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Emergent Circularly Polarized Luminescence from Self-Assembled Chiral-Ligand-Functionalized CsPbBr3 Nanocrystals

Mandal, Prasenjit LU orcid ; Chaudhary, Mohit ; Cloarec, Jeanne LU ; Prezhdo, Oleg V. and Baranov, Dmitry LU orcid (2026) In Nano Letters 26(38). p.12716-12724
Abstract
Chiral surface ligands can impart optical activity to
all-inorganic
perovskite nanocrystals, but how this affects chiroptical properties
of their assemblies remains unclear. Here we show that self-assembly
of CsPbBr3 nanocubes synthesized with a small amount of
added chiral ligand N-benzylcinchonidinium bromide
(BCD-Br) results in measurable circularly polarized luminescence (CPL).
BCD-Br-treated nanocrystals show weak circular dichroism but no detectable
CPL in colloidal dispersion. Upon assembly into CsPbBr3 and mixed halide superlattices, they exhibit CPL with a luminescence
dissymmetry factor, glum, of (5 ±
2) × 10–3, whereas untreated... (More)
Chiral surface ligands can impart optical activity to
all-inorganic
perovskite nanocrystals, but how this affects chiroptical properties
of their assemblies remains unclear. Here we show that self-assembly
of CsPbBr3 nanocubes synthesized with a small amount of
added chiral ligand N-benzylcinchonidinium bromide
(BCD-Br) results in measurable circularly polarized luminescence (CPL).
BCD-Br-treated nanocrystals show weak circular dichroism but no detectable
CPL in colloidal dispersion. Upon assembly into CsPbBr3 and mixed halide superlattices, they exhibit CPL with a luminescence
dissymmetry factor, glum, of (5 ±
2) × 10–3, whereas untreated controls remain
near the noise level. Polarization-resolved transient absorption (TA)
reveals an extended spin lifetime of hundreds of picoseconds in BCD-Br-treated
nanocrystals, while linear-response time-dependent density functional
theory (LR-TDDFT) calculations suggest that inter-nanocrystal coupling
can enhance the chiroptical response. These results support the idea
that ordered nanocrystal assembly can convert weak ligand-induced
chirality into an emergent chiroptical response in perovskite nanocrystal
solids. (Less)
Please use this url to cite or link to this publication:
@article{0ed1c524-1693-4011-a2f6-34a594168bc2,
  abstract     = {{Chiral surface ligands can impart optical activity to<br>
all-inorganic<br>
perovskite nanocrystals, but how this affects chiroptical properties<br>
of their assemblies remains unclear. Here we show that self-assembly<br>
of CsPbBr<sub>3</sub> nanocubes synthesized with a small amount of<br>
added chiral ligand <em>N</em>-benzylcinchonidinium bromide<br>
(BCD-Br) results in measurable circularly polarized luminescence (CPL).<br>
BCD-Br-treated nanocrystals show weak circular dichroism but no detectable<br>
CPL in colloidal dispersion. Upon assembly into CsPbBr<sub>3</sub> and mixed halide superlattices, they exhibit CPL with a luminescence<br>
dissymmetry factor, <em>g</em><sub>lum</sub>, of (5 ±<br>
2) × 10<sup>–3</sup>, whereas untreated controls remain<br>
near the noise level. Polarization-resolved transient absorption (TA)<br>
reveals an extended spin lifetime of hundreds of picoseconds in BCD-Br-treated<br>
nanocrystals, while linear-response time-dependent density functional<br>
theory (LR-TDDFT) calculations suggest that inter-nanocrystal coupling<br>
can enhance the chiroptical response. These results support the idea<br>
that ordered nanocrystal assembly can convert weak ligand-induced<br>
chirality into an emergent chiroptical response in perovskite nanocrystal<br>
solids.}},
  author       = {{Mandal, Prasenjit and Chaudhary, Mohit and Cloarec, Jeanne and Prezhdo, Oleg V. and Baranov, Dmitry}},
  issn         = {{1530-6992}},
  language     = {{eng}},
  month        = {{09}},
  number       = {{38}},
  pages        = {{12716--12724}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{Nano Letters}},
  title        = {{Emergent Circularly Polarized Luminescence from Self-Assembled Chiral-Ligand-Functionalized CsPbBr<sub>3</sub> Nanocrystals}},
  url          = {{http://dx.doi.org/10.1021/acs.nanolett.6c02634}},
  doi          = {{10.1021/acs.nanolett.6c02634}},
  volume       = {{26}},
  year         = {{2026}},
}