Polarization of photoluminescence by optically driven orbital reconstruction in magnetically ordered CrCl3

Fuente: arXiv
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Hauptverfasser: Zhou, Lanqing, Ležaić, Marjana, Mokrousov, Yuriy, Bui, Minh N., Rani, Renu, Grützmacher, Detlev, Kardynał, Beata E.
Format: Preprint
Veröffentlicht: 2025
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author Zhou, Lanqing
Ležaić, Marjana
Mokrousov, Yuriy
Bui, Minh N.
Rani, Renu
Grützmacher, Detlev
Kardynał, Beata E.
author_facet Zhou, Lanqing
Ležaić, Marjana
Mokrousov, Yuriy
Bui, Minh N.
Rani, Renu
Grützmacher, Detlev
Kardynał, Beata E.
contents In this paper, we show that photoluminescence from CrCl3 bulk crystal exhibits a preferential polarization direction when films are magnetically ordered or strained. We verify the magnetization as responsible for the polarization by measuring the signal as a function of the temperature in Voigt configuration while applying the in-plane magnetic field. We show that phonon coupling contributing to vibronic transitions depolarizes the signal compared with zero phonon lines. We explain the data using DFT calculations, which reveal a magnetization-selective occupation of the low energy d-orbital triplet state of Cr3+ upon photon absorption. In addition, the calculations find that the excitation of one electron results in the excited state acquiring out-of-plane components of spin and very large orbital magnetic moments, in addition to a lattice deformation.
format Preprint
id arxiv_https___arxiv_org_abs_2502_16285
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Polarization of photoluminescence by optically driven orbital reconstruction in magnetically ordered CrCl3
Zhou, Lanqing
Ležaić, Marjana
Mokrousov, Yuriy
Bui, Minh N.
Rani, Renu
Grützmacher, Detlev
Kardynał, Beata E.
Materials Science
Optics
In this paper, we show that photoluminescence from CrCl3 bulk crystal exhibits a preferential polarization direction when films are magnetically ordered or strained. We verify the magnetization as responsible for the polarization by measuring the signal as a function of the temperature in Voigt configuration while applying the in-plane magnetic field. We show that phonon coupling contributing to vibronic transitions depolarizes the signal compared with zero phonon lines. We explain the data using DFT calculations, which reveal a magnetization-selective occupation of the low energy d-orbital triplet state of Cr3+ upon photon absorption. In addition, the calculations find that the excitation of one electron results in the excited state acquiring out-of-plane components of spin and very large orbital magnetic moments, in addition to a lattice deformation.
title Polarization of photoluminescence by optically driven orbital reconstruction in magnetically ordered CrCl3
topic Materials Science
Optics
url https://arxiv.org/abs/2502.16285