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In 1964, Keldysh laid the groundwork for strong-field physics in atomic, molecular, and solid-state systems by delineating a ubiquitous transition from multiphoton absorption to quantum electron tunneling under intense AC driving forces. While both processes in semiconductors can generate carriers and result in photon emission through electron-hole recombination, the low quantum yields in most materials have hindered direct observation of the Keldysh crossover. Leveraging the large quantum yields of photoluminescence in lead halide perovskites, we show that we can not only induce bright light emission from extreme sub-bandgap light excitation but also distinguish between photon-induced and electric-field-induced processes. Our results are rationalized by the Landau-Dykhne formalism, providing insights into the non-equilibrium dynamics of strong-field light-matter interactions. These findings open new avenues for light upconversion and sub-bandgap photon detection, highlighting the potential of lead halide perovskites in advanced optoelectronic applications.

Floquet engineering is a novel method of manipulating quantum phases of matter via periodic driving [1, 2]. It has successfully been utilized in different platforms ranging from photonic systems [3] to optical lattice of ultracold atoms [4, 5]. In solids, light can be used as the periodic drive via coherent light-matter interaction. This leads to hybridization of Bloch electrons with photons resulting in replica bands known as Floquet-Bloch states. After the direct observation of Floquet-Bloch states in a topological insulator [6], their manifestations have been seen in a number of other experiments [7-14]. By engineering the electronic band structure using Floquet-Bloch states, various exotic phase transitions have been predicted [15-22] to occur. To realize these phases, it is necessary to better understand the nature of Floquet-Bloch states in different materials. However, direct energy and momentum resolved observation of these states is still limited to only few material systems [6, 10, 14, 23, 24]. Here, we report direct observation of Floquet-Bloch states in monolayer epitaxial graphene which was the first proposed material platform [15] for Floquet engineering. By using time- and angle-resolved photoemission spectroscopy (trARPES) with mid-infrared (mid-IR) pump excitation, we detected replicas of the Dirac cone. Pump polarization dependence of these replica bands unequivocally shows that they originate from the scattering between Floquet-Bloch states and photon-dressed free-electron-like photoemission final states, called Volkov states. Beyond graphene, our method can potentially be used to directly observe Floquet-Bloch states in other systems paving the way for Floquet engineering in a wide range of quantum materials.

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., Comment: To appear in PRL

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 competition between two coexisting $2\times2\times2$ 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., Comment: 10 pages, 4 figures with supplemental Material

The control of antiferromagnets with ultrashort optical pulses has emerged as a prominent field of research. Tailored laser excitation can launch coherent spin waves at terahertz frequencies, yet a comprehensive description of their generation mechanisms is still lacking despite extensive efforts. Using terahertz emission spectroscopy, we investigate the generation of a coherent magnon mode in the van der Waals antiferromagnet NiPS$_3$ under a range of photoexcitation conditions. By tuning the pump photon energy from transparency to resonant with a $d$-$d$ transition, we reveal a striking change in the coherent magnon's dependence on the pump polarization, indicating two distinct excitation mechanisms. Our findings provide a strategy for the manipulation of magnetic modes via photoexcitation around sub-gap electronic states., Comment: 15 pages, 14 figures

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 ultrafast electronic devices of the future. However, the ability to induce long-lasting metastable electronic states yet in a fully reversible manner is a long standing challenge. Here, by using ultrafast laser excitation with distinct pulse sequences and fluences, we were able to regulate the symmetry and electronic properties in a polar charge-density-wave material EuTe4. We demonstrated the capability of nonvolatile writing and erasing the polar order, a process that is completely reversible and is achieved at room temperature in an all optical manner. Each induced state brings about modifications to the electric resistance and second harmonic generation intensity. The results point to a distinct dynamical symmetry inversion mechanism in which photoexcitation mediates the polar phases of long-range electronic order. Our finding extends the scope of nonvolatile all-optical control of electronic states to ambient conditions, thus providing possibilities for applications in ultrafast optoelectronics.

Atomically thin transition metal dichalcogenides can exhibit markedly different electronic properties compared to their bulk counterparts. In the case of NbSe$_2$, the question of whether its charge density wave (CDW) phase is enhanced in the monolayer limit has been the subject of intense debate, primarily due to the difficulty of decoupling this order from its environment. Here, we address this challenge by using a misfit crystal that comprises NbSe$_2$ monolayers separated by SnSe rock-salt spacers, a structure that allows us to investigate a monolayer crystal embedded in a bulk matrix. We establish an effective monolayer electronic behavior of the misfit crystal by studying its transport properties and visualizing its electronic structure by angle-resolved photoemission measurements. We then investigate the emergence of the CDW by tracking the temperature dependence of its collective modes. Our findings reveal a nearly sixfold enhancement in the CDW transition temperature, providing compelling evidence for the profound impact of dimensionality on charge order formation in NbSe$_2$.

Sr$_2$IrO$_4$ has attracted a lot of attention due to its structural and electronic similarities to La$_2$CuO$_4$ which is the parent compound of high-T$_c$ superconducting cuprates. It was proposed to be a strong spin-orbit coupled J$_{eff}$ = 1/2 Mott insulator, but the Mott nature of its insulating ground state and the origin of the gap have not been conclusively established. Here, we use ultrafast laser pulses to realize an insulator-metal transition in Sr$_2$IrO$_4$ and probe the resulting dynamics using time- and angle-resolved photoemission spectroscopy. We observe a closing of the gap and the formation of weakly-renormalized electronic bands in the gap region. Comparing these observations to the expected temperature and doping evolution of Mott gaps and Hubbard bands provides clear evidence that the insulating state does not originate from Mott correlations. We instead propose a correlated band insulator picture, where antiferromagnetic correlations play a key role in the opening of the gap. More broadly, our results demonstrate that energy-momentum resolved nonequilibrium dynamics can be used to clarify the nature of equilibrium states in correlated materials.

Strong interactions between different degrees of freedom lead to exotic phases of matter with complex order parameters and emergent collective excitations. Conventional techniques, such as scattering and transport, probe the amplitudes of these excitations, but they are typically insensitive to phase. Therefore, novel methods with phase sensitivity are required to understand ground states with phase modulations and interactions that couple to the phase of collective modes. Here, by performing phase-resolved coherent phonon spectroscopy (CPS), we reveal a hidden spin-lattice coupling in a vdW antiferromagnet FePS$_{3}$ that eluded other phase-insensitive conventional probes, such as Raman and X-ray scattering. With comparative analysis and analytical calculations, we directly show that the magnetic order in FePS$_{3}$ selectively couples to the trigonal distortions through partially filled t$_{2g}$ orbitals. This magnetoelastic coupling is linear in magnetic order and lattice parameters, rendering these distortions inaccessible to inelastic scattering techniques. Our results not only capture the elusive spin-lattice coupling in FePS$_3$, but also establish phase-resolved CPS as a tool to investigate hidden interactions., Comment: 6 pages, 4 figures

A new group of kagome metals AV$_3$Sb$_5$ (A = K, Rb, Cs) exhibit a variety of intertwined unconventional electronic phases, which emerge from a puzzling charge density wave phase. Understanding of this parent charge order phase is crucial for deciphering the entire phase diagram. However, the mechanism of the charge density wave is still controversial, and its primary source of fluctuations - the collective modes - have not been experimentally observed. Here, we use ultrashort laser pulses to melt the charge order in CsV$_3$Sb$_5$ and record the resulting dynamics using femtosecond angle-resolved photoemission. We resolve the melting time of the charge order and directly observe its amplitude mode, imposing a fundamental limit for the fastest possible lattice rearrangement time. These observations together with ab-initio calculations provide clear evidence for a structural rather than electronic mechanism of the charge density wave. Our findings pave the way for better understanding of the unconventional phases hosted on the kagome lattice., Comment: 17 pages, 4 figures

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., Comment: 14 pages, 15 figures, including supplemental material

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.

Electron-lattice coupling effects in low dimensional materials give rise to charge density wave (CDW) order and phase transitions. These phenomena are critical ingredients for superconductivity and predominantly occur in metallic model systems such as doped cuprates, transition metal dichalcogenides, and more recently, in Kagome lattice materials. However, CDW in semiconducting systems, specifically at the limit of low carrier concentration region, is uncommon. Here, we combine electrical transport, synchrotron X-ray diffraction and optical spectroscopy to discover CDW order in a quasi-one-dimensional (1D), dilute d-band semiconductor, BaTiS3, which suggests the existence of strong electron-phonon coupling. The CDW state further undergoes an unusual transition featuring a sharp increase in carrier mobility. Our work establishes BaTiS3 as a unique platform to study the CDW physics in the dilute filling limit to explore novel electronic phases.

We report a transport, thermodynamic, and spectroscopic study of the recently identified topological semiconductor ZrTe$_5$ with a focus on elucidating the connections between its band structure and unusual thermoelectric properties. Using time and angle resolved photoemission spectroscopy (tr-ARPES) we observe a small electronic band gap and temperature dependent Fermi level which traverses from a single valence to conduction band with lowering temperature, consistent with previous reports. This low temperature Fermi surface closely matches that derived from quantum oscillations, suggesting it is reflective of the bulk electronic structure. The Seebeck and low field Nernst response is characterized by an unusually large and non-monotonic temperature evolution. We find this can be quantitatively explained using a semiclassical model based on the observed band character and a linear temperature shifting of the Fermi level. Additionally, we observe a large, non-saturating enhancement of both thermoelectric coefficients in magnetic field. We show this can be captured by the Zeeman energy associated with a large effective $g$-factor of 25.8 consistent with that derived from Lifshitz-Kosevich analysis of the quantum oscillations. Together these observations provide a comprehensive picture of ZrTe$_{5}$ as a model high mobility semiconductor and potential platform for significant magnetic field driven thermoelectricity., Comment: 10 pages, 4 figures

In van der Waals (vdW) materials, strong coupling between different degrees of freedom can hybridize elementary excitations into bound states with mixed character. Correctly identifying the nature and composition of these bound states is key to understanding their ground state properties and excitation spectra. Here, we use ultrafast spectroscopy to reveal bound states of d-orbitals and phonons in 2D vdW antiferromagnet NiPS3. These bound states manifest themselves through equally spaced phonon replicas in frequency domain. These states are optically dark above the N\'eel 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. These results demonstrate NiPS3 as a platform to study strong interactions between spins, orbitals and lattice, and open pathways to coherent control of 2D magnets.

Charge-density-wave order in a solid can be temporarily "melted" by a strong laser pulse. Here we use the discrete Gross-Pitaevskii equation on a cubic lattice to simulate the recovery of the CDW long-range phase coherence following such a pulse. Our simulations indicate that the recovery process is dramatically slowed down by the three-dimensional topological defects - CDW dislocations - created as a result of strongly nonequilibrium heating and cooling of the system. Overall, the simulated CDW recovery was found to be remarkably reminiscent of a recent pump-probe experiment in LaTe$_3$., Comment: v2. Main text: 5 pages, 4 figures. Supplemental Material: 7 pages, 8 figures

Continuous and concerted development of colloidal quantum-dot light-emitting diodes over the past two decades has established them as a bedrock technology for the next generation of displays. However, a fundamental issue that limits the performance of these devices is the quenching of photoluminescence due to excess charges from conductive charge transport layers. Although device designs have leveraged various workarounds, doing so often comes at the cost of limiting efficient charge injection. Here we demonstrate that high-field terahertz (THz) pulses can dramatically brighten quenched QDs on metallic surfaces, an effect which persists for minutes after THz irradiation. This phenomenon is attributed to the ability of the THz field to remove excess charges, thereby reducing trion and non-radiative Auger recombination. Our findings show that THz technologies can be used to suppress and control such undesired non-radiative decay, potentially in a variety of luminescent materials for future device applications., Comment: 28 pages, 4 figures

Engineering novel states of matter with light is at the forefront of materials research. An intensely studied direction is to realize broken-symmetry phases that are "hidden" under equilibrium conditions but can be unleashed by an ultrashort laser pulse. Despite a plethora of experimental discoveries, the nature of these orders and how they transiently appear remain unclear. To this end, we investigate a nonequilibrium charge density wave (CDW) in rare-earth tritellurides, which is suppressed in equilibrium but emerges after photoexcitation. Using a pump-pump-probe protocol implemented in ultrafast electron diffraction, we demonstrate that the light-induced CDW consists solely of order parameter fluctuations, which bear striking similarities to critical fluctuations in equilibrium despite differences in the length scale. By calculating the dynamics of CDW fluctuations in a nonperturbative model, we further show that the strength of the light-induced order is governed by the amplitude of equilibrium fluctuations. These findings highlight photoinduced fluctuations as an important ingredient for the emergence of transient orders out of equilibrium. Our results further suggest that materials with strong fluctuations in equilibrium are promising platforms to host "hidden" orders after laser excitation.