Ligand Induced Size-Dependent Circular Dichroism in Quantum Dots

Fuente: arXiv
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Autores principales: Chabeda, Daniel, Gee, Stephen, Rabani, Eran
Formato: Preprint
Publicado: 2024
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author Chabeda, Daniel
Gee, Stephen
Rabani, Eran
author_facet Chabeda, Daniel
Gee, Stephen
Rabani, Eran
contents Recent experiments have probed the chiral properties of semiconductor nanocrystal (NC) quantum dots (QDs), but understanding the circular dichroism lineshape, excitonic features, and ligand 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 spectra, predicting consistent bisignate lineshapes with decreasing CD magnitude as size increases. Our analysis reveals the origin of bisignate lineshapes, arising from nondegenerate excitons with opposing angular momenta. We also explore the impact of chiral ligand orientation on QD surfaces, observing changes in optical activity magnitude and sign. This orientation sensitivity offers means to distinguish ordered from disordered ligand configurations, facilitating the study of order-disorder transitions at ligand-QD interfaces.
format Preprint
id arxiv_https___arxiv_org_abs_2404_10862
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Ligand Induced Size-Dependent Circular Dichroism in Quantum Dots
Chabeda, Daniel
Gee, Stephen
Rabani, Eran
Materials Science
Recent experiments have probed the chiral properties of semiconductor nanocrystal (NC) quantum dots (QDs), but understanding the circular dichroism lineshape, excitonic features, and ligand 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 spectra, predicting consistent bisignate lineshapes with decreasing CD magnitude as size increases. Our analysis reveals the origin of bisignate lineshapes, arising from nondegenerate excitons with opposing angular momenta. We also explore the impact of chiral ligand orientation on QD surfaces, observing changes in optical activity magnitude and sign. This orientation sensitivity offers means to distinguish ordered from disordered ligand configurations, facilitating the study of order-disorder transitions at ligand-QD interfaces.
title Ligand Induced Size-Dependent Circular Dichroism in Quantum Dots
topic Materials Science
url https://arxiv.org/abs/2404.10862