Ligand-Induced Size-Dependent Circular Dichroism in Quantum Dots

Chabeda, Daniel; Gee, Stephen; Rabani, Eran

doi:10.1021/acs.jpclett.4c01682

Ligand-Induced Size-Dependent Circular Dichroism in Quantum Dots

Journal Article · Thu Jul 25 00:00:00 EDT 2024 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.4c01682· OSTI ID:2500822

^[1]; Gee, Stephen ^[2]; ^[3]

Univ. of California, Berkeley, CA (United States)
Univ. of California, Santa Barbara, CA (United States)
Univ. of California, Berkeley, CA (United States); Tel Aviv Univ., Tel Aviv (Israel); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Recent experiments have probed the chiral properties of semiconductor nanocrystal (NC) quantum dots (QDs), but understanding the circular dichroism line shape, excitonic features, and chirality induction mechanism remains a challenge. We propose an atomistic pseudopotential method to model chiral ligand passivated QDs, computing circular dichroism (CD) spectra for CdSe QDs (2.6-3.8 nm). We find strong agreement between calculated and measured line shapes, predicting consistent bisignate line shapes with decreasing CD magnitude as size increases. Further, our analysis reveals the origin of bisignate line shapes, arising from nondegenerate excitons with opposing angular momenta. We also explore the impact of chiral ligand orientation on QD surfaces, observing changes in the optical activity magnitude and sign. This orientation sensitivity offers the means to distinguish ordered from disordered ligand configurations, facilitating the study of order-disorder transitions at ligand-QD interfaces.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2500822

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 31 Vol. 15; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Absorption
Chirality
Circular dichroism spectroscopy
Ligands
Quantum dots

Ligand-Induced Size-Dependent Circular Dichroism in Quantum Dots

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