arXiv subjects

Alfred Zong

Publications and source records attributed to Alfred Zong.

At least 19 recordsLinked to original sources

arXiv2026

A table-top few-femtosecond broadband extreme-ultraviolet absorption spectrometer with cryogenic cooling

We present a table-top cryogenic ultrafast broadband XUV absorption spectroscopy (c-UBXAS) beamline designed for temperature-dependent and time-resolved investigations of quantum materials. The instrument combines a broadband high-harmonic generation source spanning 22-73 eV with automated image registration and cryogenic sample control down to 20 K, enabling element-specific measurements under both equilibrium and nonequilibrium conditions. The beamline provides sub-50-meV energy resolution and a sub-10-fs instrument response function, while maintaining long-term stability suitable for extended, ultrasensitive measurements. Benchmark experiments on NiI$_2$, a van der Waals multiferroic, reveal temperature-dependent spectral evolution across its magnetic phase transitions, demonstrating the ability to identify element-specific contributions to the ground state and its transient response in the femtosecond regime. This instrument introduces the opportunity to unravel the very first response of a solid-state material during light-matter interaction, paving the way for understanding the complex phase space of nonequilibrium dynamics and emergent states in strongly correlated systems where the few-femtosecond electronic response has eluded most other types of time-resolved techniques.

physics.ins-det↗

arXiv2026

Room-temperature multistage metastability in a moir\'e superstructure

Metastability is fundamental not only to phase ordering and transitions, but also to a broad range of modern technologies, from memory devices to metallic glasses. In condensed-matter physics, charge density waves (CDWs) offer versatile platforms for accessing metastable states due to their sensitivity to external stimuli. However, most metastable CDW states are stabilized only at low temperatures, limiting their practical utility. In this study, we report the observation of electrically driven, room-temperature, nonvolatile metastable states in the bulk form of EuTe$_4$, a recently discovered compound that hosts an innate moir\'e superlattice characterized by the stacking of incommensurate monolayer and bilayer CDWs. Systematic transport measurements reveal discrete resistivity plateaus and strong electric-field sensitivity, with a large number of metastable states readily induced across a wide temperature window within a giant hysteresis loop, making them well-suited for high-temperature, multi-bit memory applications. By integrating photoemission spectroscopy, diffraction, and in-situ transport measurements, we uncover that these metastable states do not stem from conventional mechanisms such as the emergence of new ordered phases or changes in incommensurate periodicity. Instead, they are characterized by a suppression of the original CDW amplitude and a reduction in correlation length, pointing to a unique electric-field-induced switching of out-of-plane CDW phases in the moir\'e superstructure. Our findings not only provide critical insights into metastable phenomena in moir\'e systems with stacked electronic orders but also establish EuTe$_4$ as a promising platform for developing room-temperature, multi-bit memory devices.

cond-mat.str-el↗

arXiv2026

Atomically Resolved Acoustic Dynamics Coupled with Magnetic Order in a van der Waals Antiferromagnet

Magnetoelastic coupling in van der Waals (vdW) magnetic materials enables a unique interplay between the spin and lattice degrees of freedom. Characterizing the elastic responses with atomic and femtosecond resolution across the magnetic transition is essential for guiding the design of magnetically tunable actuators and strain-mediated spintronic devices. Here, ultrafast x-ray diffraction employed at a free-electron laser reveals that the atomic displacements, wave vectors, and dispersion relations of acoustic phonon modes in a vdW antiferromagnet FePS$_3$ are coupled with the magnetic order, by tracking both in-plane and out-of-plane Bragg peaks upon optical excitation across the N\'eel temperature (T$_N$). One transverse mode shows that a quasi-out-of-plane atomic displacement undergoes a significant directional change across T$_N$. Its quasi-in-plane wave vector is derived by the comparison between the measured sound velocity and the first-principles calculations. The other transverse mode is an interlayer shear acoustic mode whose amplitude is strongly enhanced in the antiferromagnetic phase, exhibiting eight times stronger amplitude than the longitudinal acoustic mode below T$_N$. The atomically resolved characterization of acoustic phonon dynamics that couple with magnetic ordering opens opportunities for harnessing unique magnetoelastic coupling in vdW magnets on ultrafast timescales.

cond-mat.mtrl-sci↗

arXiv2025

Bidirectional ultrafast control of charge density waves via phase competition

The intricate competition between coexisting charge density waves (CDWs) can lead to rich phenomena, offering unique opportunities for phase manipulation through electromagnetic stimuli. Leveraging time-resolved X-ray diffraction, we demonstrate ultrafast control of a CDW in EuTe$_4$ upon optical excitation. At low excitation intensities, the amplitude of one of the coexisting CDW orders increases at the expense of the competing CDW, whereas at high intensities, it exhibits a nonmonotonic temporal evolution characterized by both enhancement and reduction. This transient bidirectional controllability, tunable by adjusting photo-excitation intensity, arises from the interplay between optical quenching and phase-competition-induced enhancement. Our findings, supported by phenomenological time-dependent Ginzburg-Landau theory simulations, not only clarify the relationship between the two CDWs in EuTe$_4$, but also highlight the versatility of optical control over order parameters enabled by phase competition.

cond-mat.str-el↗

arXiv2025

Dynamics of a jointly commensurate moir\'e charge density wave

The advent of two-dimensional moir\'e systems has revolutionized the exploration of phenomena arising from strong correlations and nontrivial band topology. Recently, a moir\'e superstructure formed by two coexisting charge density waves (CDWs) with slightly mismatched wavevectors has been realized. These incommensurate CDWs can collectively exhibit commensurability, resulting in the jointly commensurate CDW (JC-CDW) and establishing a new paradigm for controlling moir\'e potential and periodicity. Achieving such functionality, however, hinges on a key open question: how do the amplitude, phase coherence, and periodicity of this order respond to external perturbations? Here, we address this question using a suite of time- and momentum-resolved diffraction and spectroscopic techniques to probe light-induced CDW dynamics in EuTe$_4$. Our time-resolved diffraction measurements distinguish the instantaneous quenching of the JC-CDW amplitude, as verified by time-resolved photoemission spectroscopy, from the much slower evolution of phase fluctuations. Furthermore, while the JC-CDW wavevector remains locked along the CDW direction upon photoexcitation, indicating a preserved moir\'e periodicity, the correlation length of JC-CDW shows an exclusive reduction perpendicular to its wavevector, unveiling the formation of previously unexplored shear-type defects. Together, this multimodal methodology reconstructs the spatiotemporal evolution of the JC-CDW upon excitation. These findings not only highlight the remarkable robustness of JC-CDWs out of equilibrium, but also provide insight into optical manipulation and engineering of moir\'e quantum materials through defect control.

cond-mat.str-el↗

arXiv2025

Structural contribution to light-induced gap suppression in Ta$_2$NiSe$_5$

An excitonic insulator is a material that hosts an exotic ground state, where an energy gap opens due to spontaneous condensation of bound electron-hole pairs. Ta$_2$NiSe$_5$ is a promising candidate for this type of material, but the coexistence of a structural phase transition with the gap opening has led to a long-standing debate regarding the origin of the insulating gap. Here we employ MeV ultrafast electron diffraction to obtain quantitative insights into the atomic displacements in Ta$_2$NiSe$_5$ following photoexcitation, which has been overlooked in previous time-resolved spectroscopy studies. In conjunction with first-principles calculations using the measured atomic displacements, we find that the structural change can largely account for the photoinduced reduction in the energy gap without considering excitonic effects. Our work illustrates the importance of a quantitative reconstruction of individual atomic pathways during nonequilibrium phase transitions, paving the way for a mechanistic understanding of a diverse array of phase transitions in correlated materials where lattice dynamics can play a pivotal role.

cond-mat.mtrl-sci↗

arXiv2025

Time-domain identification of distinct mechanisms for competing charge density waves in a rare-earth tritelluride

Understanding the origin of phase transitions and the interactions between distinct phases remains a central task in condensed matter physics. Charge density wave (CDW) systems provide an ideal platform for investigating these phenomena. While the dominant CDW phases in many materials can be explained through Fermi surface nesting or electron-phonon interactions, certain CDW phase transitions remain poorly understood, challenging conventional paradigms. One notable example is rare-earth tritelluride ErTe3, which hosts two competing CDW orders. While the dominant CDW phase fits within the electron-phonon coupling framework, the formation mechanism of the subdominant CDW remains enigmatic. In this study, we combine time-and-angle-resolved photoemission spectroscopy (trARPES) with time-dependent Ginzburg-Landau (TDGL) theory to establish a time-domain approach for probing phase transitions in solid-state systems. By analyzing the distinct recovery dynamics of the two CDW orders in ErTe3 following light excitation, we reveal a novel nucleation-like growth mechanism that likely drives the secondary CDW phase transition. This work not only uncovers a previously unknown CDW formation mechanism in rare-earth tritellurides but also introduces a non-equilibrium framework for understanding phase transitions and phase competition in quantum materials.

cond-mat.str-el↗

arXiv2025

Revisiting the charge-density-wave superlattice of 1$T$-TiSe$_2$

A number of intriguing phenomena, including exciton condensation, orbital ordering, and emergence of chirality, have been proposed to accompany charge-density-wave (CDW) formation in the layered transition metal dichalcogenide 1$T$-TiSe$_2$. Explaining these effects relies on knowledge of the atomic displacement pattern underlying the CDW, yet structural proposals based on spatially-averaging bulk crystal diffraction and surface-dependent scanning tunneling microscopy have remained inconsistent. Here, we revisit the CDW superlattice structure with selected-area electron diffraction, a bulk-sensitive probe capable of capturing sub-micrometer spatial variations while maintaining high momentum resolution. We resolved two distinct, spatially separated CDW phases characterized by different interlayer ordering. In both phases, previously reported atomic displacement patterns fail to account for the observed extinction rules. Instead, our analysis reveals a new superlattice structure, which features a large number of nearly degenerate CDW domains. These findings not only provide a new basis for understanding the gyrotropic electronic order and metastability in 1$T$-TiSe$_2$, they also underscore the importance of bulk-sensitive mesoscopic techniques in investigating materials that host unconventional superlattices.

cond-mat.str-el↗

arXiv2025

Large moir\'{e} superstructure of stacked incommensurate charge density waves

Recent advances in van der Waals heterostructures have opened the new frontier of moir\'{e} physics, whereby tuning the interlayer twist angle or adjusting lattice parameter mismatch have led to a plethora of exotic phenomena such as unconventional superconductivity and fractional quantum spin Hall effect. We extend the concept of moir\'{e} engineering to materials that host incommensurate orders, where we discovered a long-period, thermally-hysteretic moir\'{e} superlattice in a layered charge density wave (CDW) compound, EuTe$_\text{4}$. Using high-momentum-resolution X-ray diffraction performed on ultrathin flakes, we found two coexisting, incommensurate CDWs with slightly mismatched in-plane wavevectors. The interaction between these two CDWs leads to their joint commensuration with the high-symmetry lattice as well as a large moir\'{e} superstructure with an in-plane period of 13.6~nm. Due to different out-of-plane orders of the incommensurate CDWs, the moir\'{e} superstructure exhibits a clear thermal hysteresis, accounting for the large hysteresis observed in electrical resistivity and numerous metastable states induced by light or electrical pulses. Our findings pave the way for a new development in moir\'{e} engineering based on an incommensurate lattice. They further highlight the important role of interlayer ordering in determining the macroscopic properties of these stacked incommensurate structures.

cond-mat.str-el↗

arXiv2025

Time-domain study of coupled collective excitations in quantum materials

Quantum materials hold immense promises for future applications due to their intriguing electronic, magnetic, thermal, and mechanical properties that often arise from a complex interplay between microscopic degrees of freedom. Important insights of such interactions come from studying the collective excitations of electrons, spins, orbitals, and lattice, whose cooperative motions play a crucial role in determining the novel behavior of these systems and offer us a key tuning knob to modify material properties on-demand through external perturbations. In this regard, ultrafast light-matter interaction has shown great potential in controlling the couplings of collective excitations, and rapid progress in a plethora of time-resolved techniques down to the attosecond regime has significantly advanced our understanding of the coupling mechanisms and guided us in manipulating the dynamical properties of quantum materials. This review aims to highlight recent experiments on visualizing collective excitations in the time domain, focusing on the coupling mechanisms between different collective modes such as phonon-phonon, phonon-magnon, phonon-exciton, magnon-magnon, magnon-exciton, and various polaritons. We introduce how these collective modes are excited by an ultrashort laser pulse and probed by different ultrafast techniques, and we explain how the coupling between collective excitations governs the ensuing nonequilibrium dynamics. We also provide some perspectives on future studies that can lead to discoveries of the emergent properties of quantum materials both in and out of equilibrium.

cond-mat.str-el↗

arXiv2024

Observation of Orbital-Selective Dual Modulations in an Anisotropic Antiferromagnetic Kagome Metal TbTi3Bi4

Orbital selectivity is pivotal in dictating the phase diagrams of multiorbital systems, with prominent examples including the orbital-selective Mott phase and superconductivity, etc. The intercalation of anisotropic layers represents an effective method for enhancing orbital selectivity and, thereby shaping the low-energy physics of multiorbital systems. Despite its potential, related experimental studies remain limited. In this work, we systematically examine the interplay between orbital selectivity and magnetism in the newly discovered anisotropic kagome TbTi3Bi4 single crystal, and report a unidirectional, orbital-selective band reconstruction within the antiferromagnetic (AFM) state. By combining soft X-ray and vacuum ultraviolet angle-resolved photoemission spectroscopy (ARPES) measurements with orbital-resolved density functional theory (DFT) calculations, we identify that the band reconstruction is a manifestation of the AFM order, driven by a 1/3 nesting instability of the intercalated Tb 5dxz orbitals. Such an orbital-selective modulation leads the unusual momentum-dependent band folding and the emergence of symmetry-protected Dirac cones only at the M1 point. More importantly, the discovery of orbital-selective 3 x 1 AFM order offers crucial insights into the underlying mechanism of the fractional magnetization plateau in this Kagome AFM metal. Our findings not only underscore the essential role of both conducting and localized electrons in determining the magnetic orders of LnTi3Bi4 (Ln = Lanthanide) kagome metals but also offer a pathway for manipulating magnetism through selective control of anisotropic electronic structures.

cond-mat.str-el↗

arXiv2024

Core-level signature of long-range density-wave order and short-range excitonic correlations probed by attosecond broadband spectroscopy

Advances in attosecond core-level spectroscopies have successfully unlocked the fastest dynamics involving high-energy electrons. Yet, these techniques are not conventionally regarded as an appropriate probe for low-energy quasiparticle interactions that govern the ground state of quantum materials, nor for studying long-range order because of their limited sensitivity to local charge environments. Here, by employing a unique cryogenic attosecond beamline, we identified clear core-level signatures of long-range charge-density-wave (CDW) formation in a quasi-2D excitonic insulator candidate, even though equilibrium photoemission and absorption measurements of the same core levels showed no spectroscopic singularity at the phase transition. Leveraging the high time resolution and intrinsic sensitivity to short-range charge excitations in attosecond core-level absorption, we observed compelling time-domain evidence for excitonic correlations in the normal-state of the material, whose presence has been subjected to a long-standing debate in equilibrium experiments because of interfering phonon fluctuations in a similar part of the phase space. Our findings support the scenario that short-range excitonic fluctuations prelude long-range order formation in the ground state, providing important insights in the mechanism of exciton condensation in a quasi-low-dimensional system. These results further demonstrate the importance of a simultaneous access to long- and short-range order with underlying dynamical processes spanning a multitude of time- and energy-scales, making attosecond spectroscopy an indispensable tool for both understanding the equilibrium phase diagram and for discovering novel, nonequilibrium states in strongly correlated materials.

cond-mat.str-el↗

arXiv2024

Hidden correlations in stochastic photoinduced dynamics of a solid-state electrolyte

Photoexcitation by ultrashort laser pulses plays a crucial role in controlling reaction pathways, creating nonequilibrium material properties, and offering a microscopic view of complex dynamics at the molecular level. The photo response following a laser pulse is, in general, non-identical between multiple exposures due to spatiotemporal fluctuations in a material or the stochastic nature of dynamical pathways. However, most ultrafast experiments using a stroboscopic pump-probe scheme struggle to distinguish intrinsic sample fluctuations from extrinsic apparatus noise, often missing seemingly random deviations from the averaged shot-to-shot response. Leveraging the stability and high photon-flux of time-resolved X-ray micro-diffraction at a synchrotron, we developed a method to quantitatively characterize the shot-to-shot variation of the photoinduced dynamics in a solid-state electrolyte. By analyzing temporal evolutions of the lattice parameter of a single grain in a powder ensemble, we found that the sample responses after different shots contain random fluctuations that are, however, not independent. Instead, there is a correlation between the nonequilibrium lattice trajectories following adjacent laser shots with a characteristic "correlation length" of approximately 1,500 shots, which represents an energy barrier of 0.38~eV for switching the photoinduced pathway, a value interestingly commensurate with the activation energy of lithium ion diffusion. Not only does our nonequilibrium noise correlation spectroscopy provide a new strategy for studying fluctuations that are central to phase transitions in both condensed matter and molecular systems, it also paves the way for discovering hidden correlations and novel metastable states buried in oft-presumed random, uncorrelated fluctuating dynamics.

cond-mat.mtrl-sci↗

arXiv2024

Coexistence of interacting charge density waves in a layered semiconductor

Coexisting orders are key features of strongly correlated materials and underlie many intriguing phenomena from unconventional superconductivity to topological orders. Here, we report the coexistence of two interacting charge-density-wave (CDW) orders in EuTe4, a layered crystal that has drawn considerable attention owing to its anomalous thermal hysteresis and a semiconducting CDW state despite the absence of perfect FS nesting. By accessing unoccupied conduction bands with time- and angle-resolved photoemission measurements, we find that mono- and bi-layers of Te in the unit cell host different CDWs that are associated with distinct energy gaps. The two gaps display dichotomous evolutions following photoexcitation, where the larger bilayer CDW gap exhibits less renormalization and faster recovery. Surprisingly, the CDW in the Te monolayer displays an additional momentum-dependent gap renormalization that cannot be captured by density-functional theory calculations. This phenomenon is attributed to interlayer interactions between the two CDW orders, which account for the semiconducting nature of the equilibrium state. Our findings not only offer microscopic insights into the correlated ground state of EuTe4 but also provide a general non-equilibrium approach to understand coexisting, layer-dependent orders in a complex system.

cond-mat.str-el↗

arXiv2023

Room-temperature non-volatile optical manipulation of polar order in a charge density wave

Utilizing ultrafast light-matter interaction to manipulate electronic states of quantum materials is an emerging area of research in condensed matter physics. It has significant implications for the development of future ultrafast electronic devices. However, the ability to induce long-lasting metastable electronic states in a fully reversible manner is a long-standing challenge.Here, by using ultrafast laser excitations, we demonstrate the capability to manipulate the electronic polar states in the charge-density-wavematerial EuTe4 in a non-volatile manner. The process is completely reversible and is achieved at room temperature with an all-optical approach. Each induced non-volatile state brings about modifications to the electrical resistance and second harmonic generation intensity. The results point to layer-specific phase inversion dynamics by which photoexcitation mediates the stacking polar order of the system. Our findings extend the scope of non-volatile all-optical control of electronic states to ambient conditions, and highlight a distinct role of layerdependent phase manipulation in quasi-two-dimensional systems with inherent sublayer stacking orders.

cond-mat.str-el↗

arXiv2023

A solid-state high harmonic generation spectrometer with cryogenic cooling

Solid-state high harmonic generation spectroscopy (sHHG) is a promising technique for studying electronic structure, symmetry, and dynamics in condensed matter systems. Here, we report on the implementation of an advanced sHHG spectrometer based on a vacuum chamber and closed-cycle helium cryostat. Using an in situ temperature probe, it is demonstrated that the sample interaction region retains cryogenic temperature during the application of high-intensity femtosecond laser pulses that generate high harmonics. The presented implementation opens the door for temperature-dependent sHHG measurements down to few Kelvin, which makes sHHG spectroscopy a new tool for studying phases of matter that emerge at low temperatures, which is particularly interesting for highly correlated materials.

physics.app-ph↗

arXiv2023

Evidence for bootstrap percolation dynamics in a photo-induced phase transition

Upon intense femtosecond photo-excitation, a many-body system can undergo a phase transition through a non-equilibrium route, but understanding these pathways remains an outstanding challenge. Here, we use time-resolved second harmonic generation to investigate a photo-induced phase transition in Ca$_3$Ru$_2$O$_7$ and show that mesoscale inhomogeneity profoundly influences the transition dynamics. We observe a marked slowing down of the characteristic time, $\tau$, that quantifies the transition between two structures. $\tau$ evolves non-monotonically as a function of photo-excitation fluence, rising from below 200~fs to $\sim$1.4~ps, then falling again to below 200~fs. To account for the observed behavior, we perform a bootstrap percolation simulation that demonstrates how local structural interactions govern the transition kinetics. Our work highlights the importance of percolating mesoscale inhomogeneity in the dynamics of photo-induced phase transitions and provides a model that may be useful for understanding such transitions more broadly.

cond-mat.str-el↗

arXiv2022

Delamination-assisted ultrafast wrinkle formation in a freestanding film

The ability to synthesize and control two-dimensional (2D) crystals creates numerous opportunities for studying emergent states of matter and their novel functionalities. Freestanding films provide a particularly versatile platform for materials engineering in 2D thanks to additional structural motifs not found in films adhered to a flat substrate. A ubiquitous example is wrinkles, yet little is known about how they can develop over as fast as a few picoseconds due to a lack of experimental probes to visualize their dynamics in real time at the nanoscopic scale. Here, we use ultrafast electron diffraction to directly observe light-activated wrinkling formation in a freestanding La$_{2/3}$Ca$_{1/3}$MnO$_3$ film. Via a ``lock-in'' analysis of a single mode of oscillation in the diffraction peak position, intensity, and width, we are able to quantitatively reconstruct how wrinkles develop at the picosecond timescale. Contrary to the common assumption of a fixed boundary condition for freestanding films, we found that wrinkle development is associated with ultrafast delamination at the contact point between the film boundary and the underlying substrate, avoiding a strain build-up in the film. Not only does our work provide a generic protocol to quantify wrinkling dynamics in freestanding films, it also highlights the importance of film-substrate interaction for determining the properties of freestanding structures.

cond-mat.mtrl-sci↗