Single-shot electro-optic sampling (EOS) is a powerful method enabling the measurement of weak terahertz signals that would otherwise require prohibitively long acquisition times. This is generally achieved by encoding the EOS time delay into a spatial, angular, or frequency coordinate. In general, angular-encoding techniques operate well up to 3 THz but become more challenging for larger bandwidths, due to dispersion and imaging imperfections. Here, we demonstrate a reliable angular-encoding single-shot EOS implementation that reaches frequencies beyond 6 THz. Diffraction simulations are used to design the experimental setup and adapt this technique to commercial reflection gratings, removing the need for custom-built echelon mirrors. Furthermore, we show that, contrary to earlier reports, group delay dispersion from angular dispersion does not reduce the bandwidth of single-shot EOS.

Is it feasible to alter the ground-state properties of a material by engineering its electromagnetic environment? Inspired by theoretical predictions1-12, experimental realizations of such cavity-controlled properties without optical excitation are beginning to emerge13-19. Here we devised and implemented a new platform to realize cavity-altered materials. Single crystals of hyperbolic van der Waals (vdW) compounds provide a resonant electromagnetic environment with enhanced density of photonic states and prominent mode confinement20-24. We interfaced hexagonal boron nitride (hBN) with the molecular superconductor κ-(BEDT-TTF)2Cu[N(CN)2]Br (κ-ET). The frequencies of infrared hyperbolic modes (HMs) of hBN (refs. 25,26) match the infrared-active carbon-carbon (C=C) stretching molecular resonance of κ-ET implicated in superconductivity27. Nano-optical data supported by first-principles molecular Langevin dynamics simulations confirm the presence of resonant coupling between the hBN hyperbolic cavity modes and the C=C stretching mode in κ-ET. Meissner-effect measurements using magnetic force microscopy (MFM) demonstrate a strong suppression of superfluid density near the hBN/κ-ET interface. Non-resonant control heterostructures, including RuCl3/κ-ET and hBN/Bi2Sr2CaCu2O8+x (BSCCO), do not show the pronounced superfluid suppression. These observations suggest that hBN/κ-ET realizes a cavity-altered superconducting ground state. Our work highlights the potential of dark cavities devoid of external photons for engineering electronic ground-state properties of complex quantum materials.

High temperature superconductivity is typically associated with strong coupling and a large superconducting gap, yet these characteristics have not been demonstrated in the nickelates. Here, we provide experimental evidence that Eu substitution in the spacer layer of Nd1-xEuxNiO2 (NENO) thin films enhances the superconducting gap, driving the system toward a strong-coupling regime. This is accompanied by a magnetic-exchange-driven magnetic-field-enhanced superconductivity. We investigate the upper critical magnetic field, Hc2, and the superconducting gap of superconducting NENO thin films with x = 0.2 to 0.35. Magnetoresistance measurements reveal magnetic-field-enhanced superconductivity in NENO films. We interpret this phenomenon as a result of an interaction between magnetic Eu ions and superconducting states in the Ni dx2-y2 orbital. The upper critical magnetic field strongly violates the weak-coupling Pauli limit. Infrared spectroscopy confirms a large gap-to-Tc ratio 2 Δ / k B T c ≃ 5 - 6 , indicating a stronger coupling pairing mechanism in NENO relative to the Sr-doped NdNiO2. The substitution of Eu in the rare-earth layer causes pronounced modifications of the superconducting gap and magnetic interactions in Nd-based nickelates, opening new pathways to engineer high-Tc superconductivity in infinite-layer nickelates.

A long-standing challenge in ultrafast magnetism and functional materials research, in general, has been the generation of a universal, ultrafast stimulus able to switch between stable magnetic states. Solving this problem would open up many new opportunities for fundamental studies, potentially impacting future data storage technologies. Ideally, step-like magnetic field transients with infinitely fast rise time would serve this purpose. Here we develop a new approach to generate ultrafast magnetic field steps by quenching supercurrents in a superconductor. We achieve magnetic field steps with millitesla amplitude, picosecond rise times and slew rates approaching 1 GT s-1. We test the potential of this technique by coherently rotating the magnetization in a ferrimagnet. Although in the current geometry, the magnetic field step is not sufficient to achieve complete switching, suitable improvements in the device geometry could make these magnetic steps both larger and faster. We foresee new applications ranging from quenches across phase transitions to complete switching of magnetic order parameters.

Signatures of photo-induced superconductivity have been reported in cuprate materials subjected to a coherent phonon drive. A 'cold' superfluid was extracted from the transient Terahertz conductivity and was seen to coexist with 'hot' uncondensed quasi-particles, a hallmark of a driven-dissipative system of which the interplay between coherent and incoherent responses are not well understood. Here, time resolved spontaneous Raman scattering was used to probe the lattice temperature in the photo-induced superconducting state of YBa2Cu3O6.48. An increase in lattice temperature of approximately 80 K was observed by measuring the time dependent Raman scattering intensity of an undriven 'spectator' phonon mode. This is to be compared with an estimated increase in quasi-particle temperatures of nearly 200 K. These temperature changes provide quantitative information on the nature of the driven state and its decay, and may provide a strategy to optimize this effect.

Motivated by recent experiments that observed low-frequency second-order optical responses in doped striped superconductors, here we investigate the nonlinear electrodynamics of systems exhibiting a charge density wave (CDW) order parameter. Due to the Bragg scattering off the CDW order, an incoming spatially homogeneous electric field in addition to zero momentum current generates Umklapp currents that are modulated in space at momenta of the reciprocal CDW lattice. In particular, here we predict and microscopically evaluate the Umklapp shift current, a finite momentum analog of the regular shift current which represents the second-order optical process that downconverts homogeneous AC electric field into low-frequency, zero momentum current. Specifically, we evaluate real-time response functions within mean-field theory via the Keldysh technique and use the Peierls substitution to compute observables at finite momenta in lattice models. We find that systems with certain lattice symmetries (such as inversion symmetry), where the regular shift current is disallowed, may give rise to the Umklapp one. We apply our framework to investigate lattice symmetries in layered materials with helical-like stripes and show that both types of shift currents provide insight into the nature of intertwined phases of matter. Finally, we discuss the relation of our findings to recent experiments in striped superconductors.

Crystal lattice fluctuations, which are known to influence phase transitions of quantum materials in equilibrium, are also expected to determine the dynamics of light-induced phase changes. However, they have only rarely been explored in these dynamical settings. Here we study the time evolution of lattice fluctuations in the quantum paraelectric SrTiO 3 , in which mid-infrared drives have been shown to induce a metastable ferroelectric state. Crucial in these physics is the competition between polar instabilities and antiferrodistortive rotations, which in equilibrium frustrate the formation of long-range ferroelectricity. We make use of high-intensity mid-infrared optical pulses to resonantly drive the Ti–O-stretching mode at 17 THz, and we measure the resulting change in lattice fluctuations using time-resolved X-ray diffuse scattering at a free-electron laser. After a prompt increase, we observe a long-lived quench in R-point antiferrodistortive lattice fluctuations. Their enhancement and reduction are theoretically explained by considering the fourth-order nonlinear phononic interactions to the driven optical phonon and third-order coupling to lattice strain, respectively. These observations provide a number of testable hypotheses for the physics of light-induced ferroelectricity.

Chirality is a pervasive form of symmetry that is intimately connected to the physical properties of solids, as well as the chemical and biological activity of molecular systems. However, its control with light is challenging, because inducing chirality in a non-chiral material requires that all mirrors and all roto-inversions be simultaneously broken. Electromagnetic fields exert only oscillatory forces that vanish on average, mostly leading to entropy increase that does not break symmetries, per se. Here, we show that chirality of either handedness can be generated in the non-chiral piezoelectric material BPO_4, in which two compensated sub-structures of opposite handedness coexist within the same unit cell. By resonantly driving either one of two orthogonal, doubly degenerate vibrational modes at Terahertz frequency, we rectify the lattice distortion and exert a displacive force onto the crystal. The staggered chirality is in this way uncompensated in either direction, inducing chiral structure with either handedness. The rotary power of the photo-induced phases is comparable to the static value of prototypical chiral alpha-quartz, limited by the strength of the pump laser pulse.

Coherent optical driving in quantum solids is emerging as a research frontier, with many reports of interesting non-equilibrium quantum phases1-4 and transient photo-induced functional phenomena such as ferroelectricity5,6, magnetism7-10 and superconductivity11-14. In high-temperature cuprate superconductors, coherent driving of certain phonon modes has resulted in a transient state with superconducting-like optical properties, observed far above their transition temperature Tc and throughout the pseudogap phase15-18. However, questions remain on the microscopic nature of this transient state and how to distinguish it from a non-superconducting state with enhanced carrier mobility. For example, it is not known whether cuprates driven in this fashion exhibit Meissner diamagnetism. Here we examine the time-dependent magnetic field surrounding an optically driven YBa2Cu3O6.48 crystal by measuring Faraday rotation in a magneto-optic material placed in the vicinity of the sample. For a constant applied magnetic field and under the same driving conditions that result in superconducting-like optical properties15-18, a transient diamagnetic response was observed. This response is comparable in size with that expected in an equilibrium type II superconductor of similar shape and size with a volume susceptibility χv of order -0.3. This value is incompatible with a photo-induced increase in mobility without superconductivity. Rather, it underscores the notion of a pseudogap phase in which incipient superconducting correlations are enhanced or synchronized by the drive.

Optically driven quantum materials exhibit a variety of non-equilibrium functional phenomena [1-11], which are potentially associated with unique transport properties. However, these transient electrical responses have remained largely unexplored, primarily because of the challenges associated with integrating quantum materials into ultrafast electrical devices. Here, thin films of K3C60 grown by Molecular Beam Epitaxy were connected by coplanar terahertz waveguides to a series of photo-conductive switches. This geometry enabled ultrafast transport measurements at high current densities, providing new information on the photo-induced phase created in the high temperature metal by mid-infrared excitation [12-16]. Nonlinearities in the current-voltage charactersitics of the transient state validate the assignment of transient superconductivity, and point to an inhomogeneous phase in which superconducting regions of the sample are connected by resistive weak links [17-23]. This work opens up the possibility of systematic transport measurements in driven quantum materials, both to probe their properties and to integrate them into ultrafast optoelectronic platforms.

The physics of optically-induced superconductivity remains poorly understood, with questions that range from the underlying microscopic mechanism to the macroscopic electrical response of the non-equilibrium phase. In this paper, we study optically-induced superconductivity in K$_{3}$C$_{60}$ thin films, which display signatures of granularity both in the equilibrium state below T$_{c}$ and in the nonequilibrium photo-induced phase above T$_{c}$. Photo-conductive switches are used to measure the ultrafast voltage drop across a K$_{3}$C$_{60}$ film as a function of time after irradiation, both below and above T$_{c}$. These measurements reveal fast changes associated with the kinetic inductance of in-grain superconductivity, and a slower response attributed to the Josephson dynamics at the weak links. Fits to the data yield estimates of the in-grain photo-induced superfluid density after the drive and the dynamics of phase slips at the weak links. This work underscores the increasing ability to make electrical measurements at ultrafast speeds in optically-driven quantum materials, and demonstrates a striking new platform for optoelectronic device applications.

Optically driven quantum materials exhibit a variety of non-equilibrium functional phenomena, which to date have been primarily studied with ultrafast optical, X-Ray and photo-emission spectroscopy. However, little has been done to characterize their transient electrical responses, which are directly associated with the functionality of these materials. Especially interesting are linear and nonlinear current-voltage characteristics at frequencies below 1 THz, which are not easily measured at picosecond temporal resolution. Here, we report on ultrafast transport measurements in photo-excited K 3 C 60 . Thin films of this compound were connected to photo-conductive switches with co-planar waveguides. We observe characteristic nonlinear current-voltage responses, which in these films point to photo-induced granular superconductivity. Although these dynamics are not necessarily identical to those reported for the powder samples studied so far, they provide valuable new information on the nature of the light-induced superconducting-like state above equilibrium T c . Furthermore, integration of non-equilibrium superconductivity into optoelectronic platforms may lead to integration in high-speed devices based on this effect.

Coherent optical excitation of certain phonon modes in YBa_2Cu_3O_6+x has been shown to induce superconducting-like interlayer coherence at temperatures higher than T_c. Recent work has associated these phenomena to a parametric excitation and amplification of Josephson plasma polaritons, which are overdamped above T_c but are made coherent by the phonon drive. However, the dissipative response of uncondensed quasiparticles, which do not couple in the same way to the phonon drive, has not been addressed. Here, we investigate both the enhancement of the superfluid density, ωσ_2(ω), and the dissipative response of quasiparticles, σ_1(ω), by systematically tuning the duration and energy of the mid-infrared pulse while keeping the peak field fixed. We find that the photo-induced superfluid density saturates to the zero-temperature equilibrium value for pulses made longer than the phonon dephasing time, whilst the dissipative component continues to grow with increasing pulse duration. We show that superfluid and dissipation remain uncoupled as long as the drive is on, and identify an optimal regime of pump pulse durations for which the superconducting response is maximum and dissipation is minimized.

In the manuscript arXiv:2210.01114, Dodge and co-authors discuss the influence of pump-probe profile deformations on the reconstructed non-equilibrium optical conductivity of K$_3$C$_{60}$. They state that when pump-induced saturation of the probe response is taken into account, the reconstructed optical properties are not superconducting-like, as was claimed in a number of experimental reports by our group. We show here that the conclusion reached by Dodge et al. is unjustified. In fact, independent of the specific model, including the problematic saturation profile proposed by the authors, the reconstructed optical properties are those of a finite temperature superconductor. The true fingerprint of superconductivity, which is the $1/\omega$ divergence of the imaginary conductivity, $\sigma_{2}(\omega)$, is retained and is virtually independent of the chosen model. The only model-dependent feature is the degree of gapping in $\sigma_{1}(\omega)$. In all cases the extracted optical properties reflect the presence of residual quasiparticles, which at finite temperatures are inevitably present alongside the superfluid.

Recent experiments in the doped cuprates La_2-xBa_xCuO_4 have revealed the emission of anomalous terahertz radiation after impulsive optical excitation. Here, we theoretically investigate the nonlinear electrodynamics of such striped superconductors and explore the origin of the observed radiation. We argue that photoexcitation is converted into a photocurrent by a second-order optical nonlinearity, which is activated by the breaking of inversion symmetry in certain stripe configurations. We point out the importance of including Umklapp photocurrents modulated at the stripe periodicity itself, which impulsively drive surface Josephson plasmons and lead to a resonant structure of outgoing radiation, consistent with the experiments. We speculate on the utility of the proposed mechanism in the context of generating tunable terahertz radiation.

Photo-excitation at terahertz and mid-infrared frequencies has emerged as an effective way to manipulate functionalities in quantum materials, in some cases creating non-equilibrium phases that have no equilibrium analogue. In K3C60, a metastable zero-resistance phase was observed that has optical properties, nonlinear electrical transport and pressure dependencies compatible with non-equilibrium high-temperature superconductivity. Here we demonstrate a two-orders-of-magnitude increase in photo-susceptibility near 10 THz excitation frequency. At these drive frequencies, a metastable superconducting-like phase is observed up to room temperature. The discovery of a dominant frequency scale sheds light on the microscopic mechanism underlying photo-induced superconductivity. It also indicates a path towards steady-state operation, limited at present by the availability of a suitable high-repetition-rate optical source at these frequencies.

In the manuscript arXiv:2306.07869v1, N. L. Wang and co-authors report the results of a near-infrared pump / terahertz probe study in the stripe-ordered cuprate La$_{1.875}$Ba$_{0.125}$CuO$_4$. They measured a change in optical conductivity, but did not find signatures of transient superconductivity. From this observation they extrapolate that in all cuprates in which striped states have been excited with light, there must be no light-induced superconductivity. They conclude that "transient superconductivity cannot be induced by melting of the competing stripe orders with pump pulses whose photon energy is much higher than the superconducting gap of cuprates." Here we show that this extrapolation is unwarranted. First, the absence of light-induced superconductivity in this particular compound was already reported in a previous paper, which instead showed positive evidence for La$_{1.885}$Ba$_{0.115}$CuO$_4$. In addition, the experiment discussed here used photo-excitation with too low fluence and at a suboptimal wavelength. More broadly, a negative result in one compound is rarely compelling indication of the absence of an effect in an entire class of materials.

Interlayer transport in high-TC cuprates is mediated by superconducting tunneling across the CuO2 planes. For this reason, the terahertz frequency optical response is dominated by one or more Josephson plasma resonances and becomes highly nonlinear at fields for which the tunneling supercurrents approach their critical value, IC. These large terahertz nonlinearities are in fact a hallmark of superconducting transport. Surprisingly, however, they have been documented in La2-xBaxCuO4 also above TC for doping values near x =1/8, and interpreted as an indication of superfluidity in the stripe phase. Here, Electric Field Induced Second Harmonic (EFISH) is used to study the dynamics of time-dependent interlayer voltages when La2-xBaxCuO4 is driven with largeamplitude terahertz pulses, in search of other characteristic signatures of Josephson tunnelling in the normal state. We show that this method is sensitive to the voltage anomalies associated with 2p Josephson phase slips, which near x =1/8 are observed both below and above TC. These results document a new regime of nonlinear transport that shares features of sliding charge-densitywaves and superconducting phase dynamics.

Pavel E. Dolgirev, ∗ Marios H. Michael, Jonathan B. Curtis, 2 Daniel E. Parker, Daniele Nicoletti, Michele Buzzi, Michael Fechner, Andrea Cavalleri, 4 and Eugene Demler Department of Physics, Harvard University, Cambridge, Massachusetts 02138, USA. John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138. Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761 Hamburg, Germany. Clarendon Laboratory, University of Oxford, Parks Road, Oxford OX1 3PU, UK. Institute for Theoretical Physics, ETH Zurich, 8093 Zurich, Switzerland. (Dated: March 10, 2022)

We report on element-resolved ultrafast magnetization dynamics in multiferroic CoCr2O4 and Co0.975Ge0.025Cr2O4 after optical excitation above the electronic band gap. We observe demagnetization dynamics in the range of several picoseconds, up to two orders of magnitude faster than previously reported demagnetization in other ferrimagnetic insulators. Moreover, we find that the dynamics of the two magnetic ions differ significantly just below the Curie point. The dynamics of the low-temperature multiferroic phase are almost two times slower than those in the ferrimagnetic phase. This suggests that the additional magnetic cycloidal component, which is coupled to electric polarization at low temperatures, might influence the ultrafast magnetization dynamics.