Enhanced Magnetization by Defect-Assisted Exciton Recombination in Atomically Thin CrCl$_3$

Fuente: arXiv
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Autori principali: Zhang, Xin-Yue, Graham, Thomas K. M., Bae, Hyeonhu, Wang, Yu-Xuan, Delegan, Nazar, Ahn, Jonghoon, Wang, Zhi-Cheng, Regner, Jakub, Watanabe, Kenji, Taniguchi, Takashi, Jung, Minkyung, Sofer, Zdeněk, Tafti, Fazel, Awschalom, David D., Heremans, F. Joseph, Yan, Binghai, Zhou, Brian B.
Natura: Preprint
Pubblicazione: 2023
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author Zhang, Xin-Yue
Graham, Thomas K. M.
Bae, Hyeonhu
Wang, Yu-Xuan
Delegan, Nazar
Ahn, Jonghoon
Wang, Zhi-Cheng
Regner, Jakub
Watanabe, Kenji
Taniguchi, Takashi
Jung, Minkyung
Sofer, Zdeněk
Tafti, Fazel
Awschalom, David D.
Heremans, F. Joseph
Yan, Binghai
Zhou, Brian B.
author_facet Zhang, Xin-Yue
Graham, Thomas K. M.
Bae, Hyeonhu
Wang, Yu-Xuan
Delegan, Nazar
Ahn, Jonghoon
Wang, Zhi-Cheng
Regner, Jakub
Watanabe, Kenji
Taniguchi, Takashi
Jung, Minkyung
Sofer, Zdeněk
Tafti, Fazel
Awschalom, David D.
Heremans, F. Joseph
Yan, Binghai
Zhou, Brian B.
contents Two dimensional (2D) semiconductors present unique opportunities to intertwine optical and magnetic functionalities and to tune these performances through defects and dopants. Here, we integrate exciton pumping into a quantum sensing protocol on nitrogen-vacancy centers in diamond to image the optically-induced transient stray fields in few-layer, antiferromagnetic CrCl$_3$. We discover that exciton recombination enhances the in-plane magnetization of the CrCl$_3$ layers, with a predominant effect in the surface monolayers. Concomitantly, time-resolved photoluminescence measurements reveal that nonradiative exciton recombination intensifies in atomically thin CrCl$_3$ with tightly localized, nearly dipole-forbidden excitons and amplified surface-to-volume ratio. Supported by experiments under controlled surface exposure and density functional theory calculations, we interpret the magnetically enhanced state to result from a defect-assisted Auger recombination that optically activates electron transfer between water vapor related surface impurities and the spin-polarized conduction band. Our work validates defect engineering as a route to enhance intrinsic magnetism in single magnetic layers and opens a novel experimental platform for studying optically-induced, transient magnetism in condensed matter systems.
format Preprint
id arxiv_https___arxiv_org_abs_2312_08476
institution arXiv
publishDate 2023
record_format arxiv
spellingShingle Enhanced Magnetization by Defect-Assisted Exciton Recombination in Atomically Thin CrCl$_3$
Zhang, Xin-Yue
Graham, Thomas K. M.
Bae, Hyeonhu
Wang, Yu-Xuan
Delegan, Nazar
Ahn, Jonghoon
Wang, Zhi-Cheng
Regner, Jakub
Watanabe, Kenji
Taniguchi, Takashi
Jung, Minkyung
Sofer, Zdeněk
Tafti, Fazel
Awschalom, David D.
Heremans, F. Joseph
Yan, Binghai
Zhou, Brian B.
Materials Science
Mesoscale and Nanoscale Physics
Two dimensional (2D) semiconductors present unique opportunities to intertwine optical and magnetic functionalities and to tune these performances through defects and dopants. Here, we integrate exciton pumping into a quantum sensing protocol on nitrogen-vacancy centers in diamond to image the optically-induced transient stray fields in few-layer, antiferromagnetic CrCl$_3$. We discover that exciton recombination enhances the in-plane magnetization of the CrCl$_3$ layers, with a predominant effect in the surface monolayers. Concomitantly, time-resolved photoluminescence measurements reveal that nonradiative exciton recombination intensifies in atomically thin CrCl$_3$ with tightly localized, nearly dipole-forbidden excitons and amplified surface-to-volume ratio. Supported by experiments under controlled surface exposure and density functional theory calculations, we interpret the magnetically enhanced state to result from a defect-assisted Auger recombination that optically activates electron transfer between water vapor related surface impurities and the spin-polarized conduction band. Our work validates defect engineering as a route to enhance intrinsic magnetism in single magnetic layers and opens a novel experimental platform for studying optically-induced, transient magnetism in condensed matter systems.
title Enhanced Magnetization by Defect-Assisted Exciton Recombination in Atomically Thin CrCl$_3$
topic Materials Science
Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2312.08476