Optical activity of chiral excitons

Fuente: arXiv
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Main Authors: Sercel, Peter C., Hautzinger, Matthew P., Song, Ruyi, Blum, Volker, Beard, Matthew C.
Format: Preprint
Published: 2024
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author Sercel, Peter C.
Hautzinger, Matthew P.
Song, Ruyi
Blum, Volker
Beard, Matthew C.
author_facet Sercel, Peter C.
Hautzinger, Matthew P.
Song, Ruyi
Blum, Volker
Beard, Matthew C.
contents Recent activity in the area of chiroptical phenomena has been focused on the connection between structural asymmetry, electron spin configuration and light matter interactions in chiral semiconductors. In these systems, spin-splitting phenomena emerge due to inversion symmetry breaking and the presence of extended electronic states, yet the connection to chiroptical phenomena is lacking. Here, we develop an analytical effective mass model of chiral excitons, parameterized by density functional theory. The model accounts for parity mixing of the band edge Bloch functions resulting from polar distortions, resulting in magnetic dipole allowed transitions. Through the study of a prototypical chiral 2D hybrid perovskite semiconductor, we show that circular dichroism of the chiral exciton and its interband continuum emerges from spin-splitting via cross coupling of Rashba-like and chiral/helical spin-texture components. As a counterpoint, we apply our model to describe chiroptical properties of excitons in perovskite nanocrystals that occur without chiral lattice distortions.
format Preprint
id arxiv_https___arxiv_org_abs_2412_00602
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Optical activity of chiral excitons
Sercel, Peter C.
Hautzinger, Matthew P.
Song, Ruyi
Blum, Volker
Beard, Matthew C.
Mesoscale and Nanoscale Physics
Recent activity in the area of chiroptical phenomena has been focused on the connection between structural asymmetry, electron spin configuration and light matter interactions in chiral semiconductors. In these systems, spin-splitting phenomena emerge due to inversion symmetry breaking and the presence of extended electronic states, yet the connection to chiroptical phenomena is lacking. Here, we develop an analytical effective mass model of chiral excitons, parameterized by density functional theory. The model accounts for parity mixing of the band edge Bloch functions resulting from polar distortions, resulting in magnetic dipole allowed transitions. Through the study of a prototypical chiral 2D hybrid perovskite semiconductor, we show that circular dichroism of the chiral exciton and its interband continuum emerges from spin-splitting via cross coupling of Rashba-like and chiral/helical spin-texture components. As a counterpoint, we apply our model to describe chiroptical properties of excitons in perovskite nanocrystals that occur without chiral lattice distortions.
title Optical activity of chiral excitons
topic Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2412.00602