Giant optical anisotropy in CrSBr from giant exciton oscillator strength

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Main Authors: Ermolaev, Georgy, Mazitov, Tagir, Mazitov, Arslan, Toksumakov, Adilet, Grudinin, Dmitriy, Minnekhanov, Anton, Tselikov, Gleb, Yakubovsky, Dmitry, Tikhonowski, Gleb, Pak, Nikolay, Ahsan, Umer, Slavich, Aleksandr, Mironov, Mikhail, Tsapenko, Alexey, Vyshnevyy, Andrey, Kruglov, Ivan, Sofer, Zdenek, Arsenin, Aleksey, Novoselov, Kostya, Katanin, Andrey, Volkov, Valentyn
Format: Preprint
Published: 2025
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author Ermolaev, Georgy
Mazitov, Tagir
Mazitov, Arslan
Toksumakov, Adilet
Grudinin, Dmitriy
Minnekhanov, Anton
Tselikov, Gleb
Yakubovsky, Dmitry
Tikhonowski, Gleb
Pak, Nikolay
Ahsan, Umer
Slavich, Aleksandr
Mironov, Mikhail
Tsapenko, Alexey
Vyshnevyy, Andrey
Kruglov, Ivan
Sofer, Zdenek
Arsenin, Aleksey
Novoselov, Kostya
Katanin, Andrey
Volkov, Valentyn
author_facet Ermolaev, Georgy
Mazitov, Tagir
Mazitov, Arslan
Toksumakov, Adilet
Grudinin, Dmitriy
Minnekhanov, Anton
Tselikov, Gleb
Yakubovsky, Dmitry
Tikhonowski, Gleb
Pak, Nikolay
Ahsan, Umer
Slavich, Aleksandr
Mironov, Mikhail
Tsapenko, Alexey
Vyshnevyy, Andrey
Kruglov, Ivan
Sofer, Zdenek
Arsenin, Aleksey
Novoselov, Kostya
Katanin, Andrey
Volkov, Valentyn
contents The interplay between dimensionality and electronic correlations in van der Waals (vdW) materials offers a powerful toolkit for engineering light-matter interactions at the nanoscale. Excitons, bound electron-hole pairs, are central to this endeavor, yet maximizing their oscillator strength, which dictates the interaction cross-section, remains a challenge. Conventional wisdom suggests a trade-off, where the observable oscillator strength often decreases in strongly bound systems due to population dynamics. Here, we unveil a colossal oscillator strength associated with the quasi-one-dimensional (quasi-1D) excitons in the layered magnetic semiconductor CrSBr, which fundamentally defies this established scaling law. Through comprehensive optical characterization and ab initio calculations, we establish that this anomalous enhancement originates directly from the reduced dimensionality, which enforces an increased electron-hole wavefunction overlap. Moreover, we find a close connection between fundamental exciton and local spin fluctuations that contribute to the opening of the gap in the electronic spectrum. The resulting optical anisotropy shows a giant in-plane birefringence (Delta_n = 1.45) and profoundly anisotropic waveguiding, which we directly visualize using nano-optical imaging. Leveraging this extreme response, we realize a true zero-order quarter-wave plate with an unprecedented wavelength-to-thickness ratio (lambda/t) exceeding 3.4, surpassing the limits of current miniaturization technologies, including state-of-the-art metasurfaces. Our findings underscore the profound impact of dimensionality engineering in magnetic vdW materials for realizing novel regimes of light-matter coupling and developing next-generation ultracompact photonic architectures.
format Preprint
id arxiv_https___arxiv_org_abs_2509_18866
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Giant optical anisotropy in CrSBr from giant exciton oscillator strength
Ermolaev, Georgy
Mazitov, Tagir
Mazitov, Arslan
Toksumakov, Adilet
Grudinin, Dmitriy
Minnekhanov, Anton
Tselikov, Gleb
Yakubovsky, Dmitry
Tikhonowski, Gleb
Pak, Nikolay
Ahsan, Umer
Slavich, Aleksandr
Mironov, Mikhail
Tsapenko, Alexey
Vyshnevyy, Andrey
Kruglov, Ivan
Sofer, Zdenek
Arsenin, Aleksey
Novoselov, Kostya
Katanin, Andrey
Volkov, Valentyn
Materials Science
The interplay between dimensionality and electronic correlations in van der Waals (vdW) materials offers a powerful toolkit for engineering light-matter interactions at the nanoscale. Excitons, bound electron-hole pairs, are central to this endeavor, yet maximizing their oscillator strength, which dictates the interaction cross-section, remains a challenge. Conventional wisdom suggests a trade-off, where the observable oscillator strength often decreases in strongly bound systems due to population dynamics. Here, we unveil a colossal oscillator strength associated with the quasi-one-dimensional (quasi-1D) excitons in the layered magnetic semiconductor CrSBr, which fundamentally defies this established scaling law. Through comprehensive optical characterization and ab initio calculations, we establish that this anomalous enhancement originates directly from the reduced dimensionality, which enforces an increased electron-hole wavefunction overlap. Moreover, we find a close connection between fundamental exciton and local spin fluctuations that contribute to the opening of the gap in the electronic spectrum. The resulting optical anisotropy shows a giant in-plane birefringence (Delta_n = 1.45) and profoundly anisotropic waveguiding, which we directly visualize using nano-optical imaging. Leveraging this extreme response, we realize a true zero-order quarter-wave plate with an unprecedented wavelength-to-thickness ratio (lambda/t) exceeding 3.4, surpassing the limits of current miniaturization technologies, including state-of-the-art metasurfaces. Our findings underscore the profound impact of dimensionality engineering in magnetic vdW materials for realizing novel regimes of light-matter coupling and developing next-generation ultracompact photonic architectures.
title Giant optical anisotropy in CrSBr from giant exciton oscillator strength
topic Materials Science
url https://arxiv.org/abs/2509.18866