arXiv subjects

Ruchika Mahajan

Publications and source records attributed to Ruchika Mahajan.

3 recordsLinked to original sources

arXiv2026

Comparative study of magnetic exchange parameters and magnon dispersions in NiO and MnO from first principles

Spin-wave excitations are fundamental to understanding the behavior of magnetic materials and hold promise for future information and communication technologies. Yet, modeling these accurately in transition-metal compounds remains challenging, starting from the self-interaction errors affecting localized and partially filled $d$-orbitals in density-functional theory (DFT) with (semi-)local functionals. In this work, we compare three advanced first-principles approaches for computing magnetic exchange parameters and magnon dispersions in NiO and MnO, all based on a common DFT+$U$ ground state with ab initio Hubbard $U$ values obtained from density-functional perturbation theory. Two methods extract exchange parameters directly: one via total-energy differences using the four-state mapping ($ΔE$), and the other via the magnetic force theorem (MFT) using infinitesimal spin rotations. Magnon dispersions are then obtained from a Heisenberg Hamiltonian through linear spin-wave theory (LSWT). The third approach, time-dependent density-functional perturbation theory with $U$ (TDDFPT+$U$), yields magnon dispersions directly from the dynamical spin susceptibility, with exchange parameters fitted a posteriori, for comparison, via LSWT. Our results show that TDDFPT+$U$ and the Heisenberg model based on $ΔE$-derived parameters align well with experimental neutron scattering data, whereas the MFT-based approach shows larger discrepancies, possibly due to some inherent approximations and limitations of the particular implementation used. This study benchmarks the accuracy of state-of-the-art first-principles techniques for spin-wave modeling and contributes to advancing reliable computational tools for the study and design of magnetic materials.

cond-mat.mtrl-sci↗

arXiv2022

Pivotal Role of Intersite Hubbard Interactions in Fe-doped $α$-MnO$_2$

We present a first-principles investigation of the structural, electronic, and magnetic properties of the pristine and Fe-doped $α$-MnO$_2$ using density-functional theory with extended Hubbard functionals. The onsite $U$ and intersite $V$ Hubbard parameters are determined from first principles and self-consistently using density-functional perturbation theory in the basis of Löwdin-orthogonalized atomic orbitals. For the pristine $α$-MnO$_2$ we find that the so-called C2-AFM spin configuration is the most energetically favorable, in agreement with the experimentally observed antiferromagnetic ground state. For the Fe-doped $α$-MnO$_2$ two types of doping are considered: Fe insertion in the $2 \times 2$ tunnels and partial substitution of Fe for Mn. We find that the interstitial doping preserves the C2-AFM spin configuration of the host lattice only when both onsite $U$ and intersite $V$ Hubbard corrections are included, while for the substitutional doping the onsite Hubbard $U$ correction alone is able to preserve the C2-AFM spin configuration of the host lattice. The oxidation state of Fe is found to be $+2$ and $+4$ in the case of the interstitial and substitutional doping, respectively, while the oxidation state of Mn is $+4$ in both cases. This work paves the way for accurate studies of other MnO$_2$ polymorphs and complex transition-metal compounds when the localization of $3d$ electrons occurs in the presence of strong covalent interactions with ligands.

cond-mat.mtrl-sci↗

arXiv2021

Importance of intersite Hubbard interactions in $β$-MnO$_2$: A first-principles DFT+$U$+$V$ study

We present a first-principles investigation of the structural, electronic, and magnetic properties of pyrolusite ($β$-MnO$_2$) using conventional and extended Hubbard-corrected density-functional theory (DFT+$U$ and DFT+$U$+$V$). The onsite $U$ and intersite $V$ Hubbard parameters are computed using linear-response theory in the framework of density-functional perturbation theory. We show that while the inclusion of the onsite $U$ is crucial to describe the localized nature of the Mn($3d$) states, the intersite $V$ is key to capture accurately the strong hybridization between neighboring Mn($3d$) and O($2p$) states. In this framework, we stabilize the simplified collinear antiferromagnetic (AFM) ordering (suggested by the Goodenough-Kanamori rule) that is commonly used as an approximation to the experimentally-observed noncollinear screw-type spiral magnetic ordering. A detailed investigation of the ferromagnetic and of other three collinear AFM spin configurations is also presented. The findings from Hubbard-corrected DFT are discussed using two kinds of Hubbard manifolds - nonorthogonalized and orthogonalized atomic orbitals - showing that special attention must be given to the choice of the Hubbard projectors, with orthogonalized manifolds providing more accurate results than nonorthogonalized ones within DFT+$U$+$V$. This work paves the way for future studies of complex transition-metal compounds containing strongly localized electrons in the presence of pronounced covalent interactions.

cond-mat.mtrl-sci↗