arXiv subjects

Kyungwha Park

Publications and source records attributed to Kyungwha Park.

At least 37 records · Page 2Linked to original sources

arXiv2020

Hyperfine and quadrupole interactions for Dy isotopes in DyPc$_2$ molecules

Nuclear spin levels play an important role in understanding magnetization dynamics and implementation and control of quantum bits in lanthanide-based single-molecule magnets. We investigate the hyperfine and nuclear quadrupole interactions for $^{161}$Dy and $^{163}$Dy nucleus in anionic DyPc$_2$ (Pc=phthalocyanine) single-molecule magnets, using multiconfigurational ab-initio methods (beyond density-functional theory) including spin-orbit interaction. The two isotopes of Dy are chosen because the others have zero nuclear spin. Both isotopes have the nuclear spin $I=5/2$, although the magnitude and sign of the nuclear magnetic moment differ from each other. The large energy gap between the electronic ground and first-excited Kramers doublets, allows us to map the microscopic hyperfine and quadrupole interaction Hamiltonian onto an effective Hamiltonian with an electronic pseudo-spin $S_{\rm eff}=1/2$ that corresponds to the ground Kramers doublet. Our ab-initio calculations show that the coupling between the nuclear spin and electronic orbital angular momentum contributes the most to the hyperfine interaction and that both the hyperfine and nuclear quadrupole interactions for $^{161}$Dy and $^{163}$Dy nucleus are much smaller than those for $^{159}$Tb nucleus in TbPc$_2$ single-molecule magnets. The calculated separations of the electronic-nuclear levels are comparable to experimental data reported for $^{163}$DyPc$_2$. We demonstrate that hyperfine interaction for Dy Kramers ion leads to tunnel splitting (or quantum tunneling of magnetization) at zero field. This effect does not occur for TbPc$_2$ single-molecule magnets. The magnetic field values of the avoided level crossings for $^{161}$DyPc$_2$ and $^{163}$DyPc$_2$ are found to be noticeably different, which can be observed from experiment.

cond-mat.mtrl-sci↗

arXiv2020

Toward long-range entanglement between electrically driven single-molecule magnets

Over the past two decades, several molecules have been explored as possible building blocks of a quantum computer, a device that would provide exponential speedups for a number of problems, including the simulation of large, strongly correlated chemical systems. Achieving strong interactions and entanglement between molecular qubits remains an outstanding challenge. Here, we show that the TbPc$_2$ single-molecule magnet has the potential to overcome this obstacle due to its sensitivity to electric fields stemming from the hyperfine Stark effect. We show how this feature can be leveraged to achieve long-range entanglement between pairs of molecules using a superconducting resonator as a mediator. Our results suggest that the molecule-resonator interaction is near the edge of the strong-coupling regime and could potentially pass into it given a more detailed, quantitative understanding of the TbPc$_2$ molecule.

quant-ph↗

arXiv2020

Observation of high-temperature quantum anomalous Hall regime in intrinsic MnBi$_2$Te$_4$/Bi$_2$Te$_3$ superlattice

The quantum anomalous Hall effect is a fundamental transport response of a topologically non-trivial system in zero magnetic field. Its physical origin relies on the intrinsically inverted electronic band structure and ferromagnetism, and its most consequential manifestation is the dissipation-free flow of chiral charge currents at the edges that can potentially transform future quantum electronics. Here we report a previously unknown Berry-curvature-driven anomalous Hall regime ('Q-window') at above-Kelvin temperatures in the magnetic topological bulk crystals where through growth Mn ions self-organize into a period-ordered MnBi$_2$Te$_4$/Bi$_2$Te$_3$ superlattice. Robust ferromagnetism of the MnBi$_2$Te$_4$ monolayers opens a large surface gap, and anomalous Hall conductance reaches an $e^2/h$ quantization plateau when the Fermi level is tuned into this gap within a Q-window in which the anomalous Hall conductance from the bulk is to a high precision zero. The quantization in this new regime is not obstructed by the bulk conduction channels and thus should be present in a broad family of topological magnets.

cond-mat.mtrl-sci↗

arXiv2019

Nature of hyperfine interactions in TbPc$_2$ single-molecule magnets: Multireference ab-initio study

Lanthanide-based single-ion magnetic molecules can have large magnetic hyperfine interactions as well as large magnetic anisotropy. Recent experimental studies reported tunability of these properties by changes of chemical environments or by application of external stimuli for device applications. In order to provide insight onto the origin and mechanism of such tunability, here we investigate the magnetic hyperfine and nuclear quadrupole interactions for $^{159}$Tb nucleus in TbPc$_2$ (Pc=phthalocyanine) single-molecule magnets using multireference ab-initio methods including spin-orbit interaction. Since the electronic ground and first-excited (quasi)doublets are well separated in energy, the microscopic Hamiltonian can be mapped onto an effective Hamiltonian with an electronic pseudo-spin $S=1/2$. From the ab-initio-calculated parameters, we find that the magnetic hyperfine coupling is dominated by the interaction of the Tb nuclear spin with electronic orbital angular momentum. The asymmetric $4f$-like electronic charge distribution leads to a strong nuclear quadrupole interaction with significant non-axial terms for the molecule with low symmetry. The ab-initio calculated electronic-nuclear spectrum including the magnetic hyperfine and quadrupole interactions is in excellent agreement with experiment. We further find that the non-axial quadrupole interactions significantly influence the avoided level crossings in magnetization dynamics and that the molecular distortions affect mostly the Fermi contact terms as well as the non-axial quadrupole interactions.

cond-mat.mtrl-sci↗

arXiv2019

Zeeman-splitting-induced Topological Nodal Structure and Anomalous Hall Conductivity in ZrTe$_5$

We investigate the topological nodal structure of three-dimensional (3D) ZrTe$_5$ driven by Zeeman splitting as a function of the direction of external magnetic (B) field by using a Wannier-function-based tight-binding (WFTB) model obtained from first-principles calculations. It is known that small external stimuli can drive 3D ZrTe$_5$ into different topological phases including Dirac semimetal. In order to emphasize the effect of Zeeman splitting, we consider 3D ZrTe$_5$ in a strong TI phase with a small band gap. With Zeeman splitting greater than the band gap, the WFTB model suggests that a type-I nodal ring protected by (glide) mirror symmetry is formed when the B field aligns with the crystal $a$ or $b$ axes, and that a pair of type-I Weyl nodes are formed otherwise, when conduction and valence bands touch. We show that a pair of Weyl nodes can disappear through formation of a nodal ring, rather than requiring two Weyl nodes with opposite chirality to come together. Interestingly, a type-II nodal ring appears from crossings of the top two valence bands when the B field is applied along the $c$ axis. This nodal ring gaps out to form type-II Weyl nodes when the B field rotates in the $bc$ plane. Comparing the WFTB and linearized $k \cdot p$ model, we find inadequacy of the latter at some B field directions. Further, using the WFTB model, we numerically compute the intrinsic anomalous Hall conductivity ${σ_{ac}}$ induced by Berry curvature as a function of chemical potential and B field direction. We find that ${σ_{ac}}$ increases abruptly when the B field is tilted from the $a$ axis within the $ab$ plane. Our WFTB model also shows significant anomalous Hall conductivity induced by avoided level crossings even in the absence of Weyl nodes.

cond-mat.mes-hall↗

arXiv2019

Multireference Ab Initio Studies of Magnetic Properties of Terbium-Based Single-Molecule Magnets

We investigate how different chemical environment influences magnetic properties of terbium(III) (Tb)-based single-molecule magnets (SMMs), using first-principles relativistic multireference methods. Recent experiments showed that Tb-based SMMs can have exceptionally large magnetic anisotropy and that they can be used for experimental realization of quantum information applications, with a judicious choice of chemical environment. Here, we perform complete active space self-consistent field (CASSCF) calculations including relativistic spin-orbit interaction (SOI) for representative Tb-based SMMs such as TbPc$_2$ and TbPcNc in three charge states. We calculate low-energy electronic structure from which we compute the Tb crystal-field parameters and construct an effective pseudospin Hamiltonian. Our calculations show that ligand type and fine points of molecular geometry do not affect the zero-field splitting, while the latter varies weakly with oxidation number. On the other hand, higher-energy levels have a strong dependence on all these characteristics. For neutral TbPc$_2$ and TbPcNc molecules, the Tb magnetic moment and the ligand spin are parallel to each other and the coupling strength between them does not depend much on ligand type and details of atomic structure. However, ligand distortion and molecular symmetry play a crucial role in transverse crystal-field parameters which lead to tunnel splitting. The tunnel splitting induces quantum tunneling of magnetization by itself or by combining with other processes. Our results provide insight into mechanisms of magnetization relaxation in the representative Tb-based SMMs.

physics.chem-ph↗

arXiv2019

Intrinsic Point Defects in Ultrathin 1T-PtSe2 Layers

Among two-dimensional (2D) transition metal dichalcogenides (TMDs), platinum diselenide (PtSe2) stands at a unique place in the sense that it undergoes a phase transition from type-II Dirac semimetal to indirect-gap semiconductor as thickness decreases. Defects in 2D TMDs are ubiquitous and play crucial roles in understanding and tuning electronic, optical, and magnetic properties. Here we investigate intrinsic point defects in ultrathin 1T-PtSe2 layers grown on mica through the chemical vapor transport (CVT) method, using scanning tunneling microscopy and spectroscopy (STM/STS) and first-principles calculations. We observed five types of distinct defects from STM topography images and obtained the local density of states of the defects. By combining the STM results with the first-principles calculations, we identified the types and characteristics of these defects, which are Pt vacancies at the topmost and next monolayers, Se vacancies in the topmost monolayer, and Se antisites at Pt sites within the topmost monolayer. Our study shows that the Se antisite defects are the most abundant with the lowest formation energy in a Se-rich growth condition, in contrast to cases of 2D molybdenum disulfide (MoS2) family. Our findings would provide critical insight into tuning of carrier mobility, charge carrier relaxation, and electron-hole recombination rates by defect engineering or varying growth condition in few-layer 1T-PtSe2 and other related 2D materials.

cond-mat.mes-hall↗

arXiv2018

Magnetic Field Induced Weyl Semimetal from Wannier-Function-based Tight-Binding Model

Weyl semimetals (WSMs) have Weyl nodes where conduction and valence bands meet in the absence of inversion or time-reversal symmetry (TRS), or both. Interesting phenomena are expected in WSMs such as the chiral magnetic effect, anomalous Hall conductivity or Nernst effect, and unique quantum oscillations. The TRS-broken WSM phase can be driven from a topological Dirac semimetal (DSM) by magnetic field or magnetic dopants, considering that DSMs have degenerate Weyl nodes stabilized by rotational symmetry, i.e. Dirac nodes. Here we develop a Wannier-function-based tight-binding (WF-TB) model to investigate the formation of Weyl nodes and nodal rings induced by B field in the topological DSM Na$_3$Bi. The field is applied along the rotational axis. Remarkably, our study based on the WF-TB model shows that upon B field each Dirac node is split into four separate Weyl nodes along the rotational axis near the Fermi level; two nodes with single chiral charge (single Weyl nodes) and two with double chiral charge (double Weyl nodes). This result is in contrast to the common belief that each Dirac node splits into two Weyl nodes. In the effective models, the existence of double Weyl nodes ensures nonzero cubic terms in momentum. We further examine the evolution of Fermi arcs at a side surface as a function of chemical potential. The number of Fermi arcs is consistent with the corresponding Fermi surface Chern numbers, corroborating our finding of the double Weyl nodes. Furthermore, our study reveals the existence of nodal rings in the mirror plane below the Fermi level upon B field. These nodal rings persist with spin-orbit coupling, in contrast to typical nodal ring semimetals. Our WF-TB model can be used to compute interesting features arising from Berry curvature such as anomalous Hall and thermal conductivities, and our findings can be applied to other topological DSMs like Cd$_3$As$_2$.

cond-mat.mes-hall↗

arXiv2018

Atomically Resolved Observation of Continuous Interfaces between As-grown MoS2 Monolayer and WS2/MoS2 Heterobilayer on SiO2

Van der Waals (vdW) heterostructures synthesized through the chemical vapor deposition (CVD) method allow creation and tuning of intriguing electronic and optical properties of two- dimensional (2D) materials, the knowledge of which is critical for a wide range of potential applications. Here we report our scanning tunneling microscopy/spectroscopy (STM/STS) study of as-grown MoS2 monolayer and WS2/MoS2 heterobilayer on SiO2. The heterobilayer appears smoother than the MoS2 monolayer, with root mean square (RMS) roughness of 0.230 +- 0.021 nm in the former and 0.329 +- 0.033 nm in the latter. For the first time, to our knowledge, we directly observed a continuous interface between the MoS2 monolayer and the top layer of the heterobilayer with atomic resolution. This finding contrasts to the previously reported open edges in the top layer of the heterobilayer. Our STS results and density functional theory (DFT) calculations revealed the band gaps of the heterobilayer and the MoS2 monolayer.

cond-mat.mes-hall↗

arXiv2017

Hybridization-induced interface states in a topological insulator-magnetic metal heterostructure

Recent experiments demonstrating large spin-transfer torques in topological insulator (TI)-ferromagnetic metal (FM) bilayers have generated a great deal of excitement due to their potential applications in spintronics. The source of the observed spin-transfer torque, however, remains unclear. This is because the large charge transfer from the FM to TI layer would prevent the Dirac cone at the interface from being anywhere near the Fermi level to contribute to the observed spin-transfer torque. Moreover, there is yet little understanding of the impact on the Dirac cone at the interface from the metallic bands overlapping in energy and momentum, where strong hybridization could take place. Here, we build a simple microscopic model and perform first-principles-based simulations for such a TI-FM heterostructure, considering the strong hybridization and charge transfer effects. We find that the original Dirac cone is destroyed by the hybridization as expected. Instead, we find a new interface state which we dub 'descendent state' to form near the Fermi level due to the strong hybridization with the FM states at the same momentum. Such a `descendent state' carries a sizable weight of the original Dirac interface state, and thus inherits the localization at the interface and the same Rashba-type spin-momentum locking. We propose that the `descendent state' may be an important source of the experimentally observed large spin-transfer torque in the TI-FM heterostructure.

cond-mat.mes-hall↗

arXiv2017

Epitaxial thin films of pyrochlore iridate Bi_{2+x}Ir_{2-y}O_{7-delta}: structure, defects and transport properties

While pyrochlore iridate thin films are theoretically predicted to possess a variety of emergent topological properties, experimental verification of these predictions can be obstructed by the challenge in thin film growth. Here we report on the pulsed laser deposition and characterization of thin films of a representative pyrochlore compound Bi2Ir2O7. The films were epitaxially grown on yttria-stabilized zirconia substrates and have lattice constants that are a few percent larger than that of the bulk single crystals. The film composition shows a strong dependence on the oxygen partial pressure. Density-functional-theory calculations indicate the existence of Bi_Ir antisite defects, qualitatively consistent with the high Bi: Ir ratio found in the films. Both Ir and Bi have oxidation states that are lower than their nominal values, suggesting the existence of oxygen deficiency. The iridate thin films show a variety of intriguing transport characteristics, including multiple charge carriers, logarithmic dependence of resistance on temperature, antilocalization corrections to conductance due to spin-orbit interactions, and linear positive magnetoresistance.

cond-mat.mtrl-sci↗

arXiv2016

Magnetic-anisotropy induced spin blockade in a single-molecule transistor

We present a new mechanism for a spin blockade effect associated with a change in the type of magnetic anisotropy over oxidation state in a single molecule transistor, by taking an example of an individual Eu$_{2}$(C$_{8}$H$_{8}$)$_{3}$ molecule weakly coupled to non-magnetic electrodes without linker groups. The molecule switches its magnetization direction from in-plane to out-of-plane when it is charged. In other words, the magnetic anisotropy of the molecule changes from easy plane to easy axis when the molecule is charged. By solving the master equation based on model Hamiltonian, we find that current through the molecule is highly suppressed at low bias independently of gate voltage due to the interplay between spin selection rules and the change in the type of magnetic anisotropy. Transitions between the lowest magnetic levels in successive charge states are forbidden because the magnetic levels differ by $|ΔM| > 1/2$ due to the change in the type of magnetic anisotropy, although the total spins differ by $|ΔS|=1/2$. This current suppression can be lifted by significant B field, and the threshold B field varies as a function of the field direction and the strength of magnetic anisotropy. The spin blockade effect shed light on switching the magnetization direction by non-spin-polarized current and on exploring effects of this property coupled to other molecular degrees of freedom.

cond-mat.mes-hall↗

arXiv2016

Engineering and probing topological properties of Dirac semimetal films by asymmetric charge transfer

Dirac semimetals (DSMs) have topologically robust three-dimensional Dirac (doubled Weyl) nodes with Fermi-arc states. In heterostructures involving DSMs, charge transfer occurs at the interfaces, which can be used to probe and control their bulk and surface topological properties through surface-bulk connectivity. Here we demonstrate that despite a band gap in DSM films, asymmetric charge transfer at the surface enables one to accurately identify locations of the Dirac-node projections from gapless band crossings and to examine and engineer properties of the topological Fermi-arc surface states connecting the projections, by simulating adatom-adsorbed DSM films using a first-principles method with an effective model. The positions of the Dirac-node projections are insensitive to charge transfer amount or slab thickness except for extremely thin films. By varying the amount of charge transfer, unique spin textures near the projections and a separation between the Fermi-arc states change, which can be observed by gating without adatoms.

cond-mat.mes-hall↗

arXiv2014

Electron-vibron coupling effects on electron transport via a single-molecule magnet

We investigate how the electron-vibron coupling influences electron transport via an anisotropic magnetic molecule, such as a single-molecule magnet (SMM) Fe$_4$, by using a model Hamiltonian with parameter values obtained from density-functional theory (DFT). Magnetic anisotropy parameters, vibrational energies, and electron-vibron coupling strengths of the Fe$_4$ are computed using DFT. A giant spin model is applied to the Fe$_4$ with only two charge states, specifically a neutral state with the total spin $S=5$ and a singly charged state with $S=9/2$, which is consistent with our DFT result and experiments on Fe$_4$ single-molecule transistors. In sequential electron tunneling, we find that the magnetic anisotropy gives rise to new features in conductance peaks arising from vibrational excitations. In particular, the peak height shows a strong, unusual dependence on the direction as well as magnitude of applied B field. The magnetic anisotropy also introduces vibrational satellite peaks whose position and height are modified with the direction and magnitude of applied B field. Furthermore, when multiple vibrational modes with considerable electron-vibron coupling have energies close to one another, a low-bias current is suppressed, independently of gate voltage and applied B field, although that is not the case for a single mode with the similar electron-vibron coupling. In the former case, the conductance peaks reveal a stronger B-field dependence than in the latter case. The new features appear because the magnetic anisotropy barrier is of the same order of magnitude as the energies of vibrational modes with significant electron-vibron coupling. Our findings clearly show the interesting interplay between magnetic anisotropy and electron-vibron coupling in electron transport via the Fe$_4$. The similar behavior can be observed in transport via other anisotropic magnetic molecules.

cond-mat.mes-hall↗

arXiv2014

Magnetic proximity effect at Bi$_2$Se$_3$/EuS interface with broken inversion symmetry

We investigate a magnetic proximity effect on Dirac surface states of topological insulator (TI) induced by a Bi$_2$Se$_3$/EuS interface, using density-functional theory (DFT) and a low-energy effective model, motivated by a recent experimental realization of the interface. We consider a thin ferromagnetic insulator EuS film stacked on top of Bi$_2$Se$_3$(111) slabs of three or five quintuple layers (QLs) with the magnetization of EuS normal to the interface ($z$ axis), which breaks both time-reversal and inversion symmetry. It is found that a charge transfer and surface relaxation makes the Dirac cones electron-doped. For both 3 and 5 QLs, the top-surface Dirac cone has an energy gap of 9 meV, while the bottom surface Dirac cone remains gapless. This feature is due to the short-ranged induced magnetic moment of the EuS film. For the 5 QLs, an additional Dirac cone with an energy gap of 2 meV is formed right below the bottom-surface Dirac point, while for 3 QLs, there is no additional Dirac cone. We also examine the spin-orbital texture of the Dirac surface states with broken inversion symmetry, using DFT and the effective model. We find that the $p_z$ orbital is coupled to the $z$ component of the spin moment in the opposite sign to the $p_x$ and $p_y$ orbitals. The $p_z$ and radial $p$ orbitals are coupled to the in-plane spin texture in the opposite handedness to the tangential $p$ orbital. The result obtained from the effective model agrees with our DFT calculations. The calculated spin-orbital texture may be tested from spin-polarized angle-resolved photoemission spectroscopy.

cond-mat.mes-hall↗

arXiv2014

Effects of surface-bulk hybridization in 3D topological `metals'

Identifying the effects of surface-bulk coupling is a key challenge towards exploiting the topological nature of the surface states in many available three-dimensional topological `metals'. Here we combine an effective-model calculation and an ab-initio slab calculation to study the effects of the lowest order surface-bulk interaction: the hybridization. In the effective-model study, we discretize an established low-energy effective four-band model and introduce the hybridization between the surface bands and bulk bands in the spirit of the Fano model. We find that the hybridization enhances the energy gap between bulk and Dirac surface states and preserves the latter's spin texture qualitatively albeit with a reduced spin-polarization magnitude. Our ab-initio study finds the energy gap between the bulk and surface states to grow upon an increase in the slab thickness, very much in qualitative agreement with the effective model study. Comparing the results of our two approaches, we deduce that the experimentally observed low magnitude of spin polarization can be attributed to a hybridization-type surface-bulk interaction. We discuss evidences for such hybridization in existing ARPES data.

cond-mat.mes-hall↗

arXiv2011

Antiferromagnetic coupling of the single-molecule magnet Mn12 to a ferromagnetic substrate

We investigate magnetic coupling between a monolayer of prototype single-molecule magnets Mn12 and a ferromagnetic Ni(111) substrate through S, using density-functional theory (DFT) and a DFT+U method. Our DFT and DFT+U calculations show that the Mn12 molecules favor antiferromagnetic coupling to the Ni substrate, and that they possess magnetic moments deviated from the magnetic moments of isolated Mn12 molecules. We find that the magnetic easy axis of the Mn12 on Ni (whole system) is dictated by that of the Ni substrate. The antiferromagnetic coupling is, dominantly, caused by superexchange interactions between the magnetic moments of the Mn and the Ni substrate via the S, C, and O anions. Our findings can be observed from x-ray magnetic circular dichroism or scanning tunneling microscopy.

cond-mat.mes-hall↗

arXiv2010

Robustness of topologically protected surface states in layering of Bi2Te3 thin films

Bulk Bi2Te3 is known to be a topological insulator. We investigate surface states of Bi2Te3(111) thin films using density-functional theory including spin-orbit coupling. We construct a method to unambiguously identify surface states of thin film topological insulators. Applying this method for one to six quintuple layers of Bi2Te3, we find that the topological nature of the surface states remains robust with the film thickness and that the films of three or more quintuple layers have topologically non-trivial or protected surface states, in agreement with recent experiments.

cond-mat.mes-hall↗