arXiv subjects

Andrei Shumilin

Publications and source records attributed to Andrei Shumilin.

12 recordsLinked to original sources

arXiv2026

Switchable Altermagnetism in a Layered van der Waals Metal-Organic Framework Driven by Spin-Crossover

Dynamical control of altermagnetism is a key requirement for translating its unique spin-dependent functionalities into practical spintronic devices, yet effective switching mechanisms remain largely unexplored. Here, we open an unprecedented, versatile and programmable route based on spin-crossover to switch altermagnetism on demand in molecular materials. Using density functional calculations, we demonstrate an altermagnetic ground state in the layered van der Waals MOFs MnX$_2$(tdz)$_2$ (X = Cl, Br; tdz = thiadiazole), stabilized by anisotropic interlayer exchange interactions, which gives rise to a characteristic d-wave momentum-space spin splitting and an associated spin-splitter transport response. Our findings reveal that under hydrostatic pressure, a high-spin to low-spin transition reconfigures the Mn d-orbital occupation, thus modifying the magnetic exchange network, and stabilizing a different antiferromagnetic ground state whose symmetry suppresses the nonrelativistic spin splitting. Crucially, spin-crossover switches altermagnetism not by directly altering the electronic structure, but by changing the symmetry of the magnetic ground state. These results establish molecular spin-crossover altermagnets as a platform for externally reconfigurable spintronic devices.

cond-mat.mtrl-sci↗

arXiv2026

Altermagnetic Metal-Organic Frameworks

Altermagnetism has recently emerged as a new class of spin compensated magnetic materials that exhibit momentum dependent spin splitting despite having zero net magnetization. The origin of these electronic signatures lies in symmetry operations that connect opposite spin sublattices while allowing spin splitting in momentum space. While most candidate materials identified so far belong to inorganic crystals with fixed lattice symmetries, the realization of altermagnetism ultimately requires platforms in which magnetic symmetry can be deliberately engineered. In this Perspective, we discuss how metal-organic frameworks (MOFs) provide a unique chemical platform to address this challenge. We first place altermagnetism in the broader context of magnetic and electronically active metal-organic networks, highlighting how reticular chemistry enables precise control over lattice geometry, dimensionality and electronic structure. We then discuss how these features position framework materials as promising candidates for realizing altermagnetism and highlight the key challenges that must be addressed to translate theoretical proposals into experimentally accessible systems. Finally, we critically assess current experimental challenges and outline emerging directions for realizing and controlling altermagnetism in coordination framework materials, which emerge as a versatile and powerful platform for exploring new paradigms in spintronics.

cond-mat.mtrl-sci↗

arXiv2026

Intrinsic (non)-Gilbert damping in magnetic insulators calculated from a minimal model and \textit{ab initio} spin Hamiltonians

We present an analytically solvable minimal model for the relaxation of low-frequency magnons in magnetic insulators arising from magnon-phonon and magnon-magnon interactions. The model establishes a direct connection between microscopic relaxation processes and Gilbert damping, and reveals how magnon decay evolves from bulk systems to the monolayer limit. We find that magnon-phonon coupling produces Gilbert damping of comparable magnitude in three- and two-dimensional magnets, with qualitative differences between flexural phonons in free-standing monolayers and three-dimensional phonons in substrate-supported layers. By contrast, non-Gilbert damping due to four-magnon scattering is strongly enhanced in two dimensions, where it becomes independent of spin-orbit coupling. To benchmark the model against real materials, we introduce a numerical approach for computing magnon damping from ab initio-derived spin Hamiltonians. We demonstrate that the central conclusions of the model remain valid for magnons in bulk YIG and in a monolayer of the van der Waals magnetic insulator CrSBr.

cond-mat.mtrl-sci↗

arXiv2026

Twist-induced altermagnetism in a metallic van der Waals antiferromagnet

Altermagnetism -a magnetic state characterized by spin-polarized electronic bands at zero net magnetization- offers a promising route for next-generation spintronic devices. In two-dimensional (2D) magnets, twist engineering enables its realization by breaking the combined inversion and time-reversal symmetry (PT) while preserving crystal symmetries that ensure the altermagnetic order. Here, by means of first-principles calculations and symmetry analysis, we demonstrate that twist engineering applied to the recently synthesized metallic van der Waals antiferromagnet Co-doped bilayer Fe$_3$GaTe$_2$ (Fe$_2$CoGaTe$_2$) provides a robust platform for altermagnetism. By twisting two layers of Fe$_2$CoGaTe$_2$, the PT symmetry between opposite spin sublattices is broken, resulting in a non-relativistic $i$-wave altermagnetic state with spin splitting up to 138 meV. In the absence of spin-orbit coupling (SOC), the electronic states are spin-degenerate along six high-symmetry directions, while the inclusion of SOC preserves this degeneracy along the three directions protected by twofold rotation axes. Furthermore, we unveil the microscopic mechanisms governing the magnetic behavior in twisted Fe$_2$CoGaTe$_2$. Our results establish twist engineering and metallic Fe-based van der Waals antiferromagnets as versatile platforms to realize 2D van der Waals altermagnetism, with potential for designing high-efficiency ultrathin nanodevices.

cond-mat.mtrl-sci↗

arXiv2025

Switchable Magnonic Crystals Based on Spin Crossover/CrSBr Heterostructures

The progress of magnonics ultimately depends on material platforms that offer precise control of spin waves propagation. Here, we put forward a chemical strategy to create locally tunable magnonic crystals by integrating switchable spin-crossover (SCO) molecules with 2D van der Waals magnets. Specifically, we investigate from first principles a hybrid molecular/2D heterostructure formed by [Fe((3,5-(CH3)2Pz)3BH)2] molecules (Fe-pz) deposited on a single-layer of semiconducting CrSBr. We show that Fe-pz molecules are stable on CrSBr while preserving its SCO bistability, particularly in densely packed molecular arrays. By patterning Fe-pz into periodic stripes separated by pristine CrSBr regions, the interface becomes a magnonic crystal that filters spin waves at selected frequencies. Crucially, light-driven excited spin-state trapping (LIESST) enables LS-HS switching and induces up to ~1.3% local strain in CrSBr, which in turn reshapes the magnonic band structure in a dynamic and reversible manner. These results establish Fe-pz@CrSBr as a switchable platform for on-chip, programmable magnonic devices.

cond-mat.mtrl-sci↗

arXiv2025

Chemical Engineering of Altermagnetism in Two-Dimensional Metal-Organic Frameworks

Altermagnetism represents a novel class of collinear antiferromagnetism exhibiting non-relativistic spin splitting without net magnetization, driven by lattice symmetry rather than spin-orbit coupling (SOC). Here, we introduce a coordination-driven chemical strategy to realize altermagnetic (AM) spin splitting in two-dimensional (2D) planar tetracoordinated Cr-based metal-organic frameworks (MOFs). Using density functional theory (DFT) calculations, we demonstrate that replacing centrosymmetric pyrazine (pyz) ligands with non-centrosymmetric imidazole (imz) linkers in Cr-based MOFs reduces lattice symmetry, enabling g-wave AM spin splitting up to 65 meV. Furthermore, frontier molecular orbital engineering (FMOE) allows selective ligand spin polarization, inducing a shift to d-wave AM anisotropy in polycyclic ligand-based 2D MOFs with spin splitting up to 83.9 meV. Microscopic magnetic exchange interactions (J) analysis reveals that ligand-mediated interactions dominate over metal-metal coupling, stabilizing AM order in systems with radical ligands. Interestingly, we further confirm AM spin splitting in spin wave spectrum, where chiral magnon splitting is observed. Finally, we show that AM spin splitting gives rise to experimentally accessible charge to spin conversion, emerging as a linear response in d-wave and as a symmetry-allowed nonlinear effect in g-wave 2D AM MOFs. This work establishes coordination chemistry as a powerful and versatile route to symmetry control in 2D MOFs, enabling rational design of 2D molecular materials with tunable electronic and AM properties for next-generation spintronic devices.

cond-mat.mtrl-sci↗

arXiv2025

Confinement-Induced One-Dimensional Magnetism in CrSBr Chains via Carbon Nanotube Encapsulation

Encapsulating low-dimensional magnetic materials within carbon nanotubes (CNTs) offers a compelling route to stabilize unconventional magnetic states and engineer quantum functionalities at the limit of miniaturization. In this work, we systematically investigate the structural, electronic, and magnetic properties of one-dimensional (1D) CrSBr chains encapsulated within CNTs using density functional theory (DFT) and spin dynamics simulations. We demonstrate the structural stability of CrSBr@CNT, where confinement and charge transfer cooperate to stabilize ferromagnetism in the 1D limit, which persists up to 50 K. These findings position CrSBr@CNT as a model platform for realizing 1D magnetism and establish CNT encapsulation as a powerful strategy for exploring emergent quantum spin phenomena and engineering nanoscale spintronic devices.

cond-mat.mtrl-sci↗

arXiv2025

Controlling Magnetism in the 2D van der Waals Antiferromagnet CrPS$_4$ via Ion Intercalation

Two-dimensional van der Waals (vdW) magnetic materials are versatile platforms for tailoring electronic and magnetic properties, in which the insertion of chemical species into their interlayer gaps offers a powerful route to engineer magnetism. Here, we focus on the A-type antiferromagnetic semiconductor CrPS$_4$ (T$_N$ = 38 K) and investigate its electronic and magnetic properties upon intercalation of lithium (Li$^+$) and organic tetrabutylammonium (TBA$^+$) ions using first-principles calculations. Our results show that Li$^+$ incorporation induces a semiconductor-to-metal transition in CrPS$_4$ and selectively modifies its magnetic behaviour: switching from out-of-plane to in-plane antiferromagnetism, followed by an in-plane ferromagnetic ground state at higher intercalation levels. This is accompanied by a continuous increase of the ordering temperature, reaching a fivefold enhancement for Li$_{0.5}$CrPS$_4$. Similarly, TBA$^+$ intercalation expands the vdW gap, decoupling CrPS$_4$ layers and stabilising in-plane ferromagnetism with a T$_C$ above 100 K. Furthermore, it also modifies magnon propagation, leading to enhanced group velocities and a more isotropic magnon transport. This work highlights intercalation as a powerful and versatile approach for controlling magnetic behaviour and spin dynamics, paving the way for the design of tunable 2D layered magnetic materials for spintronic and magnonic applications.

cond-mat.mtrl-sci↗

arXiv2025

Strain Engineering of Magnetoresistance and Magnetic Anisotropy in CrSBr

Tailoring magnetoresistance and magnetic anisotropy in van der Waals magnetic materials is essential for advancing their integration into technological applications. In this regard, strain engineering has emerged as a powerful and versatile strategy to control magnetism at the two-dimensional (2D) limit. Here, we demonstrate that compressive biaxial strain significantly enhances the magnetoresistance and magnetic anisotropy of few-layer CrSBr flakes. Strain is efficiently transferred to the flakes from the thermal compression of a polymeric substrate upon cooling, as confirmed by temperature-dependent Raman spectroscopy. This strain induces a remarkable increase in the magnetoresistance ratio and in the saturation fields required to align the magnetization of CrSBr along each of its three crystalographic directions, reaching a twofold enhancement along the magnetic easy axis. This enhancement is accompanied by a subtle reduction of the Néel temperature by ~10K. Our experimental results are fully supported by first-principles calculations, which link the observed effects to a strain-driven modification in interlayer exchange coupling and magnetic anisotropy energy. These findings establish strain engineering as a key tool for fine-tuning magnetotransport properties in 2D magnetic semiconductors, paving the way for implementation in spintronics and information storage devices.

cond-mat.mtrl-sci↗

arXiv2025

Tunable Itinerant Ferromagnetism in the Two-Dimensional FePd$_2$Te$_2$ Hosting 1D Spin Chains

One-dimensional (1D) magnetism offers unidirectional spin interactions that allow unique tunable properties and unconventional spin phenomena. However, it often suffers from poor stability, limiting practical applications. In this regard, integrating 1D magnetism into two-dimensional (2D) materials enables a promising route to stabilize these systems while preserving their anisotropic magnetic characteristics. Here, we focus on the 2D ferromagnet FePd$_2$Te$_2$ (T$_C$ = 183K), which hosts 1D spin chains and strong in-plane anisotropy. Our first-principles calculations reveal highly anisotropic magnetic exchange interactions, confirming its 1D ferromagnetic nature. We modulate this behavior by Co and Ni substitution and introduce two new members of this family, CoPd$_2$Te$_2$ -- a ferromagnet -- and NiPd$_2$Te$_2$. Our results unveil the microscopic mechanisms governing the behaviour of FePd$_2$Te$_2$ and CoPd$_2$Te$_2$. Furthermore, we also demonstrate that the variation of the chain length is key to modulate magnetism. Finally, we determine the magnon dispersion, showcasing a pronounced anisotropy that enables unidirectional magnon propagation.

cond-mat.mtrl-sci↗

arXiv2025

Coupling molecular spin qubits with 2D magnets for coherent magnon manipulation

Magnonics is an emerging field widely considered as a paradigm shift in information technology that uses spin waves for data storage, processing and transmission. However, the coherent control of spin waves in 2D magnets still remains a challenge. Herein, we investigate the interplay between molecular spins and magnons in hybrid heterostructures formed by [CpTi(cot)] and VOPc spin qubits deposited on the surface of the air-stable 2D van der Waals ferromagnet CrSBr using first principles. Our results show that different molecular rotation configurations significantly impact on qubit relaxation time and alter the magnon spectra of the underlying 2D magnet, allowing the chemical coherent control of spin waves in this material. We predict the feasibility of an ultrafast magnon-qubit interface with minimized decoherence, where exchange coupling plays a crucial role. This work opens new avenues for hybrid quantum magnonics, enabling selective tailoring through a versatile chemical approach.

cond-mat.mes-hall↗

arXiv2025

Collapse of the standard ferromagnetic domain structure in hybrid Co/Molecule bilayers

We show that, upon the chemisorption of organic molecules, Co thin films display a number of unique magnetic properties, including the giant magnetic hardening and the violation of the Rayleigh law in magnetization reversal. These novel properties originate from the modification of the surface magnetic anisotropy induced by the molecule/film interaction: the π-d molecule/metal hybridization modifies the orbital population of the associated cobalt atoms and induces an additional and randomly oriented local anisotropy. Strong effects arise when the induced surface anisotropy is correlated over scales of a few molecules, and particularly when the correlation length of the random anisotropy field is comparable to the characteristic exchange length. This leads to the collapse of the standard domain structure and to the emergency of a glassy-type ferromagnetic state, defined by blurred pseudo-domains intertwined by diffuse and irregular domain walls. The magnetization reversal in such state was predicted to include topological vortex-like structures, successfully measured in this research by magnetic-force microscopy. Our work shows how the strong electronic interaction of standard components, Co thin films and readily available molecules, can generate structures with remarkable new magnetic properties, and thus opens a new avenue for the design of tailored-on-demand magnetic composites.

cond-mat.mtrl-sci↗