Showing 1–37 of 37 results for author: Mosina, K

Excitonic fingerprints of magnetic configurations and switching in multilayer CrSBr

Authors: Lukas Krelle, Ryan Tan, Jakob Conradi, Priyanka Mondal, Wenze Lan, Kseniia Mosina, Regine von Klitzing, Zdenek Sofer, Bernhard Urbaszek

Abstract: The coupling between electronic states and magnetism provides a route towards optical readout and control of magnetic information. In the magnetic semiconductor CrSBr, excitons are coupled to magnetic order, making their optical response sensitive to the underlying magnetization. Here, we show that the energy and oscillator strength of bulk and surface excitons provide distinct spectroscopic finge… ▽ More The coupling between electronic states and magnetism provides a route towards optical readout and control of magnetic information. In the magnetic semiconductor CrSBr, excitons are coupled to magnetic order, making their optical response sensitive to the underlying magnetization. Here, we show that the energy and oscillator strength of bulk and surface excitons provide distinct spectroscopic fingerprints of magnetic configurations and switching pathways. We distinguish domain-wall-mediated magnetization reversal, manifested by continuous spectral evolution as a domain wall traverses the optical spot, from abrupt, large-area magnetization reversal. Using the resulting excitonic fingerprints, we reconstruct successive magnetic configurations in 4- and 5-layer CrSBr during the transition from ferromagnetic to antiferromagnetic order. We further find that the sensitivity to magnetic order is strongly exciton-dependent: low-energy excitons resolve intermediate and surface-related configurations, whereas a higher-energy exciton predominantly exhibits a transfer of oscillator strength between ferromagnetic and antiferromagnetic resonances. These results establish excitonic spectroscopy as a sensitive probe of layer-dependent magnetic configurations and their switching pathways in layered magnetic semiconductors. △ Less

Submitted 25 August, 2026; originally announced August 2026.

Detecting Magnetic Phase Transitions in Ion-Irradiated CrSBr Through Resonant Raman Scattering

Authors: Daria I. Markina, Alison Pfister, Priyanka Mondal, Lukas Krelle, Sai Shradha, Regine von Klitzing, Kseniia Mosina, Zdenek Sofer, Fangchao Long, Ulrich Kentsch, Shengqiang Zhou, Bernhard Urbaszek

Abstract: Controlling magnetic phases and accurately determining their transition temperatures are essential for the development of low-dimensional magnetic materials. Here, we demonstrate that He$^+$ ion irradiation provides a versatile route for engineering magnetic phases in layered CrSBr and establish temperature-dependent polarization-resolved Raman spectroscopy as a sensitive optical probe for identif… ▽ More Controlling magnetic phases and accurately determining their transition temperatures are essential for the development of low-dimensional magnetic materials. Here, we demonstrate that He$^+$ ion irradiation provides a versatile route for engineering magnetic phases in layered CrSBr and establish temperature-dependent polarization-resolved Raman spectroscopy as a sensitive optical probe for identifying irradiation-induced magnetic phase transitions. We reveal that the magnetic response of the modified CrSBr is governed by both irradiation dose and crystal thickness. The temperature evolution of the Raman tensor elements resolves the antiferromagnetic transition in pristine CrSBr at T$_N \approx 132$ K as well as irradiation-induced magnetic transitions at T$_C \approx 105-110$ K and T$_D \approx 40$ K corresponding to ferromagnetic and defect-related magnetic phase transitions. Complementary magneto-optical measurements confirm the progressive suppression of antiferromagnetic order and the emergence of new defect-engineered magnetic phases, including pure ferromagnetic behavior at high irradiation doses. These findings establish irradiated CrSBr as a platform for controllable magnetic phase engineering while demonstrating polarization-resolved Raman spectroscopy as a rapid, non-destructive, and broadly applicable method for probing magnetic phase transitions in van der Waals magnets. △ Less

Submitted 19 August, 2026; originally announced August 2026.

Comments: Main and supplement

Tunable Magneto-Excitonic Coupling in Alloyed van der Waals Antiferromagnet

Authors: Maciej Smiertka, Oliwia Janikowska, Katarzyna Olkowska-Pucko, Grzegorz Krasucki, Katarzyna Posmyk, Paulina Peksa, Alessandro Surrente, Dimitar Pashov, Kseniia Mosina, Zdenek Sofer, Mark van Schilfgaarde, Adam Babinski, Maciej R. Molas, Gabriela Komorowska, Esteban Zamora-Amo, Andres Castellanos-Gomez, Federico Mompean, Mar Garcia-Hernandez, Michal Baranowski, Swagata Acharya, Paulina Plochocka

Abstract: The unique coupling between magnetic order and photo-generated excitons, electron-hole pairs bound by Coulomb interaction, in layered magnetic semiconductors offers a powerful mechanism for controlling light-matter interactions. In the van der Waals antiferromagnet CrSBr, this coupling is exceptionally strong and manifests distinctly between two coexisting excitonic states: the localised, Frenkel-… ▽ More The unique coupling between magnetic order and photo-generated excitons, electron-hole pairs bound by Coulomb interaction, in layered magnetic semiconductors offers a powerful mechanism for controlling light-matter interactions. In the van der Waals antiferromagnet CrSBr, this coupling is exceptionally strong and manifests distinctly between two coexisting excitonic states: the localised, Frenkel-like XA exciton and the more delocalised, Wannier-Mott-like XB exciton, providing a unique playground for the optical control of magnetism. Here, we reveal how chlorine incorporation reshapes the magneto-optical interplay in CrSBr1-xClx by simultaneously modifying its electronic structure, excitonic properties, and magnetic interactions. Combining magneto-optical spectroscopy up to 85 T with state-of-the-art quasiparticle self-consistent GW (QSGW) calculations on alloy supercells, we show that Cl insertion progressively localises the excitonic wavefunctions and drives both states toward a more Frenkel-like regime. This evolution is accompanied by a systematic reduction of the magnetic-field-induced energy renormalisation, most prominently for the XB exciton. Our work connects exciton character directly to magneto-excitonic coupling. Furthermore, it establishes compositional alloying as an effective strategy for engineering the coupling between magnetic and optical properties in van der Waals magnetic semiconductors. △ Less

Submitted 16 July, 2026; originally announced July 2026.

Anisotropic nanoscale coherent polariton transport in CrSBr

Authors: Paritosh Malik, Dogyun Ko, Vita Solovyeva, Chirag Chandrakant Palekar, Imad Limame, Sven Rodt, Kseniia Mosina, Zdeněk Sofer, Alexander Steinhoff, Martin Esmann, Stephan Reitzenstein, Bo Han, Christopher Gies, Christian Schneider

Abstract: In a combined experimental and theoretical study, we demonstrate anisotropic polariton transport on the nanoscale in the van der Waals antiferromagnet CrSBr. While effective cavity-polariton formation emerges via the self-hybridization of ultra-high oscillator strength excitons with a thin slab photonic mode, the absence of external mirrors facilitates spectroscopic investigation of these polarito… ▽ More In a combined experimental and theoretical study, we demonstrate anisotropic polariton transport on the nanoscale in the van der Waals antiferromagnet CrSBr. While effective cavity-polariton formation emerges via the self-hybridization of ultra-high oscillator strength excitons with a thin slab photonic mode, the absence of external mirrors facilitates spectroscopic investigation of these polaritons via cathodoluminescence (CL) on length scales determined by the electron wavelength. This direct access allows us to perform precise charting of the polariton landscape with nanometric resolution, and to probe polariton interference phenomena. The main finding of the work highlights that the coherent polariton transport follows the $C_{2v}$ symmetry of CrSBr, allowing exclusive transport along the crystallographic a-axis, while no coherent feature is found along the b-axis direction. Our work sets the foundation to use CL spectroscopy in cavity-polaritonics in more advanced landscapes, such as photonic crystals or optical lattices, and establishes the technique as a powerful tool to probe anisotropic expansion and relaxation phenomena on the nanoscale △ Less

Submitted 2 July, 2026; originally announced July 2026.

Comments: 11 pages, 5 figures

Microwave-to-optical transduction using magnon-exciton coupling in a layered antiferromagnet

Authors: Pratap Chandra Adak, Iris McDaniel, Suvodeep Paul, Caleb Heuvel-Horwitz, Bikash Das, Vitali Kozlov, Kseniia Mosina, Arun Ramanathan, Xavier Roy, Zdeněk Sofer, Tian Zhong, Akashdeep Kamra, Arno Thielens, Andrea Alù, Vinod M. Menon

Abstract: Coherent interfaces between microwave-frequency quantum systems and low-loss optical links are essential for quantum networks. However, existing microwave-optical transducers often trade conversion efficiency against added noise, bandwidth, and device integrability. Here, we demonstrate coherent microwave-to-optical transduction based on magnon-exciton coupling in the layered antiferromagnet CrSBr… ▽ More Coherent interfaces between microwave-frequency quantum systems and low-loss optical links are essential for quantum networks. However, existing microwave-optical transducers often trade conversion efficiency against added noise, bandwidth, and device integrability. Here, we demonstrate coherent microwave-to-optical transduction based on magnon-exciton coupling in the layered antiferromagnet CrSBr. Driving the antiferromagnetic resonance with microwave signals imprints coherent modulation on a reflected optical probe, generating optical sidebands that are resonantly enhanced near excitonic transitions. While prior magnon-based approaches to microwave-to-optical transduction have typically relied on intrinsically weak off-resonant magneto-optical effects (e.g., Faraday rotation), our scheme exploits strong light-matter interactions at exciton resonances. Even in a bulk crystal without cavity enhancement, we observe coherent conversion over an intrinsically broadband window of ~ 300 MHz. We further show that multiple exciton-polariton resonances inherit the magnon-coupled response, suggesting a route to broaden the usable optical detuning range and to mitigate optical dissipation. Our results establish magnon-coupled excitons in layered magnets as a scalable platform for broadband microwave-optical interfaces, with pathways to higher cooperativity via reduced magnetic volume and cavity integration. △ Less

Submitted 3 April, 2026; originally announced April 2026.

Comments: 19 pages, 4 figures

Ultrafast Formation and Annihilation of Strongly Bound, Anisotropic Excitons

Authors: Lawson T. Lloyd, Tommaso Pincelli, Mohamed Amine Wahada, Alessandro De Vita, Ferdinand Menzel, Kseniia Mosina, Túlio H. L. G. Castro, Alexander Neef, Andreas V. Stier, Nathan P. Wilson, Zdeněk Sofer, Jonathan J. Finley, Martin Wolf, Laurenz Rettig, Ralph Ernstorfer

Abstract: Van der Waals (vdW) layered materials with long-range magnetic order have the potential to enable novel optoelectronic and spintronic applications. Among these, CrSBr is an air-stable, direct band gap semiconductor that hosts interlayer antiferromagnetic order, a highly anisotropic electronic structure, and strongly bound excitons. In particular, excitons in CrSBr have been shown to inherit the qu… ▽ More Van der Waals (vdW) layered materials with long-range magnetic order have the potential to enable novel optoelectronic and spintronic applications. Among these, CrSBr is an air-stable, direct band gap semiconductor that hosts interlayer antiferromagnetic order, a highly anisotropic electronic structure, and strongly bound excitons. In particular, excitons in CrSBr have been shown to inherit the quasi-one-dimensional nature of the material and also couple to the underlying spinorder. However, mechanisms of exciton formation, dissociation, and interaction with free carriers remain largely unexplored, despite being crucial for spintronic and optoelectronic applications. Here, we employ time- and angle-resolved photoemission spectroscopy to map the electronic structure and excited state dynamics in CrSBr. We directly resolve an exceptionally large exciton binding energy (~800 meV) and a highly anisotropic momentum space distribution of the exciton, revealing its quasi-1D real-space character. We observe an excitation-density-dependent interconversion between bound excitons and quasi-free carriers on sub- to few-picosecond timescales, indicating that many-body effects govern the excited-state dynamics and optical properties during the initial stages of relaxation. Our work highlights the strongly bound, anisotropic character of excitons in CrSBr, as well as the microscopic interactions steering relaxation pathways after photoexcitation in elevated density regimes relevant for future device applications. △ Less

Submitted 25 August, 2026; v1 submitted 27 March, 2026; originally announced March 2026.

Optical Readout of Reconfigurable Layered Magnetic Domain Structure in CrSBr

Authors: Aleksandra Łopion, Pierre-Maurice Piel, Thomas Kliewer, Manuel Terbeck, Jan-Hendrik Larusch, Jakob Henz, Marie-Christin Heißenbüttel, Kseniia Mosina, Thorsten Deilmann, Michael Rohlfing, Zdenek Sofer, Ursula Wurstbauer

Abstract: The van der Waals magnetic semiconductor CrSBr combines multistable magnetic order with strong light--matter coupling, enabling optical access to a rich and reconfigurable layered magnetic domain structure. A purely optical, non-destructive, and non-contact readout of layered magnetic configurations is realized here by magneto-reflectance measurements and interpreted using an optical multilayer mo… ▽ More The van der Waals magnetic semiconductor CrSBr combines multistable magnetic order with strong light--matter coupling, enabling optical access to a rich and reconfigurable layered magnetic domain structure. A purely optical, non-destructive, and non-contact readout of layered magnetic configurations is realized here by magneto-reflectance measurements and interpreted using an optical multilayer model. The magnetic state is tunable by applied magnetic fields and by interfacing CrSBr with the antiferromagnet MnPS$_3$. Applying an external magnetic field along the easy axis drives the hysteretic antiferromagnetic--to--ferromagnetic transition, which is not universally binary but instead develops through a cascade of intermediate magnetic configurations whose multiplicity and stability scale systematically with layer thickness and can be tailored by magnetic interfaces. The intertwined optical and magnetic properties of CrSBr provide a readout mechanism for information encoded in and processed through its magnetic configuration that is compatible with modern on- and off-chip photonic and electronic technologies. These properties identify CrSBr as a promising platform for intelligent matter and for spin-optoelectronics, in particular for neuromorphic architectures that can learn and evolve in response to changing environments. △ Less

Submitted 20 April, 2026; v1 submitted 4 December, 2025; originally announced December 2025.

Comments: 10 pages, 4 figures, SI: 4 pages, 6 figures

Anisotropic Phonon Dynamics and Directional Transport in Actinide van der Waals Semiconductor USe$_3$

Authors: Aljoscha Söll, Valentino Jadrisko, Sourav Dey, Nassima Benchtaber, Kalyan Sarkar, Borna Radatovic, Jan Luxa, Fedor Lipilin, Kseniia Mosina, Vojtech Kundrat, Jakub Zalesak, Jana Vejpravova, Martin Zacek, Christoph Gadermaier, José J. Baldoví, Zdeněk Sofer

Abstract: Direction-dependent charge transport and optical responses are characteristic of van der Waals (vdW) materials with strong in-plane anisotropy. While transition-metal trichalcogenides (TMTCs) exemplify this behavior, heavier analogs remain largely unexplored. In this study we examine USe$_3$ as an anisotropic vdW material and a heavier analog of the well-studied TMTCs. We reveal strong in-plane an… ▽ More Direction-dependent charge transport and optical responses are characteristic of van der Waals (vdW) materials with strong in-plane anisotropy. While transition-metal trichalcogenides (TMTCs) exemplify this behavior, heavier analogs remain largely unexplored. In this study we examine USe$_3$ as an anisotropic vdW material and a heavier analog of the well-studied TMTCs. We reveal strong in-plane anisotropy using polarization-resolved Raman spectroscopy, investigate strain-induced shifts of phonon modes, and quantify direction-dependent charge-carrier mobility through transport measurements on field-effect devices. First-principles calculations based on density-functional theory corroborate our findings, providing a theoretical basis for our experimental observations. Casting USe$_3$ as an actinide analog of a TMTC establishes a platform for exploring low-dimensional semiconductors that combine strong in-plane anisotropy with f-electron physics. △ Less

Submitted 3 December, 2025; originally announced December 2025.

Space-Charge-Limited van der Waals Spin Transistor

Authors: Thomas K. M. Graham, Yu-Xuan Wang, Niranjana Renjith Nair, Kseniia Mosina, Kenji Watanabe, Takashi Taniguchi, Zdenek Sofer, Brian B. Zhou

Abstract: Integrating semiconducting and magnetic materials could combine transistor-like operation with nonvolatility and enable architectures such as logic-in-memory. Here, we employ correlated electrical transport and scanning nitrogen-vacancy (NV) center magnetic imaging to elucidate a spin transistor concept that amalgamates vertical and lateral hopping transport inside a 2D antiferromagnetic semicondu… ▽ More Integrating semiconducting and magnetic materials could combine transistor-like operation with nonvolatility and enable architectures such as logic-in-memory. Here, we employ correlated electrical transport and scanning nitrogen-vacancy (NV) center magnetic imaging to elucidate a spin transistor concept that amalgamates vertical and lateral hopping transport inside a 2D antiferromagnetic semiconductor, mechanistically distinct from vertical tunneling devices. Our device, based on a monolayer-bilayer junction in CrSBr, displays giant, gate-tunable magnetoresistance driven by the dual action of electrostatic doping on space-charge-limited lateral conduction and interlayer exchange coupling. Moreover, we visualize a field-trainable, layer-sharing effect that selects between coherent or domain-wall reversal at the spin-flip transition, enabling multilevel, memristive conductance states. Our layer-dependent space charge mechanism for convergent electrical and magnetic control opens opportunities to address limitations in contemporary computing. △ Less

Submitted 29 July, 2026; v1 submitted 2 December, 2025; originally announced December 2025.

Comments: 9 pages, 6 figures

Journal ref: Phys. Rev. Lett. 137, 040802 (2026)

Twist-tuned exchange and hysteresis in a bilayer van der Waals magnet

Authors: Priyanka Mondal, Sonu Verma, Wenze Lan, Lukas Krelle, Ryan Tan, Regine von Klitzing, Kenji Watanabe, Takashi Taniguchi, Kseniia Mosina, Zdenek Sofer, Akashdeep Kamra, Bernhard Urbaszek

Abstract: Moiré superlattices in twisted bilayers enable profound reconstructions of the electronic bandstructure, giving rise to correlated states with remarkable tunability. Extending this paradigm to van der Waals magnets, twisting creates spatially varying interlayer exchange interactions that stabilize emergent spin textures and the coexistence of ferromagnetic and antiferromagnetic domains. Here, we d… ▽ More Moiré superlattices in twisted bilayers enable profound reconstructions of the electronic bandstructure, giving rise to correlated states with remarkable tunability. Extending this paradigm to van der Waals magnets, twisting creates spatially varying interlayer exchange interactions that stabilize emergent spin textures and the coexistence of ferromagnetic and antiferromagnetic domains. Here, we demonstrate the emergence of robust magnetic hysteresis in bilayer CrSBr upon twisting by an angle of ~ 3°. This is observed as the corresponding hysteretic evolution of the exciton energy, that directly correlates with the bilayer magnetic state, in magnetic field dependent photoluminescence measurements. A two-sublattice model captures this behavior, attributing it to the twist-induced reduction of interlayer exchange that stabilizes both parallel and antiparallel spin configurations across a broad field range. Comparison with experiment enables quantitative extraction of the effective exchange strength. Remarkably, the system exhibits coherent averaging across the moiré supercell, yielding an effective monodomain response characterized by switching into the antiferromagnetic state, rather than forming spin textures or fragmented domains. Spatially resolved measurements further uncover local variations in hysteresis loops, consistent with position-dependent modulation of the average exchange interaction. Our results establish twist engineering as a powerful route to programmable magnetic memories in two-dimensional magnets, harnessing the robustness of antiferromagnetic order. △ Less

Submitted 9 October, 2025; originally announced October 2025.

Comments: Main and Supplement

Journal ref: Nature Communications 17, 75186 (2026)

Interplay of vibrational, electronic, and magnetic states in CrSBr

Authors: Daria I. Markina, Priyanka Mondal, Lukas Krelle, Sai Shradha, Mikhail M. Glazov, Regine von Klitzing, Kseniia Mosina, Zdenek Sofer, Bernhard Urbaszek

Abstract: The van der Waals antiferromagnet CrSBr exhibits coupling of vibrational, electronic, and magnetic degrees of freedom, giving rise to distinctive quasi-particle interactions. We investigate these interactions across a wide temperature range using polarization-resolved Raman spectroscopy at various excitation energies, complemented by optical absorption and photoluminescence excitation (PLE) spectr… ▽ More The van der Waals antiferromagnet CrSBr exhibits coupling of vibrational, electronic, and magnetic degrees of freedom, giving rise to distinctive quasi-particle interactions. We investigate these interactions across a wide temperature range using polarization-resolved Raman spectroscopy at various excitation energies, complemented by optical absorption and photoluminescence excitation (PLE) spectroscopy. Under 1.96 eV excitation, we observe pronounced changes in the A$_g^1$, A$_g^2$, and A$_g^3$ Raman modes near the Néel temperature, coinciding with modifications in the oscillator strength of excitonic transitions and clear resonances in PLE. The distinct temperature evolution of Raman tensor elements and polarization anisotropy for Raman modes indicates that they couple to different excitonic and electronic states. The suppression of the excitonic state's oscillation strength above the Néel temperature could be related to the magnetic phase transition, thereby connecting these excitonic states and Raman modes to a specific spin alignment. These observations make CrSBr a versatile platform for probing quasi-particle interactions in low-dimensional magnets and provide insights for applications in quantum sensing and quantum communication. △ Less

Submitted 12 September, 2025; originally announced September 2025.

Magneto-Excitonic Duality From Monolayer to Trilayer CrSBr

Authors: Igor Antoniazzi, Łucja Kipczak, Bruno Camargo, Gayatri, Chinmay Mohanty, Kseniia Mosina, Zdeněk Sofer, Adam Babiński, Arka Karmakar, Maciej R. Molas

Abstract: Two-dimensional (2D) layered magnetic materials (LMMs) are a newly emerging class of van der Waals materials, opening new opportunities to study magneto-excitonic coupling. The air-stable, structurally and optically anisotropic A-type antiferromagnetic chromium sulfur bromide (CrSBr) is one of the most prominent examples of such LMMs. We investigate photoluminescence (PL) and PL excitation of mono… ▽ More Two-dimensional (2D) layered magnetic materials (LMMs) are a newly emerging class of van der Waals materials, opening new opportunities to study magneto-excitonic coupling. The air-stable, structurally and optically anisotropic A-type antiferromagnetic chromium sulfur bromide (CrSBr) is one of the most prominent examples of such LMMs. We investigate photoluminescence (PL) and PL excitation of mono- to tri-layers CrSBr and find that it exhibits a unique duplexity, supporting both Frenkel- and Wannier-Mott-like excitons. Our magneto-optical experiments reveal a similar excitonic response from the mono- and trilayer systems and a completely different signature in the bilayer flake. This shows a different origin of the low-lying excitonic species (A, A', and B) in the band structure. We confirm the robustness of the magneto-excitonic coupling in few-layer CrSBr. Our work enables a more comprehensive exploration of the dual excitonic behavior in 2D materials. △ Less

Submitted 29 August, 2025; originally announced August 2025.

Comments: 9 pages, 5 figures

Report number: 2D Mater. 12 (2025) 045019

Exciton transport driven by spin excitations in an antiferromagnet

Authors: Florian Dirnberger, Sophia Terres, Zakhar A. Iakovlev, Kseniia Mosina, Zdenek Sofer, Akashdeep Kamra, Mikhail M. Glazov, Alexey Chernikov

Abstract: A new class of optical quasiparticles called magnetic excitons recently emerged in magnetic van der Waals materials. Akin to the highly effective strategies developed for electrons, the strong interactions of these excitons with the spin degree of freedom may provide innovative solutions for long-standing challenges in optics, such as steering the flow of energy and information. Here, we demonstra… ▽ More A new class of optical quasiparticles called magnetic excitons recently emerged in magnetic van der Waals materials. Akin to the highly effective strategies developed for electrons, the strong interactions of these excitons with the spin degree of freedom may provide innovative solutions for long-standing challenges in optics, such as steering the flow of energy and information. Here, we demonstrate transport of excitons by spin excitations in the van der Waals antiferromagnetic semiconductor CrSBr. Key results of our study are the observations of ultrafast, nearly isotropic exciton propagation substantially enhanced at the Neel temperature, transient contraction and expansion of the exciton clouds at low temperatures, as well as superdiffusive behavior in bilayer samples. These signatures largely defy description by commonly known exciton transport mechanisms and are related to the currents of incoherent magnons induced by laser excitation instead. We propose that the drag forces exerted by these currents can effectively imprint characteristic properties of spin excitations onto the motion of excitons. The universal nature of the underlying exciton-magnon scattering promises driving of excitons by magnons in other magnetic semiconductors and even in non-magnetic materials by proximity in heterostructures, merging the rich physics of magneto-transport with optics and photonics. △ Less

Submitted 10 July, 2025; v1 submitted 9 July, 2025; originally announced July 2025.

Comments: 12 pages, 4 main figures

Journal ref: Nat. Nanotechnol. 21, 65-70 (2026)

Distinct Magneto-Optical Response of Frenkel and Wannier Excitons in CrSBr

Authors: Maciej Smiertka, Michal Rygala, Katarzyna Posmyk, Paulina Peksa, Mateusz Dyksik, Dimitar Pashov, Kseniia Mosina, Zdenek Sofer, Mark van Schilfgaarde, Florian Dirnberger, Michal Baranowski, Swagata Acharya, Paulina Plochocka

Abstract: This study shows that CrSBr hosts Frenkel-like and Wannier-Mott-like excitons whose distinct spatial character explains their contrasting sensitivity to magnetic order and lattice vibrations, challenging the standard dichotomy in describing excitons. This study shows that CrSBr hosts Frenkel-like and Wannier-Mott-like excitons whose distinct spatial character explains their contrasting sensitivity to magnetic order and lattice vibrations, challenging the standard dichotomy in describing excitons. △ Less

Submitted 22 January, 2026; v1 submitted 19 June, 2025; originally announced June 2025.

ACM Class: J.2

Defect complexes in CrSBr revealed through electron microscopy and deep learning

Authors: Mads Weile, Sergii Grytsiuk, Aubrey Penn, Daniel G. Chica, Xavier Roy, Kseniia Mosina, Zdenek Sofer, Jakob Schiøtz, Stig Helveg, Malte Rösner, Frances M. Ross, Julian Klein

Abstract: Atomic defects underpin the properties of van der Waals materials, and their understanding is essential for advancing quantum and energy technologies. Scanning transmission electron microscopy is a powerful tool for defect identification in atomically thin materials, and extending it to multilayer and beam-sensitive materials would accelerate their exploration. Here we establish a comprehensive de… ▽ More Atomic defects underpin the properties of van der Waals materials, and their understanding is essential for advancing quantum and energy technologies. Scanning transmission electron microscopy is a powerful tool for defect identification in atomically thin materials, and extending it to multilayer and beam-sensitive materials would accelerate their exploration. Here we establish a comprehensive defect library in a bilayer of the magnetic quasi-1D semiconductor CrSBr by combining atomic-resolution imaging, deep learning, and ab-initio calculations. We apply a custom-developed machine learning work flow to detect, classify and average point vacancy defects. This classification enables us to uncover several distinct Cr interstitial defect complexes, combined Cr and Br vacancy defect complexes and lines of vacancy defects that extend over many unit cells. We show that their occurrence is in agreement with our computed structures and binding energy densities, reflecting the intriguing layer interlocked crystal structure of CrSBr. Our ab-initio calculations show that the interstitial defect complexes give rise to highly localized electronic states. These states are of particular interest due to the reduced electronic dimensionality and magnetic properties of CrSBr and are furthermore predicted to be optically active. Our results broaden the scope of defect studies in challenging materials and reveal new defect types in bilayer CrSBr that can be extrapolated to the bulk and to over 20 materials belonging to the same FeOCl structural family. △ Less

Submitted 9 June, 2025; originally announced June 2025.

Comments: main: 13 pages, 6 figures, 1 table; SM: 32 pages, 25 figures, 4 tables

Journal ref: Phys. Rev. X 15, 021080 (2025)

Magnetic control of an exciton-polariton condensate in a van der Waals magnet

Authors: Heng Zhang, Niloufar Nilforoushan, Christian Weidgans, Tobias Inzenhofer, Marlene Liebich, Josef Riepl, Julian Hirschmann, Imke Gronwald, Kseniia Mosina, Zdeněk Sofer, Ritaj Tyagi, Jan Wilhelm, Fabian Mooshammer, Florian Dirnberger, Rupert Huber

Abstract: Quasiparticle condensates are among the most spectacular solid-state manifestations of quantum physics. Coupling macroscopic real-space wavefunctions to additional degrees of freedom, such as the electron spin, would add valuable control knobs for quantum applications. While creating spin-carrying superconducting condensates has attracted enormous attention, man-made condensates of light-matter hy… ▽ More Quasiparticle condensates are among the most spectacular solid-state manifestations of quantum physics. Coupling macroscopic real-space wavefunctions to additional degrees of freedom, such as the electron spin, would add valuable control knobs for quantum applications. While creating spin-carrying superconducting condensates has attracted enormous attention, man-made condensates of light-matter hybrids known as exciton-polaritons have lacked an analogous spin-based perspective. Here we open a new door by demonstrating magnetically tunable exciton-polariton condensation in the van der Waals magnet CrSBr. Under photoexcitation, CrSBr microwires embedded in an optical cavity show the hallmarks of polariton condensation: a dramatic increase of the emission intensity from an excited laterally confined polariton state by multiple orders of magnitude, spectral narrowing of the emission line, and a continuous shift of the peak energy. Interferometry evidences an increase in spatial and temporal coherence. Owing to the strong coupling between the spin order and excitonic correlation, the energy of the condensate can be tuned by up to 10.5 meV by an external magnetic field of only 2 Tesla. Our results establish CrSBr microcavities as a powerful platform for exploring magnetic control of polariton condensates and mark a significant step toward spin-controlled coherent quantum light sources. △ Less

Submitted 13 June, 2026; v1 submitted 6 June, 2025; originally announced June 2025.

Lithium Intercalation in the Anisotropic van der Waals Magnetic Semiconductor CrSBr

Authors: Kseniia Mosina, Aljoscha Söll, Jiri Sturala, Martin Veselý, Petr Levinský, Florian Dirnberger, Giuliana Materzanini, Nicola Marzari, Gian-Marco Rignanese, Borna Radatović, David Sedmidubsky, Zdeněk Sofer

Abstract: Alkali metal intercalation is an important strategy for doping van der Waals materials. Lithium, in particular, was shown to achieve exceptional charge carrier densities, reaching levels at which fundamental electrical, optical, and magnetic material properties begin to be strongly modified. While lithium is known to be highly volatile, its migration dynamics in anisotropic layered crystals remain… ▽ More Alkali metal intercalation is an important strategy for doping van der Waals materials. Lithium, in particular, was shown to achieve exceptional charge carrier densities, reaching levels at which fundamental electrical, optical, and magnetic material properties begin to be strongly modified. While lithium is known to be highly volatile, its migration dynamics in anisotropic layered crystals remain poorly understood. In this work, we investigate the intercalation of lithium in-between layers of the anisotropic magnetic semiconductor CrSBr. Using exfoliated crystals, we are able to monitor the dynamics of the intercalation process in real time through optical and electrical characterization methods. Our measurements reveal highly anisotropic migration of Lithium characterized by diffusion coefficients that differ by more than one order of magnitude along a- and b-directions. This finding is in good agreement with our molecular dynamics simulations which show trajectories of lithium atoms primarily follow the Br-chains in the a-direction. Beyond that, we find that partially covering CrSBr crystals by thin hexagonal boron nitride (hBN) flakes has a significant impact on the intercalation process, and that lithium strongly enhances the electrical conductivity along the a-axis. Our method offers a new platform for lithium diffusion studies and encourages further research to pursue the fabrication of lithium-doped devices. △ Less

Submitted 21 May, 2025; originally announced May 2025.

All-electrical near-field injection of excitons in a van der Waals antiferromagnet

Authors: Jonas D. Ziegler, Sotirios Papadopoulos, Antti J. Moilanen, Marcelo M. Valenzuela, Qia Lin, Kseniia Mosina, Takashi Taniguchi, Kenji Watanabe, Zdenek Sofer, Florian Dirnberger, Lukas Novotny

Abstract: Van der Waals materials have become a promising building block for future electronics and photonics. The two-dimensional magnet CrSBr came into the spotlight of solid state research due to its intriguing combination of antiferromagnetic order, strong light-matter coupling and unusual quasi-1D electronic bandstructure. This study reports the electrical excitation of excitons in CrSBr layers from cr… ▽ More Van der Waals materials have become a promising building block for future electronics and photonics. The two-dimensional magnet CrSBr came into the spotlight of solid state research due to its intriguing combination of antiferromagnetic order, strong light-matter coupling and unusual quasi-1D electronic bandstructure. This study reports the electrical excitation of excitons in CrSBr layers from cryogenic temperatures up to room temperature. By exploiting the energy transfer via tunneling electrons in a graphene tunnel junction strongly bound excitons are excited in proximate CrSBr layers. This facilitates electrically-excited emission from CrSBr crystals ranging in thickness from a bilayer up to 250 nm, in which the strong linear polarization of the electroluminescence confirms the excitonic origin. For thicker layers, clear evidence for the electrically excited emission from self-hybridized exciton polaritons is observed, highlighting the strong coupling between optical excitations and confined photon modes in CrSBr. These results pave the way for future applications in spintronic and optical readout of magnetic properties. △ Less

Submitted 21 May, 2025; originally announced May 2025.

Magnetically Modulated Electrical Switching in an Antiferromagnetic Transistor

Authors: Chung-Tao Chou, Eugene Park, Josep Ingla-Aynes, Julian Klein, Kseniia Mosina, Jagadeesh S. Moodera, Zdenek Sofer, Frances M. Ross, Luqiao Liu

Abstract: A spin version of transistor, where magnetism is used to influence electrical behaviors of the semiconductor, has been a long-pursued device concept in spintronics. In this work, we experimentally study a field-effect transistor with CrSBr, a van der Waals (vdW) antiferromagnetic semiconductor, as the channel material. Unlike the weak magnetic tunability of in-plane currents previously reported in… ▽ More A spin version of transistor, where magnetism is used to influence electrical behaviors of the semiconductor, has been a long-pursued device concept in spintronics. In this work, we experimentally study a field-effect transistor with CrSBr, a van der Waals (vdW) antiferromagnetic semiconductor, as the channel material. Unlike the weak magnetic tunability of in-plane currents previously reported in vdW magnets, the channel current of our transistor is efficiently tuned by both gate voltage and magnetic transitions, achieving a magnetoresistance ratio as high as 1500%. Combining measurement and theoretical modeling, we reveal magnetically modulated carrier concentration as the origin of the large magnetoresistance. The strategy of using both magnetic ordering and electric field in the same device to control ON/OFF states of a transistor opens a new avenue of energy-efficient spintronics for memory, logic and magnetic sensing applications. △ Less

Submitted 13 May, 2025; originally announced May 2025.

Magnetic Correlation Spectroscopy in CrSBr

Authors: Lukas Krelle, Ryan Tan, Daria Markina, Priyanka Mondal, Kseniia Mosina, Kevin Hagmann, Regine von Klitzing, Kenji Watanabe, Takashi Taniguchi, Zdenek Sofer, Bernhard Urbaszek

Abstract: CrSBr is an air-stable magnetic van der Waals semiconductor with strong magnetic anisotropy, where the interaction of excitons with the magnetic order enables the optical identification of different magnetic phases. Here, we study the magnetic anisotropy of multi-layer CrSBr inside a three-axis vector magnet and correlate magnetic order and optical transitions in emission and absorption. We identi… ▽ More CrSBr is an air-stable magnetic van der Waals semiconductor with strong magnetic anisotropy, where the interaction of excitons with the magnetic order enables the optical identification of different magnetic phases. Here, we study the magnetic anisotropy of multi-layer CrSBr inside a three-axis vector magnet and correlate magnetic order and optical transitions in emission and absorption. We identify layer by layer switching of the magnetization through drastic changes of the optical emission and absorption energy and strength as a function of the applied magnetic field. We correlate optical transitions in reflection spectra with photoluminescence (PL) emission using a transfer-matrix analysis and find that ferromagnetic and antiferromagnetic order between layers can coexist in the same crystal. In the multi-peak PL emission the intensity of energetically lower lying transitions reduces monotonously with increasing field strength whereas energetically higher lying transitions around the bright exciton $X_B$ brighten close to the saturation field. Using this contrasting behavior we can therefore correlate transitions with each other. △ Less

Submitted 11 March, 2025; originally announced March 2025.

Comments: 7 pages, 7 figures

Journal ref: ACS Nano 2025, 19, 37, 33156

Resonance Raman Scattering and Anomalous Anti-Stokes Phenomena in CrSBr

Authors: Satyam Sahu, Charlotte Berrezueta-Palacios, Sabrina Juergensen, Kseniia Mosina, Zdeněk Sofer, Matěj Velický, Patryk Kusch, Otakar Frank

Abstract: CrSBr, a van der Waals material, stands out as an air-stable magnetic semiconductor with appealing intrinsic properties such as crystalline anisotropy, quasi-1D electronic characteristics, layer-dependent antiferromagnetism, and non-linear optical effects. In this study, we investigate the differences between the absorption and emission spectra, focusing on the origin of the emission peak near 1.7… ▽ More CrSBr, a van der Waals material, stands out as an air-stable magnetic semiconductor with appealing intrinsic properties such as crystalline anisotropy, quasi-1D electronic characteristics, layer-dependent antiferromagnetism, and non-linear optical effects. In this study, we investigate the differences between the absorption and emission spectra, focusing on the origin of the emission peak near 1.7 eV observed in the photoluminescence spectrum of CrSBr. Our findings are corroborated by excitation-dependent Raman experiments. Additionally, we explore the anti-Stokes Raman spectra and observe an anomalously high anti-Stokes to Stokes intensity ratio of up to 0.8, which varies significantly with excitation laser power and crystallographic orientation relative to the polarization of the scattered light. This ratio is notably higher than that observed in graphene ($\approx$ 0.1) and MoS$_2$ ($\approx$ 0.4), highlighting the unique vibrational and electronic interactions in CrSBr. Lastly, we examine stimulated Raman scattering and calculate the Raman gain in CrSBr, which attains a value of 1 $\times$ 10$^{8}$ cm/GW, nearly four orders of magnitude higher than that of previously studied three-dimensional systems. △ Less

Submitted 15 May, 2025; v1 submitted 3 February, 2025; originally announced February 2025.

Comments: 8 pages, 4 figures

Journal ref: Nanoscale 17(18), 11539-46 (2025)

Raman Polarization Switching in CrSBr

Authors: Priyanka Mondal, Daria I. Markina, Lennard Hopf, Lukas Krelle, Sai Shradha, Julian Klein, Mikhail M. Glazov, Iann Gerber, Kevin Hagmann, Regine v. Klitzing, Kseniia Mosina, Zdenek Sofer, Bernhard Urbaszek

Abstract: Semiconducting CrSBr is a layered A-type antiferromagnet, with individual layers antiferromagnetically coupled along the stacking direction. Due to its unique orthorhombic crystal structure, CrSBr exhibits highly anisotropic mechanical and optoelectronic properties acting itself as a quasi-1D material. CrSBr demonstrates complex coupling phenomena involving phonons, excitons, magnons, and polarito… ▽ More Semiconducting CrSBr is a layered A-type antiferromagnet, with individual layers antiferromagnetically coupled along the stacking direction. Due to its unique orthorhombic crystal structure, CrSBr exhibits highly anisotropic mechanical and optoelectronic properties acting itself as a quasi-1D material. CrSBr demonstrates complex coupling phenomena involving phonons, excitons, magnons, and polaritons. Here we show through polarization-resolved resonant Raman scattering the intricate interaction between the vibrational and electronic properties of CrSBr. For samples spanning from few-layer to bulk thickness, we observe that the polarization of the A$_g^2$ Raman mode can be rotated by 90 degrees, shifting from alignment with the crystallographic a (intermediate magnetic) axis to the b (easy magnetic) axis, depending on the excitation energy. In contrast, the A$_g^1$ and A$_g^3$ modes consistently remain polarized along the b axis, regardless of the laser energy used. We access real and imaginary parts of the Raman tensor in our analysis, uncovering resonant electron-phonon coupling. △ Less

Submitted 29 October, 2024; originally announced October 2024.

Comments: Main text + Supplementary Information

Magnon-mediated exciton-exciton interaction in a van der Waals antiferromagnet

Authors: Biswajit Datta, Pratap Chandra Adak, Sichao Yu, Agneya V. Dharmapalan, Siedah J. Hall, Anton Vakulenko, Filipp Komissarenko, Egor Kurganov, Jiamin Quan, Wei Wang, Kseniia Mosina, Zdeněk Sofer, Dimitar Pashov, Mark van Schilfgaarde, Swagata Acharya, Akashdeep Kamra, Matthew Y. Sfeir, Andrea Alù, Alexander B. Khanikaev, Vinod M. Menon

Abstract: Excitons are fundamental excitations that govern the optical properties of semiconductors. Interacting excitons can lead to various emergent phases of matter and large nonlinear optical responses. In most semiconductors, excitons interact via exchange interaction or phase space filling. Correlated materials that host excitons coupled to other degrees of freedom offer hitherto unexplored pathways f… ▽ More Excitons are fundamental excitations that govern the optical properties of semiconductors. Interacting excitons can lead to various emergent phases of matter and large nonlinear optical responses. In most semiconductors, excitons interact via exchange interaction or phase space filling. Correlated materials that host excitons coupled to other degrees of freedom offer hitherto unexplored pathways for controlling these interactions. Here, we demonstrate magnon-mediated excitonic interactions in CrSBr, an antiferromagnetic semiconductor. This interaction manifests as the dependence of exciton energy on exciton density via a magnonic adjustment of the spin canting angle. Our study demonstrates the emergence of quasiparticle-mediated interactions in correlated quantum materials, leading to large nonlinear optical responses and potential device concepts such as magnon-mediated quantum transducers. △ Less

Submitted 27 September, 2024; originally announced September 2024.

Comments: 33 pages, 14 figures

Journal ref: Nature Materials (2025)

Colossal magneto-excitonic effects in 2D van der Waals magnetic semiconductor CrSBr

Authors: R. Komar, M. Goryca, A. Łopion, M. Rybak, T. Woźniak, M. Raczyński, K. M. Gałązka, K. Mosina, A. Söll, Z. Sofer, W. Pacuski, C. Faugeras, M. Birowska, P. Kossacki, T. Kazimierczuk

Abstract: 2D magnetic semiconductors, which intrinsically couple a rich landscape of magnetic orders with tightly bound electron-hole pairs (excitons), present an exciting platform to investigate the interplay between optical and magnetic phenomena at the atomic scale. In such systems, the strength of magneto-optical effects determines how deeply the magnetic properties can be revealed. Here, we report the… ▽ More 2D magnetic semiconductors, which intrinsically couple a rich landscape of magnetic orders with tightly bound electron-hole pairs (excitons), present an exciting platform to investigate the interplay between optical and magnetic phenomena at the atomic scale. In such systems, the strength of magneto-optical effects determines how deeply the magnetic properties can be revealed. Here, we report the observation of remarkably strong magneto-excitonic effects in the 2D magnetic semiconductor CrSBr that allow probing its magnetic order with unprecedented sensitivity. By investigating optical transitions above the fundamental exciton energy, we discover a massive spectral shift approaching 100 meV under applied magnetic fields - an order of magnitude larger than previously observed magneto-excitonic responses. Our comprehensive magneto-optical experiments accompanied by detailed DFT calculations indicate the possible origin of the transitions exhibiting such intriguing behavior. These findings open avenues for exploiting magneto-excitonic phenomena at newly accessible regimes, enabling novel opto-spintronic applications previously limited by weak magnetic responses. △ Less

Submitted 8 June, 2026; v1 submitted 30 August, 2024; originally announced September 2024.

Comments: list of authors updated; in review in Nature Communications, Supplementary Material included

Phonon and magnon dynamics across antiferromagnetic transition in 2D layered van der Waals material CrSBr

Authors: E. Uykur, A. A. Tsirlin, F. Long, M. Wenzel, M. Dressel, K. Mosina, Z. Sofer, M. Helm, S. Zhou

Abstract: We report temperature-dependent reflectivity spectra of the layered van der Waals magnet CrSBr in the far-infrared region. Polarization-dependent measurements resolve the vibrational modes along the E$\|a$- and $b$-axes and reveal the clear structural anisotropy. While the $a$-axis phonons notably harden on cooling, the $b$-axis phonon frequencies are almost temperature-independent. A phonon split… ▽ More We report temperature-dependent reflectivity spectra of the layered van der Waals magnet CrSBr in the far-infrared region. Polarization-dependent measurements resolve the vibrational modes along the E$\|a$- and $b$-axes and reveal the clear structural anisotropy. While the $a$-axis phonons notably harden on cooling, the $b$-axis phonon frequencies are almost temperature-independent. A phonon splitting due to the antiferromagnetic phase transition is observed for the 180~cm$^{-1}$ $a$-axis vibrational mode, accompanied by a phonon softening below $T_N$. Furthermore, an additional mode with strong magnetic characteristics at $\sim$360~cm$^{-1}$ is identified and attributed to the magnon excitation of CrSBr. △ Less

Submitted 13 May, 2024; originally announced May 2024.

Comments: 6 pages, 3 figures

Journal ref: Phys. Rev. B 111, 174434 (2025)

Doping-control of excitons and magnetism in few-layer CrSBr

Authors: Farsane Tabataba-Vakili, Huy P. G. Nguyen, Anna Rupp, Kseniia Mosina, Anastasios Papavasileiou, Kenji Watanabe, Takashi Taniguchi, Patrick Maletinsky, Mikhail M. Glazov, Zdenek Sofer, Anvar S. Baimuratov, Alexander Högele

Abstract: Magnetism in two-dimensional materials reveals phenomena distinct from bulk magnetic crystals, with sensitivity to charge doping and electric fields in monolayer and bilayer van der Waals magnet CrI3. Within the class of layered magnets, semiconducting CrSBr stands out by featuring stability under ambient conditions, correlating excitons with magnetic order and thus providing strong magnon-exciton… ▽ More Magnetism in two-dimensional materials reveals phenomena distinct from bulk magnetic crystals, with sensitivity to charge doping and electric fields in monolayer and bilayer van der Waals magnet CrI3. Within the class of layered magnets, semiconducting CrSBr stands out by featuring stability under ambient conditions, correlating excitons with magnetic order and thus providing strong magnon-exciton coupling, and exhibiting peculiar magneto-optics of exciton-polaritons. Here, we demonstrate that both exciton and magnetic transitions in bilayer and trilayer CrSBr are sensitive to voltage-controlled field-effect charging, exhibiting bound exciton-charge complexes and doping-induced metamagnetic transitions. Moreover, we demonstrate how these unique properties enable optical probes of local magnetic order, visualizing magnetic domains of competing phases across metamagnetic transitions induced by magnetic field or electrostatic doping. Our work identifies few-layer CrSBr as a rich platform for exploring collaborative effects of charge, optical excitations, and magnetism. △ Less

Submitted 8 June, 2024; v1 submitted 18 December, 2023; originally announced December 2023.

Comments: 18 pages, 11 figures

Journal ref: Nat. Commun. 15, 4735 (2024)

Valley Polarization-Electric Dipole Interference and Nonlinear Chiral Selection Rules in Monolayer WSe$_2$

Authors: Paul Herrmann, Sebastian Klimmer, Till Weickhardt, Anastasios Papavasileiou, Kseniia Mosina, Zdeněk Sofer, Ioannis Paradisanos, Daniil Kartashov, Giancarlo Soavi

Abstract: In monolayer transition metal dichalcogenides time-reversal symmetry, combined with space-inversion symmetry, defines the spin-valley degree of freedom. As such, engineering and control of time-reversal symmetry by optical or magnetic fields constitutes the foundation of valleytronics. Here, we propose a new approach for the detection of broken time-reversal symmetry and valley polarization in mon… ▽ More In monolayer transition metal dichalcogenides time-reversal symmetry, combined with space-inversion symmetry, defines the spin-valley degree of freedom. As such, engineering and control of time-reversal symmetry by optical or magnetic fields constitutes the foundation of valleytronics. Here, we propose a new approach for the detection of broken time-reversal symmetry and valley polarization in monolayer WSe$_2$ based on second harmonic generation. Our method can selectively and simultaneously generate and detect a valley polarization at the $\pm K$ valleys of transition metal dichalcogenides at room temperature. Furthermore, it allows to measure the interference between the real and imaginary parts of the intrinsic (electric dipole) and valley terms of the second order nonlinear susceptibility. This work demonstrates the potential and unique capabilities of nonlinear optics as a probe of broken time-reversal symmetry and as a tool for ultrafast and non-destructive valleytronic operations. △ Less

Submitted 25 October, 2023; originally announced October 2023.

Comments: 27 pages 6 figures

Intrinsic magnetic properties of the layered antiferromagnet CrSBr

Authors: Fangchao Long, Kseniia Mosina, René Hübner, Zdenek Sofer, Julian Klein, Slawomir Prucnal, Manfred Helm, Florian Dirnberger, Shengqiang Zhou

Abstract: Van der Waals magnetic materials are an ideal platform to study low-dimensional magnetism. Opposed to other members of this family, the magnetic semiconductor CrSBr is highly resistant to degradation in air, which, besides its exceptional optical, electronic, and magnetic properties, is the reason the compound is receiving considerable attention at the moment. For many years, its magnetic phase di… ▽ More Van der Waals magnetic materials are an ideal platform to study low-dimensional magnetism. Opposed to other members of this family, the magnetic semiconductor CrSBr is highly resistant to degradation in air, which, besides its exceptional optical, electronic, and magnetic properties, is the reason the compound is receiving considerable attention at the moment. For many years, its magnetic phase diagram seemed to be well-understood. Recently, however, several groups observed a magnetic transition in magnetometry measurements at temperatures of around 40 K that is not expected from theoretical considerations, causing a debate about the intrinsic magnetic properties of the material. In this letter, we report the absence of this particular transition in magnetization measurements conducted on high-quality CrSBr crystals, attesting to the extrinsic nature of the low-temperature magnetic phase observed in other works. Our magnetometry results obtained from large bulk crystals are in very good agreement with the magnetic phase diagram of CrSBr previously predicted by the mean-field theory; A-type antiferromagnetic order is the only phase observed below the Néel temperature at TN = 131 K. Moreover, numerical fits based on the Curie-Weiss law confirm that strong ferromagnetic correlations are present within individual layers even at temperatures much larger than TN. △ Less

Submitted 9 September, 2023; originally announced September 2023.

Comments: 13 pages, submitted to Appl. Phys. Lett

Journal ref: Appl. Phys. Lett. 123, 222401 (2023)

A high-$κ$ wide-gap layered dielectric for two-dimensional van der Waals heterostructures

Authors: A. Söll, E. Lopriore, A. K. Ottesen, J. Luxa, G. Pasquale, J. Sturala, F. Hájek, V. Jarý, D. Sedmidubský, K. Mosina, A. Kis, Z. Sofer

Abstract: Van der Waals heterostructures of two-dimensional materials have opened up new frontiers in condensed matter physics, unlocking unexplored possibilities in electronic and photonic device applications. However, the investigation of wide-gap high-$κ$ layered dielectrics for devices based on van der Waals structures has been relatively limited. In this work, we demonstrate an easily reproducible synt… ▽ More Van der Waals heterostructures of two-dimensional materials have opened up new frontiers in condensed matter physics, unlocking unexplored possibilities in electronic and photonic device applications. However, the investigation of wide-gap high-$κ$ layered dielectrics for devices based on van der Waals structures has been relatively limited. In this work, we demonstrate an easily reproducible synthesis method for the rare earth oxyhalide LaOBr, and we exfoliate it as a 2D layered material with a measured static dielectric constant of $ε_{0, \perp} \simeq 9$ and a wide bandgap of 5.3 eV. Furthermore, our research demonstrates that LaOBr can be used as a high-$κ$ dielectric in van der Waals field-effect transistors with high performance and low interface defect concentrations. Additionally, it proves to be an attractive choice for electrical gating in excitonic devices based on 2D materials. Our work demonstrates the versatile realization and functionality of 2D systems with wide-gap and high-$κ$ van der Waals dielectric environments. △ Less

Submitted 25 July, 2023; originally announced July 2023.

Charge transfer-induced Lifshitz transition and magnetic symmetry breaking in ultrathin CrSBr crystals

Authors: Marco Bianchi, Kimberly Hsieh, Esben Juel Porat, Florian Dirnberger, Julian Klein, Kseniia Mosina, Zdenek Sofer, Alexander N. Rudenko, Mikhail I. Katsnelson, Yong P. Chen, Malte Rösner, Philip Hofmann

Abstract: Ultrathin CrSBr flakes are exfoliated \emph{in situ} on Au(111) and Ag(111) and their electronic structure is studied by angle-resolved photoemission spectroscopy. The thin flakes' electronic properties are drastically different from those of the bulk material and also substrate-dependent. For both substrates, a strong charge transfer to the flakes is observed, partly populating the conduction ban… ▽ More Ultrathin CrSBr flakes are exfoliated \emph{in situ} on Au(111) and Ag(111) and their electronic structure is studied by angle-resolved photoemission spectroscopy. The thin flakes' electronic properties are drastically different from those of the bulk material and also substrate-dependent. For both substrates, a strong charge transfer to the flakes is observed, partly populating the conduction band and giving rise to a highly anisotropic Fermi contour with an Ohmic contact to the substrate. The fundamental CrSBr band gap is strongly renormalized compared to the bulk. The charge transfer to the CrSBr flake is substantially larger for Ag(111) than for Au(111), but a rigid energy shift of the chemical potential is insufficient to describe the observed band structure modifications. In particular, the Fermi contour shows a Lifshitz transition, the fundamental band gap undergoes a transition from direct on Au(111) to indirect on Ag(111) and a doping-induced symmetry breaking between the intra-layer Cr magnetic moments further modifies the band structure. Electronic structure calculations can account for non-rigid Lifshitz-type band structure changes in thin CrSBr as a function of doping and strain. In contrast to undoped bulk band structure calculations that require self-consistent $GW$ theory, the doped thin film properties are well-approximated by density functional theory if local Coulomb interactions are taken into account on the mean-field level and the charge transfer is considered. △ Less

Submitted 24 July, 2023; originally announced July 2023.

Journal ref: Physical Review B 108, 195410 (2023)

Ferromagnetic interlayer coupling in CrSBr crystals irradiated by ions

Authors: Fangchao Long, Mahdi Ghorbani-Asl, Kseniia Mosina, Yi Li, Kaiman Lin, Fabian Ganss, René Hübner, Zdenek Sofer, Florian Dirnberger, Akashdeep Kamra, Arkady V. Krasheninnikov, Slawomir Prucnal, Manfred Helm, Shengqiang Zhou

Abstract: Layered magnetic materials are becoming a major platform for future spin-based applications. Particularly the air-stable van der Waals compound CrSBr is attracting considerable interest due to its prominent magneto-transport and magneto-optical properties. In this work, we observe a transition from antiferromagnetic to ferromagnetic behavior in CrSBr crystals exposed to high-energy, non-magnetic i… ▽ More Layered magnetic materials are becoming a major platform for future spin-based applications. Particularly the air-stable van der Waals compound CrSBr is attracting considerable interest due to its prominent magneto-transport and magneto-optical properties. In this work, we observe a transition from antiferromagnetic to ferromagnetic behavior in CrSBr crystals exposed to high-energy, non-magnetic ions. Already at moderate fluences, ion irradiation induces a remanent magnetization with hysteresis adapting to the easy-axis anisotropy of the pristine magnetic order up to a critical temperature of 110 K. Structure analysis of the irradiated crystals in conjunction with density functional theory calculations suggest that the displacement of constituent atoms due to collisions with ions and the formation of interstitials favors ferromagnetic order between the layers. △ Less

Submitted 27 September, 2023; v1 submitted 30 May, 2023; originally announced May 2023.

Comments: 25 pages including the supporting information, published as Nano Lett. 23, 8468-8473 (2023)

Journal ref: Nano Lett. 23, 8468-8473 (2023)

Optical markers of magnetic phase transition in CrSBr

Authors: W. M. Linhart, M. Rybak, M. Birowska, K. Mosina, V. Mazanek, P. Scharoch, D. Kaczorowski, Z. Sofer, R. Kudrawiec

Abstract: Here, we investigate the role of the interlayer magnetic ordering of CrSBr in the framework of $\textit{ab initio}$ calculations and by using optical spectroscopy techniques. These combined studies allow us to unambiguously determine the nature of the optical transitions. In particular, photoreflectance measurements, sensitive to the direct transitions, have been carried out for the first time. We… ▽ More Here, we investigate the role of the interlayer magnetic ordering of CrSBr in the framework of $\textit{ab initio}$ calculations and by using optical spectroscopy techniques. These combined studies allow us to unambiguously determine the nature of the optical transitions. In particular, photoreflectance measurements, sensitive to the direct transitions, have been carried out for the first time. We have demonstrated that optically induced band-to-band transitions visible in optical measurement are remarkably well assigned to the band structure by the momentum matrix elements and energy differences for the magnetic ground state (A-AFM). In addition, our study reveals significant differences in electronic properties for two different interlayer magnetic phases. When the magnetic ordering of A-AFM to FM is changed, the crucial modification of the band structure reflected in the direct-to-indirect band gap transition and the significant splitting of the conduction bands along the $Γ-Z$ direction are obtained. In addition, Raman measurements demonstrate a splitting between the in-plane modes $B^2_{2g}$/$B^2_{3g}$, which is temperature dependent and can be assigned to different interlayer magnetic states, corroborated by the DFT+U study. Moreover, the $B^2_{2g}$ mode has not been experimentally observed before. Finally, our results point out the origin of interlayer magnetism, which can be attributed to electronic rather than structural properties. Our results reveal a new approach for tuning the optical and electronic properties of van der Waals magnets by controlling the interlayer magnetic ordering in adjacent layers. △ Less

Submitted 31 March, 2023; originally announced March 2023.

Comments: 33 pages, 15 figures

Magneto-optical sensing of the pressure driven magnetic ground states in bulk CrSBr

Authors: A. Pawbake, T. Pelini, I. Mohelsky, D. Jana, I. Breslavetz, C. -W. Cho, M. Orlita, M. Potemski, M. -A. Measson, N. Wilson, K. Mosina, A. Soll, Z. Sofer, B. A. Piot, M. E. Zhitomirsky, C. Faugeras

Abstract: Competition between exchange interactions and magnetocrystalline anisotropy may bring new magnetic states that are of great current interest. An applied hydrostatic pressure can further be used to tune their balance. In this work we investigate the magnetization process of a biaxial antiferromagnet in an external magnetic field applied along the easy axis. We find that the single metamagnetic tran… ▽ More Competition between exchange interactions and magnetocrystalline anisotropy may bring new magnetic states that are of great current interest. An applied hydrostatic pressure can further be used to tune their balance. In this work we investigate the magnetization process of a biaxial antiferromagnet in an external magnetic field applied along the easy axis. We find that the single metamagnetic transition of the Ising type observed in this material under ambient pressure transforms under hydrostatic pressure into two transitions, a first-order spin flop transition followed by a second order transition towards a polarized ferromagnetic state near saturation. This reversible tuning into a new magnetic phase is obtained in layered bulk CrSBr at low temperature by varying the interlayer distance using high hydrostatic pressure, which efficiently acts on the interlayer magnetic exchange, and is probed by magneto-optical spectroscopy. △ Less

Submitted 24 October, 2023; v1 submitted 3 March, 2023; originally announced March 2023.

Comments: 3 Figures, 6 pages. To appear in ACS NanoLetters

Paramagnetic Electronic Structure of CrSBr: Comparison between Ab Initio GW Theory and Angle-Resolved Photoemission Spectroscopy

Authors: Marco Bianchi, Swagata Acharya, Florian Dirnberger, Julian Klein, Dimitar Pashov, Kseniia Mosina, Zdenek Sofer, Alexander N. Rudenko, Mikhail I. Katsnelson, Mark van Schilfgaarde, Malte Rösner, Philip Hofmann

Abstract: We explore the electronic structure of paramagnetic CrSBr by comparative first principles calculations and angle-resolved photoemission spectroscopy. We theoretically approximate the paramagnetic phase using a supercell hosting spin configurations with broken long-range order and applying quasiparticle self-consistent $GW$ theory, without and with the inclusion of excitonic vertex corrections to t… ▽ More We explore the electronic structure of paramagnetic CrSBr by comparative first principles calculations and angle-resolved photoemission spectroscopy. We theoretically approximate the paramagnetic phase using a supercell hosting spin configurations with broken long-range order and applying quasiparticle self-consistent $GW$ theory, without and with the inclusion of excitonic vertex corrections to the screened Coulomb interaction (QS$GW$ and QS$G\hat{W}$, respectively). Comparing the quasi-particle band structure calculations to angle-resolved photoemission data collected at 200 K results in excellent agreement. This allows us to qualitatively explain the significant broadening of some bands as arising from the broken magnetic long-range order and/or electronic dispersion perpendicular to the quasi two-dimensional layers of the crystal structure. The experimental band gap at 200 K is found to be at least 1.51 eV at 200 K. At lower temperature, no photoemission data can be collected as a result of charging effects, pointing towards a significantly larger gap, which is consistent with the calculated band gap of $\approx$ 2.1 eV. △ Less

Submitted 2 March, 2023; originally announced March 2023.

Comments: 11 pages, 12 figures

Magneto-optics in a van der Waals magnet tuned by self-hybridized polaritons

Authors: Florian Dirnberger, Jiamin Quan, Rezlind Bushati, Geoffrey Diederich, Matthias Florian, Julian Klein, Kseniia Mosina, Zdenek Sofer, Xiaodong Xu, Akashdeep Kamra, Francisco J. García-Vidal, Andrea Alù, Vinod M. Menon

Abstract: Controlling quantum materials with light is of fundamental and technological importance. By utilizing the strong coupling of light and matter in optical cavities (1-3), recent studies were able to modify some of their most defining features (4-6). In this work, we study the magneto-optical properties of a van der Waals magnet that supports strong coupling of photons and excitons even in the absenc… ▽ More Controlling quantum materials with light is of fundamental and technological importance. By utilizing the strong coupling of light and matter in optical cavities (1-3), recent studies were able to modify some of their most defining features (4-6). In this work, we study the magneto-optical properties of a van der Waals magnet that supports strong coupling of photons and excitons even in the absence of external cavity mirrors. In this material - the layered magnetic semiconductor CrSBr - emergent light-matter hybrids called polaritons are shown to significantly increase the spectral bandwidth of correlations between the magnetic, electronic, and optical properties, enabling largely tunable optical responses to applied magnetic fields and magnons. Our results highlight the importance of exciton-photon self-hybridization in van der Waals magnets and motivate novel directions for the manipulation of quantum material properties by strong light-matter coupling. △ Less

Submitted 23 September, 2024; v1 submitted 18 January, 2023; originally announced January 2023.

Microscopic parameters of the van der Waals CrSBr antiferromagnet from microwave absorption experiments

Authors: C. W. Cho, A. Pawbake, N. Aubergier, A. L. Barra, K. Mosina, Z. Sofer, M. E. Zhitomirsky, C. Faugeras, B. A. Piot

Abstract: Microwave absorption experiments employing a phase-sensitive external resistive detection are performed for a topical van der Waals antiferromagnet CrSBr. The field dependence of two resonance modes is measured in an applied field parallel to the three principal crystallographic directions, revealing anisotropies and magnetic transitions in this material. To account for the observed results, we fo… ▽ More Microwave absorption experiments employing a phase-sensitive external resistive detection are performed for a topical van der Waals antiferromagnet CrSBr. The field dependence of two resonance modes is measured in an applied field parallel to the three principal crystallographic directions, revealing anisotropies and magnetic transitions in this material. To account for the observed results, we formulate a microscopic spin model with a bi-axial single-ion anisotropy and inter-plane exchange. Theoretical calculations give an excellent description of full magnon spectra enabling us to precisely determine microscopic interaction parameters for CrSBr. △ Less

Submitted 25 November, 2022; originally announced November 2022.

Comments: includes a supplementary information document

Raman scattering signatures of the strong spin-phonon coupling in the bulk magnetic van der Waals material CrSBr

Authors: Amit Pawbake, Thomas Pelini, Nathan P. Wilson, Kseniia Mosina, Zdenek Sofer, Rolf Heid, Clement Faugeras

Abstract: Magnetic excitations in layered magnetic materials that can be thinned down the two-dimensional (2D) monolayer limit are of high interest from a fundamental point of view and for applications perspectives. Raman scattering has played a crucial role in exploring the properties of magnetic layered materials and, even-though it is essentially a probe of lattice vibrations, it can reflect magnetic ord… ▽ More Magnetic excitations in layered magnetic materials that can be thinned down the two-dimensional (2D) monolayer limit are of high interest from a fundamental point of view and for applications perspectives. Raman scattering has played a crucial role in exploring the properties of magnetic layered materials and, even-though it is essentially a probe of lattice vibrations, it can reflect magnetic ordering in solids through the spin-phonon interaction or through the observation of magnon excitations. In bulk CrSBr, a layered A type antiferromagnet (AF), we show that the magnetic ordering can be directly observed in the temperature dependence of the Raman scattering response i) through the variations of the scattered intensities, ii) through the activation of new phonon lines reflecting the change of symmetry with the appearance of the additional magnetic periodicity, and iii) through the observation, below the Neel temperature (TN) of second order Raman scattering processes. We additionally show that the three different magnetic phases encountered in CrSBr, including the recently identified low temperature phase, have a particular Raman scattering signature. This work demonstrates that magnetic ordering can be observed directly in the Raman scattering response of bulk CrSBr with in-plane magnetization, and that it can provide a unique insight into the magnetic phases encountered in magnetic layered materials. △ Less

Submitted 23 November, 2022; originally announced November 2022.

Journal ref: Phys. Rev. B 107, 075421, (2023)