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Evidence for Many-Body States in NiPS$_3$ Revealed by Angle-Resolved Photoelectron Spectroscopy
Authors:
Miłosz Rybak,
Benjamin Pestka,
Biplab Bhattacharyya,
Jeff Strasdas,
Adam K. Budniak,
Adi Harchol,
Vitaliy Feyer,
Iulia Cojocariu,
Daniel Baranowski,
Yaron Amouyal,
Efrat Lifshitz,
Markus Morgenstern,
Magdalena Birowska,
Krzysztof Wohlfeld
Abstract:
We present $μ$-ARPES spectra of the Mott-insulating van der Waals antiferromagnet NiPS$_3$. Signatures of strong correlations -- such as the onset of atomic or atomic-ligand multiplets and spin-orbit-entangled exciton have been observed in this material by various two-particle spectroscopies, but not previously in photoemission. Our measurements reveal a weakly dispersive feature at the valence-ba…
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We present $μ$-ARPES spectra of the Mott-insulating van der Waals antiferromagnet NiPS$_3$. Signatures of strong correlations -- such as the onset of atomic or atomic-ligand multiplets and spin-orbit-entangled exciton have been observed in this material by various two-particle spectroscopies, but not previously in photoemission. Our measurements reveal a weakly dispersive feature at the valence-band edge that is absent in DFT+$U$ calculations and remains unchanged across the Néel transition. After critically examining and ruling out alternative interpretations, we show that an exact diagonalization of a NiS$_6$ cluster yields low-energy final-state configurations of mixed multiplet $d^7$ and $d^8\underline{L}$ character, whose energy differences are consistent with the observed additional feature. This implies that ARPES directly accesses local Ni-S multiplet physics in NiPS$_3$, revealing a many-body structure beyond mean-field theory. Our results confirm that NiPS$_3$ is an excellent model platform in which strong correlations, reduced dimensionality, and covalent metal-ligand bonding jointly shape both two- and single-particle spectroscopies, underscoring the need for a genuinely quantum many-body description of two-dimensional quantum materials.
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Submitted 27 April, 2026; v1 submitted 3 February, 2026;
originally announced February 2026.
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Symmetry-Breaking Phenomena in MnPS3/TMDC Heterostructures: Non-relativistic Spin Splitting, Altermagnetism and Spin-Valley Effects
Authors:
Kamil Wrzos,
Magdalena Birowska,
Milosz Rybak
Abstract:
We explore symmetry-breaking phenomena in MnPS3/TMDC (MoS2, WS2, MoSe2, WSe2) heterostructures using first-principles calculations, considering two high-symmetry stacking configurations, S1 and S2, which differ not only by their interfacial registry but also by a 30° twist between the layers. Depending on the stacking geometry, the systems exhibit two distinct types of nonrelativistic spin splitti…
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We explore symmetry-breaking phenomena in MnPS3/TMDC (MoS2, WS2, MoSe2, WSe2) heterostructures using first-principles calculations, considering two high-symmetry stacking configurations, S1 and S2, which differ not only by their interfacial registry but also by a 30° twist between the layers. Depending on the stacking geometry, the systems exhibit two distinct types of nonrelativistic spin splitting (NRSS): S2 hosts altermagnetic-like band crossings, while S1 shows global spin splitting characteristic of symmetry-breaking NRSS. Magnetic exchange and anisotropy parameters indicate that the intrinsic magnetic properties of MnPS3 are largely preserved upon interfacing. Including spin-orbit coupling, we find tunable conduction-valley splitting controlled by the MnPS3 spin orientation. Our results identify MnPS3 as a symmetry-tunable antiferromagnetic substrate capable of inducing and controlling spin and valley effects in 2D heterostructures without relying on net magnetization or strong SOC, offering a route toward nonvolatile valleytronic functionalities.
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Submitted 27 November, 2025;
originally announced November 2025.
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Probing the band structure of the strongly correlated antiferromagnet NiPS3 across its phase transition
Authors:
Benjamin Pestka,
Biplab Bhattacharyya,
Milosz Rybak,
Jeff Strasdas,
Adam K. Budniak,
Adi Harchol,
Marcus Liebmann,
Niklas Leuth,
Honey Boban,
Vitaliy Feyer,
Iulia Cojocariu,
Daniel Baranowski,
Simone Mearini,
Lutz Waldecker,
Bernd Beschoten,
Christoph Stampfer,
Yaron Amouyal,
Lukasz Plucinski,
Efrat Lifshitz,
Krzysztof Wohlfeld,
Magdalena Birowska,
Markus Morgenstern
Abstract:
NiPS3 is an exfoliable van-der-Waals intralayer antiferromagnet with zigzag-type spin arrangement. It is distinct from other TMPS3 (TM: transition metal) materials by optical excitations into a strongly correlated state that is tied to the magnetic properties. However, the related, fundamental band structure across the antiferromagnetic phase transition has not been probed yet. Here, we use angula…
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NiPS3 is an exfoliable van-der-Waals intralayer antiferromagnet with zigzag-type spin arrangement. It is distinct from other TMPS3 (TM: transition metal) materials by optical excitations into a strongly correlated state that is tied to the magnetic properties. However, the related, fundamental band structure across the antiferromagnetic phase transition has not been probed yet. Here, we use angular-resolved photoelectron spectroscopy with μm resolution in combination with DFT+U calculations for that purpose. We identify a characteristic band shift across TN. It is attributed to bands of mixed Ni and S character related to the superexchange interaction of Ni 3t2g orbitals. Moreover, we find a structure above the valence band maximum with little angular dispersion that could not be reproduced by the calculations. The discrepancy suggests the influence of many-body interactions beyond the DFT+U approximations in striking contrast to the results on MnPS3 and FePS3, where these calculations were sufficient for an adequate description.
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Submitted 3 January, 2026; v1 submitted 20 July, 2025;
originally announced July 2025.
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Atomic-Scale Investigation of an Asymmetric SrTiO$_{3}$ Grain Boundary
Authors:
Janina Malin Rybak,
Jonas Arlt,
Qian Ma,
Carmen Fuchs,
Baptiste Gault,
Timo Jacob,
Christian Jooss,
Tobias Meyer,
Cynthia A. Volkert
Abstract:
Grain boundaries (GBs) in oxide perovskites significantly influence their functional properties. This study examines the atomic-scale structure and composition of a faceted asymmetric grain boundary in strontium titanate (SrTiO$_3$) using scanning transmission electron microscopy (STEM), atom probe tomography (APT), and density functional theory (DFT). STEM and APT reveal an atomically sharp bound…
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Grain boundaries (GBs) in oxide perovskites significantly influence their functional properties. This study examines the atomic-scale structure and composition of a faceted asymmetric grain boundary in strontium titanate (SrTiO$_3$) using scanning transmission electron microscopy (STEM), atom probe tomography (APT), and density functional theory (DFT). STEM and APT reveal an atomically sharp boundary with asymmetric and symmetric facets, marked by strong Sr depletion over a width of less than 1 nm. STEM-EELS shows Ti concentration variations of up to 20% between facets, while APT constrains this variation to less than 10%. DFT$+U$ calculations of a symmetric $Σ$5 facet confirm that Sr depletion minimizes boundary energy while maintaining Ti content. The variation in Ti suggests cation mobility that enables local energy minimization. Differences in facet surface energies likely drive Ti redistribution, offering strategies for GB structure control. This combined experimental-theoretical approach provides key insights into the structure and energy landscape of GBs in SrTiO$_3$, aiding in the prediction of their impact on ionic and electronic transport.
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Submitted 14 March, 2025;
originally announced March 2025.
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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…
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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.
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Submitted 8 June, 2026; v1 submitted 30 August, 2024;
originally announced September 2024.
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Direct Optical Probing of the Magnetic Properties of the Layered Antiferromagnet CrPS$_4$
Authors:
Tomasz Fąs,
Mateusz Wlazło,
Magdalena Birowska,
Miłosz Rybak,
Małgorzata Zinkiewicz,
Leon Oleschko,
Mateusz Goryca,
Łukasz Gondek,
Bruno Camargo,
Jacek Szczytko,
Adam K. Budniak,
Yaron Amouyal,
Efrat Lifshitz,
Jan Suffczyński
Abstract:
Unusual magnetic properties of Van der Waals type antiferromagnetic semiconductors make them highly attractive for spintronics and optoelectronics. A link between the magnetic and optical properties of those materials, required for practical applications, has not been, however, established so far. Here, we report on a combined experimental and theoretical study of magnetic, optical, and structural…
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Unusual magnetic properties of Van der Waals type antiferromagnetic semiconductors make them highly attractive for spintronics and optoelectronics. A link between the magnetic and optical properties of those materials, required for practical applications, has not been, however, established so far. Here, we report on a combined experimental and theoretical study of magnetic, optical, and structural properties of bulk CrPS$_{4}$ samples. We find that the magnetic-field-dependent circular polarization degree of the photoluminescence is a direct measure of the net magnetization of CrPS$_{4}$. Complementary, Raman scattering measured as a function of magnetic field and temperature enables the determination of the magnetic susceptibility curve of the material. Our experimental results are backed by Our experimental results are supported by density functional theory calculations that take as input the lattice parameters determined from temperature-dependent X-ray diffraction measurements. This allows us to explain the impact of spin ordering on the spectral position of Raman transitions in CrPS$_4$, as well as anomalous temperature shifts of selected of them. The presented method for all-optical determination of the magnetic properties is highly promising for studies of spin ordering and magnetic phase transitions in single- or a few-layer samples of magnetic layered materials, for which a poor signal-to-noise ratio precludes any reliable neutron scattering or magnetometry measurements.
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Submitted 25 July, 2024;
originally announced July 2024.
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Tuning Magnetic and Optical Properties in MnxZn1-xPS3 Single Crystals by the Alloying Composition
Authors:
Adi Harchol,
Shahar Zuri,
Esther Ritov,
Faris Horani,
Miłosz Rybak,
Tomasz Woźniak,
Anna Eyal,
Yaron Amouyal,
Magdalena Birowska,
Efrat Lifshitz
Abstract:
The exploration of two-dimensional (2D) antiferromagnetic (AFM) materials has shown great promise and interest in tuning the magnetic and electronic properties as well as studying magneto-optical effects. The current work investigates the control of magneto-optical interactions in alloyed MnxZn1-xPS3 lamellar semiconductor single crystals, with the Mn/Zn ratio regulating the coupling strength. Mag…
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The exploration of two-dimensional (2D) antiferromagnetic (AFM) materials has shown great promise and interest in tuning the magnetic and electronic properties as well as studying magneto-optical effects. The current work investigates the control of magneto-optical interactions in alloyed MnxZn1-xPS3 lamellar semiconductor single crystals, with the Mn/Zn ratio regulating the coupling strength. Magnetic susceptibility results show a retention of AFM order followed by a decrease in Néel temperatures down to ~ 40% Mn concentration, below which a paramagnetic behavior is observed. Absorption measurements reveal an increase in bandgap energy with higher Zn(II) concentration, and the presence of Mn(II) d-d transition below the absorption edge. DFT+U approach qualitatively explained the origin and the position of the experimentally observed mid band-gap states in pure MnPS3, and corresponding peaks visible in the alloyed systems MnxZn1-xPS3. Accordingly, emission at 1.3 eV in all alloyed compounds results from recombination from a 4T1g Mn(II) excited state to a hybrid p-d state at the valence band. Most significant, temperature-dependent photoluminescence (PL) intensity trends demonstrate strong magneto-optical coupling in compositions with x > 0.65. This study underscores the potential of tailored alloy compositions as a means to control magnetic and optical properties in 2D materials, paving the way for advances in spin-based technologies.
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Submitted 11 April, 2024;
originally announced April 2024.
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Magneto-optical anisotropies of 2D antiferromagnetic MPX$_3$ from first principles
Authors:
Miłosz Rybak,
Paulo E. Faria Junior,
Tomasz Woźniak,
Paweł Scharoch,
Jaroslav Fabian,
Magdalena Birowska
Abstract:
Here we systematically investigate the impact of the spin direction on the electronic and optical properties of transition metal phosphorus trichalcogenides (MPX$_3$, M=Mn, Ni, Fe; X=S, Se) exhibiting various antiferromagnetic arrangement within the 2D limit. Our analysis based on the density functional theory and versatile formalism of Bethe-Salpeter equation reveals larger exciton binding energi…
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Here we systematically investigate the impact of the spin direction on the electronic and optical properties of transition metal phosphorus trichalcogenides (MPX$_3$, M=Mn, Ni, Fe; X=S, Se) exhibiting various antiferromagnetic arrangement within the 2D limit. Our analysis based on the density functional theory and versatile formalism of Bethe-Salpeter equation reveals larger exciton binding energies for MPS$_3$ (up to 1.1 eV in air) than MPSe$_3$(up to 0.8 eV in air), exceeding the values of transition metal dichalcogenides (TMDs). For the (Mn,Fe)PX$_3$ we determine the optically active band edge transitions, revealing that they are sensitive to in-plane magnetic order, irrespective of the type of chalcogen atom. We predict the anistropic effective masses and the type of linear polarization as an important fingerprints for sensing the type of magnetic AFM arrangements. Furthermore, we identify the spin-orientation-dependent features such as the valley splitting, the effective mass of holes, and the exciton binding energy. In particular, we demonstrate that for MnPX$_3$ (X=S, Se) a pair of non equivalent K+ and K- points exists yielding the valley splittings that strongly depend on the direction of AFM aligned spins. Notably, for the out-of-plane direction of spins, two distinct peaks are expected to be visible below the absorption onset, whereas one peak should emerge for the in-plane configuration of spins. These spin-dependent features provide an insight into spin flop transitions of 2D materials. Finally, we propose a strategy how the spin valley polarization can be realized in 2D AFM within honeycomb lattice.
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Submitted 24 August, 2023;
originally announced August 2023.
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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…
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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.
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Submitted 31 March, 2023;
originally announced March 2023.
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Electronic band structure changes across the antiferromagnetic phase transition of exfoliated MnPS$_3$ probed by $μ$-ARPES
Authors:
Jeff Strasdas,
Benjamin Pestka,
Milosz Rybak,
Adam K. Budniak,
Niklas Leuth,
Honey Boban,
Vitaliy Feyer,
Iulia Cojocariu,
Daniel Baranowski,
José Avila,
Pavel Dudin,
Aaron Bostwick,
Chris Jozwiak,
Eli Rotenberg,
Carmine Autieri,
Yaron Amouyal,
Lukasz Plucinski,
Efrat Lifshitz,
Magdalena Birowska,
Markus Morgenstern
Abstract:
Exfoliated magnetic 2D materials enable versatile tuning of magnetization, e.g., by gating or providing proximity-induced exchange interaction. However, their electronic band structure after exfoliation has not been probed, most likely due to their photochemical sensitivity. Here, we provide micron-scale angle-resolved photoelectron spectroscopy of the exfoliated intralayer antiferromagnet MnPS…
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Exfoliated magnetic 2D materials enable versatile tuning of magnetization, e.g., by gating or providing proximity-induced exchange interaction. However, their electronic band structure after exfoliation has not been probed, most likely due to their photochemical sensitivity. Here, we provide micron-scale angle-resolved photoelectron spectroscopy of the exfoliated intralayer antiferromagnet MnPS$_3$ above and below the Néel temperature down to one monolayer. The favorable comparison with density functional theory calculations enables to identify the orbital character of the observed bands. Consistently, we find pronounced changes across the Néel temperature for bands that consist of Mn 3d and 3p levels of adjacent S atoms. The deduced orbital mixture indicates that the superexchange is relevant for the magnetic interaction. There are only minor changes between monolayer and thicker films demonstrating the predominant 2D character of MnPS$_3$. The novel access is transferable to other MPX$_3$ materials (M: transition metal, P: phosphorus, X: chalcogenide) providing a multitude of antiferromagnetic arrangements.
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Submitted 22 June, 2023; v1 submitted 10 November, 2022;
originally announced November 2022.
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Stress-Tuned Optical Transitions in Layered 1T-MX2 (M= Hf, Zr, Sn; X= S, Se) Crystals
Authors:
Miłosz Rybak,
Tomasz Woźniak,
Magdalena Birowska,
Filip Dybała,
Alfredo Segura,
Konrad J. Kapcia,
Paweł Scharoch,
Robert Kudrawiec
Abstract:
Optical measurements under externally applied stresses allow us to study the materials' electronic structure by comparing the pressure evolution of optical peaks obtained from experiments and theoretical calculations. We examine the stress-induced changes in electronic structure for the thermodynamically stable 1T polytype of selected MX2 compounds (M=Hf, Zr, Sn; X=S, Se), using the density functi…
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Optical measurements under externally applied stresses allow us to study the materials' electronic structure by comparing the pressure evolution of optical peaks obtained from experiments and theoretical calculations. We examine the stress-induced changes in electronic structure for the thermodynamically stable 1T polytype of selected MX2 compounds (M=Hf, Zr, Sn; X=S, Se), using the density functional theory. We demonstrate that considered 1T-MX2 materials are semiconducting with indirect character of the band gap, irrespective to the employed pressure as predicted using modified Becke-Johnson potential. We determine energies of direct interband transitions between bands extrema and in band-nesting regions close to Fermi level. Generally, the studied transitions are optically active, exhibiting in-plane polarization of light. Finally, we quantify their energy trends under external hydrostatic, uniaxial, and biaxial stresses by determining the linear pressure coefficients. Generally, negative pressure coefficients are obtained implying the narrowing of the band gap. The semiconducting-to-metal transition are predicted under hydrostatic pressure. We discuss these trends in terms of orbital composition of involved electronic bands. In addition, we demonstrate that the measured pressure coefficients of HfS2 and HfSe2 absorption edges are in perfect agreement with our predictions. Comprehensive and easy-to-interpret tables containing the optical features are provided to form the basis for assignation of optical peaks in future measurements.
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Submitted 21 October, 2022;
originally announced October 2022.
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Crystal anisotropy implications on the intrinsic magnetic and optical properties in van der Waals FePS3
Authors:
Ellenor Geraffy,
Shahar Zuri,
Milosz Marcin Rybak,
Faris Horani,
Adam K. Budniak,
Yaron Amouyal,
Magdalena Birowska,
Efrat Lifshitz
Abstract:
Antiferromagnetic (AFM) FePS3 has gained significant interest recently for its potential applications in spin-related devices. A single layer is comprised of a honeycomb network, stabilized by long-range spin-exchange interactions, with a zigzag or Neel arrangement of the Fe-atoms. This study exposed, for the first time, a strong impact of lateral crystal distortion on the magnetic arrangement and…
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Antiferromagnetic (AFM) FePS3 has gained significant interest recently for its potential applications in spin-related devices. A single layer is comprised of a honeycomb network, stabilized by long-range spin-exchange interactions, with a zigzag or Neel arrangement of the Fe-atoms. This study exposed, for the first time, a strong impact of lateral crystal distortion on the magnetic arrangement and optical properties of FePS3. This impact was deciphered by correlating photoluminescence (PL) observations with single-crystal XRD which uncovered anisotropy in the a/b crystallographic plane. Thus, induceing a breakage in the inversion symmetry in FePS3 causing changes in it's electronic and optical transitions. The MPL observations exhibited an unexpected band-edge circularly polarized recombination emission, while off-band-edge transitions were linearly polarized. Also, temperature-dependent MPL measurements reflected zigzag-AFM at low temperatures and the coexistence of zigzag or Neel at mid temperatures. Theoretical calculation implementing anisotropy in spin-exchange interactions among Fe atom's nearest neighbors revealed stabilized zigzag arrangement tilted away from the a-axis. Furthermore, DFT calculations of the electronic band-edge predicted split states in degenerate symmetric points (K+/K-) for zigzag structure and non-degenerate for the Neel arrangement. Highlighting the importance of the inclusion of a crystallographic anisotropy parameter for the simulation of the experimental observations.
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Submitted 6 May, 2024; v1 submitted 23 August, 2022;
originally announced August 2022.
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Anisotropic Magnetodielectric Coupling in Layered Antiferromagnetic FePS$_3$
Authors:
Anudeepa Ghosh,
Magdalena Birowska,
Pradeepta Kumar Ghose,
Miłosz Rybak,
Sujan Maity,
Somsubhra Ghosh,
Bikash Das,
Koushik Dey,
Satyabrata Bera,
Suresh Bhardwaj,
Shibabrata Nandi,
Subhadeep Datta
Abstract:
We report anisotropic magnetodielectric (MD) coupling in layered van der Waals (vdW) antiferromagnetic (AFM) FePS$_3$ (Néel temperature $T_{\mathrm{N}}$ $\sim$ 120K) with perpendicular anisotropy. Above $T_N$, while dielectric response function along \textit{c}-axis shows frequency dependent relaxations, in-plane data is frequency independent and reveals a deviation from phonon-anharmonicity in th…
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We report anisotropic magnetodielectric (MD) coupling in layered van der Waals (vdW) antiferromagnetic (AFM) FePS$_3$ (Néel temperature $T_{\mathrm{N}}$ $\sim$ 120K) with perpendicular anisotropy. Above $T_N$, while dielectric response function along \textit{c}-axis shows frequency dependent relaxations, in-plane data is frequency independent and reveals a deviation from phonon-anharmonicity in the ordered state, thereby implying a connection to spin-phonon coupling known to be indicative of onset of magnetic ordering. At low temperature (below 40 K), atypical anomaly in the dielectric constant is corroborated with temperature dependent DC and AC susceptibility. The magnetodielectric response across this anomaly differs significantly for both, in-plane and out-of-plane cases. We have explained this in terms of preferential orientation of magnetic AFM-z alignment, implied by the in-plane structural anisotropy as confirmed by \textit{ab-initio} calculations. Controlling relative strength of magnetodielectric coupling with magnetic anisotropy opens up a strategy for tracking subtle modifications of structure, such as in-plane anisotropy, with potential application to spintronic technologies.
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Submitted 4 August, 2023; v1 submitted 4 August, 2022;
originally announced August 2022.
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Controlling magnetic exchange and anisotropy by non-magnetic ligand substitution in layered MPX3 (M = Ni, Mn; X = S, Se)
Authors:
Rabindra Basnet,
K. Kotur,
M. Rybak,
Cory Stephenson,
Samuel Bishop,
C. Autieri,
M. Birowska,
Jin Hu
Abstract:
Recent discoveries in two-dimensional (2D) magnetism have intensified the investigation of van der Waals (vdW) magnetic materials and further improved our ability to tune their magnetic properties. Tunable magnetism has been widely studied in antiferromagnetic metal thiophosphates MPX3. Substitution of metal ions M has been adopted as an important technique to engineer the magnetism in MPX3. In th…
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Recent discoveries in two-dimensional (2D) magnetism have intensified the investigation of van der Waals (vdW) magnetic materials and further improved our ability to tune their magnetic properties. Tunable magnetism has been widely studied in antiferromagnetic metal thiophosphates MPX3. Substitution of metal ions M has been adopted as an important technique to engineer the magnetism in MPX3. In this work, we have studied the previously unexplored chalcogen X substitutions in MPX3 (M = Mn/Ni; X = S/Se). We synthesized the single crystals of MnPS3-xSex (0 < x < 3) and NiPS3-xSex (0 < x < 1.3) and investigated the systematic evolution of the magnetism with varying x. Our study reveals the effective tuning of magnetic interactions and anisotropies in both MnPS3 and NiPS3 upon Se substitution. Such efficient engineering of the magnetism provides a suitable platform to understand the low-dimensional magnetism and develop future magnetic devices.
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Submitted 9 May, 2022;
originally announced May 2022.
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Limited ferromagnetic interactions in monolayers of MPS$_3$ (M=Mn, Ni)
Authors:
Carmine Autieri,
Giuseppe Cuono,
Canio Noce,
Milosz Rybak,
Kamila M. Kotur,
Cliò Efthimia Agrapidis,
Krzysztof Wohlfeld,
Magdalena Birowska
Abstract:
We present a systematic study of the electronic and magnetic properties of two-dimensional ordered alloys, consisting of two representative hosts (MnPS$_3$ and NiPS$_3$) of transition metal phosphorus trichalcogenides doped with $3d$ elements. For both hosts our DFT+U calculations are able to qualitatively reproduce the ratios and signs of all experimentally observed magnetic couplings. The relati…
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We present a systematic study of the electronic and magnetic properties of two-dimensional ordered alloys, consisting of two representative hosts (MnPS$_3$ and NiPS$_3$) of transition metal phosphorus trichalcogenides doped with $3d$ elements. For both hosts our DFT+U calculations are able to qualitatively reproduce the ratios and signs of all experimentally observed magnetic couplings. The relative strength of all antiferromagnetic exchange couplings, both in MnPS$_3$ as well as in NiPS$_3$, can successfully be explained using an effective direct exchange model: they reveal that the third-neighbor exchange dominates in NiPS$_3$ due to the filling of the $t_{2g}$ subshell, whereas for MnPS$_3$ the first neighbor exchange is prevailed owing to the presence of the $t_{2g}$ magnetism. On the other hand, the nearest neighbor ferromagnetic coupling in NiPS$_3$ can only be explained using a more complex superexchange model and is (also) largely triggered by the absence of the $t_{2g}$ magnetism. For the doped systems, the DFT+U calculations revealed that magnetic impurities do not affect the magnetic ordering observed in the pure phases and thus in general in these systems ferromagnetism may not be easily induced by such a kind of elemental doping. However, unlike for the hosts, the first and second (dopant-host) exchange couplings are of similar order of magnitude. This leads to frustration in case of antiferromagnetic coupling and may be one of the reasons of the observed lower magnetic ordering temperature of the doped systems.
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Submitted 17 March, 2022; v1 submitted 29 November, 2021;
originally announced November 2021.
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Competing contact processes in the Watts-Strogatz network
Authors:
Marcin Rybak,
Krzysztof Malarz,
Krzysztof Kułakowski
Abstract:
We investigate two competing contact processes on a set of Watts--Strogatz networks with the clustering coefficient tuned by rewiring. The base for network construction is one-dimensional chain of $N$ sites, where each site $i$ is directly linked to nodes labelled as $i\pm 1$ and $i\pm 2$. So initially, each node has the same degree $k_i=4$. The periodic boundary conditions are assumed as well.…
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We investigate two competing contact processes on a set of Watts--Strogatz networks with the clustering coefficient tuned by rewiring. The base for network construction is one-dimensional chain of $N$ sites, where each site $i$ is directly linked to nodes labelled as $i\pm 1$ and $i\pm 2$. So initially, each node has the same degree $k_i=4$. The periodic boundary conditions are assumed as well.
For each node $i$ the links to sites $i+1$ and $i+2$ are rewired to two randomly selected nodes so far not-connected to node $i$. An increase of the rewiring probability $q$ influences the nodes degree distribution and the network clusterization coefficient $\mathcal{C}$. For given values of rewiring probability $q$ the set $\mathcal{N}(q)=\{\mathcal{N}_1, \mathcal{N}_2, \cdots, \mathcal{N}_M \}$ of $M$ networks is generated.
The network's nodes are decorated with spin-like variables $s_i\in\{S,D\}$. During simulation each $S$ node having a $D$-site in its neighbourhood converts this neighbour from $D$ to $S$ state. Conversely, a node in $D$ state having at least one neighbour also in state $D$-state converts all nearest-neighbours of this pair into $D$-state. The latter is realized with probability $p$.
We plot the dependence of the nodes $S$ final density $n_S^T$ on initial nodes $S$ fraction $n_S^0$. Then, we construct the surface of the unstable fixed points in $(\mathcal{C}, p, n_S^0)$ space. The system evolves more often toward $n_S^T=1$ for $(\mathcal{C}, p, n_S^0)$ points situated above this surface while starting simulation with $(\mathcal{C}, p, n_S^0)$ parameters situated below this surface leads system to $n_S^T=0$. The points on this surface correspond to such value of initial fraction $n_S^*$ of $S$ nodes (for fixed values $\mathcal{C}$ and $p$) for which their final density is $n_S^T=\frac{1}{2}$.
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Submitted 20 January, 2015; v1 submitted 18 November, 2014;
originally announced November 2014.