SearcharxivSearch

arXiv subjects

Jong-Woo Kim

Publications and source records attributed to Jong-Woo Kim.

At least 19 recordsLinked to original sources

Soft-Phonon-Driven Effective Inversion-Symmetry Crossover in Quantum Paraelectrics

Symmetry lays the foundation of condensed matter physics and its experimental manifestation provides fundamental insight into the collective behaviors of quantum materials. Optical second-harmonic generation (SHG) is widely regarded as a fingerprint of inversion-symmetry breaking, yet whether and how collective lattice dynamics govern the nonlinear optical manifestation of local inversion-symmetry breaking remains unknown. Here, combining optical SHG, diffuse X-ray scattering, and microscopic theory, we reveal a phonon-regulated mechanism governing the temperature-dependent manifestation of local inversion-symmetry breaking in quantum paraelectric material KTaO3. We demonstrate that an oxygen-defect-mediated nonlinear optical channel is strongly coupled to the host soft polar mode, whose thermal fluctuations scramble the associated electronic phase coherence and thereby suppress the nonlinear manifestation of local inversion-symmetry breaking at elevated temperatures. Consequently, the nonlinear response exhibits a temperature-driven crossover from a regime in which local inversion-symmetry breaking is optically manifest to one that appears effectively centrosymmetric, without any accompanying structural change. Our findings revise the conventional picture of the temperature-dependent manifestation of inversion-symmetry breaking in quantum paraelectrics and establish a framework for understanding and engineering defect-mediated nonlinear optical responses in materials hosting low-energy polar excitations.

cond-mat.mtrl-sci

Ferroaxial and nematic transitions in the charge density wave phase of 1T-TiSe$_2$

Charge density waves (CDWs) with multi-component order parameters can break unexpected symmetries through the interplay of nearly degenerate instabilities. In the widely investigated material 1T-TiSe$_2$, a central question is whether the observed CDW has a chiral character, which would manifest as the spontaneous breaking of mirror and inversion symmetries. Previous experiments have reported conflicting results about the broken symmetries in the CDW phase of 1T-TiSe$_2$. Here, we resolve this controversy by identifying the bulk broken symmetry as ferroaxial, corresponding to the breaking of vertical mirrors while preserving inversion symmetry. Using symmetry-resolved elastoresistivity, we detect the spontaneous emergence of intrinsic off-diagonal elastoresistivity coefficients that satisfy an antisymmetric relation ($m_{xx-yy,xy} \approx -m_{xy,xx-yy}$), providing an unambiguous bulk transport signature of a macroscopic electric toroidal moment. Simultaneous elastocaloric measurements reveal that the onset of ferroaxial order occurs just below the CDW transition. As the temperature is lowered further, a diverging nematic susceptibility signals a distinct rotational symmetry-breaking instability inside the ferroaxial CDW state. Our findings demonstrate that the proposed ``chiral'' CDW in 1T-TiSe$_2$ is actually a centrosymmetric ferroaxial state, reconciling previous surface-sensitive observations with bulk symmetry constraints.

cond-mat.str-el

Large asymmetric anomalous Nernst effect in the antiferromagnet SrIr$_{0.8}$Sn$_{0.2}$O$_3$

A large anomalous Nernst effect is essential for thermoelectric energy harvesting in the transverse geometry without external magnetic field. It is often connected with anomalous Hall effect, especially when electronic Berry curvature is believed to be the driving force. This approach implicitly assumes the same symmetry for the Nernst and Hall coefficients, which is however not necessarily true. Here we report a large anomalous Nernst effect in antiferromagnetic SrIr$_{0.8}$Sn$_{0.2}$O$_3$ that defies the antisymmetric constraint on the anomalous Hall effect imposed by the Onsager reciprocal relation. The observed spontaneous Nernst thermopower quickly reaches the sub-$μ$V/K level below the Néel transition around 250 K, which is comparable with many topological antiferromagnetic semimetals and far excels other magnetic oxides. Our analysis indicates that the coexistence of significant symmetric and antisymmetric contributions plays a key role, pointing to the importance of extracting both contributions and a new pathway to enhanced anomalous Nernst effect for transverse thermoelectrics

cond-mat.mtrl-sci

The Classical-to-Quantum Crossover in strain-induced ferroelectric transition in SrTiO$_3$ membranes

Mechanical strain presents an effective control over symmetry-breaking phase transitions. In quantum paralelectric SrTiO3, strain can induce the ferroelectric transition via modification of local Ti potential landscape. However, brittle bulk materials can only withstand limited strain range (~0.1%). Taking advantage of nanoscopically-thin freestanding membranes, we demonstrated in-situ strain-induced reversible ferroelectric transition in a single freestanding SrTiO3 membranes. We measure the ferroelectric order by detecting the local anisotropy of the Ti 3d orbital using X-ray linear dichroism at the Ti-K pre-edge, while the strain is determined by X-ray diffraction. With reduced thickness, the SrTiO3 membranes remain elastic with >1% tensile strain cycles. A robust displacive ferroelectricity appears beyond a temperature-dependent critical strain. Interestingly, we discover a crossover from a classical ferroelectric transition to a quantum regime at low temperatures, which enhances strain-induced ferroelectricity. Our results offer a new opportunities to strain engineer functional properties in low dimensional quantum materials and provide new insights into the role of the ferroelectric fluctuations in quantum paraelectric SrTiO3.

cond-mat.mtrl-sci

Pulling order back from the brink of disorder: Observation of a nodal line spin liquid and fluctuation stabilized order in K$_2$IrCl$_6$

Competing interactions in frustrated magnets can give rise to highly degenerate ground states from which correlated liquid-like states of matter often emerge. The scaling of this degeneracy influences the ultimate ground state, with extensive degeneracies potentially yielding quantum spin liquids, while sub-extensive or smaller degeneracies yield static orders. A longstanding problem is to understand how ordered states precipitate from this degenerate manifold and what echoes of the degeneracy survive ordering. Here, we use neutron scattering to experimentally demonstrate a new "nodal line" spin liquid, where spins collectively fluctuate within a sub-extensive manifold spanning one-dimensional lines in reciprocal space. Realized in the spin-orbit coupled, face-centered cubic iridate K$_2$IrCl$_6$, we show that the sub-extensive degeneracy is robust, but remains susceptible to fluctuations or longer range interactions which cooperate to select a magnetic order at low temperatures. Proximity to the nodal line spin liquid influences the ordered state, enhancing the effects of quantum fluctuations and stabilizing it through the opening of a large spin-wave gap. Our results demonstrate quantum fluctuations can act counter-intuitively in frustrated materials: instead of destabilizing ordering, at the brink of the nodal spin liquid they can act to stabilize it and dictate its low-energy physics.

cond-mat.str-el

Chiral Spin-Liquid-Like State in Pyrochlore Iridate Thin Films

The pyrochlore iridates have become ideal platforms to unravel fascinating correlated and topolog?ical phenomena that stem from the intricate interplay among strong spin-orbit coupling, electronic correlations, lattice with geometric frustration, and itinerancy of the 5d electrons. The all-in-all?out antiferromagnetic state, commonly considered as the magnetic ground state, can be dramatically altered in reduced dimensionality, leading to exotic or hidden quantum states inaccessible in bulk. Here, by means of magnetotransport, resonant elastic and inelastic x-ray scattering experiments, we discover an emergent quantum disordered state in (111) Y2Ir2O7 thin films (thickness less than 30 nm) per?sisting down to 5 K, characterized by dispersionless magnetic excitations. The anomalous Hall effect observed below an onset temperature near 135 K corroborates the presence of chiral short-range spin configurations expressed in non-zero scalar spin chirality, breaking the macroscopic time-reversal symmetry. The origin of this chiral state is ascribed to the restoration of magnetic frustration on the pyrochlore lattice in lower dimensionality, where the competing exchange interactions together with enhanced quantum fluctuations suppress any long-range order and trigger spin-liquid-like behavior with degenerate ground-state manifold.

cond-mat.str-el

Elastocaloric evidence for a multicomponent superconductor stabilized within the nematic state in Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$

The iron-based high-$T_c$ superconductors exhibit rich phase diagrams with intertwined phases, including magnetism, nematicity and superconductivity. The superconducting $T_c$ in many of these materials is maximized in the regime of strong nematic fluctuations, making the role of nematicity in influencing the superconductivity a topic of intense research. Here, we use the AC elastocaloric effect (ECE) to map out the phase diagram of Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$ near optimal doping. The ECE signature at $T_c$ on the overdoped side, where superconductivity condenses without any nematic order, is quantitatively consistent with other thermodynamic probes that indicate a single-component superconducting state. In contrast, on the slightly underdoped side, where superconductivity condenses within the nematic phase, ECE reveals a second thermodynamic transition proximate to and below $T_c$. We rule out magnetism and re-entrant tetragonality as the origin of this transition, and find that our observations strongly suggest a phase transition into a multicomponent superconducting state. This implies the existence of a sub-dominant pairing instability that competes strongly with the dominant $s^\pm$ instability. Our results thus motivate a re-examination of the pairing state and its interplay with nematicity in this extensively studied iron-based superconductor, while also demonstrating the power of ECE in uncovering strain-tuned phase diagrams of quantum materials.

cond-mat.supr-con

Magneto-synthesis effect on magnetic order, phonons, and magnons in single-crystal Sr$_2$IrO$_4$

It was shown earlier that applying a magnetic field during the growth of Sr$_2$IrO$_4$, also known as "field-alteration", induces significant changes to its structural, magnetic, and transport properties. However, the microscopic nature of these changes is enigmatic. In this study, we employed resonant elastic and inelastic x-ray scattering, as well as Raman scattering, to investigate samples from two batches of Sr$_2$IrO$_4$ grown in magnetic fields of different strengths. Our findings reveal that samples grown in a weaker magnetic field have similar magnetic order to non-altered samples, whereas those grown in a stronger field show a different stacking of weak in-plane ferromagnetic moments. Additionally, we observed significant softening and broadening of select Raman-active phonons in the field altered samples, with a stronger effect in the samples grown in the stronger field. We discuss insights that our results provide into the microscopic nature of field-alteration in Sr$_2$IrO$_4$.

cond-mat.str-el

Extraordinary magnetic response of an anisotropic 2D antiferromagnet via site-dilution

A prominent character of two-dimensional magnetic systems is the enhanced spin fluctuations, which however reduce the ordering temperature. Here we report that a magnetic field of only one-thousandth of the Heisenberg superexchange interaction can induce a crossover, which for practical purposes is the effective ordering transition, at temperatures about 6 times of the Neel transition in a site-diluted two-dimensional anisotropic quantum antiferromagnet. Such a strong magnetic response is enabled because the system directly enters the antiferromagnetically ordered state from the isotropic disordered state skipping the intermediate anisotropic stage. The underlying mechanism is achieved on a pseudospin-half square lattice realized in the [(SrIrO3)1/(SrTiO3)2] superlattice thin film that is designed to linearly couple the staggered magnetization to external magnetic fields by virtue of the rotational symmetry-preserving Dzyaloshinskii Moriya interaction. Our model analysis shows that the skipping of the anisotropic regime despite the finite anisotropy is due to the enhanced isotropic fluctuations under moderate dilution.

cond-mat.str-el

Discovery of Charge Order in the Transition Metal Dichalcogenide Fe$_{x}$NbS$_2$

The Fe intercalated transition metal dichalcogenide (TMD), Fe$_{1/3}$NbS$_2$, exhibits remarkable resistance switching properties and highly tunable spin ordering phases due to magnetic defects. We conduct synchrotron X-ray scattering measurements on both under-intercalated ($x$ = 0.32) and over-intercalated ($x$ = 0.35) samples. We discover a new charge order phase in the over-intercalated sample, where the excess Fe atoms lead to a zigzag antiferromagnetic order. The agreement between the charge and magnetic ordering temperatures, as well as their intensity relationship, suggests a strong magnetoelastic coupling as the mechanism for the charge ordering. Our results reveal the first example of a charge order phase among the intercalated TMD family and demonstrate the ability to stabilize charge modulation by introducing electronic correlations, where the charge order is absent in bulk 2H-NbS$_2$ compared to other pristine TMDs.

cond-mat.str-el

Single crystal growth and characterization of antiferromagnetically ordering EuIn$_2$

We report the single crystal growth and characterization of EuIn$_2$, a magnetic topological semimetal candidate according to our density functional theory (DFT) calculations. We present results from electrical resistance, magnetization, Mössbauer spectroscopy, and X-ray resonant magnetic scattering (XRMS) measurements. We observe three magnetic transitions at $T_{\text{N}1}\sim 14.2~$K, $T_{\text{N}2}\sim12.8~$K and $T_{\text{N}3}\sim 11~$K, signatures of which are consistently seen in anisotropic temperature dependent magnetic susceptibility and electrical resistance data. Mössbauer spectroscopy measurements on ground crystals suggest an incommensurate sinusoidally modulated magnetic structure below the transition at $T_{\text{N}1}\sim 14~$K, followed by the appearance of higher harmonics in the modulation on further cooling roughly below $T_{\text{N}2}\sim13~$K, before the moment distribution squaring up below the lowest transition around $T_{\text{N}3}\sim 11~$K. XRMS measurements showed the appearance of magnetic Bragg peaks below $T_{\text{N}1}\sim14~$K, with a propagation vector of $\bmτ$ $=(τ_h,\barτ_h,0)$, with $τ_h$varying with temperature, and showing a jump at $T_{\text{N}3}\sim11$~K. The temperature dependence of $τ_h$ between $\sim11$~K and $14$~K shows incommensurate values consistent with the Mössbauer data. XRMS data indicate that $τ_h$ remains incommensurate at low temperatures and locks into $τ_h=0.3443(1)$.

cond-mat.mtrl-sci

Spontaneous orbital polarization in the nematic phase of FeSe

The origin of nematicity in FeSe remains a critical outstanding question towards understanding unconventional superconductivity in proximity to nematic order. To understand what drives the nematicity, it is essential to determine which electronic degree of freedom admits a spontaneous order parameter independent from the structural distortion. Here, we use X-ray linear dichroism at the Fe K pre-edge to measure the anisotropy of the 3d orbital occupation as a function of in situ applied stress and temperature across the nematic transition. Along with X-ray diffraction to precisely quantify the strain state, we reveal a lattice-independent, spontaneously-ordered orbital polarization within the nematic phase, as well as an orbital polarizability that diverges as the transition is approached from above. These results provide strong evidence that spontaneous orbital polarization serves as the primary order parameter of the nematic phase.

cond-mat.supr-con

Incommensurate Magnetic Order in the $\mathbb{Z}_2$ Kagome Metal GdV$_6$Sn$_6$

We characterize the magnetic ground state of the topological kagome metal GdV$_6$Sn$_6$ via resonant X-ray diffraction. Previous magnetoentropic studies of GdV$_6$Sn$_6$ suggested the presence of a modulated magnetic order distinct from the ferromagnetism that is easily polarized by the application of a magnetic field. Diffraction data near the Gd-$L_2$ edge directly resolve a $c$-axis modulated spin structure order on the Gd sublattice with an incommensurate wave vector that evolves upon cooling toward a partial lock-in transition. While equal moment (spiral) and amplitude (sine) modulated spin states can not be unambiguously discerned from the scattering data, the overall phenomenology suggests an amplitude modulated state with moments predominantly oriented in the $ab$-plane. Comparisons to the ``double-flat" spiral state observed in Mn-based $R$Mn$_6$Sn$_6$ kagome compounds of the same structure type are discussed.

cond-mat.str-el

Strain-Switchable Field-Induced Superconductivity

Field-induced superconductivity is a rare phenomenon where an applied magnetic field enhances or induces superconductivity. This fascinating effect arises from a complex interplay between magnetism and superconductivity, and it offers the tantalizing technological possibility of an infinite magnetoresistance superconducting spin valve. Here, we demonstrate field-induced superconductivity at a record-high temperature of T=9K in two samples of the ferromagnetic superconductor Eu(Fe$_{0.88}$Co$_{0.12}$)$_{2}$As$_{2}$. We combine tunable uniaxial stress and applied magnetic field to shift the temperature range of the zero-resistance state between 4K and 10K. We use x-ray diffraction and spectroscopy measurements under stress and field to demonstrate that stress tuning of the nematic order and field tuning of the ferromagnetism act as independent tuning knobs of the superconductivity. Finally, DFT calculations and analysis of the Eu dipole field reveal the electromagnetic mechanism of the field-induced superconductivity.

cond-mat.supr-con

Quasi-2D anomalous Hall Mott insulator of topologically engineered Jeff =1/2 electrons

We investigate an experimental toy-model system of a pseudospin-half square-lattice Hubbard Hamiltonian in [(SrIrO3)1/(CaTiO3)1] to include both nontrivial complex hopping and moderate electronic correlation. While the former induces electronic Berry phases as anticipated from the weak-coupling limit, the later stabilizes an antiferromagnetic (AFM) Mott insulator ground state in analogous to the strong-coupling limit. Their combined results in the real system are found to be an anomalous Hall effect with a non-monotonic temperature dependence due to the self-competition of the electron-hole pairing in the Mott state, and an exceptionally large Ising anisotropy that is captured as a giant magnon gap beyond the superexchange approach. The unusual phenomena highlight the rich interplay of electronic topology and electronic correlation in the intermediate-coupling regime that is largely unexplored and challenging in theoretical modelling.

cond-mat.str-el

Reconciling monolayer and bilayer $J_{\rm eff} = 1/2$ square lattices in hybrid oxide superlattice

The number of atomic layers confined in a two-dimensional structure is crucial for the electronic and magnetic properties. Single-layer and bilayer $J_{\rm eff} = 1/2$ square lattices are well-known examples where the presence of the extra layer turns the XY-anisotropy to the $c$-axis anisotropy. We report on experimental realization of a hybrid SrIrO$_3$/SrTiO$_3$ superlattice that integrates monolayer and bilayer square lattices in one layered structure. By synchrotron x-ray diffraction, resonant x-ray magnetic scattering, magnetization, and resistivity measurements, we found that the hybrid superlattice exhibits properties that are distinct from both the single-layer and bilayer systems and cannot be explained by a simple addition of them. In particular, the entire hybrid superlattice orders simultaneously through a single antiferromagnetic transition at temperatures similar to the bilayer system but with all the $J_{\rm eff} = 1/2$ moments mainly pointing in the $ab$-plane similar to the single-layer system. The results show that bringing monolayer and bilayer with orthogonal properties in proximity to each other in a hybrid superlattice structure is a powerful way to stabilize a unique state not obtainable in a uniform structure.

cond-mat.mtrl-sci

Quantitative relationship between structural orthorhombicity, shear modulus and heat capacity anomaly of the nematic transition in iron-based superconductors

Electronic nematicity in iron pnictide materials has been extensively studied by various experimental techniques, yet its heat capacity anomaly at the phase transition has not been examined quantitatively. In this work we review the thermodynamic description of nematicity in $Ba(Fe_{1-x}Co_{x})_{2}As_{2}$ using the Landau free energy, which defines the behavior of three thermodynamic quantities: the structural orthorhombicity that develops below the nematic transition, the softening shear modulus above the transition, and the discontinuous heat capacity at the transition. We derive a quantitative relationship between these three quantities, which is found to hold for a range of dopings. This result shows that the nematic transition is exceedingly well described by a mean-field model in the underdoped regime of the phase diagram.

cond-mat.supr-con

Local atomic configuration control of superconductivity in the undoped pnictide parent compound BaFe2As2

Emergent superconductivity is strongly correlated with the symmetry of local atomic configuration in the parent compounds of iron-based superconductors. While chemical doping or hydrostatic pressure can change the local geometry, these conventional approaches do not provide a clear pathway in tuning the detailed atomic arrangement predictably, due to the parent compounds complicated structural deformation in the presence of the tetragonal-to-orthorhombic phase transition. Here, we demonstrate a systematic approach to manipulate the local structural configurations in BaFe2As2 epitaxial thin films by controlling two independent structural factors orthorhombicity (in-plane anisotropy) and tetragonality (out-of-plane/in-plane balance) from lattice parameters. We tune superconductivity without chemical doping utilizing both structural factors separately, controlling local tetrahedral coordination in designed thin film heterostructures with substrate clamping and bi-axial strain. We further show that this allows quantitative control of both the structural phase transition, associated magnetism, and superconductivity in the parent material BaFe2As2. This approach will advance the development of tunable thin film superconductors in reduced dimension.

cond-mat.supr-con