arXiv subjects

Shih-Wen Huang

Publications and source records attributed to Shih-Wen Huang.

At least 19 recordsLinked to original sources

arXiv2026

Quantifying angular momentum of coherently driven circular phonons

The use of intense terahertz (THz) pulses to manipulate low-energy excitations offers a powerful approach for ultrafast control of electronic and magnetic properties in materials. Theory suggests that circular ionic motions driven by THz fields carry angular momentum, potentially generating internal magnetic fields. Recent experiments in nonmagnetic SrTiO3 (STO) have hinted at such THz-induced fields, but their origin remains debated. Here, we employ ultrafast x-ray diffraction to resolve the time-dependent ionic trajectories in STO following excitation by circularly polarized THz pulses. Our analysis reveals that oxygen ions, despite their lower mass, contribute around 90% of the phonon angular momentum. The resulting imbalance between the negatively and positively charged ions provides a clear explanation for the mechanism behind induced magnetism in STO. This work further provides the first quantitative measurement of circular ionic motions and their angular momentum and establishes a general methodology for the investigation of angular momentum transfer in solids, paving the way for new strategies to control topological phonon transport and phonon-driven magnetism in quantum materials.

cond-mat.mtrl-sci↗

arXiv2026

Chemical and optical control of chiral-domain dynamics in 1T-TaS$_2$

Optical control of symmetry-breaking quantum phases is often constrained when one domain is strongly favored in equilibrium. This limitation is exemplified by the chiral charge-density-wave (CDW) order in 1T-TaS$_2$, where pristine samples predominantly select a single chirality. Here we show that free-energy landscape engineering through Ti substitution enables a distinct nonthermal pathway for ultrafast chiral-domain redistribution. Ti doping stabilizes coexisting chiral domains and tunes their relative stability, allowing femtosecond excitation to drive an asymmetric and anisotropic redistribution from the dominant toward the minority chirality. The subpicosecond response follows a $\sim2$ THz amplitude mode and is consistent with a phonon-assisted pathway involving transient domain-wall configurations. Our results establish free-energy landscape engineering as a strategy for selecting nonequilibrium transition pathways.

cond-mat.str-el↗

arXiv2026

In-situ Straining of Epitaxial Freestanding Ferroic Films by a MEMS Device

Mechanical strain can be used to control physical properties in materials. The experimental investigation of strain-induced effects at the nanoscale is of importance not only for its fundamental aspects, but also for the development of device applications. Transmission X-ray microscopy is a particularly well-suited technique for nanoscale imaging of magnetic materials, but its compatibility with in-situ mechanical straining of samples is limited. In this work, we present a setup for applying tailored in-situ mechanical strains to freestanding thin films by means of a micro electromechanical system (MEMS) actuator. We then present a proof-of-concept experiment in which a freestanding 80 nm thick (001) BiFeO3 multiferroic thin film is strained with the MEMS device, allowing us to control the coupled ferroelectric/spin cycloidal configuration.

cond-mat.mes-hall↗

arXiv2026

Electric field switching of chiral phonons

Lattice vibrations carrying angular momentum, known as chiral phonons, have emerged as a promising route to control and understand complex material properties, yet their deterministic manipulation remains largely unexplored. Here we demonstrate electric-field switching of phonon angular momentum in the technologically relevant ferroelectric BaTiO3. Using circularly dichroic resonant inelastic X-ray scattering (CD-RIXS) at the oxygen K edge, we directly probe the phonon angular momentum and compare the measured dichroism with first-principles predictions of phonon-mode chirality. We find excellent agreement, revealing a momentum-dependent circular-dichroism contrast that exhibits a reversible gyroelectric effect, stable for at least 15 hours. Our results establish a robust mechanism for non-volatile control of chiral phonons and point towards new opportunities for phonon-based information and energy technologies.

cond-mat.mtrl-sci↗

arXiv2026

Hierarchical quasiparticle dynamics in antiferromagnets revealed by time- and momentum-resolved X-ray scattering

Energy flows among coupled subsystems are essential for ultrafast dynamics and high-speed technologies. In magnetic materials, spin fluctuations -- magnons -- mediate these flows in ultrafast magnetism. Yet momentum-resolved access to low-energy magnons governing the microscopic dynamics has been lacking. Using time-resolved resonant diffuse scattering alongside complementary time-resolved X-ray techniques and quantum-kinetic simulations, we unveil the hierarchical energy pathways among correlated systems in the photoexcited antiferromagnet CuO. Above-bandgap excitation triggers near-instantaneous spin disorder, generating non-thermal magnons throughout reciprocal space within femtoseconds. Real-time momentum-resolved tracking reveals picosecond magnon quasi-thermalization, followed by nanosecond recovery via momentum-selective magnon-phonon scattering. The quasiparticle dispersion mismatch creates recovery bottlenecks that control non-equilibrium lifetimes. This microscopic framework transcends phenomenological models and generalizes across materials, establishing design principles for ultrafast control of material properties.

cond-mat.str-el↗

arXiv2025

Three-dimensional electronic domain correlations in 1T-TaS2

The interplay of nanoscale electronic domains underpins many emergent phenomena of quantum materials, including the competition between charge density waves (CDW) and superconductivity in high-Tc cuprates, or the storage of information in phase-change memory devices. Coupling to electronic domains provides an observable for pinpointing key interactions, e.g. affecting phase transitions. While the equilibrium phase diagram of 1T-TaS2 - characterized by unique transport properties and varying degrees of CDW commensurability - has been studied extensively, an understanding of how the electronic domains in the bulk behave across phase boundaries is lacking. We reveal the three-dimensional evolution of electronic domains in 1T-TaS2 using temperature-dependent X-ray diffraction and reciprocal space mapping, complemented by structure factor simulations based on the Hendricks-Teller method. With this methodology, we identify an increasing number of stacking faults near the phase transitions, and a growing fraction of dimerized layers in the commensurate phase upon cooling. We provide structural evidence that the CDW domains mediate the transport properties at phase boundaries, and that they also account for an anomalous intermediate electronic phase within the triclinic regime upon heating. As a paradigmatic material with potential in phase-change memory applications, our study underscores the importance of domain sizes and layer stacking in defining electronic behaviors of van der Waals materials.

cond-mat.str-el↗

arXiv2025

Imaging of electrically controlled van der Waals layer stacking in 1T-TaS2

Van der Waals (vdW) materials exhibit a variety of states that can be switched with low power at low temperatures, offering a viable cryogenic "flash memory" required for the classical control electronics for solid-state quantum information processing. In 1T-TaS2, a non-volatile metallic 'hidden' state can be induced from an insulating equilibrium charge-density wave ground state using either optical or electrical pulses. Given that conventional memristors form localized, filamentary channels which support the current, a key question for design concerns the geometry of the conduction region in highly energy-efficient 1T-TaS2 devices. Here, we report in operando micro-beam X-ray diffraction, fluorescence, and concurrent transport measurements, allowing us to spatially image the non-thermal hidden state induced by electrical switching of 1T-TaS2. Our results reveal a long-range ordered, non-filamentary switched state that extends well below the electrodes, implying that the self-organized, collective growth of the hidden phase is driven by a combination of charge flow and lattice strain. Our unique combination of techniques showcases the potential of non-destructive, three-dimensional X-ray imaging to study bulk switching properties in microscopic detail, namely electrical control of the vdW layer stacking.

cond-mat.str-el↗

arXiv2025

Imaging ferroelectric domains with soft X-ray ptychography at the oxygen K-edge

The ferroelectric domain structure of a freestanding BiFeO$_3$ film was visualized by ptychographic dichroic imaging with linearly polarized X-rays at the O K-edge around 530 eV. The dichroic contrast is maximized at the energy of the hybridization of the O 2p state and the Fe 3d orbitals, which is split by the octahedral crystal field of the perovskite structure. The microscopy images thus obtained complement the ptychographic imaging of the antiferromagnetic contribution at the Fe L$_3$-edge. The approach can be extended to the separation of different ferroic contributions in other multiferroic oxides.

cond-mat.mtrl-sci↗

arXiv2024

Ptychographic nanoscale imaging of the magnetoelectric coupling in freestanding BiFeO$_3$

Understanding the magnetic and ferroelectric ordering of magnetoelectric multiferroic materials at the nanoscale necessitates a versatile imaging method with high spatial resolution. Here, soft X-ray ptychography is employed to simultaneously image the ferroelectric and antiferromagnetic domains in an 80 nm thin freestanding film of the room-temperature multiferroic BiFeO$_3$ (BFO). The antiferromagnetic spin cycloid of period 64 nm is resolved by reconstructing the corresponding resonant elastic X-ray scattering in real space and visualized together with mosaic-like ferroelectric domains in a linear dichroic contrast image at the Fe L$_3$ edge. The measurements reveal a near perfect coupling between the antiferromagnetic and ferroelectric ordering by which the propagation direction of the spin cycloid is locked orthogonally to the ferroelectric polarization. In addition, the study evinces both a preference for in-plane propagation of the spin cycloid and changes of the ferroelectric polarization by 71° between multiferroic domains in the epitaxial strain-free, freestanding BFO film. The results provide a direct visualization of the strong magnetoelectric coupling in BFO and of its fine multiferroic domain structure, emphasizing the potential of ptychographic imaging for the study of multiferroics and non-collinear magnetic materials with soft X-rays.

cond-mat.mtrl-sci↗

arXiv2024

Unraveling the Mn $L_3$-edge RIXS spectrum of lightly manganese doped Sr$_{3}$Ru$_{2}$O$_{7}$

Resonant inelastic x-ray scattering (RIXS) experiment was performed at the Mn $L_3$ edge. A 10 $\%$ Mn-doped Sr$_{3}$Ru$_{2}$O$_{7}$ compound, where the Mn$^{3+}$ ions are in the 3$d^4$ state, were probed for $dd$ excitations. The dilute doping concentration allows one to treat the dopant Mn$^{3+}$ ions as effectively free in the host ruthenium compound. The local nature of $dd$ RIXS spectroscopy permits one to use a single-site model to simulate the experimental spectra. The simulated spectra reproduces the in-plane [100] experimental RIXS spectrum. We also predict the intensity for the in-plane [110] direction and the out-of-plane spin orientation configuration [001]. Based on our single-ion model we were able to fit the experimental data to obtain the crystal field parameters, the 10Dq value, and the intra-orbital spin-flip energy 2$\mathcal{J}$(or $3J_{H}$, where $J_{H}$ is the Hund's energy) of the Mn$^{3+}$ ion. Utilizing our computed RIXS quantum transition amplitudes between the various $d$ orbitals of the Mn$^{3+}$ ion, the expression for the Kramers-Heisenberg cross section, and a self-consistent fitting procedure we also identify the energy boundaries of the non-spin-flip and spin-flip $dd$ excitations present in the experimental data. From our fitting procedure we obtain $2\mathcal{J} (3J_{H})=2.06$ eV, a value which is in excellent agreement with that computed from the free ion Racah parameters. We also identified the charge transfer boundary. In addition to predicting the microscopic parameters, we find a quantum spin-flip transition in the non-cross ($σ_{in}-σ_{out}$, $π_{in}-π_{out}$) x-ray polarization channels of the $dd$ RIXS spectra. A similar transition, was previously predicted to occur in the $π-π$ channel of the magnon spectrum in the non-collinear non-coplanar Kagome compound composed of Cu$^{2+}$ 3d$^{9}$ ion.

cond-mat.str-el↗

arXiv2024

Octahedral and polar phase transitions in freestanding films of SrTiO3

From extreme strain to bending, the possibilities in the manipulation of freestanding films of oxide perovskites bring a novel landscape to their properties and brings them one step closer to their application. It is therefore of great importance to fully understand the inherent properties of such films, in which dimensionality and surface effects can play a major role in defining the properties of the materials ground state. This paper reports the properties of freestanding (FS) films of the canonical oxide, SrTiO3 (STO) with thicknesses 20, 30, 40 and 80 nm. We show that the relaxed ultrathin STO FS films become polar at temperatures as high as 85 K, in contrast to the quantum paraelectric behavior of bulk. Our findings are based on the softening of the ferroelectric mode towards the ferroelectric transition temperature Tc and its consecutive hardening below Tc with further decreasing temperature, probed with THz time domain spectroscopy in transmission mode. We find almost no thickness dependence in Tc. Moreover, we characterize the antiferrodistortive (AFD) phase transition in STO FS by X-ray diffraction (XRD) probing superlattice reflections characteristic for the rotation of the TiO6 octahedra. Our results point to a higher phase transition temperature in comparison to bulk STO, as well as an unbalanced domain population favoring the rotation axis to be in plane. X-ray linear dichroism results further show a preferential Ti xz/yz orbital occupancy at the surface, but with a complete degeneracy in the t2g states in the inner part of the film indicating that the AFD distortion does not strongly affect the t2g splitting. These findings demonstrate that STO FS films have clearly different properties than bulk.

cond-mat.mtrl-sci↗

arXiv2024

Flexomagnetoelectric effect in Sr2IrO4 thin films

Symmetry engineering is explicitly effective to manipulate and even create phases and orderings in strongly correlated materials. Flexural stress is universally practical to break the space-inversion or time-reversal symmetry. Here, by introducing strain gradient in a centrosymmetric antiferromagnet Sr2IrO4, the space-inversion symmetry is broken accompanying a non-equivalent O p-Ir d orbital hybridization along z axis. Thus, emergent polar phase and out-of-plane magnetic moment have been simultaneously observed in these asymmetric Sr2IrO4 thin films, which both are absent in its ground state. Furthermore, upon the application of magnetic field, such polarization can be controlled by modifying the occupied d orbitals through spin-orbit interaction, giving rise to a flexomagnetoelectric effect. This work provides a general strategy to artificially design multiple symmetries and ferroic orderings in strongly correlated systems.

cond-mat.str-el↗

arXiv2023

Provoking topology by octahedral tilting in strained SrNbO$_3$

Transition metal oxides with a wide variety of electronic and magnetic properties offer an extraordinary possibility to be a platform for developing future electronics based on unconventional quantum phenomena, for instance, the topology. The formation of topologically non-trivial states is related to crystalline symmetry, spin-orbit coupling, and magnetic ordering. Here, we demonstrate how lattice distortions and octahedral rotation in SrNbO$_3$ films induce the band topology. By employing angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT) calculations, we verify the presence of in-phase $a^0a^0c^+$ octahedral rotation in ultra-thin SrNbO$_3$ films, which causes the formation of topologically-protected Dirac band crossings. Our study illustrates that octahedral engineering can be effectively exploited for implanting and controlling quantum topological phases in transition metal oxides.

cond-mat.mtrl-sci↗

arXiv2023

Structural and magnetic properties of $β$-Li$_2$IrO$_3$ after grazing-angle focused ion beam thinning

Manipulating the size and orientation of quantum materials is often used to tune emergent phenomena, but precise control of these parameters is also necessary from an experimental point of view. Various synthesis techniques already exist, such as epitaxial thin film growth and chemical etching, that are capable of producing specific sample dimensions with high precision. However, certain materials exist as single crystals that are often difficult to manipulate, thereby limiting their studies to a certain subset of experimental techniques. One particular class of these materials are the lithium and sodium iridates that are promising candidates for hosting a Kitaev quantum spin liquid state. Here we present a controlled method of using a focused ion beam at grazing incidence to reduce the size of a $β$-Li$_2$IrO$_3$ single crystal to a thickness of 1 $μm$. Subsequent x-ray diffraction measurements show the lattice remains intact, albeit with a larger mosaic spread. The integrity of the magnetic order is also preserved as the temperature dependent magnetic diffraction peak follows the same trend as its bulk counterpart with a transition temperature at TN = 37.5 K. Our study demonstrates a technique that opens up the possibility of nonequilibrium experiments where submicron thin samples are often essential.

cond-mat.mtrl-sci↗

arXiv2023

Precise dd excitations and commensurate intersite Coulomb interactions in the dissimilar cuprate YBa_2Cu_3O_(7-x) and La_(2-x)Sr_xCuO_4

Using high-resolution extreme ultraviolet resonant inelastic X-ray scattering (EUVRIXS) spectroscopy at Cu M-edge, we observed the doping dependent spectral shifts of inter-orbital (dd) excitations of YBa_2Cu_3O_(7-x) and La_(2-x)Sr_xCuO_4. With increasing hole doping level from undoped to optimally doped superconducting compositions, the leading edge of dd excitations is found to shift towards lower energy loss in a roughly linear trend that is irrespective to the cuprate species. The magnitude of energy shift can be explained by including a 0.15 eV Coulomb attraction between Cu 3d_(x^2-y^2) electrons and the doped holes on the surrounding oxygens in the atomic multiplet calculations. The consistent energy shift between distinct cuprate families suggests that this inter-site Coulomb interaction energy scale is relatively material-independent, and provides an important reference point for understanding charge density wave phenomena in the cuprate phase diagram.

cond-mat.supr-con↗

arXiv2022

Resonant Soft X-Ray Scattering on LaPt$_2$Si$_2$

X-ray absorption (XAS) and Resonant Inelastic X-ray Scattering (RIXS) spectra of LaPt$_2$Si$_2$ single crystal at the Si L and La N edges are presented. The data are interpreted in terms of density functional theory, showing that the Si spectra can be described in terms of Si $s$ and $d$ local partial density of states (LPDOS), and the La spectra are due to quasi-atomic local $4f$ excitations. Calculations show that Pt $d$-LPDOS dominates the occupied states, and a sharp localized La $f$ state is found in the unoccupied states, in line with the observations.

cond-mat.mtrl-sci↗

arXiv2016

Experimental signatures of phase interference and sub-femtosecond time dynamics on the incident energy axis of resonant inelastic X-ray scattering

Core hole resonance is used in X-ray spectroscopy to incisively probe the local electronic states of many-body systems. Here, resonant inelastic X-ray scattering (RIXS) is studied as a function of incident photon energy on Mott insulators SrCuO2 and NiO to examine how resonance states decay into different excitation symmetries at the transition metal M-, L- and K-edges. Quantum interference patterns characteristic of the two major RIXS mechanisms are identified within the data, and used to distinguish the attosecond scale scattering dynamics by which fundamental excitations of a many-body system are created. A function is proposed to experimentally evaluate whether a particular excitation has constructive or destructive interference in the RIXS cross-section, and corroborates other evidence that an anomalous excitation is present at the leading edge of the Mott gap in quasi-one dimensional SrCuO2.

cond-mat.str-el↗

arXiv2015

Spectroscopic determination of the atomic f-electron symmetry underlying hidden order in URu$_2$Si$_2$

The low temperature hidden order state of URu$_2$Si$_2$ has long been a subject of intense speculation, and is thought to represent an as yet undetermined many-body quantum state not realized by other known materials. Here, X-ray absorption spectroscopy (XAS) and high resolution resonant inelastic X-ray scattering (RIXS) are used to observe electronic excitation spectra of URu$_2$Si$_2$, as a means to identify the degrees of freedom available to constitute the hidden order wavefunction. Excitations are shown to have symmetries that derive from a correlated $5f^2$ atomic multiplet basis that is modified by itinerancy. The features, amplitude and temperature dependence of linear dichroism are in agreement with ground states that closely resemble the doublet $Γ_5$ crystal field state of uranium.

cond-mat.mtrl-sci↗