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Kyungwha Park

Publications and source records attributed to Kyungwha Park.

At least 19 recordsLinked to original sources
arXiv2026

Cluster-configurational study of G-center in Silicon

Understanding the properties of defects is imperative for proper use for variety of applications including quantum computing. In this paper, we use the multiconfigurational self consistent field (MCSCF) combined with DFT optimized geometry in order to investigate the spin and optical properties of G centers in Silicon. By utilizing quantum chemistry based methods, we show excellent agreement with the Zero Phonon Line and Zero Field Splitting Tensor components of the G center. We also calculate the theoretical spin decoherence time of the G centers using Cluster Correlation Expansion (CCE) methods.

quant-ph↗
arXiv2026

Improving Jet A-1 Thermal-Oxidative Stability through Selective Removal of Unwanted Trace Species via 3.7 Å Chabazite Filtration

The thermal stability of Jet A-1 fuel is strongly affected by trace heteroatomic species that promote thermal oxidative deposit formation, as well as antioxidant additives such as butylated hydroxytoluene, which preserve fuel stability. 3.7 Å chabazite is a tunable microporous adsorbent, but optimizing its composition requires balancing promoter removal against antioxidant loss. Here, we use density functional theory and \textit{ab initio} molecular dynamics (AIMD) to evaluate this trade-off using two compositional descriptors: framework acidity (Si/Al $= 35$--$8$) and bimetallic substitution (Co, Mg, Zn) at fixed Al content. Lowering Si/Al strengthens adsorption of all species, including BHT, confirming an intrinsic selectivity penalty for acidity-only tuning. In contrast, bimetallic substitution introduces chemically selective behavior, strengthening uptake of specific promoters while either suppressing or enhancing antioxidant adsorption depending on dopant identity. AIMD simulations at 400 K further show that adsorption energy alone is insufficient to describe calculated trends, because molecular mobility inside chabazite can influence residence time and effective capture during fuel treatment. Analysis of the density of states and the participating wavefunctions reveals signatures that are consistent with dopant-dependent adsorption shifts. These results establish a unified adsorption--transport--electronic screening framework for selecting chabazite compositions that remove deposit promoters while preserving antioxidant functionality in Jet A-1 treatment.

physics.chem-ph↗
arXiv2026

Influence of Magnetic Order on Proximity-Induced Superconductivity in Mn Layers on Nb(110) from First Principles

We investigate the influence of magnetic order on the proximity-induced superconducting state in the Mn layers of a Mn-Nb(110) heterostructure by using a first-principles method. For this study, we use the recently developed Bogoliubov-de Gennes (BdG) solver for superconducting heterostructures [Csire et al., Phys. Rev. B 97, 024514 (2018)] within the first-principles calculations based on multiple scattering theory and the screened Korringa-Kohn-Rostoker (SKKR) Green's function method. In our calculations, we first study the normal-state density of states (DOS) in the single- and double-Mn-layer heterostructures, and calculate the induced magnetic moments in the Nb layers. Next, we compute the momentum-resolved spectral functions in the superconducting state for the heterostructure with a single Mn layer, and find bands crossing the Fermi level within the superconducting (SC) gap. We also study the SC state DOS in the single- and double-Mn-layer heterostructures and compare some of our results with experimental findings, revealing secondary gaps, plateau-like regions, and central V-shaped in-gap states within the bulk SC Nb gap that are magnetic-order-dependent. Finally, we compute the singlet and internally antisymmetric triplet (IAT) order parameters for each layer for both heterostructures, and find an order of magnitude difference in the induced singlet part of the SC order parameter in the Mn layer/s between the FM and AFM cases in favor of the AFM pairing with the maximum still being only 4.44% of the bulk Nb singlet order parameter value. We also find a negligible induced triplet part, yet comparable to the induced singlet values, indicating some singlet-triplet mixing in the Mn layer/s.

cond-mat.supr-con↗
arXiv2024

Probing Berry curvature in magnetic topological insulators through resonant infrared magnetic circular dichroism

Probing the quantum geometry and topology in condensed matter systems has relied heavily on static electronic transport experiments in magnetic fields. Yet, contact-free optical measurements have rarely been explored. Magnetic dichroism (MCD), the nonreciprocal absorption of circular polarized light, was theoretically linked to the quantized anomalous Hall effect in magnetic insulators and can identify the bands and momenta responsible for the underlying Berry Curvature (BC). Detecting BC through MCD faces two challenges: First, the relevant inter-band transitions usually generate MCD in the infrared (IR) range, requiring large samples with high quality. Second, while most magnetic materials are metallic, the relation between MCD and BC in metals remains unclear. Here, we report the observation of MCD in the IR range along with the anomalous Hall effect in thin film MnBi2Te4. Both phenomena emerge with a field-driven phase transition from an antiferromagnet to a canted ferromagnet. By theoretically relating the MCD to the anomalous Hall effect via BC in a metal, we show that this transition accompanies an abrupt onset of BC, signaling a topological phase transition from a topological insulator to a doped Chern insulator. Our density functional theory calculation suggests the MCD signal mainly originates from an optical transition at the Brillouin zone edge, hinting at a potential new source of BC away from the commonly considered Γ point. Our findings demonstrate a novel experimental approach for detecting BC and identifying the responsible bands and momenta, generally applicable to magnetic materials.

cond-mat.mes-hall↗
arXiv2024

Competing d$_{xy}$ and s$_{\pm }$ Pairing Symmetries in Superconducting La$_{3}$Ni$_{2}$O$_{7}$ emerge from LDA+FLEX Calculations

With recent discoveries of superconductivity in infinite--layer nickelates, and in La$_{3}$Ni$_{2}$O$_{7}$ under high pressure, new opportunities appeared that yet another family of high--temperature superconductors based on Ni element may exist in Nature as was previously the case of cuprates and iron based materials. With their famous strong Coulomb correlations among 3d electrons and the proximity to antiferromagnetic instability these systems represent a challenge for their theoretical description, and most previous studies of superconductivity relied on the solutions of simplified few--orbital model Hamiltonians. Here, on the other hand, we use a recently developed combination of density functional theory with momentum and frequency resolved self--energies deduced from the so--called Fluctuational--Exchange (FLEX)--type Random Phase Approximation (RPA) to study spin fluctuation mediated pairing tendencies in La$_{3}$Ni$_{2}$O$_{7}$ under pressure. This methodology uses first--principle electronic structures of an actual material and is free of tight--binding parametrizations employed in model Hamiltonian approach. Based on our numerical diagonalization of the BCS Gap equation we show that competing d$_{xy}$ and s$_{\pm }$ pairing symmetries emerge in superconducting La$_{3}$Ni$_{2}$O$% _{7}$ with the corresponding coupling constants becoming large in the proximity of spin density wave instability. The results presented here are discussed in light of numerous other calculations and provide on--going experimental efforts with predictions that will allow further tests of our understanding of unconventional superconductors.

cond-mat.supr-con↗
arXiv2023

Hydrogen induces chiral conduction channels in the topological magnet

Chirality, a characteristic handedness that distinguishes 'left' from 'right', cuts widely across all of nature$^1$, from the structure of DNA$^2$ to opposite chirality of particles and antiparticles$^3$. In condensed matter chiral fermions have been identified in Weyl semimetals$^4$ through their unconventional electrodynamics arising from 'axial' charge imbalance between chiral Weyl nodes of topologically nontrivial electronic bands. Up to now it has been challenging or impossible to create transport channels of Weyl fermions in a single material that could be easily configured for advancing chiral logic or spintronics$^{5,6}$. Here we generate chirality-directed conduction channels in inversion-symmetric Weyl ferromagnet (FM) $MnSb_2Te_4$, emergent from a deep connection between chirality in reciprocal and real space. We alter the bandstructure on-demand with an intake and a subsequent release of ionic hydrogen ($H^+$) $-$ a process we show to induce the tilt and rotation of Weyl bands. The transformed Weyl FM states feature a doubled Curie temperature $\geq50K$ and an enhanced angular transport chirality synchronous with a rare field-antisymmetric longitudinal resistance $-$ a low-field tunable 'chiral switch' that roots in the interplay of Berry curvature$^7$, chiral anomaly$^8$ and hydrogen-engendered mutation of Weyl nodes.

cond-mat.mtrl-sci↗
arXiv2023

Relativistic Douglas-Kroll-Hess Calculations of Hyperfine Interactions within First Principles Multireference Methods

Relativistic magnetic hyperfine interaction Hamiltonian based on the Douglas-Kroll-Hess (DKH) theory up to the second order is implemented within the ab initio multireference methods including spin-orbit coupling in the Molcas/OpenMolcas package. This implementation is applied to calculate relativistic hyperfine coupling (HFC) parameters for atomic systems and diatomic radicals with valence s or d orbitals by systematically varying active space size in the restricted active space self-consistent field (RASSCF) formalism with restricted active space state interaction (RASSI) for spin-orbit coupling. The DKH relativistic treatment of the hyperfine interaction reduces the Fermi contact contribution to the HFC due to the presence of kinetic factors that regularize the singularity of the Dirac delta function in the nonrelativitic Fermi contact operator. This effect is more prominent for heavier nuclei. As the active space size increases, the relativistic correction of the Fermi contact contribution converges well to the experimental data for light and moderately heavy nuclei. The relativistic correction, however, does not significantly affect the spin-dipole contribution to the hyperfine interaction. In addition to the atomic and molecular systems, the implementation is applied to calculate the relativistic HFC parameters for large trivalent and divalent Tb-based single-molecule magnets (SMMs) such as Tb(III)Pc$_2$ and Tb(II)(Cp$^\text{iPr5}$)$_2$ without ligand truncation using well-converged basis sets. In particular, for the divalent SMM which has an unpaired valence 6s/5d hybrid orbital, the relativistic treatment of HFC is crucial for a proper description of the Fermi contact contribution. Even with the relativistic hyperfine Hamiltonian, the divalent SMM is shown to exhibit strong tunability of HFC via an external electric field (i.e., strong hyperfine Stark effect).

cond-mat.mtrl-sci↗
arXiv2023

Higher-order topological superconductivity in a topological metal 1T$^\prime$-MoTe$_2$

One key challenge in the field of topological superconductivity (Tsc) has been the rareness of material realization. This is true not only for the first-order Tsc featuring Majorana surface modes, but also for the higher-order Tsc, which host Majorana hinge and corner modes. Here, we propose a four-step strategy that mathematically derives comprehensive guiding principles for the search and design for materials of general higher-order Tsc phases. Specifically, such recipes consist of conditions on the normal state and pairing symmetry that can lead to a given higher-order Tsc state. We demonstrate this strategy by obtaining recipes for achieving three-dimensional higher-order Tsc phases protected by the inversion symmetry. Following our recipe, we predict that the observed superconductivity in centrosymmetric MoTe$_2$ is a candidate for higher-order Tsc with corner modes. Our proposed strategy enables systematic materials search and design for higher-order Tsc, which can mobilize the experimental efforts and accelerate the material discovery for higher-order Tsc phases.

cond-mat.supr-con↗
arXiv2023

Superconducting topological Dirac semimetals: $P6/m$-Si$_6$ and $P6/m$-NaSi$_6$

We theoretically propose that hexagonal silicon-based crystals, $P6/m$-Si$_6$ and $P6/m$-NaSi$_6$, are topological Dirac semimetals with superconducting critical temperatures of 12 K and 13 K, respectively, at ambient pressure. Band inversion occurs with the Fu-Kane topological invariant $\mathbb{Z}_2=1$, even in the absence of spin-orbit coupling. The Dirac nodes protected by $C_6$ crystal rotational symmetry remain gapless with spin-orbit coupling. Using first-principles calculations, we find pressure-induced topological phase transitions for $P6/m$-Si$_6$ and $P6/m$-NaSi$_6$ with critical external pressures of 11.5 GPa and 14.9 GPa, respectively. Above the critical pressures, the Dirac bands are gapped with $\mathbb{Z}_2=0$, while the superconducting states and the crystal symmetries are retained.Our results may shed light into a search for silicon-based topological materials with superconductivity.

cond-mat.supr-con↗
arXiv2022

Computational Insights into Electronic Excitations, Spin-Orbit Coupling Effects, and Spin Decoherence in Cr(IV)-based Molecular Qubits

The great success of point defects and dopants in semiconductors for quantum information processing has invigorated a search for molecules with analogous properties. Flexibility and tunability of desired properties in a large chemical space have great advantages over solid-state systems. The properties analogous to point defects were demonstrated in Cr(IV)-based molecular family, Cr(IV)(aryl)$_4$, where the electronic spin states were optically initialized, read out, and controlled. Despite this kick-start, there is still a large room for enhancing properties crucial for molecular qubits. Here we provide computational insights into key properties of the Cr(IV)-based molecules aimed at assisting chemical design of efficient molecular qubits. Using the multireference ab-initio methods, we investigate the electronic states of Cr(IV)(aryl)$_4$ molecules with slightly different ligands, showing that the zero-phonon line energies agree with the experiment, and that the excited spin-triplet and spin-singlet states are highly sensitive to small chemical perturbations. By adding spin-orbit interaction, we find that the sign of the uniaxial zero-field splitting (ZFS) parameter is negative for all considered molecules, and discuss optically-induced spin initialization via non-radiative intersystem crossing. We quantify (super)hyperfine coupling to the $^{53}$Cr nuclear spin and to the $^{13}$C and $^1$H nuclear spins, and we discuss electron spin decoherence. We show that the splitting or broadening of the electronic spin sub-levels due to superhyperfine interaction with $^1$H nuclear spins decreases by an order of magnitude when the molecules have a substantial transverse ZFS parameter.

cond-mat.mtrl-sci↗
arXiv2021

Spin-polarized zero-bias peak from a single magnetic impurity at an s-wave superconductor: first-principles study

Magnetic impurities at surfaces of superconductors can induce bound states referred to as Yu-Shiba-Rusinov (YSR) states within superconducting gaps. Understanding of YSR states with spin-orbit coupling (SOC) plays a pivotal role in studies of Majorana zero modes. Spin polarization of a zero-bias peak (ZBP) is used to determine its topological nature. Here we investigate the YSR states of single magnetic impurities at the surface of Pb using the fully relativistic first-principles simulations including band structure of Pb and five 3$d$ orbitals of the impurity in the superconducting state. We show that for single Fe and Co impurities, strong SOC can induce a ZBP with rotation of the impurity magnetic moment and that the ZBP has large spin polarization in contrast to effective model studies. Conditions for a ZBP from a single magnetic impurity are discussed. Our results are relevant to longer atomic chains considering their canting and noncollinear magnetism.

cond-mat.supr-con↗
arXiv2021

Systemic Consequences of Disorder in Magnetically Self-Organized Topological MnBi$_{2}$Te$_{4}/$(Bi$_{2}$Te$_{3}$)$_{n}$ Superlattices

MnBi$_{2}$Te$_{4}/$(Bi$_{2}$Te$_{3}$)$_{n}$ materials system has recently generated strong interest as a natural platform for realization of the quantum anomalous Hall (QAH) state. The system is magnetically much better ordered than substitutionally doped materials, however, the detrimental effects of certain disorders are becoming increasingly acknowledged. Here, from compiling structural, compositional, and magnetic metrics of disorder in ferromagnetic MnBi$_{2}$Te$_{4}/$(Bi$_{2}$Te$_{3}$)$_{n}$ it is found that migration of Mn between MnBi$_{2}$T$e_{4}$ septuple layers (SLs) and otherwise non-magnetic Bi$_{2}$Te$_{3}$ quintuple layers (QLs) has systemic consequences - it induces ferromagnetic coupling of Mn-depleted SLs with Mn-doped QLs, seen in ferromagnetic resonance as an acoustic and optical resonance mode of the two coupled spin subsystems. Even for a large SL separation (n $\gtrsim$ 4 QLs) the structure cannot be considered as a stack of uncoupled two-dimensional layers. Angle-resolved photoemission spectroscopy and density functional theory studies show that Mn disorder within an SL causes delocalization of electron wavefunctions and a change of the surface bandstructure as compared to the ideal MnBi$_{2}$Te$_{4}/$(Bi$_{2}$Te$_{3}$)$_{n}$. These findings highlight the critical importance of inter- and intra-SL disorder towards achieving new QAH platforms as well as exploring novel axion physics in intrinsic topological magnets.

cond-mat.mtrl-sci↗
arXiv2021

Relativistic first principles theory of Yu--Shiba--Rusinov states applied to an Mn adatom and Mn dimers on Nb(110)

We present a fully relativistic first principles based theoretical approach for the calculation of the spectral properties of magnetic impurities on the surface of a superconducting substrate, providing a material specific framework for the investigation of the Yu--Shiba--Rusinov (YSR) states. By using a suitable orbital decomposition of the local densities of states we discuss in great details the formation of the YSR states for an Mn adatom and for two kinds of Mn dimers placed on the Nb(110) surface and compare our results to recent experimental findings. In case of the adatom we find that the spin-orbit coupling slightly shifts some of the YSR peaks and also the local spin-polarization on the Nb atoms have marginal effects to the their positions. Moreover, by scaling the exchange field on the Mn site we could explain the lack of the $d_{x^2-y^2}$-like YSR state in the spectrum. While our results for a close packed ferromagnetic dimer are in satisfactory agreement with the experimentally observed splitting of the YSR states, in case of an antiferromagnetic dimer we find that the spin-orbit coupling is not sufficiently large to explain the splitting of the YSR states seen in the experiment. Changing the relative orientation of the magnetic moments in this dimer induces splitting of the YSR states and also shifts their energy, leading even to the formation of a zero bias peak in case of the deepest YSR state.

cond-mat.supr-con↗
arXiv2021

Electronic Structure of Mononuclear Cu-based Molecule from Density-Functional Theory with Self-Interaction Correction

We investigate the electronic structure of a planar mononuclear Cu-based molecule [Cu(C$_6$H$_4$S$_2$)$_2$]$^z$ in two oxidation states ($z$$=$$-2$, $-$1) using density-functional theory (DFT) with Fermi-Löwdin orbital (FLO) self-interaction correction (SIC). The dianionic Cu-based molecule was proposed to be a promising qubit candidate. Self-interaction error within approximate DFT functionals renders severe delocalization of electron and spin densities arising from 3$d$ orbitals. The FLO-SIC method relies on optimization of Fermi-Löwdin orbital descriptors (FODs) with which localized occupied orbitals are constructed to create the SIC potentials. Starting with many initial sets of FODs, we employ a frozen-density loop algorithm within the FLO-SIC method to study the Cu-based molecule. We find that the electronic structure of the molecule remains unchanged despite somewhat different final FOD configurations. In the dianionic state (spin $S=1/2$), FLO-SIC spin density originates from the Cu $d$ and S $p$ orbitals with an approximate ratio of 2:1, in quantitative agreement with multireference calculations, while in the case of SIC-free DFT, the orbital ratio is reversed. Overall, FLO-SIC lowers the energies of the occupied orbitals and in particular the 3$d$ orbitals unhybridized with the ligands significantly, which substantially increases the energy gap between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) compared to SIC-free DFT results. The FLO-SIC HOMO-LUMO gap of the dianionic state is larger than that of the monoionic state, which is consistent with experiment. Our results suggest a positive outlook of the FLO-SIC method in the description of magnetic exchange coupling within 3$d$-element based systems.

cond-mat.mes-hall↗
arXiv2021

Topological surface currents accessed through reversible hydrogenation of the three-dimensional bulk

Hydrogen, the smallest and most abundant element in nature, can be efficiently incorporated within a solid and drastically modify its electronic state - it has been known to induce novel magnetoelectric effects in complex perovskites and modulate insulator-to-metal transition in a correlated Mott oxide. Here we demonstrate that hydrogenation resolves an outstanding challenge in chalcogenide classes of three-dimensional (3D) topological insulators and magnets - the control of intrinsic bulk conduction that denies access to quantum surface transport. With electrons donated by a reversible binding of H+ ions to Te(Se) chalcogens, carrier densities are easily changed by over 10^20 cm^-3, allowing tuning the Fermi level into the bulk bandgap to enter surface/edge current channels. The hydrogen-tuned topological materials are stable at room temperature and tunable disregarding bulk size, opening a breadth of platforms for harnessing emergent topological states.

cond-mat.mtrl-sci↗
arXiv2020

A multiconfigurational study of the negatively charged nitrogen-vacancy center in diamond

Deep defects in wide band gap semiconductors have emerged as leading qubit candidates for realizing quantum sensing and information applications. Due to the spatial localization of the defect states, these deep defects can be considered as artificial atoms/molecules in a solid state matrix. Here we show that unlike single-particle treatments, the multiconfigurational quantum chemistry methods, traditionally reserved for atoms/molecules, accurately describe the many-body characteristics of the electronic states of these defect centers and correctly predict properties that single-particle treatments fail to obtain. We choose the negatively charged nitrogen-vacancy (NV$^-$) center in diamond as the prototype defect to study with these techniques due to its importance for quantum information applications and because its properties are well-known, which makes it an ideal benchmark system. By properly accounting for electron correlations and including spin-orbit coupling and dipolar spin-spin coupling in the quantum chemistry calculations, for the NV$^-$ center in diamond clusters, we are able to: (i) show the correct splitting of the ground (first-excited) triplet state into two levels (four levels), (ii) calculate zero-field splitting values of the ground and excited triplet states, in good agreement with experiment, and (iii) calculate the energy differences between ground and exited spin-triplet and spin-singlet states, as well as their ordering, which are also found to be in good agreement with recent experimental data. The numerical procedure we have developed is general and it can screen other color centers whose properties are not well known but promising for applications.

quant-ph↗
arXiv2020

Electrically tuned hyperfine spectrum in neutral Tb(II)(Cp$^{\rm{iPr5}}$)$_2$ single-molecule magnet

Molecular spin qubits with long spin coherence time as well as non-invasive operation methods on such qubits are in high demand. It was shown that both molecular electronic and nuclear spin levels can be used as qubits. In solid state systems with dopants, an electric field was shown to effectively change the spacing between the nuclear spin qubit levels when the electron spin density is high at the nucleus of the dopant. Inspired by such solid-state systems, we propose that divalent lanthanide (Ln) complexes with an unusual electronic configuration of Ln$^{2+}$ have a strong interaction between the Ln nuclear spin and the electronic degrees of freedom, which renders electrical tuning of the interaction. As an example, we study electronic structure and hyperfine interaction of the $^{159}$Tb nucleus in a neutral Tb(II)(Cp$^{\rm{iPr5}}$)$_2$ single-molecule magnet (SMM) using the complete active space self-consistent field method with spin-orbit interaction included within the restricted active space state interaction. Our calculations show that the low-energy states arise from $4f^8(6s,5d_{z^2})^1$, 4$f^8$(5$d_{x^2-y^2}$)$^1$, and $4f^8(5d_{xy})^1$ configurations. We compute the hyperfine interaction parameters and the electronic-nuclear spectrum within our multiconfigurational approach. We find that the hyperfine interaction is about one order of magnitude greater than that for Tb(III)Pc$_2$ SMMs. This stems from the strong Fermi contact interaction between the Tb nuclear spin and the electron spin density at the nucleus that originates from the occupation of the $(6s,5d)$ orbitals. We also uncover that the response of the Fermi contact term to electric field results in electrical tuning of the electronic-nuclear level separations. This hyperfine Stark effect may be useful for applications of molecular nuclear spins for quantum computing.

cond-mat.mtrl-sci↗
arXiv2020

Proximity effect in a superconductor-topological insulator heterostructure based on first principles

Superconductor-topological insulator (SC-TI) heterostructures were proposed to be a possible platform to realize and control Majorana zero-modes. Despite experimental signatures indicating their existence, univocal interpretation of the observed features demands theories including realistic electronic structures. To achieve this, we solve the Kohn-Sham-Dirac-Bogoliubov-de Gennes equations for ultrathin Bi$_2$Se$_3$ films on superconductor PdTe, within the fully relativistic Korringa-Kohn-Rostoker method, and investigate quasiparticle spectra as a function of chemical potential and film thickness. We find a strongly momentum-dependent proximity-induced gap feature where the gap sizes highly depend on characteristics of the TI states. The interface TI Dirac state is relevant to the induced gap only when the chemical potential is close to the Dirac-point energy. Otherwise, at a given chemical potential, the largest induced gap arises from the highest-energy quantum-well states, whereas the smallest gap arises from the TI topological surface state with its gap size depending on the TI pairing potential.

cond-mat.supr-con↗