Faraday waves, typically observed in driven fluids, result from the confluence of nonlinearity and parametric amplification. Here we show that optical pulses can generate analogous phenomena that persist much longer than the pump time-scales in ordered quantum solids. We present a theory of ultrafast light-matter interactions within a symmetry-broken state; dynamical nonlinear coupling between the Higgs (amplitude) and the Goldstone (phase) modes drives an emergent phason texture that oscillates in space and in time: Faraday-Goldstone waves. Calculated signatures of this spatiotemporal order compare well with measurements on K0.3MoO3; Higgs-Goldstone beating, associated with coherent energy exchange between these two modes, is also predicted. We show this light-generated crystalline state is robust to thermal noise, even when the original Goldstone mode is not. Our results offer a pathway for the design of periodic structures in quantum materials with ultrafast light pulses.
Pump-probe experiments performed on K_3C_60 have unveiled both optical and transport signatures of metastable light-induced superconductivity up to room temperature, far above T_c. Recent experiments have uncovered that excitation in the vicinity of 50 meV enables the observation of high temperature light-induced superconductivity at significantly lower fluences. Inspired by these experiments we develop a mechanism which can explain such a giant resonant enhancement of light-induced superconductivity. Within a minimal non-linear Holstein model, we show that resonantly driving optical Raman modes leads to a time-dependent electron-phonon coupling. Such a coupling then modulates the effective electron-electron attraction, with the strongest modulations occurring when the drive is resonant with the phonon frequency. These dynamical modulations of the pairing interactions lead to Floquet-BCS instabilities at temperatures far exceeding equilibrium T_c, as observed in experiments. We conclude by discussing the implications of our general analysis on the K_3C_60 experiments specifically and suggesting experimental signatures of our mechanism.
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.
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.
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.
Strong optical drives have been shown to induce transient superconducting-like response in materials above their equilibrium T_c. Many of these materials already exhibit short-range superconducting correlations in equilibrium. This motivates the question: can external driving enhance coherence in systems with superconducting correlations but no long-range order? We explore this scenario in the two-dimensional XY model with a periodically modulated stiffness using overdamped Langevin dynamics. We find that, even though the modulation leaves the average coupling unchanged, the drive can markedly increase long-range, time-averaged correlations in systems well above the equilibrium Berezinskii-Kosterlitz-Thouless temperature. The outcome depends on the ratio of the drive frequency to the intrinsic relaxation rate: faster drives primarily heat the system, suppressing correlations and conductivity. For slower drives, the optical conductivity is modified so that the real part exhibits a prolonged effective Drude scattering time, while the imaginary part has a strengthened low-frequency 1/ω behavior. We map out these regimes across temperature, frequency, and amplitude, and rationalize them via simple analytics and vortex-thermalization arguments. Overall, we identify a generic nonequilibrium route to enhance coherence in XY-like systems, with potential relevance to experiments reporting light-induced superconductivity.
Polaritons are quantum mechanical superpositions of photon states with elementary excitations in molecules and solids. The light-matter admixture causes a characteristic frequency-momentum dispersion shared by all polaritons irrespective of the microscopic nature of material excitations that could entail charge, spin, lattice or orbital effects. Polaritons retain the strong nonlinearities of their matter component and simultaneously inherit ray-like propagation of light. Polaritons prompt new properties, enable new opportunities for spectroscopy/imaging, empower quantum simulations and give rise to new forms of synthetic quantum matter. Here, we review the emergent effects rooted in polaritonic quasiparticles in a wide variety of their physical implementations. We present a broad portfolio of the physical platforms and phenomena of what we term polaritonic quantum matter. We discuss the unifying aspects of polaritons across different platforms and physical implementations and focus on recent developments in: polaritonic imaging, cavity electrodynamics and cavity materials engineering, topology and nonlinearities, as well as quantum polaritonics.
We present a novel theoretical approach for computing and analyzing two-dimensional spectroscopy of bosonic collective excitations in disordered many-body systems. Specifically, we employ the Keldysh formalism to derive, within a non-pertubative treatment of disorder effects, the third-order nonlinear response and obtain two-dimensional spectroscopy maps. In the weak nonlinear regime of our formalism, we demonstrate the ability of the echo peak to distinguish between elastic and inelastic scattering processes, in perfect agreement with the intuition developed in isolated two-level systems. Furthermore, we discuss unique many-body effects on the echo peak signature arising from interaction induced quantum fluctuations. In particular, we show that these quantum fluctuations induce a finite nonrephasable broadening and examine how the echo peak is influenced by the attractive or repulsive nature of the collective excitations.
Inspired by the striking discovery of metastable superconductivity in K3C60 at 100K, far above Tc = 20 K, we discuss possible mechanisms for long-lived, photo-induced superconductivity. Starting from a model of optically-driven Raman phonons coupled to inter-band electronic transitions, we develop a microscopic mechanism for photo-controlling the pairing interaction. Leveraging this mechanism, we first investigate long-lived superconductivity arising from the thermodynamic metastable trapping of the driven phonon. We then propose an alternative route, where the superconducting gap created by an optical drive leads to a dynamical bottleneck in the equilibration of quasi-particles. We conclude by discussing the implications of both scenarios for experiments that can be used to discriminate between them. Our work provides falsifiable explanations for the nanosecond-scale photo-induced superconductivity found in K3C60, while simultaneously offering a theoretical basis for exploring metastable superconductivity in other quantum materials.
Novel theoretical developments have allowed to connect microscopic disorder in bosonic collective excitations to the signatures in two-dimensional terahertz spectroscopy (Gómez Salvador et al. 2025). Here, we employ this framework to analyze the recently measured Josepshon echoes in optimally doped La_2-xSr_xCuO_4 (Liu et al. 2024). We consider the spatial gap inhomogeneities -observed in scanning tunneling microscopy- as input for the disorder in the superfluid density, and compute the resulting echo peaks. The excellent agreement supports the interpretation that the gap inhomogeneity arises solely from pairing gap fluctuations, with no evidence for non-superconducting competing local orders. Finally, we study the microscopic origin of the inelastic processes, contributing to the damping of the Josephson plasmon at low temperatures, and conclude that it can be attributed to nodal quasiparticles.
The nature of the "failed" ferroelectric transition in SrTiO3 has been a long-standing puzzle in condensed matter physics. A compelling explanation is the competition between ferroelectricity and an instability with a mesoscopic modulation of the polarization. These polarization density waves, which should become especially strong near the quantum critical point, break local inversion symmetry and are difficult to probe with conventional x-ray scattering methods. Here we combine a femtosecond x-ray free electron laser (XFEL) with THz coherent control methods to probe inversion symmetry breaking at finite momenta and visualize the instability of the polarization on nanometer lengthscales in SrTiO3. We find polar-acoustic collective modes that are soft particularly at the tens of nanometer lengthscale. These precursor collective excitations provide evidence for the conjectured mesoscopic modulated phase in SrTiO3.
The spatial and temporal dynamics of wave propagation are intertwined. A common manifestation of this duality emerges in the spatial and temporal decay of waves as they propagate through a lossy medium. A complete description of the non-Hermitian wave dynamics in such a lossy system, capturing temporal and spatial decays, necessitates the use of complex-valued frequency and/or wavenumber Eigen-values. Here, we demonstrate that the propagation of polaritons - hybrid light-matter quasiparticles - can be broadly controlled in space and time by temporally shaping their photonic excitation. Using time-domain terahertz near-field nanoscopy, we study plasmon polaritons in bilayer graphene at sub-picosecond time scales. Suppressed spatial decay of polaritons is implemented by temporally engineering the excitation waveform. Polaritonic space-time metrology data agree with our dynamic model. Through the experimental realization and visualization of polaritonic space-time duality, we uncover the effects of the spatio-temporal engineering of wave dynamics; these are applicable to acoustic, photonic, plasmonic, and electronic systems.
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.
Two-dimensional terahertz spectroscopy (2DTS), a terahertz analogue of nuclear magnetic resonance, is a new technique poised to address many open questions in complex condensed matter systems. The conventional theoretical framework used ubiquitously for interpreting multidimensional spectra of discrete quantum level systems is, however, insufficient for the continua of collective excitations in strongly correlated materials. Here, we develop a theory for 2DTS of a model collective excitation, the Josephson plasma resonance in layered superconductors. Starting from a mean-field approach at temperatures well below the superconducting phase transition, we obtain expressions for the multidimensional nonlinear responses that are amenable to intuition derived from the conventional single-mode scenario. We then consider temperatures near the superconducting critical temperature $T_c$, where dynamics beyond mean-field become important and conventional intuition fails. As fluctuations proliferate near $T_c$, the dominant contribution to nonlinear response comes from an optical parametric drive of counter-propagating Josephson plasmons, which gives rise to 2D spectra that are qualitatively different from the mean-field predictions. As such, and in contrast to one-dimensional spectroscopy techniques, such as third harmonic generation, 2DTS can be used to directly probe thermally excited finite-momentum plasmons and their interactions. Our theory provides a clear interpretation of recent 2DTS measurements on cuprates, and we discuss implications beyond the present context of Josephson plasmons.
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.
The physics of driven collective modes in quantum materials underpin a number of striking non-equilibrium functional responses, which include enhanced magnetism, ferroelectricity and superconductivity. However, the coherent coupling between multiple modes at once are difficult to capture by single-pump probe (one-dimensional) spectroscopy, and often remain poorly understood. One example is phonon-mediated amplification of Josephson plasmons in YBa$_2$Cu$_3$O$_{6+x}$, in which at least three normal modes of the solid are coherently mixed as a source of enhanced superconductivity. Here, we go beyond previous pump-probe experiments in this system and acquire two-dimensional frequency maps using pairs of mutually delayed, carrier envelope phase stable mid-infrared pump pulses, combined with measurements of the time-modulated second-order nonlinear optical susceptibility. We find that the driven zone-center phonons amplify coherent pairs of opposite-momentum Josephson plasma polaritons, generating a squeezed state of interlayer phase fluctuations. The squeezed state is a potentially important ingredient in the microscopic physics of photo-induced superconductivity in this and other materials.