arXiv subjects

Qiaomei Liu

Publications and source records attributed to Qiaomei Liu.

15 recordsLinked to original sources

arXiv2026

Sublattice-resolved coherent phonon dynamics in charge density waves

Phonons govern fundamental material properties and play a central role in various electronic phase transitions. Coherent driving of specific phonon modes enables on-demand phase control, motivating sublattice-resolved identification of real-space phonon motions. Yet experimentally resolving these motions remains challenging, limiting precise phonon-based control. Here, we introduce a dynamical protocol to track element-resolved phonon dynamics in the charge density wave material EuTe4, in which the dominant Te-sublattice charge order is accompanied by a previously unreported Eu-sublattice component. We leverage the elemental selectivity of time-resolved resonant X-ray scattering to reveal three coherent phonon modes with distinct sublattice character, thereby disentangling Eu- and Te-dominated lattice dynamics, in good agreement with theoretical calculations of the phonon eigenvectors. This time-domain approach, which surpasses the energy-resolution limits of conventional frequency-domain inelastic scattering, provides a broadly applicable framework for decomposing coherent phonons in multi-element materials, which is crucial for the targeted control of phases of matter.

cond-mat.mtrl-sci↗

arXiv2026

Dynamics of a jointly commensurate moiré charge density wave

The advent of two-dimensional moiré systems has revolutionized the exploration of phenomena arising from strong correlations and nontrivial band topology. Recently, a moiré 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 moiré 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 moiré 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 moiré quantum materials through defect control.

cond-mat.str-el↗

arXiv2026

Ultrafast giant enhancement of second harmonic generation in a strongly correlated cobaltite

In quantum materials, nonlinear optical responses are highly sensitive to electronic structure and many-body interactions. Probing and manipulating such nonlinear processes is a complex and subtle endeavor, yet it offers deep insights into emerging physics and functionalities. Here, we report an anomalous ultrafast enhancement of second harmonic generation (SHG) in a strongly correlated cobaltite YbBaCo$_4$O$_7$. Above-bandgap femtosecond pumping increases SHG intensity by up to 60 % within 200 fs, with the enhancement persisting for tens of picoseconds. The enhancement is strongly anisotropic, with substantial amplification of in-plane susceptibility tensors, whereas the out-of-plane counterpart shows negligible change. We attribute these anomalies to ultrafast photodoping-induced modulation of the on-site Coulomb repulsion, which dynamically renormalizes the band structure and selectively amplifies specific $χ^{(2)}$ components. These nonlinear dynamics encode rich information about the orbital symmetries and energies of the states involved, opening new avenues for all-optical probing of electronic structure in strongly correlated materials.

cond-mat.str-el↗

arXiv2026

Coherent seeding and control of dynamical ferroelectricity by phonon anharmonicity

Optical control of quantum materials has progressed along two separate directions: creating non-equilibrium states inaccessible at equilibrium, and coherently controlling ultrafast dynamics with multi-pulse protocols. Ferroelectricity is especially attractive in this context because its order parameter, macroscopic polarization, directly links inversion-symmetry breaking to functional response. Yet light-induced ferroelectricity has so far been confined to quantum paraelectrics near the ferroelectric instability, where critical fluctuations obscure the formation of a homogeneous ferroelectric state and complicate its deterministic coherent control. Unifying these capabilities -- preparing a symmetry-broken state and then coherently steering its functionality -- remains a central challenge. Here we show that intense terahertz excitation of a soft phonon mode induces a ferroelectric state in centrosymmetric PbTe, a thermoelectric material with strong lattice anharmonicity but no ferroelectric transition at finite temperature. The light-induced symmetry-broken state can be realized up to about 100 K, without relying on local dipolar fluctuations. Experiment and theory together reveal that terahertz-driven anharmonic coupling between degenerate transverse optical phonons underlies this ferroelectric induction. Furthermore, we demonstrate coherent amplification and suppression of the induced polarization via a double-pulse-excitation protocol. These results establish terahertz-driven anharmonic mode coupling as a general strategy for controlling mode-mediated functionalities in quantum materials, opening a route to ultrafast information processing.

cond-mat.mtrl-sci↗

arXiv2026

Room-temperature multistage metastability in a moiré 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 moiré 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 moiré superstructure. Our findings not only provide critical insights into metastable phenomena in moiré 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

Efficient high-harmonic generation in van der Waals ferroelectric NbOI$_2$ crystals

Layered NbOX$_2$ ($X=\mathrm{Cl,\,Br,\,I}$), a member of the van der Waals ferroelectric family, exhibits intrinsic ferroelectricity and pronounced nonlinear optical responses, making it a promising candidate for integrated nanophotonics applications. While previous studies have emphasized the material's strong second-order nonlinear responses, higher-order nonlinear responses are still mostly unexplored. This work systematically investigates NbOI$_2$ using high harmonic generation (HHG) spectroscopy. Driven by an intense mid-infrared laser field centered at $\sim4~μ\mathrm{m}$ wavelength, highly anisotropic odd- and even-order harmonics up to the 16th order are generated at a low peak intensity of $0.4~\mathrm{TW\,cm^{-2}}$, extending beyond the material's bandgap. Both bulk and flake forms of NbOI$_2$ display pronounced harmonic emission from the near-infrared to the deep-ultraviolet spectral region, with a notably high overall conversion efficiency compared to other known materials. Polarization-resolved measurements reveal that even-order harmonics remain aligned with the crystal polar axis regardless of the driving-field orientation, whereas odd-order harmonics are dynamically affected. First-principles calculations suggest that the flat valence band associated with Peierls dimerization enhances HHG efficiency through electron correlation. These findings provide fresh perspectives on HHG in van der Waals ferroelectric materials and facilitate the development of compact and tunable quantum light sources.

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

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

Large moiré superstructure of stacked incommensurate charge density waves

Recent advances in van der Waals heterostructures have opened the new frontier of moiré 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 moiré engineering to materials that host incommensurate orders, where we discovered a long-period, thermally-hysteretic moiré 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 moiré superstructure with an in-plane period of 13.6~nm. Due to different out-of-plane orders of the incommensurate CDWs, the moiré 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 moiré 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↗

arXiv2024

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

Revealing the frequency-dependent oscillations in the nonlinear terahertz response induced by the Josephson current

Nonlinear responses of superconductors to intense terahertz radiation has been an active research frontier. Using terahertz pump-terahertz probe spectroscopy, we investigate the c-axis nonlinear optical response of a high-temperature superconducting cuprate. After excitation by a single-cycle terahertz pump pulse, the reflectivity of the probe pulse oscillates as the pump-probe delay is varied. Interestingly, the oscillatory central frequency scales linearly with the probe frequency, a fact widely overlooked in pump-probe experiments. By theoretically solving the nonlinear optical reflection problem on the interface, we show that our observation is well explained by the Josephson-type third-order nonlinear electrodynamics, together with the emission coefficient from inside the material into free space. The latter results in a strong enhancement of the emitted signal whose physical frequency is around the Josephson plasma edge. Our result offers a benchmark for and new insights into strong-field terahertz spectroscopy of related quantum materials.

cond-mat.supr-con↗

arXiv2023

Pump-induced terahertz conductivity response and peculiar bound state in Mn3Si2Te6

We report the significant enhancement on ultrafast terahertz optical conductivity and the unexpected formation of a polaronic-like state in semiconductor Mn3Si2Te6 at room temperature. With the absorption of pump photons, the low-frequency terahertz photoconductivity spectrum exhibits a significant rise, quickly forming a broad peak and subsequently shifting to higher energy. The short-lived nature of the broad peak, as well as the distribution of optical constants, strongly points towards a transient polaron mechanism. Our study not only provides profound insights into the remarkable photoelectric response of Mn3Si2Te6 but also highlights its significant potential for future photoelectric applications.

cond-mat.mtrl-sci↗

arXiv2023

Giant nonlinear optical wave mixing in van der Waals compound MnPSe3

Optical nonlinearities, one of the most fascinating properties of two-dimensional (2D) materials, are essential for exploring novel physics in 2D systems and developing next-generation nonlinear optical applications. While tremendous efforts have been made to discover and optimize second-order nonlinear optical responses in various 2D materials, higher odd-order nonlinear processes, which are in general much less efficient than second order ones, have been paid less attention despite their scientific and applicational significance. Here we report giant odd-order nonlinear optical wave mixing in a correlated van der Waals insulator MnPSe3 at room temperature. Illuminated by two near-infrared femtosecond lasers simultaneously, it generates a series of degenerate and non-degenerate four- and six-wave mixing outputs, with conversion efficiencies up to the order of $10^{-4}$ and $10^{-6}$ for the four- and six-wave mixing processes, respectively, far exceeding the efficiencies of several prototypical nonlinear optical materials (GaSe, LiNbO3). This work highlights the intriguing prospect of transition metal phosphorous trichalcogenides for future research of the nonlinear light matter interactions in 2D systems and for potential nonlinear photonic applications.

physics.optics↗

arXiv2023

Optical spectroscopy and band structure calculations of structural phase transition in the Vanadium-based kagome metal ScV$_6$Sn$_6$

In condensed matter physics, materials with kagome lattice display a range of exotic quantum states, including charge density wave (CDW), superconductivity and magnetism. Recently, the intermetallic kagome metal ScV6Sn6 was discovered to undergo a first-order structural phase transition with the formation of a root3xroot3x3 CDW at around 92 K. The bulk electronic band properties are crucial to understanding the origin of the structural phase transition. Here, we conducted an optical spectroscopy study in combination with band structure calculations across the structural transition. Our findings showed abrupt changes in the optical reflectivity/conductivity spectra as a result of the structural transition, without any observable gap formation behavior. The optical measurements and band calculations actually reveal a sudden change of the band structure after transition. It is important to note that this phase transition is of the first-order type, which distinguishes it from conventional density-wave type condensations. Our results provide an insight into the origin of the structural phase transition in this new and unique kagome lattice.

cond-mat.str-el↗

arXiv2022

Strong nonlinear optical response and transient symmetry switching in Type-II Weyl semimetal $β$-WP2

The topological Weyl semimetals with peculiar band structure exhibit novel nonlinear optical enhancement phenomena even for light at optical wavelengths. While many intriguing nonlinear optical effects were constantly uncovered in type-I semimetals, few experimental works focused on basic nonlinear optical properties in type-II Weyl semimetals. Here we perform a fundamental static and time-resolved second harmonic generation (SHG) on the three dimensional Type-II Weyl semimetal candidate $β$-WP$_2$. Although $β$-WP$_2$ exhibits extremely high conductivity and an extraordinarily large mean free path, the second harmonic generation is unscreened by conduction electrons, we observed rather strong SHG response compared to non-topological polar metals and archetypal ferroelectric insulators. Additionally, our time-resolved SHG experiment traces ultrafast symmetry switching and reveals that polar metal $β$-WP$_2$ tends to form inversion symmetric metastable state after photo-excitation. Intense femtosecond laser pulse could optically drive symmetry switching and tune nonlinear optical response on ultrafast timescales although the interlayer coupling of $β$-WP$_2$ is very strong. Our work is illuminating for the polar metal nonlinear optics and potential ultrafast topological optoelectronic applications.

cond-mat.mtrl-sci↗