arXiv subjects

Noejung Park

Publications and source records attributed to Noejung Park.

At least 19 recordsLinked to original sources

arXiv2026

Real-time dynamics of the two-step charge-density-wave transition in bulk 1T-TaS$_2$

The charge-density wave (CDW) of bulk 1T-TaS2 is built from Star-of-David (SoD) clusters tiling a sqrt{13} x sqrt{13} superlattice, and it melts through a two-step sequence accompanied by order-of-magnitude changes in resistivity. Whether these steps proceed by collapse of the SoD amplitude or by rearrangement of the SoD lattice has remained unresolved, because the relevant dynamics occur on length and time scales beyond the reach of ab initio molecular dynamics. Here we follow the CDW transitions in real time using a machine-learning force field trained on first-principles data, giving access to 1404-atom supercells over 5 ns. The two steps are mechanistically distinct. Above 200 K, SoD clusters translate coherently by transiently dissolving and re-forming about shifted centers, a deformation-formation process that preserves the local SoD amplitude while randomizing the interlayer stacking order and nucleating domain walls. Only near 350 K does the SoD distortion itself collapse. These results provide microscopic support for the recently proposed two-step model of the CDW transition and offer a framework for interpreting light-induced hidden phases and cavity-modified transition temperatures in 1T-TaS2.

cond-mat.mtrl-sci↗

arXiv2026

Gauge-Field-Mediated Symmetry Breaking of Matters Under Electromagnetic Fields and Its Impact on Spin Dynamics

When a condensed-matter system is subjected to external electromagnetic fields, the gauge-invariant formulation of physical operators must explicitly incorporate the gauge-field contribution. However, in the context of spin-orbit coupling (SOC), this gauge-field term is often regarded as negligible or merely additive compared to the canonical SOC, which is typically localized near atomic cores. Here, we demonstrate that the symmetry breaking and consequent spin dynamics are governed by the gauge-field term, without which the spins remain symmetry-constrained. We perform real-time time-dependent density functional theory calculations to investigate spin-orbit dynamics, focusing on representative cases with mirror, glide, and screw-rotational symmetry. We demonstrate that when the gauge-field term in the time-dependent Hamiltonian perturbs the symmetry of the canonical term, a dynamical spin state gradually develops during the time evolution, beyond the symmetry-frozen states. We suggest that, for nonequilibrium spin-orbit dynamics, the gauge-invariant formulation of SOC is not only formally required but also quantitatively essential, even for a weak external field.

cond-mat.mtrl-sci↗

arXiv2026

Current-Driven Symmetry Breaking and Spin-Orbit Polarization in Chiral Wires

The spin dynamics of electrons in chiral molecular systems remain a topic of intense interest, particularly regarding whether geometric chirality inherently induces spin polarization in current-carrying electrons. In this work, we employ ab initio real-time time-dependent density functional theory (rt-TDDFT) to directly simulate the interplay between charge current, spin, and orbital. This real-time tracking extends beyond perturbative treatments, and we analyze how nonequilibrium currents effectively lift the symmetry constraints of screw rotation and time-reversal symmetry. We find that the emergence of spin and orbital angular momenta is dynamically correlated with a concomitant loss of translational (linear) momentum, which we interpret as an intrinsic consequence of current-driven symmetry lowering. The implications of this mechanism for chirality-induced spin selectivity and spintronic device design are discussed.

physics.comp-ph↗

arXiv2025

Spin and Orbital Angular Momentum Polarization in Thouless Topological Charge Pumping

Quantized charge pumping in one-dimensional chiral wires has been widely studied in the context of topological physics in a (1+1)-dimensional synthetic space, yet the role of orbital and spin degrees of freedom in such topological pumps remains largely unexplored. Here, we examine how the topologically quantized charge pump in insulators generates spin polarizations, and assess whether this mechanism may offer distinct insight into the widely known spin-selective transport in chiral wires-commonly referred to as chirality-induced spin selectivity. We performed time-dependent Schrodinger equations of multi-orbital tight-binding Hamiltonians driven by a circularly polarized electric field. Our main findings are twofold. First, the intrinsic screw-like geometry of the system generates a distinctive winding structure governed by a single control parameter, in contrast to conventional adiabatic pumping mechanisms that require at least two independently modulated parameters, thereby providing a clear interpretation of one-dimensional pumping in terms of the topological structure in a (1+1)-dimensional Brillouin zone. Second, while the energy gap remains open throughout the pumping cycle, the Berry-phase driven real-time dynamics of the charge flow induces a nonequilibrium orbital polarization. Through spin-orbit coupling, this orbital response is partially converted into spin polarization whose direction is determined by the current and chirality. On the analogy between the synthetic (1+1)- and 2-dimensional topological insulators, we suggest that non-trivial spin-orbital dynamics may accompany the anomalous quantum charge Hall states of even-dimensional real materials.

cond-mat.mes-hall↗

arXiv2025

Real Space Imaging of Spin Scattering in Chirality-Induced Spin Selectivity

The interaction between electron spin and molecular chirality plays a fundamental role in quantum phenomena, with significant implications for spintronics and quantum computing. The chirality-induced spin selectivity (CISS) effect, where chiral materials preferentially transmit electrons of a particular spin, has sparked intense interest and debate regarding its underlying mechanism. Despite extensive research, the spatial distribution of spin polarization in chiral systems, the key evidence to reveal the spin scattering mechanism in CISS, has remained experimentally elusive particularly due to complications arising from spin-orbit coupling in metal electrodes typically used in such studies. Here we show, through reflective magnetic circular dichroism measurements on chiral tellurium nanowires with graphene electrodes, that current-induced spin polarization exhibits identical signs in both the nanowire and electrodes, distinct from the presumed spin filter scenario. The observed spin polarization scales linearly with current amplitude, aligns parallel to the current direction, reverses with chirality or current flow, and demonstrates spin relaxation lengths of several micrometers into graphene. Our findings provide the first direct visualization of spatial spin distribution in chiral devices. This work establishes a new paradigm for investigating spin-dependent phenomena in chiral materials and opens avenues for developing chirality-based spintronic and quantum devices.

cond-mat.mes-hall↗

arXiv2025

Relativistic Spin-Lattice Interaction Compatible with Discrete Translation Symmetry in Solids

Recent interest in orbital angular momentum has led to a rapid expansion of research on spin-orbit coupling effects in solids, while also highlighting significant technical challenges. The breaking of rotational symmetry renders the orbital angular momentum operator ill-defined, causing conceptual and computational issues in describing orbital motion. To address these issues, here we propose an alternative framework. Based on the Bloch representation of the full relativistic interaction, we derive a field that directly couples to electron spins while preserving discrete translational symmetry, thereby eliminating the need for the position operator. Our approach is fully compatible with existing first-principles computational frameworks for both static and time-dependent density functional theory. We demonstrate that this method offers a more effective description of the Edelstein and spin Hall effects compared to conventional orbital angular momentum formalisms.

cond-mat.mes-hall↗

arXiv2025

Multistate Control of Nonlinear Photocurrents in Optoferroelectrics via phase manipulation of light field

Ultrafast optical control of ferroelectricity based on short and intense light can be utilized to achieve accurate manipulations of ferroelectric materials, which may pave a basis for future breakthrough in nonvolatile memories. Here, we demonstrate that phase manipulation of electric field in the strong field sub-cycle regime induces a nonlinear injection current, efficiently coupling with the topology of band structure and enabling dynamic reversal of both current and polarization. Our time-dependent first-principles calculations reveal that tuning the phase of linearly or circularly polarized light through time-varying chirp, or constant carrier envelop phases within sub-laser-cycle dynamics effectively breaks the time-reversal symmetry, allowing the control over current and electronic polarization reversal over multi-ferroelectric states. Our time- and momentum-resolved transverse current analysis reveal the significance of Berry curvature higher order poles in the apparent association between the odd (even) orders of Berry curvature multipoles to odd (even) pseudo-harmonics in driving polarization dynamics reversal. We suggest that these phase manipulations of short pulse waveform may lead to unprecedented accurate control of nonlinear photocurrents and polarization states, which facilitate the development of precise ultrafast opto-ferroelectric devices.

cond-mat.mtrl-sci↗

arXiv2023

Suppressed terahertz dynamics of water confined in nanometer gaps

Nanoconfined waters have been extensively studied within various systems, demonstrating low permittivity under static conditions; however, their dynamics have been largely unexplored due to the lack of a robust platform, particularly in the terahertz (THz) regime where hydrogen bond dynamics occur. We report the THz complex refractive index of nanoconfined water within metal gaps ranging in width from 2 to 20 nanometers, spanning mostly interfacial waters all the way to quasi-bulk waters. These loop nanogaps, encasing water molecules, sharply enhance light-matter interactions, enabling precise measurements of refractive index, both real and imaginary parts, of nanometer-thick layers of water. Under extreme confinement, the suppressed dynamics of the long-range correlation of hydrogen bond networks corresponding to the THz frequency regime result in a significant reduction in the terahertz permittivity of even 'non-interfacial' water. This platform provides valuable insights into the long-range collective dynamics of water molecules which is crucial to understanding water-mediated processes such as protein folding, lipid rafts, and molecular recognition.

physics.optics↗

arXiv2023

Dynamics of electronic states in the insulating Intermediate surface phase of 1T-TaS$_2$

This article reports a comparative study of bulk and surface properties in the transition metal dichalcogenide 1T-TaS$_2$. When heating the sample, the surface displays an intermediate insulating phase that persists for $\sim 10$ K on top of a metallic bulk. The weaker screening of Coulomb repulsion and stiffer Charge Density Wave (CDW) explain such resilience of a correlated insulator in the topmost layers. Both time resolved ARPES and transient reflectivity are employed to investigate the dynamics of electrons and CDW collective motion. It follows that the amplitude mode is always stiffer at the surface and displays variable coupling to the Mott-Peierls band, stronger in the low temperature phase and weaker in the intermediate one.

cond-mat.str-el↗

arXiv2023

Optoelectronic manifestation of orbital angular momentum driven by chiral hopping in helical Se chains

Chiral materials have garnered significant attention in the field of condensed matter physics. Nevertheless, the magnetic moment induced by the chiral spatial motion of electrons in helical materials, such as elemental Te and Se, remains inadequately understood. In this work, we investigate the development of quantum angular momentum enforced by chirality using static and time-dependent density functional theory calculations for an elemental Se chain. Our findings reveal the emergence of an unconventional orbital texture driven by the chiral geometry, giving rise to a non-vanishing current-induced orbital moment. By incorporating spin-orbit coupling, we demonstrate that a current-induced spin accumulation arises in the chiral chain, which fundamentally differs from the conventional Edelstein effect. Furthermore, we demonstrate the optoelectronic detection of the orbital angular momentum in the chiral Se chain, providing a conceptually novel alternative to the interband Berry curvature, which is ill-defined in low dimensions.

cond-mat.mes-hall↗

arXiv2023

Electronic dispersion, correlations and stacking in the photoexcited state of 1T-TaS$_2$

Here we perform angle and time-resolved photoelectron spectroscopy on the commensurate Charge Density Wave (CDW) phase of 1T-TaS$_2$. Data with different probe pulse polarization are employed to map the dispersion of electronic states below and above the chemical potential. Upon photoexcitation, the fluctuations of CDW order erase the band dispersion near to the chemical potential and halve the charge gap size. This transient phase sets within half a period of the coherent lattice motion and is favored by strong electronic correlations. The experimental results are compared to Density-Functional Theory (DFT) calculations with a self-consistent evaluation of the Coulomb repulsion. Our simulations indicate that the screening of Coulomb repulsion depends on the stacking order of the TaS$_2$ layers. The entanglement of such degrees of freedom suggest that both the structural order and electronic repulsion are locally modified by the photoinduced CDW fluctuations.

cond-mat.str-el↗

arXiv2022

Unusual Spin Polarization in the Chirality Induced Spin Selectivity

Chirality-induced spin selectivity (CISS) refers to the fact that electrons get spin polarized after passing through organic chiral molecules in a nanoscale device. In CISS, chiral molecules are commonly believed to be a spin filter through which one favored spin transmits and the opposite spin gets reflected, i.e., transmitted and reflected electrons exhibit opposite spin polarization. In this work, we point out that such a spin filter scenario contradicts the principle that equilibrium spin current must vanish. Instead, we find that both transmitted and reflected electrons present the same type spin polarization, which is actually ubiquitous for a two-terminal device. More accurately, chiral molecules play the role of a spin polarizer rather than a spin filter. The direction of spin polarization is determined by the molecule chirality and the electron incident direction. And the magnitude of spin polarization replies on local spin-orbit coupling in the device. Our work brings a deeper understanding on CISS and interprets recent experiments, for example, the CISS-driven anomalous Hall effect.

cond-mat.mes-hall↗

arXiv2021

Tracing out the Berry curvature dipole and multipoles in second harmonic Hall responses of time-reversal symmetric insulators

Various nonlinear characteristics of solid states, such as the circular photogalvanic effect of time-reversal symmetric insulators, the quantized photogalvanic effect of Weyl semimetals, and the nonlinear Hall effect of time-reversal symmetric metals, have been associated with the Berry curvature dipole (BCD). Here, we explore the question of whether the Berry curvature dipole and multipoles of time-reversal symmetric insulators can be traced in the nonlinear optical responses. We performed real-time time-dependent density functional theory calculations and examined the second harmonic generation susceptibility tensors. The two-band term of the susceptibility tensor is sharply proportional to the interband BCD, dominating over the Hall response once the cancellation effect of the multiple reflection symmetries is lifted. We suggest that the nonlinear Hall component of the second-harmonic spectra of insulators can also be utilized as an effective tool to extract the band structure geometry through Berry curvature dipole and possibly multipoles.

cond-mat.mes-hall↗

arXiv2021

Identification of the Mott insulating CDW state in 1T-TaS$_2$

We investigate the low-temperature charge-density-wave (CDW) state of bulk TaS$_2$ with a fully self-consistent DFT+U approach, over which the controversy has remained unresolved regarding the out-of-plane metallic band. By examining the innate structure of the Hubbard U potential, we reveal that the conventional use of atomic-orbital basis could seriously misevaluate the electron correlation in the CDW state. By adopting a generalized basis, covering the whole David star, we successfully reproduce the Mott insulating nature with the layer-by-layer antiferromagnetic order. Similar consideration should be applied for description of the electron correlation in molecular solid.

cond-mat.str-el↗

arXiv2020

Nonlinear phononics in 2D SnTe: a ferroelectric material with phonon dynamical amplification of electric polarization

Ultrafast optical control of ferroelectricity using intense terahertz fields has attracted significant interest. Here we show that the nonlinear interactions between two optical phonons in SnTe, a two-dimensional in-plane ferroelectric material, enables a dynamical amplification of the electric polarization within subpicoseconds time domain. Our first principles time dependent simulations show that the infrared-active out-of-plane phonon mode, pumped to nonlinear regimes, spontaneously generates in-plane motions, leading to rectified oscillations in the in-plane electric polarization. We suggest that this dynamical control of ferroelectric material, by nonlinear phonon excitation, can be utilized to achieve ultrafast control of the photovoltaic or other non-linear optical responses.

cond-mat.mtrl-sci↗

arXiv2019

Prediction of ferroelectricity-driven Berry curvature enabling charge- and spin-controllable photocurrent in tin telluride monolayers

In symmetry-broken crystalline solids, pole structures of Berry curvature (BC) can emerge, and they have been utilized as a versatile tool for controlling transport properties. For example, the monopole component of the BC is induced by the time-reversal symmetry breaking, and the BC dipole arises from a lack of inversion symmetry, leading to the anomalous Hall and nonlinear Hall effects, respectively. Based on first-principles calculations, we show that the ferroelectricity in a tin telluride monolayer produces a unique BC distribution, which offers charge- and spin-controllable photocurrents. Even with the sizable band gap, the ferroelectrically driven BC dipole is comparable to those of small-gap topological materials. By manipulating the photon handedness and the ferroelectric polarization, charge and spin circular photogalvanic currents are generated in a controllable manner. The ferroelectricity in group-IV monochalcogenide monolayers can be a useful tool to control the BC dipole and the nonlinear optoelectronic responses.

cond-mat.mes-hall↗

arXiv2019

Spin-split band hybridization in graphene proximitized with $α$-RuCl$_3$ nanosheets

Proximity effects induced in the 2D Dirac material graphene potentially open access to novel and intriguing physical phenomena. Thus far, the coupling between graphene and ferromagnetic insulators has been experimentally established. However, only very little is known about graphene's interaction with antiferromagnetic insulators. Here, we report a low temperature study of the electronic properties of high quality van der Waals heterostructures composed of a single graphene layer proximitized with $α$-RuCl$_3$. The latter is known to become antiferromagnetically ordered below 10 K. Shubnikov de Haas oscillations in the longitudinal resistance together with Hall resistance measurements provide clear evidence for a band realignment that is accompanied by a transfer of electrons originally occupying the graphene's spin degenerate Dirac cones into $α$-RuCl$_3$ band states with in-plane spin polarization. Left behind are holes in two separate Fermi pockets, only the dispersion of one of which is distorted near the Fermi energy due to spin selective hybridization with these spin polarized $α$-RuCl$_3$ band states. This interpretation is supported by our DFT calculations. An unexpected damping of the quantum oscillations as well as a zero field resistance upturn close to the N$é$el temperature of $α$-RuCl$_3$ suggests the onset of additional spin scattering due to spin fluctuations in the $α$-RuCl$_3$.

cond-mat.mtrl-sci↗

arXiv2018

Unraveling materials Berry curvature and Chern-Simons numbers from real-time evolution of Bloch states

Materials can be classified by the topological character of their electronic structure and, in this perspective, global attributes immune to local deformations have been discussed in terms of Berry curvature and Chern numbers. Except for instructional simple models, linear response theories have been ubiquitously employed in calculations of topological properties of real materials. Here we propose a completely different and versatile approach to get the topological characteristics of materials by calculating physical observables from the real-time evolving Bloch states: the cell-averaged current density reveals the anomalous velocities whose integration leads to the conductivity quantum. Results for prototypical cases are shown, including a spin-frozen valley-Hall and a quantum anomalous Hall insulator. The advantage of this method is best illustrated by the example of a quantum spin Hall insulator: the quantized spin Hall conductivity is straightforwardly obtained irrespective of the non-Abelian nature in its Berry curvature. Moreover, the method can be extended to the description of real observables in non-equilibrium states of topological materials.

cond-mat.mes-hall↗