Polarized Luminescence in the Strong Confinement Regime

Cao, Qinxuan; Song, Ruyi; Chan, Christopher C. S.; Wang, Zhiyu; Wong, Pui Ying; Wong, Kam Sing; Blum, Volker; Lu, Haipeng

doi:10.1002/adom.202203125

Chiral Perovskite Nanoplatelets with Tunable Circularly Polarized Luminescence in the Strong Confinement Regime

Journal Article · Tue Mar 21 00:00:00 UTC 2023 · Advanced Optical Materials

DOI:https://doi.org/10.1002/adom.202203125· OSTI ID:2422891

Cao, Qinxuan ^[1]; Song, Ruyi ^[2]; Chan, Christopher C. S. ^[1]; Wang, Zhiyu ^[1]; Wong, Pui Ying ^[1]; Wong, Kam Sing ^[1]; Blum, Volker ^[2]; ^[1]

Hong Kong University of Science and Technology (HKUST) (Hong Kong)
Duke Univ., Durham, NC (United States)

Chiral perovskite nanocrystals have emerged as an interesting chiral excitonic platform that combines both structural flexibility and superior optoelectronic properties. Despite several recent demonstrations of optical activity in various chiral perovskite nanocrystals, efficient circularly polarized luminescence (CPL) with tunable energies remains a challenge. The chirality imprinting mechanism as a function of perovskite nanocrystal dimensionality remains elusive. Here, in this study, atomically thin inorganic perovskite nanoplatelets (NPLs) are synthesized with precise control of layer thickness and are functionalized by chiral surface ligands, serving as a unique platform to probe the chirality transfer mechanism at the organic/perovskite interface. It is found that chirality is successfully imprinted into mono-, bi-, and tri-layer inorganic perovskite NPLs, exhibiting tunable circular dichroism (CD) and CPL responses. However, chirality transfer decreases in thicker NPLs, resulting in decreased CD and CPL dissymmetry factors for thicker NPLs. Aided by large-scale first-principles calculations, it is proposed that chirality transfer is mainly mediated through a surface distortion rather than a hybridization of electronic states, giving rise to symmetry breaking in the perovskite lattice and spin-split conduction bands. The findings described here provide an in-depth understanding of chirality transfer and design principles for distorted-surface perovskites for chiral photonic applications.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: Hong Kong Research Grants Council (RGC); National Natural Science Foundation of China (NSFC); National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2422891

Alternate ID(s):: OSTI ID: 1995935

Journal Information:: Advanced Optical Materials, Journal Name: Advanced Optical Materials Journal Issue: 12 Vol. 11; ISSN 2195-1071

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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