arXiv subjects

Aleksandar Razpopov

Publications and source records attributed to Aleksandar Razpopov.

15 recordsLinked to original sources

arXiv2026

Quetzalcoatlite as a Disorder-Free Platform for Chiral Magnetism and Frustration

The natural mineral quetzalcoatlite Zn$_6$Cu$_3$(TeO$_6$)$_2$(OH)$_6$ $\cdot$ (Ag$_x$Pb$_y$Cl$_{x+2y}$) is a structurally ideal kagome magnet, providing a platform for exploring the interplay of geometric frustration, chirality, and tunability in a disorder-free framework. Here, we present the (first) comprehensive ab initio study of its electronic and magnetic properties. The electronic structure is dominated by localized half-filled Cu $d_{x^2-y^2}$ orbitals that become insulating through electronic correlations. Mapping the low-energy physics onto a Heisenberg model reveals that the magnetism is governed primarily by two exchange interactions: a nearest-neighbor intralayer kagome coupling and a next-nearest-neighbor interlayer coupling. Their competition stabilizes an unconventional three-dimensional chiral magnetic state. Each kagome layer hosts a $\sqrt{3}\times\sqrt{3}$ order, while adjacent layers are rotated by $60^\circ$, producing a right-handed spiral along the crystallographic $c$-axis. This intrinsic chiral order emerges naturally from the crystal structure and magnetic interactions, establishing quetzalcoatlite as a distinctive realization of chiral magnetism on a perfect kagome lattice. At the same time, the small energy scale of the exchange interactions places the material close to competing magnetic regimes, suggesting that moderate pressure, chemical substitution, or structural modifications may strongly enhance frustration, suppress long-range order, and potentially drive the system toward a quantum spin-liquid state.

cond-mat.str-el↗

arXiv2026

Ab Initio Investigation of Pressure Effects in the Spin-Liquid Candidate Y-Kapellasite

Motivated by recent experiments showing pressure-induced suppression of magnetic order and the emergence of a dynamical ground state in the anisotropic kagome antiferromagnet Y-kapellasite Y3Cu9(OH)19Cl8, we perform ab initio density functional theory (DFT)calculations to investigate the evolution of magnetic exchange interactions under hydrostatic pressure. We show that pressure efficiently tunes the magnetic Hamiltonian by altering the CuOCu bond geometry, thereby driving the system towards a spin-liquid regime. This evolution is governed by a nonlinear dependence of the dominant exchange coupling on the CuOCu bond angle. We further examine the influence of hydrogen positions and find that both the OH bond length and the hydrogen out-of-plane angle strongly affect the magnetic interactions. Our results provide a microscopic explanation for the experimentally observed pressure-induced enhancement of frustration and highlight the key role of hydrogen geometry.

cond-mat.str-el↗

arXiv2026

Bobkingite, a new coupled sawtooth chain platform

We investigate the mineral bobkingite, \ce{Cu5(OH)8Cl2(H2O)2}, as a potential realization of the sawtooth chain. Using \textit{ab initio} methods, we estimate the magnetic exchange couplings and find that bobkingite hosts quasi-one-dimensional sawtooth chains, with residual three-dimensional interactions strongly suppressed by the crystal geometry. Examining the full exchange network, we find that the classical model exhibits an extensive manifold of nearly degenerate states with emergent two-dimensional character, which spin-wave theory shows to persist to leading order in quantum fluctuations as Ising degrees of freedom. Unlike other sawtooth candidates, bobkingite has negligible vertical interchain coupling, preserving a one-dimensional degeneracy even in the presence of ordering, suggesting that any long-range order is weak. Thermal fluctuations may thus stabilize a finite-temperature classical spin liquid regime, with a cascade of transitions upon cooling into successively lower-dimensional degenerate states, making bobkingite a compelling platform for exploring sawtooth chain physics.

cond-mat.str-el↗

arXiv2026

$α$-RuCl$_3$ intercalated into graphite: a new three-dimensional platform for exotic quantum phases

Multilayer graphene with different stacking sequences has emerged as a powerful setting for correlated and topological phases. In parallel, progress in graphene heterostructures with magnetic or correlated materials-most notably the Kitaev candidate $α$-RuCl$_3$-has demonstrated charge transfer, magnetic proximity effects, and interfacial reconstruction, creating new opportunities for engineered quantum systems. Motivated by these developments, we explore a three-dimensional analogue in which $α$-RuCl$_3$ layers are inserted directly into the van der Waals gaps of graphite, forming an intercalated system. Here, we report the successful synthesis and comprehensive characterization of graphite intercalated with $α$-RuCl$_3$. Using a combination of X-ray diffraction, quantum oscillation measurements, and first-principles electronic structure calculations, we study the structural and electronic properties of these intercalated crystals. Our results demonstrate that graphite intercalated with $α$-RuCl$_3$ offers a robust route to develop three-dimensional materials with access to novel correlated and topological states.

cond-mat.str-el↗

arXiv2025

Altermagnetic splitting of magnons in hematite ($α$-Fe$_2$O$_3$)

We develop a four-sublattice spin-wave theory for the $g$-wave altermagnet candidate hematite ($α$-Fe$_2$O$_3$), considering both its easy-axis phase below and its weak ferromagnetic phase above the Morin temperature. A key question is whether the defining altermagnetic feature - magnon spin splitting (also called chirality or polarization splitting) due to nonrelativistic time-reversal symmetry breaking - remains intact when relativistic corrections, which contribute to hematite's magnetic order, are included. Using a detailed symmetry analysis supported by density functional theory, we show that capturing the magnon splitting within a Heisenberg model requires exchange interactions extending at least to the 13th neighbor. We find an altermagnetic band splitting of approximately 2 meV, which contrasts with the total band width of about 100 meV. To evaluate the experimental observability of this splitting, we analyze relativistic corrections to the magnon spectrum in both magnetic phases. We show that spin-orbit coupling - manifesting as magnetocrystalline anisotropies and the Dzyaloshinskii-Moriya interaction (DMI) - does not obscure the key altermagnetic features. These findings indicate that inelastic neutron scattering can directly probe altermagnetic magnon splitting in hematite. We also discuss implications for magnon transport, particularly magnonic contributions to the thermal Hall effect (which requires spin-orbit coupling) and to spin splitter effects (which do not). Notably, we predict a third-order nonlinear magnon spin splitter effect. This result suggests that the $g$-wave magnon spin splitting in hematite enables transverse heat-to-spin conversion without requiring an external magnetic field.

cond-mat.str-el↗

arXiv2025

Microscopic origin of the magnetic interactions and their experimental signatures in altermagnetic La$_2$O$_3$Mn$_2$Se$_2$

Altermagnets (AM) are a recently introduced type of magnets, with no net magnetization like antiferromagnets, but displaying a non-relativistic Zeeman splitting in reciprocal space like ferromagnets. One of the lately discussed models to realize AM is the inverse Lieb lattice (ILL). Initially suggested as a purely theoretical construct, the ILL occurs in real materials such as La$_2$O$_3$Mn$_2$Se$_2$. However, AM on the ILL requires 90$^\circ$ nearest-neighbor superexchange to be {\it antiferromagnetic} and dominant over the 180$^\circ$ next-nearest-neighbor superexchange, in apparent contradiction to the Goodenough-Kanamori-Anderson (GKA) rules. Yet, AM ordering was found to be the ground state in La$_2$O$_3$Mn$_2$Se$_2$. Combining ab initio and analytical methods, we determine how direct exchange and superexchange act together to produce a large antiferromagnetic nearest-neigbor coupling. The seeming contradiction with the GKA rules is traced back to the multiorbital character of Mn$^{+2}$ ions. By calculating magnon bands, we identify universal signatures of the exchange interactions, suggesting experimental fingerprints.

cond-mat.str-el↗

arXiv2024

Exfoliation and Optical Properties of S=1 Triangular Lattice Antiferromagnet NiGa$_2$S$_4$

Two-dimensional (2D) van der Waals (vdW) materials have been an exciting area of research ever since scientists first isolated a single layer of graphene. Single layer magnetic materials can provide a pathway for vdW heterostructures with magnetic properties. While most of the magnetic vdW materials exhibit ordering transitions in the bulk, here we report a successful exfoliation of a triangular lattice S=1 antiferromagnet NiGa$_2$S$_4$, which already demonstrates exotic magnetism in the bulk material. We establish the number of layers of the material by atomic force microscopy (AFM) and detail a careful characterization using Raman and optical spectroscopy to demonstrate how the optical, electronic, and structural properties of NiGa$_2$S$_4$ change as a function of sample thickness. Optical measurements and electronic structure calculations of bulk versus monolayer NiGa$_2$S$_4$ confirm the material to be a Mott insulator with an electronic gap of about 1.5 eV, which slightly increases for layers below 10 L. We conclude with a theoretical analysis of the possibility of doping monolayer NiGa$_2$S$_4$ by proximity to a metal.

cond-mat.mtrl-sci↗

arXiv2024

$\textit{Ab initio}$ study of highly tunable charge transfer in $β$-RuCl$_3$/graphene heterostructures

Heterostructures of graphene in proximity to magnetic insulators open the possibility to investigate exotic states emerging from the interplay of magnetism, strain and charge transfer between the layers. Recent reports on the growth of self-integrated atomic wires of $β$-RuCl$_3$ on graphite suggest these materials as versatile candidates to investigate these effects. Here we present detailed first principles calculations on the charge transfer and electronic structure of $β$-RuCl$_3$/heterostructures and provide a comparison with the work function analysis of the related honeycomb family members $α$-RuX$_3$ (X = Cl,Br,I). We find that proximity of the two layers leads to a hole-doped graphene and electron-doped RuX$_3$ in all cases, which is sensitively dependent on the distance between the two layers. Furthermore, strain effects due to lattice mismatch control the magnetization which itself has a strong effect on the charge transfer. Charge accumulation in $β$-RuCl$_3$ strongly drops away from the chain making such heterostructures suitable candidates for sharp interfacial junctions in graphene-based devices.

cond-mat.str-el↗

arXiv2023

A $j_{\rm eff}=1/2$ Kitaev material on the triangular lattice: The case of NaRuO$_2$

Motivated by recent reports of a quantum disordered ground state in the triangular lattice compound NaRuO$_2$, we derive a $j_{\rm eff}=1/2$ magnetic model for this system by means of first-principles calculations. The pseudospin Hamiltonian is dominated by bond-dependent off-diagonal $Γ$ interactions, complemented by a ferromagnetic Heisenberg exchange and a notably antiferromagnetic Kitaev term. In addition to bilinear interactions, we find a sizable four-spin ring exchange contribution with a strongly anisotropic character, which has been so far overlooked when modeling Kitaev materials. The analysis of the magnetic model, based on the minimization of the classical energy and exact diagonalization of the quantum Hamiltonian, points toward the existence of a rather robust easy-plane ferromagnetic order, which cannot be easily destabilized by physically relevant perturbations.

cond-mat.str-el↗

arXiv2023

Improved effective vertices in the multi-orbital Two-Particle Self-Consistent method from Dynamical Mean-Field Theory

In this work we present a multi-orbital form of the Two-Particle Self-Consistent approach (TPSC), here the effective local and static irreducible interaction vertices are determined by means of the Dynamical Mean-Field Theory (DMFT). This approach replaces the approximate ansatz equations for the double occupations $\langle n^{}_{α,σ}n^{}_{β,σ'}\rangle$ by sampling them directly for the same model using DMFT. Compared to the usual Hartree-Fock like ansatz, this leads to more accurate local vertices in the weakly correlated regime, and provides access to stronger correlated systems that were previously out of reach. This approach is extended by replacing the local component of the TPSC self-energy by the DMFT impurity self-energy, which results in an improved self-energy that incorporates strong local correlations but retains a non-trivial momentum-dependence. We find that this combination of TPSC and DMFT provides a significant improvement over the multi-orbital formulation of multi-orbital TPSC, as it allows to determine the components of the spin vertex without artificial symmetry assumptions, and opens the possibility to include the transversal particle-hole channel. The new approach is also able to remove unphysical divergences in the charge vertices in TPSC. We find a general trend that lower temperatures can be accessed in the calculation. Benchmarking single-particle quantities such as the local spectral function with other many-body methods we find significant improvement in the more strongly correlated regime.

cond-mat.str-el↗

arXiv2023

Growth of self-integrated atomic quantum wires and junctions of a Mott semiconductor

Continued advances in quantum technologies rely on producing nanometer-scale wires. Although several state-of-the-art nanolithographic technologies and bottom-up synthesis processes have been used to engineer such wires, critical challenges remain in growing uniform atomic-scale crystalline wires and constructing their network structures. Here we discover a simple method to fabricate atomic-scale wires with various arrangements, including stripes, X-, Y-junctions, and nanorings. Single-crystalline atomic-scale wires of a Mott insulator, whose band gap is comparable to those of wide-gap semiconductors, are spontaneously grown on graphite substrates \DEL{and epitaxial monolayer graphene on SiC }by pulsed-laser deposition. These wires are one-unit-cell-thick and have an exact width of two- and four-unit-cells (1.4 and 2.8\,nm) and lengths up to a few $μm$. We show that the non-equilibrium reaction-diffusion processes may play an essential role in atomic pattern formation. Our findings offer a new perspective on the non-equilibrium self-organization phenomena on an atomic scale, paving a unique way for the quantum architecture of nano-network.

cond-mat.mes-hall↗

arXiv2022

Electronic and magnetic properties of the RuX$_3$ (X=Cl, Br, I) family: Two siblings -- and a cousin?

Motivated by recent reports of metallic behavior in the recently synthesized RuI$_3$, in contrast to the Mott-insulating nature of the actively discussed $α$-RuCl$_3$, as well as RuBr$_3$, we present a detailed comparative analysis of the electronic and magnetic properties of this family of trihalides. Using a combination of first-principles calculations and effective-model considerations, we conclude that RuI$_3$, similarly to the other two members, is most probably on the verge of a Mott insulator, but with much smaller magnetic moments and a strong magnetic frustration. We predict the ideal pristine crystal of RuI$_3$ to have a nearly vanishing conventional nearest-neighbor Heisenberg interaction and to be a quantum spin liquid candidate of possibly different kind than the Kitaev spin liquid. In order to understand the apparent contradiction to the reported resistivity $ρ$, we analyze the experimental evidence for all three compounds and propose a scenario for the observed metallicity in existing samples of RuI$_3$. Furthermore, for the Mott insulator RuBr$_3$ we obtain a magnetic Hamiltonian of a similar form to that in the much discussed $α$-RuCl$_3$ and show that this Hamiltonian is in agreement with experimental evidence in RuBr$_3$.

cond-mat.str-el↗

arXiv2022

Microscopic origin of magnetism in monolayer $3d$ transition metal dihalides

Motivated by the recent wealth of exotic magnetic phases emerging in two-dimensional frustrated lattices, we investigate the origin of possible magnetism in the monolayer family of triangular lattice materials $MX_2$ ($M$={V, Mn, Ni}, $X$={Cl, Br, I}). We first show that consideration of general properties such as filling and hybridization enables to formulate trends for the most relevant magnetic interaction parameters. In particular, we observe that the effects of spin-orbit coupling (SOC) can be effectively tuned through the ligand elements as the considered 3$d$ transition metal ions do not strongly contribute to the anisotropic component of the inter-site exchange interaction. Consequently, we find that the corresponding SOC matrix-elements differ significantly from the atomic limit. In a next step and by using two complementary approaches based on first principles, we extract realistic effective spin models and find that in the case of heavy ligand elements, SOC effects manifest in anisotropic exchange and single-ion anisotropy only for specific fillings.

cond-mat.str-el↗

arXiv2022

Multi-Center Magnon Excitations Open the Entire Brillouin Zone to Terahertz Magnetometry of Quantum Magnets

Due to the small photon momentum, optical spectroscopy commonly probes magnetic excitations only at the center of the Brillouin zone; however, there are ways to override this restriction. In the case of the distorted kagome quantum magnet Y-kapellasite, Y$_3$Cu$_9$(OH)$_{19}$Cl$_8$, under scrutiny here, the magnon density of states can be accessed over the entire Brillouin zone through three-center magnon excitations. This mechanism is aided by the three different magnetic sublattices and strong short-range correlations in the distorted kagome lattice. The results of THz time-domain experiments agree remarkably well with linear spin-wave theory. Relaxing the conventional zone-center constraint of photons gives a new aspect to probe magnetism in matter.

cond-mat.str-el↗

arXiv2021

Phase diagram of a distorted kagome antiferromagnet and application to Y-kapellasite

We investigate the magnetism of a previously unexplored distorted spin-1/2 kagome model consisting of three symmetry-inequivalent nearest-neighbor antiferromagnetic Heisenberg couplings Jhexagon, J and J', and uncover a rich ground state phase diagram even at the classical level. Using analytical arguments and numerical techniques we identify a collinear Q = 0 magnetic phase, two unusual non-collinear coplanar Q = (1/3,1/3) phases and a classical spin liquid phase with a degenerate manifold of non-coplanar ground states, resembling the jammed spin liquid phase found in the context of a bond-disordered kagome antiferromagnet. We further show with density functional theory calculations that the recently synthesized Y-kapellasite Y3Cu9(OH)19Cl8 is a realization of this model and predict its ground state to lie in the region of Q = (1/3,1/3) order, which remains stable even after inclusion of quantum fluctuation effects within variational Monte Carlo and pseudofermion functional renormalization group. The presented model opens a new direction in the study of kagome antiferromagnets.

cond-mat.str-el↗