arXiv subjects

Dao Xiang

Publications and source records attributed to Dao Xiang.

At least 19 recordsLinked to original sources

arXiv2026

Fully coherent short wavelength free-electron laser driven by a single sub-microjoule seed

High-repetition-rate, fully coherent extreme-ultraviolet (EUV) and X-ray free-electron lasers (FELs) are essential for advanced time-resolved ultrafast spectroscopies. While external seeding serves as the standard technique to achieve precise temporal coherence, conventional methods demand hundred-megawatt peak-power laser systems. Furthermore, advanced configurations like echo-enabled harmonic generation (EEHG) introduce the severe complexities of dual-laser synchronization. Together, these requirements fundamentally restrict operations to kilohertz repetition rates and compromise overall system stability. Here, we experimentally demonstrate a fully coherent EEHG-FEL driven by a single, sub-microjoule seed laser. By employing a direct-amplification enabled harmonic generation technique, we utilize an initial 0.4 microJ (2 MW peak power) ultraviolet seed to directly drive coherent lasing at nanometer wavelengths. By eliminating the need for extreme peak powers and multiple synchronized lasers, this approach significantly simplifies the seeding architecture and provides a practical and robust pathway toward megahertz-class, fully coherent EUV and X-ray light sources.

physics.acc-ph↗

arXiv2026

Extreme Terahertz Nonlinear Phononics by Coherence-Imprinted Control of Hybrid Order

Coherent control of quantum materials has progressed along two major fronts: nonlinear phononics, which reshapes lattices to induce emergent states, and Floquet engineering, which tailors electronic band reconstruction via time-periodic driving. Both mechanisms face fundamental limitations at terahertz (THz) frequencies: phononic nonlinearities are intrinsically weak in standard lattices, while electronic Floquet states are often constrained by rapid decoherence upon light-off and by a scarcity of coherence-resolved, multi-correlation probes beyond (quasi-)stationary band structures. Here we report an extreme THz nonlinear-phononics mechanism in $\text{Ta}_\text{2}\text{NiSe}_\text{5}$, where a highly susceptible non-equilibrium electronic correlation bath dramatically amplifies lattice nonlinearities under coherent driving. Utilizing THz two-dimensional spectroscopy as a coherence-tomography tool, we resolve an exceptionally rich landscape of approximately 30 distinct multi-order quantum pathways, including high-harmonic phonon generation, multi-quantum coherences, and multi-wave anharmonic cross-mode mixing. The density and complexity of this extreme manifold establishes a new benchmark for THz nonlinear phononics, as the multi-order quantum pathways surpass the limits of conventional lattice responses. These high-order signals collapse above ~100~K, defining an electronic correlation scale of a coherence-imprinted hybrid electronic-phonon order that governs the sustainability of high-order quantum correlations and nonlinear pathways beyond linear and equilibrium responses. Our results establish a route for correlation-boosted, phonon-anchored periodic Hamiltonian engineering and for certifying such periodically-driven states via multi-correlation coherence tomography.

cond-mat.str-el↗

arXiv2026

Electronic excitation of ultrafast collective amorphous-amorphous transitions in glassy phase-change material

The intrinsic nature of glass states and glass transitions remain a fundamental open question in condensed-matter physics and materials science. The key to solving the glass transition problem lies in achieving a complete understanding of the physics governing the structural relaxation. Nonetheless, directly probing dynamic atomic-scale structural changes in order to identify the precise local structural motifs and establish quantitative structure-property relationships remains an outstanding challenge. By combining femtosecond electron diffraction with time-dependent density-functional theory molecular dynamics simulations, we directly capture ultrafast amorphous-amorphous transitions indicated by collective bond stretching (0.2 ps) and angle bending (0.5-2 ps) in glassy phase-change material GeTe. The ultrafast bond stretching is accompanied by localized oscillation modes with the frequency of 3.10 THz, unambiguously signaling the local Peierls-like bonding structure and the flexibility of these polarized bonds. These ultrafast collective atomic motions, captured across timescales ranging from femtoseconds to picoseconds, directly reveals the structural origin of the boson peak and provide compelling evidence for many-body interactions in amorphous materials. Furthermore, the ultrafast amorphous-amorphous transitions induce a drastic insulator-metal transition, directly revealing both the underlying switching mechanism and the fundamental speed limit of the ovonic threshold switch. These insights establish a fundamental framework for rationally engineering relaxation pathways and phase-change/threshold switch in amorphous materials. Femtosecond electron diffraction provides a powerful novel approach to deciphering the structural complexity and functional mechanisms of amorphous materials by resolving collective atomic motions from random diffusion dynamics in the time domain.

cond-mat.mtrl-sci↗

arXiv2026

Sub-angstrom many-body localization driven by phononic flat bands in real quantum materials

Defects, fluctuations, degenerate states and correlated interactions facilitate the emergence of exotic properties in condensed matter systems while also inducing atomic-scale local correlated structures that deviate from the average long-range order. Establishing the structure-property relationship from the perspective of these atomic-scale local correlated structures remains ambiguous and controversial due to the lack of direct methods for identifying such local correlated structures. In this work, based on the photoexcited ultrafast structural response, we propose a Bragg scattering phase breaking regime to identify sub-angstrom local correlated structures in quantum materials. With this regime, we unambiguously identify the many-body-interaction driven local correlated structures in the low temperature ground state of AgCrSe2, characterized by static off-center displacements of Ag atoms ranging from 0 to 0.5 angstrom. The competition between Ag-Ag Coulomb correlations and potential wells induced by CrSe2 layers, leading to phononic flat bands and driving the system into a many body localization (MBL) regime. As temperature rising, these static local correlated structures transform to a dynamic state where the thermal fluctuations overwhelm the multiple localized states. These distinctive local correlated structures constitute the first experimental observation of MBL with vortex-like topological characteristic in a real material system. Emergent vibrational modes arising from MBL have been confirmed and show excellent agreement with inelastic neutron scattering experiments. Our work not only offers a universal approach to characterize sub-angstrom local correlated structures across a wide range of quantum materials but also deepens our understanding of the fundamental mechanism behind exotic properties from the perspective of atomic-scale local correlated structures.

cond-mat.mtrl-sci↗

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

Super-resolution femtosecond electron diffraction reveals electronic and nuclear dynamics at conical intersections

Conical intersections play a pivotal role in excited-state quantum dynamics. Capturing transient molecular structures near conical intersections remains challenging due to the rapid timescales and subtle structural changes involved. We overcome this by combining the enhanced temporal resolution of mega-electron-volt ultrafast electron diffraction with a super-resolution real-space inversion algorithm, enabling visualization of nuclear and electronic motions at conical intersections with sub-angstrom resolution, surpassing the diffraction limit. We apply this technique to the textbook example of the ring-opening reaction of 1,3-cyclohexadiene, which proceeds through two conical intersections within 100 femtoseconds. The super-resolved transient structures near conical intersections reveal a C-C bond length difference of less than 0.4 angstrom and an approximately 30-femtosecond traversal time of the nuclear wave packet between them. These findings establish super-resolution ultrafast scattering as a transformative tool for uncovering quantum dynamics in molecules and open new avenues for studying light-matter interactions at the most fundamental level.

physics.chem-ph↗

arXiv2025

Probing valence electron and hydrogen dynamics using charge-pair imaging with ultrafast electron diffraction

A key challenge in ultrafast science has been to directly track the coupled motions of electrons and nuclei in real-space and real-time. This study presents a significant step towards this goal by demonstrating the feasibility of time-resolved real-space tracking of valence electron and hydrogen dynamics during the photodissociation of ammonia (NH3) using MeV ultrafast electron diffraction. It is demonstrated that the enhanced temporal resolution, in conjunction with the analysis of the charge-pair distribution function, enables the disentanglement of the correlated motion of valence electrons and hydrogens in photoexcited ammonia molecule. The methodology employed in this study, which utilizes the charge-pair distribution function from ultrafast electron scattering to retrieve intertwined electron and nucleus dynamics, may open up new opportunities in the study of quantum dynamics for a wide range of molecules.

physics.chem-ph↗

arXiv2025

Imaging the photochemical dynamics of cyclobutanone with MeV ultrafast electron diffraction

We study the photoinduced chemical dynamics of cyclobutanone upon excitation at 200 nm to the 3s Rydberg state using MeV ultrafast electron diffraction (UED). We observe both the elastic scattering signal, which contains information about the structural dynamics, and the inelastic scattering signal, which encodes information about the electronic state. Our results suggest a sub-picosecond timescale for the photodissociation dynamics, and an excited state lifetime of about 230 femtoseconds. The dissociation is found to be dominated by the C3 channel where cyclopropane and CO are produced. The branching ratio of the C3 channel to the C2 channel where ethene and ketene are produced, is estimated to be approximately 5:3. Our data suggest that the C3 and C2 channels account for approximately 80% of the photoproducts, with the remaining 20% exhibiting ring-opened structures. It is found that the timescale associated with the dissociation process in the C2 channel is shorter compared to that in the C3 channel. Leveraging the enhanced temporal resolution of MeV UED, our results provide a real-time mapping of the nuclear wavepacket dynamics, capturing the complete photochemical dynamics from S2 minimum through the S1/S0 conical intersection, and finally to the dissociation. Our experimental results provide new insights into the Norrish Type I reaction and can be used to benchmark non-adiabatic dynamics simulations.

physics.chem-ph↗

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↗

arXiv2023

Transient dynamics of the phase transition in VO2 revealed by mega electron-volt ultrafast electron diffraction

Vanadium dioxide (VO2) exhibits an insulator-to-metal transition accompanied by a structural transition near room temperature. This transition can be triggered by an ultrafast laser pulse. Exotic transient states, such as a metallic state without structural transition, were also proposed. These unique characteristics let VO2 have great potential in thermal switchable devices and photonic applications. Although great efforts have been made, the atomic pathway during the photoinduced phase transition is still not clear. Here, we synthesized freestanding quasi-single-crystal VO2 films and examined their photoinduced structural phase transition with mega-electron-volt ultrafast electron diffraction. Leveraging the high signal-to-noise ratio and high temporal resolution, we observe that the disappearance of vanadium dimers and zigzag chains does not coincide with the transformation of crystal symmetry. After photoexcitation, the initial structure is strongly modified within 200 femtoseconds, resulting in a transient monoclinic structure without vanadium dimers and zigzag chains. Then, it continues to evolve to the final tetragonal structure in approximately 5 picoseconds. In addition, only one laser fluence threshold instead of two thresholds suggested in polycrystalline samples was observed in our quasi-single-crystal samples. Our findings provide new essential information for a comprehensive understanding of the photoinduced ultrafast phase transition in VO2.

cond-mat.mtrl-sci↗

arXiv2023

Femtosecond electron diffraction reveals local disorder and local anharmonicity in thermoelectric SnSe

The microscopic arrangement of atoms and molecules is the determining factor in how materials behave and perform. Beyond the long-range periodicity, the local disorder with local structures deviating from the average lattice structure plays a vital role in determining the physical properties of the phonon, electron and spin subsystems in crystalline functional materials. Experimentally characterizing the 3D atomic configuration of such local disorder and correlating it with the advanced functions remain a big challenge. Time-domain evolution of the local disorder, either static or dynamical, is lost due to the characterization at equilibrium state with conventional probing techniques. With the combination of femtosecond electron diffraction, structure factor calculation and TDDFT-MD simulation, we exclusively identify the static local disorder and the local anharmonicity of it in thermoelectric SnSe. The ultrafast structural dynamics in time domain reveal a dominant static off-symmetry displacement of Sn (~0.4 angstrom) and the anharmonicity of this local disorder induces an ultrafast atomic displacement within 100 fs after photoexcitation. The microscopic picture of the local anharmonicity indicates a direct and first signature of the THz Einstein oscillators in real space. Therefore, a glass-like thermal transport channel with the local disorder, the Einstein oscillators and the local anharmonicity, updates the fundamental insight into the long-debated ultralow thermal conductivity in SnSe. The local disorder over one to a few unit cells is pervasive and indispensable in thermoelectric materials, multiferroic materials and correlated electronic materials. Our method of revealing the 3D local disorder and the local correlated interactions by ultrafast structural dynamics will inspire broad interest in construction of the structure-property relationship in material science.

cond-mat.mtrl-sci↗

arXiv2023

Ultrafast Switching from the Charge Density Wave Phase to a Metastable Metallic State in 1T-TiSe$_2$

The ultrafast electronic structures of the charge density wave material 1T-TiSe$_2$ were investigated by high-resolution time- and angle-resolved photoemission spectroscopy. We found that the quasiparticle populations drove ultrafast electronic phase transitions in 1T-TiSe$_2$ within 100 fs after photoexcitation, and a metastable metallic state, which was significantly different from the equilibrium normal phase, was evidenced far below the charge density wave transition temperature. Detailed time- and pump-fluence-dependent experiments revealed that the photoinduced metastable metallic state was a result of the halted motion of the atoms through the coherent electron-phonon coupling process, and the lifetime of this state was prolonged to picoseconds with the highest pump fluence used in this study. Ultrafast electronic dynamics were well captured by the time-dependent Ginzburg-Landau model. Our work demonstrates a mechanism for realizing novel electronic states by photoinducing coherent motion of atoms in the lattice.

cond-mat.str-el↗

arXiv2022

Ultrafast formation of topological defects in a 2D charge density wave

Topological defects play a key role in nonequilibrium phase transitions, ranging from birth of the early universe to quantum critical behavior of ultracold atoms. In solids, transient defects are known to generate a variety of hidden orders not accessible in equilibrium, but how defects are formed at the nanometer lengthscale and femtosecond timescale remains unknown. Here, we employ an intense laser pulse to create topological defects in a 2D charge density wave, and track their morphology and dynamics with ultrafast electron diffraction. Leveraging its high temporal resolution and sensitivity in detecting weak diffuse signals, we discover a dual-stage growth of 1D domain walls within 1 ps, a process not dictated by the order parameter amplitude but instead mediated by a nonthermal population of longitudinal optical phonons. Our work provides a framework for ultrafast engineering of topological defects based on selective excitation of collective modes, opening new avenues for dynamical control of nonequilibrium phases in correlated materials.

cond-mat.mtrl-sci↗

arXiv2022

Anomalous contribution to the nematic electronic states from the structural transition in FeSe revealed by time- and angle-resolved photoemission spectroscopy

High-resolution time- and angle-resolved photoemission measurements were made on FeSe superconductors. With ultrafast photoexcitation, two critical excitation fluences that correspond to two ultrafast electronic phase transitions were found only in the $d_{yz}$-orbit-derived band near the Brillouin-zone center within our time and energy resolution. Upon comparison to the detailed temperature dependent measurements, we conclude that there are two equilibrium electronic phase transitions (at approximately 90 and 120 K) above the superconducting transition temperature, and an anomalous contribution on the scale of 10 meV to the nematic states from the structural transition is experimentally determined. Our observations strongly suggest that the electronic phase transition at 120 K must be taken into account in the energy band development of FeSe, and, furthermore, the contribution of the structural transition plays an important role in the nematic phase of iron-based high-temperature superconductors.

cond-mat.supr-con↗

arXiv2022

Advanced RF Structures for Wakefield Acceleration and High-Gradient Research

Structure wakefield acceleration (SWFA) is one of the most promising AAC schemes in several recent strategic reports, including DOE's 2016 AAC Roadmap, report on the Advanced and Novel Accelerators for High Energy Physics Roadmap (ANAR), and report on Accelerator and Beam Physics Research Goals and Opportunities. SWFA aims to raise the gradient beyond the limits of conventional radiofrequency (RF) accelerator technology, and thus the RF to beam energy efficiency, by reducing RF breakdowns from confining the microwave energy in a short (on the order of about 10 ns) and intense pulse excited by a drive beam. We envision that the following research topics, within the scope of AF7, are of great interest in the next decade: advanced wakefield structures, terahertz and sub-terahertz (THz) structures, and RF breakdown physics. Research on SWFA in the above directions would directly contribute to long-term large-scale applications, including AAC-based linear colliders and compact light sources. There is also potentially a strong synergy between SWFA and other AAC concepts, when structures are combined with plasmas into hybrid AAC schemes. Research on novel structures is at the core of advancing SWFA, and is critical to future AAC-based linear colliders; at the same, it has a strong synergy with other directions, such as cavity designs, high-power microwave systems and sources, and compact light sources.

physics.acc-ph↗

arXiv2022

Light-induced dimension crossover in 1T-TiSe$_2$ dictated by excitonic correlations

In low-dimensional systems with strong electronic correlations, the application of an ultrashort laser pulse often yields novel phases that are otherwise inaccessible. The central challenge in understanding such phenomena is to determine how dimensionality and many-body correlations together govern the pathway of a non-adiabatic transition. To this end, we examine a layered compound, 1T-TiSe$_2$, whose three-dimensional charge-density-wave (3D CDW) state also features exciton condensation due to strong electron-hole interactions. We find that photoexcitation suppresses the equilibrium 3D CDW while creating a nonequilibrium 2D CDW. Remarkably, the dimension reduction does not occur unless bound electron-hole pairs are broken. This relation suggests that excitonic correlations maintain the out-of-plane CDW coherence, settling a long-standing debate over their role in the CDW transition. Our findings demonstrate how optical manipulation of electronic interaction enables one to control the dimensionality of a broken-symmetry order, paving the way for realizing other emergent states in strongly correlated systems.

cond-mat.str-el↗

arXiv2021

A synchrotron-based kilowatt-level radiation source for EUV lithograph

A compact damping ring with limited circumference of about 160 m is proposed for producing kilowatt-level coherent EUV radiation. The electron bunch in the ring is modulated by a 257nm wavelength laser with the help of the angular dispersion induced micro-bunching method [C. Feng and Z. Zhao, Sci. Rep. 7, 4724 (2017)]. Coherent radiation at 13.5 nm with an average power of about 2.5 kW can be achieved with the state-of-the-art accelerator and laser technologies.

physics.acc-ph↗

arXiv2021

Stable and scalable multistage terahertz-driven particle accelerator

Particle accelerators that use electromagnetic fields to increase a charged particle's energy have greatly advanced the development of science and industry since invention. However, the enormous cost and size of conventional radio-frequency accelerators have limited their accessibility. Here we demonstrate a mini-accelerator powered by terahertz pulses with wavelengths 100 times shorter than radio-frequency pulses. By injecting a short relativistic electron bunch to a 30-mm-long dielectric-lined waveguide and tuning the frequency of a 20-period terahertz pulse to the phase-velocity-matched value, precise and sustained acceleration for nearly 100% of the electrons is achieved with the beam energy spread essentially unchanged. Furthermore, by accurately controlling the phase of two terahertz pulses, the beam is stably accelerated successively in two dielectric waveguides with close to 100% charge coupling efficiency. Our results demonstrate stable and scalable beam acceleration in a multistage mini-accelerator and pave the way for functioning terahertz-driven high-energy accelerators.

physics.acc-ph↗