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The kagome superconductor CsV 3 Sb 5 hosts a variety of charge density wave (CDW) phases, which play a fundamental role in the formation of other exotic electronic instabilities. However, identifying the precise structure of these CDW phases and their intricate relationships remain the subject of intense debate, due to the lack of static probes that can distinguish the CDW phases with identical spatial periodicity. Here, we unveil the out-of-equilibrium competition between two coexisting 2 × 2 × 2 CDWs in CsV 3 Sb 5 harnessing time-resolved X-ray diffraction. By analyzing the light-induced changes in the intensity of CDW superlattice peaks, we demonstrate the presence of both phases, each displaying a significantly different amount of melting upon excitation. The anomalous light-induced sharpening of peak width further shows that the phase that is more resistant to photo-excitation exhibits an increase in domain size at the expense of the other, thereby showcasing a hallmark of phase competition. Our results not only shed light on the interplay between the multiple CDW phases in CsV 3 Sb 5 , but also establish a non-equilibrium framework for comprehending complex phase relationships that are challenging to disentangle using static techniques., (© 2024. The Author(s).)

A polariton is a fundamental quasiparticle that arises from strong light-matter interaction and as such has attracted wide scientific and practical interest. When light is strongly coupled to the crystal lattice, it gives rise to phonon-polaritons (PPs), which have been proven useful in the dynamical manipulation of quantum materials and the advancement of terahertz technologies. Yet, current detection and characterization methods of polaritons are still limited. Traditional techniques such as Raman or transient grating either rely on fine-tuning of external parameters or complex phase extraction techniques. To overcome these inherent limitations, we propose and demonstrate a technique based on a time-of-flight measurement of PPs. We resonantly launch broadband PPs with intense terahertz fields and measure the time-of-flight of each spectral component with time-resolved second harmonic generation. The time-of-flight information, combined with the PP attenuation, enables us to resolve the real and imaginary parts of the PP dispersion relation. We demonstrate this technique in the van der Waals magnets NiI 2 and MnPS 3 and reveal a hidden magnon-phonon interaction. We believe that this approach will unlock new opportunities for studying polaritons across diverse material systems and enhance our understanding of strong light-matter interaction., (© 2024. The Author(s).)

The interplay between a multitude of electronic, spin, and lattice degrees of freedom underlies the complex phase diagrams of quantum materials. Layer stacking in van der Waals (vdW) heterostructures is responsible for exotic electronic and magnetic properties, which inspires stacking control of two-dimensional magnetism. Beyond the interplay between stacking order and interlayer magnetism, we discover a spin-shear coupling mechanism in which a subtle shear of the atomic layers can have a profound effect on the intralayer magnetic order in a family of vdW antiferromagnets. Using time-resolved X-ray diffraction and optical linear dichroism measurements, interlayer shear is identified as the primary structural degree of freedom that couples with magnetic order. The recovery times of both shear and magnetic order upon optical excitation diverge at the magnetic ordering temperature with the same critical exponent. The time-dependent Ginzburg-Landau theory shows that this concurrent critical slowing down arises from a linear coupling of the interlayer shear to the magnetic order, which is dictated by the broken mirror symmetry intrinsic to the monoclinic stacking. Our results highlight the importance of interlayer shear in ultrafast control of magnetic order via spin-mechanical coupling., (© 2022. The Author(s).)

In van der Waals (vdW) materials, strong coupling between different degrees of freedom can hybridize elementary excitations into bound states with mixed character 1-3 . Correctly identifying the nature and composition of these bound states is key to understanding their ground state properties and excitation spectra 4,5 . Here, we use ultrafast spectroscopy to reveal bound states of d-orbitals and phonons in 2D vdW antiferromagnet NiPS 3 . These bound states manifest themselves through equally spaced phonon replicas in frequency domain. These states are optically dark above the Néel temperature and become accessible with magnetic order. By launching this phonon and spectrally tracking its amplitude, we establish the electronic origin of bound states as localized d-d excitations. Our data directly yield electron-phonon coupling strength which exceeds the highest known value in 2D systems 6 . These results demonstrate NiPS 3 as a platform to study strong interactions between spins, orbitals and lattice, and open pathways to coherent control of 2D magnets., (© 2022. The Author(s).)

Collective excitations of bound electron-hole pairs-known as excitons-are ubiquitous in condensed matter, emerging in systems as diverse as band semiconductors, molecular crystals, and proteins. Recently, their existence in strongly correlated electron materials has attracted increasing interest due to the excitons' unique coupling to spin and orbital degrees of freedom. The non-equilibrium driving of such dressed quasiparticles offers a promising platform for realizing unconventional many-body phenomena and phases beyond thermodynamic equilibrium. Here, we achieve this in the van der Waals correlated insulator NiPS 3 by photoexciting its newly discovered spin-orbit-entangled excitons that arise from Zhang-Rice states. By monitoring the time evolution of the terahertz conductivity, we observe the coexistence of itinerant carriers produced by exciton dissociation and a long-wavelength antiferromagnetic magnon that coherently precesses in time. These results demonstrate the emergence of a transient metallic state that preserves long-range antiferromagnetism, a phase that cannot be reached by simply tuning the temperature. More broadly, our findings open an avenue toward the exciton-mediated optical manipulation of magnetism., (© 2021. The Author(s).)

High harmonic generation of ultrafast laser pulses can be used to perform angle-resolved photoemission spectroscopy (ARPES) to map the electronic band structure of materials with femtosecond time resolution. However, currently it is difficult to reach high momenta with narrow energy resolution. Here, we combine a gas phase extreme ultraviolet (XUV) femtosecond light source, an XUV monochromator, and a time-of-flight electron analyzer to develop XUV-based time-resolved ARPES. Our technique can produce tunable photon energy between 24-33 eV with an unprecedented energy resolution of 30 meV and time resolution of 200 fs. This technique enables time-, energy- and momentum-resolved investigation of the nonequilibrium dynamics of electrons in materials with a full access to their first Brillouin zone. We evaluate the performance of this setup through exemplary measurements on various quantum materials, including WTe 2 , WSe 2 , TiSe 2 , and Bi 2 Sr 2 CaCu 2 O 8+δ .

When the Fermi level is aligned with the Dirac point of graphene, reduced charge screening greatly enhances electron-electron scattering 1-5 . In an optically excited system, the kinematics of electron-electron scattering in Dirac fermions is predicted to give rise to novel optoelectronic phenomena 6-11 . In this paper, we report on the observation of an intrinsic photocurrent in graphene, which occurs in a different parameter regime from all the previously observed photothermoelectric or photovoltaic photocurrents in graphene 12-20 : the photocurrent emerges exclusively at the charge neutrality point, requiring no finite doping. Unlike other photocurrent types that are enhanced near p-n or contact junctions, the photocurrent observed in our work arises near the edges/corners. By systematic data analyses, we show that the phenomenon stems from the unique electron-electron scattering kinematics in charge-neutral graphene. Our results not only highlight the intriguing electron dynamics in the optoelectronic response of Dirac fermions, but also offer a new scheme for photodetection and energy harvesting applications based on intrinsic, charge-neutral Dirac fermions.

When a topological insulator (TI) is in contact with a ferromagnet, both time-reversal and inversion symmetries are broken at the interface. An energy gap is formed at the TI surface, and its electrons gain a net magnetic moment through short-range exchange interactions. Magnetic TIs can host various exotic quantum phenomena, such as massive Dirac fermions, Majorana fermions, the quantum anomalous Hall effect and chiral edge currents along the domain boundaries. However, selective measurement of induced magnetism at the buried interface has remained a challenge. Using magnetic second-harmonic generation, we directly probe both the in-plane and out-of-plane magnetizations induced at the interface between the ferromagnetic insulator (FMI) EuS and the three-dimensional TI Bi2Se3. Our findings not only allow characterizing magnetism at the TI-FMI interface but also lay the groundwork for imaging magnetic domains and domain boundaries at the magnetic TI surfaces.

Breaking space-time symmetries in two-dimensional crystals can markedly influence their macroscopic electronic properties. Monolayer transition metal dichalcogenides (TMDs) are prime examples where the intrinsically broken crystal inversion symmetry permits the generation of valley-selective electron populations, even though the two valleys are energetically degenerate, locked by time-reversal symmetry. Lifting the valley degeneracy in these materials is of great interest because it would allow for valley-specific band engineering and offer additional control in valleytronic applications. Although applying a magnetic field should, in principle, accomplish this task, experiments so far have not shown valley-selective energy level shifts in fields accessible in the laboratory. Here, we show the first direct evidence of lifted valley degeneracy in the monolayer TMD WS2. By applying intense circularly polarized light, which breaks time-reversal symmetry, we demonstrate that the exciton level in each valley can be selectively tuned by as much as 18 meV through the optical Stark effect. These results offer a new way to control the valley degree of freedom, and may provide a means to realize new Floquet topological phases in two-dimensional TMDs.