Hubbard excitons capture the many-body correlations of Mott insulators. Using ultrafast light, their quantum wavefunction can be coherently rotated, opening a path towards optical quantum control and sensing in strongly correlated materials.

We study the behavior of the 2D repulsive Hubbard model on a square lattice at half filling, under strong driving with ac electric fields, by employing a time-dependent Gaussian variational approach. Within the same theoretical framework, we analytically obtain the conventional Keldysh crossover between multiphoton and tunneling photoexcitation mechanisms, as well as two new regimes beyond the Keldysh paradigm. We discuss how dynamical renormalization of the Mott-Hubbard gap feeds back into the photoexcitation process, modulating the carrier generation rate in real time. The momentum distribution of quasiparticle excitations immediately after the drive is calculated, and shown to contain valuable information about the generation mechanism. Finally, we discuss experimental probing of the pump-induced nonequilibrium electronic state.

Photo-excited quantum materials can be driven into thermally inaccessible metastable states that exhibit structural, charge, spin, topological and superconducting orders. Metastable states typically emerge on timescales set by the intrinsic electronic and phononic energy scales, ranging from femtoseconds to picoseconds, and can persist for weeks. Therefore, studies have primarily focused on ultrafast or quasi-static limits, leaving the intermediate time window less explored. Here we reveal a metastable state with broken glide-plane symmetry in photo-doped Ca2RuO4 using time-resolved optical second-harmonic generation and birefringence measurements. We find that the metastable state appears long after intralayer antiferromagnetic order has melted and photo-carriers have recombined. Its properties are distinct from all known states in the equilibrium phase diagram and are consistent with intralayer ferromagnetic order. Furthermore, model Hamiltonian calculations reveal that a non-thermal trajectory to this state can be accessed via photo-doping. Our results expand the search space for out-of-equilibrium electronic matter to metastable states emerging at intermediate timescales. Searches for metastable states with properties not found in thermal equilibrium have been restricted to either ultrafast or slow timescales. A metastable state in an intermediate time window has now been identified in a photo-doped Mott insulator.

The relative twist angle between layers of near-lattice-matched van der Waals materials is critical for the emergent correlated phenomena associated with moire flat bands. However, the concept of angle rotation control is not exclusive to moiré superlattices in which electrons directly experience a twist-angle-dependent periodic potential. Instead, it can also be employed to induce programmable symmetry-breaking perturbations with the goal of stabilizing desired correlated states. Here, we experimentally demonstrate `moireless' twist-tuning of superconductivity together with other correlated orders in Bernal bilayer graphene proximitized by tungsten diselenide. The alignment between the two materials systematically controls the strength of the induced Ising spin-orbit coupling (SOC), profoundly altering the phase diagram. As Ising SOC is increased, superconductivity onsets at a higher displacement field and features a higher critical temperature, reaching up to 0.5K. Within the main superconducting dome and in the strong Ising SOC limit, we find an unusual phase transition characterized by a nematic redistribution of holes among trigonally warped Fermi pockets and enhanced resilience to in-plane magnetic fields. The behavior of the superconducting phase is well captured by our theoretical model, which emphasizes the role of interband interactions between Fermi pockets arising due to interaction-enhanced symmetry breaking. Moreover, we identify two additional superconducting regions, one of which descends from an inter-valley coherent normal state and exhibits a Pauli-limit violation ratio exceeding 40, among the highest for all known superconductors. Our results provide new insights into ultra-clean graphene-based superconductors and underscore the potential of utilizing moireless-twist engineering across a range of van der Waals heterostructures.

Magnetism has played a central role in the long and rich history of modern condensed matter physics, with many foundational insights originating from theoretical studies of two-dimensional (2D) spin systems. The discovery of 2D van der Waals (vdW) magnets has revolutionized this area by providing real, atomically thin magnetic systems for experimental investigation. Since the first experimental reports of antiferromagnetic vdW insulators in 2016 - followed by studies on ferromagnetic vdW systems in 2017 - the field has witnessed rapid and expansive growth, with more than two dozen vdW magnetic materials now identified, including both ferro- and antiferromagnets. In this review, we present a comprehensive overview of the major scientific and technological developments in this rapidly evolving field. These include experimental realizations of various 2D spin Hamiltonians as well as unexpected phenomena such as magnetic excitons, Floquet-engineered states, and light-induced metastable magnetic phases. In parallel, 2D vdW magnets have shown significant promise in spintronics and related applications, offering a new platform for engineering quantum functionalities. We organize this review by tracing the historical development of the field, synthesizing key milestones, and highlighting its broader impact across condensed matter physics and materials science. We conclude with an Outlook section that outlines several promising directions for future research, aiming to chart a path forward in this vibrant and still rapidly growing area.

The ability to rapidly manipulate domain walls in magnetic materials is key to developing novel high-speed spintronic memory and computing devices. Antiferromagnetic materials present a particularly promising platform due to their robustness against stray fields and their potential for exceptional domain wall velocities. Among various proposed driving mechanisms, coherent spin waves could potentially propel antiferromagnetic domain walls to the magnon group velocity while minimizing dissipation from Joule heating. However, experimental realization has remained elusive due to the dual challenges of generating coherent antiferromagnetic spin waves near isolated mobile antiferromagnetic domain walls and simultaneously measuring high-speed domain wall dynamics. Here we experimentally realize an approach where ultrafast laser pulses generate coherent spin waves that drive antiferromagnetic domain walls and develop a technique to directly map the spatiotemporal domain wall dynamics. Using the room-temperature antiferromagnetic insulator Sr2Cu3O4Cl2, we observe antiferromagnetic domain wall motion with record-high velocities up to ~50 km s-1. Remarkably, the direction of domain wall propagation is controllable through both the pump laser helicity and the sign of the domain wall winding number. This bidirectional control can be theoretically explained, and numerically reproduced, by the domain wall dynamics induced by coherent spin waves of the in-plane magnon mode-a phenomenon unique to magnets with an easy-plane anisotropy. Our work uncovers a novel domain wall propulsion mechanism that is generalizable to a wide range of antiferromagnetic materials, unlocking new opportunities for ultrafast coherent antiferromagnetic spintronics.

Two-dimensional Mott insulators host antiferromagnetic (AFM) correlations that are predicted to enhance the attractive interaction between empty (holons) and doubly occupied (doublons) sites, creating a novel pathway for exciton formation. However, experimental confirmation of this spin-mediated binding mechanism remains elusive. Leveraging the distinct magnetic critical properties of the Mott antiferromagnets Sr2IrO4 and Sr3Ir2O7, we show using time-resolved THz spectroscopy that excitons exist only at temperatures below where short-range AFM correlation develops. The excitons remain stable up to photodoping densities approaching the predicted excitonic Mott insulator-to-metal transition, revealing a unique robustness against screening. Our results establish the viability of spin-bound excitons and introduce opportunities for excitonic control through magnetic degrees of freedom.

Uncovering pathways to optically drive magnetic order-disorder transitions on ultrashort timescales can lead to the realization of novel out-of-equilibrium quantum phenomena. A long-sought pathway is to directly excite a highly non-thermal energy-momentum distribution of magnons, bypassing both charge and lattice degrees of freedom. However, this remains elusive owing to the weak coupling and large momentum mismatch between photons and magnons. Here we demonstrate strong parametric excitation of magnons across the entire Brillouin zone of the antiferromagnetic insulator Sr_2Cu_3O_4Cl_2 by periodically modulating the superexchange interaction with the electric field of light. The excitation efficiency is greatly enhanced by tuning to the van Hove singularity in the magnon spectrum, sufficient to transiently collapse the antiferromagnetic state using a pulsed laser field of 10^9 V/m. The order parameter recovery timescale increases by over 1000 times as a function of excitation density, reflecting a crossover from high- to low-energy magnon dominated decay dynamics. This electric-field induced parametric magnon pumping mechanism is applicable to a broad range of magnetic insulators and opens up the possibility of dynamically engineering magnon distributions by design.

The identification of distinct charge transport features, deriving from nontrivial bulk band and surface states, has been a challenging subject in the field of topological systems. In topological Dirac and Weyl semimetals, nontrivial conical bands with Fermi-arc surface states give rise to negative longitudinal magnetoresistance due to chiral anomaly effect and unusual thickness dependent quantum oscillation from Weyl-orbit effect, which were demonstrated recently in experiments. In this work, we report the experimental observations of large nonlinear and nonreciprocal transport effects for both longitudinal and transverse channels in an untwinned Weyl metal of SrRuO$_3$ thin film grown on a SrTiO$_{3}$ substrate. From rigorous measurements with bias current applied along various directions with respect to the crystalline principal axes, the magnitude of nonlinear Hall signals from the transverse channel exhibits a simple sin$\alpha$ dependence at low temperatures, where $\alpha$ is the angle between bias current direction and orthorhombic [001]$_{\rm o}$, reaching a maximum when current is along orthorhombic [1-10]$_{\rm o}$. On the contrary, the magnitude of nonlinear and nonreciprocal signals in the longitudinal channel attains a maximum for bias current along [001]$_{\rm o}$, and it vanishes for bias current along [1-10]$_{\rm o}$. The observed $\alpha$-dependent nonlinear and nonreciprocal signals in longitudinal and transverse channels reveal a magnetic Weyl phase with an effective Berry curvature dipole along [1-10]$_{\rm o}$ from surface states, accompanied by 1D chiral edge modes along [001]$_{\rm o}$.

Floquet engineering, the process of using a periodic driving force, like a laser, can be used to control quantum systems by changing their electronic structure. In this project, a femtosecond IR laser was used to drive a Mott insulator (specifically La 2 CuO 4 ) into transient states. Mott insulators are quantum materials which have a partially filled electron band, causing them to be insulators at low temperatures due to electron-electron correlation. Understanding their properties is of great interest as they potentially have wide-ranging applications from quantum storage devices to optical switches. Using a pump-probe technique, the La 2 CuO 4 crystal was driven out of equilibrium by the femtosecond laser pump beam with varying energies intended to limit the heating of the Mott sample by the pump. The transient reflectivity was then probed using a white-light spectrum generated by a sapphire crystal of wavelengths comparable to the band gap. In addition, a DFT code, Quantum Espresso, was used to model the electronic structure of La 2 CuO 4 and calculate various quantities such as the Fermi Energy and band gap. These transient reflectivity measurements and related spectra will be analyzed and interesting properties such as the optical conductivity can potentially be inferred.

The undoped antiferromagnetic Mott insulator naturally has one charge carrier per lattice site. When it is doped with additional carriers, they are unstable to spin-fluctuation-mediated Cooper pairing as well as other unconventional types of charge, spin and orbital current ordering. Photo-excitation can produce charge carriers in the form of empty (holons) and doubly occupied (doublons) sites that may also exhibit charge instabilities. There is evidence that antiferromagnetic correlations enhance attractive interactions between holons and doublons, which can then form bound pairs known as Hubbard excitons, and that these might self-organize into an insulating Hubbard exciton fluid. However, this out-of-equilibrium phenomenon has not been experimentally detected. Here we report the transient formation of a Hubbard exciton fluid in the antiferromagnetic Mott insulator Sr 2 IrO 4 using ultrafast terahertz conductivity. Following photo-excitation, we observe rapid spectral-weight transfer from a Drude metallic response to an insulating response. The latter is characterized by a finite-energy peak originating from intraexcitonic transitions, whose assignment is corroborated by our numerical simulations of an extended Hubbard model. The lifetime of the peak is short (approximately one picosecond) and scales exponentially with the Mott gap size, implying extremely strong coupling to magnon modes.

We explore the effects of chemical doping and photodoping in the strain-induced multiferroic EuTiO3 grown on DyScO3 substrates. The polar order is probed experimentally using second harmonic generation (SHG) and modeled using ab initio calculations. At low photodoping concentrations, we observe a reduction in SHG signal, indicating a destructive coupling between charge carriers and polar order in accordance with our simulations and expectations for a second-order Jahn-Teller driven ferroelectric. However, under increased photodoping the reduction in SHG plateaus at 84% of its original magnitude, indicating resilience of the polar order in the presence of a high concentration of delocalized electrons. This behavior stands in contrast with our first-principles simulations, indicating that EuTiO3 undergoes a transition from ferroelectric to polar metallic character under photodoping. We suggest several hypotheses for the mechanism behind this change in distortion character.

Ultrafast laser excitation provides a means to transiently realize long-range ordered electronic states of matter that are hidden in thermal equilibrium. Recently, this approach has unveiled a variety of thermally inaccessible ordered states in strongly correlated materials, including charge density wave, ferroelectric, magnetic, and intertwined charge-orbital ordered states. However, more exotic hidden states exhibiting higher multipolar ordering remain elusive owing to the challenge of directly manipulating and detecting them with light. Here we demonstrate a method to induce a dynamical transition from a thermally allowed to a thermally forbidden spin-orbit entangled quadrupolar ordered state in Ca 2 RuO 4 by coherently exciting a phonon that is strongly coupled to the order parameter. Combining probe photon energy-resolved coherent phonon spectroscopy measurements with model Hamiltonian calculations, we show that the dynamical transition is manifested through anomalies in the temperature, pump excitation fluence, and probe photon energy dependence of the strongly coupled phonon. With this procedure, we introduce a general pathway to uncover hidden multipolar ordered states and to control their re-orientation on ultrashort timescales.

Strongly driven antiferromagnetic Mott insulators have the potential to exhibit exotic transient phenomena that are forbidden in thermal equilibrium. However, such far-from-equilibrium regimes, where conventional time-dependent Ginzburg-Landau descriptions fail, are experimentally challenging to prepare and to probe especially in solid state systems. Here we use a combination of time-resolved second harmonic optical polarimetry and coherent magnon spectroscopy to interrogate n-type photo-doping induced ultrafast magnetic order parameter dynamics in the antiferromagnetic Mott insulator Sr2IrO4. We find signatures of an unusual far-from-equilibrium critical regime in which the divergences of the magnetic correlation length and relaxation time are decoupled. This violation of conventional thermal critical behavior arises from the interplay of photo-doping and non-thermal magnon population induced demagnetization effects. Our findings, embodied in a non-equilibrium phase diagram, provide a blueprint for engineering the out-of-equilibrium properties of quantum matter, with potential applications to terahertz spintronics technologies. The impulsively driven antiferromagnetic Mott insulator is a model quantum many-body system predicted to realize exotic transient phenomena, however its exploration in far-from equilibrium regimes remains experimentally challenging. Here, the authors use a combination of second harmonic optical polarimetry and coherent magnon spectroscopy to investigate the ultrafast non-equilibrium dynamics of the Mott insulator Sr2IrO4 and find evidence of a far-from-equilibrium critical regime where static and dynamic critical behaviour decouple and which could be present in a number of other quantum materials.

The fate of a Mott insulator under strong low frequency optical driving conditions is a fundamental problem in quantum many-body dynamics. Using ultrafast broadband optical spectroscopy, we measured the transient electronic structure and charge dynamics of an off-resonantly pumped Mott insulator Ca_{2}RuO_{4}. We observe coherent bandwidth renormalization and nonlinear doublon-holon pair production occurring in rapid succession within a sub-100-fs pump pulse duration. By sweeping the electric field amplitude, we demonstrate continuous bandwidth tuning and a Keldysh crossover from a multiphoton absorption to quantum tunneling dominated pair production regime. Our results provide a procedure to control coherent and nonlinear heating processes in Mott insulators, facilitating the discovery of novel out-of-equilibrium phenomena in strongly correlated systems.

Elemental tellurium is a strongly spin-orbit coupled Peierls-distorted semiconductor whose band structure features topologically protected Weyl nodes. Using time-dependent density functional theory calculations, we show that impulsive optical excitation can be used to transiently control the amplitude of the Peierls distortion, realizing a mechanism to switch tellurium between three states: Weyl semiconductor, Weyl metal and non-Weyl metal. Further, we present experimental evidence of this inverse-Peierls distortion using time-resolved optical second harmonic generation measurements. These results provide a pathway to multifunctional ultrafast Weyl devices and introduce Peierls systems as viable hosts of light-induced topological transitions.

G. Li, W. Z. Hu, J. Dong, D. Qian, D. Hsieh, M. Z. Hasan, E. Morosan, R. J. Cava, and N. L. Wang ∗ Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100080, P. R. China Department of Physics, Joseph Henry Laboratories of Physics, Princeton University, Princeton, New Jersey 08544, USA Department of Chemistry, Princeton University, Princeton, New Jersey 08544, USA

The transition metal monopnictide family of Weyl semimetals recently has been shown to exhibit anomalously strong second-order optical nonlinearity, which is theoretically attributed to a highly asymmetric polarization distribution induced by their polar structure. We experimentally test this hypothesis by measuring optical second harmonic generation (SHG) from TaAs across a pressure-tuned polar-to-nonpolar structural phase transition. Despite the high-pressure structure remaining noncentrosymmetric, the SHG yield is reduced by more than 60% by 20 GPa as compared to the ambient pressure value. By examining the pressure dependence of distinct groups of SHG susceptibility tensor elements, we find that the yield is primarily controlled by a single element that governs the response along the polar axis. Our results confirm a connection between the polar axis and the giant optical nonlinearity of Weyl semimetals and demonstrate pressure as a means to tune this effect in situ.

We report magnetic optical second-harmonic generation (SHG) polarimetry and imaging on Sr$_2$Cu$_3$O$_4$Cl$_2$, which allows direct visualization of the mesoscopic antiferromagnetic (AFM) structure of a parent cuprate. Temperature- and magnetic-field-dependent SHG reveals large domains with 90$^{\circ}$ relative orientations that are stabilized by a combination of uniaxial magnetic anisotropy and the Earth's magnetic field. Below a temperature $T_R$ $\sim$ 97 K, we observe an unusual 90$^{\circ}$ spin reorientation transition, possibly driven by competing magnetic anisotropies of the two copper sublattices, which swaps the AFM domain states while preserving the domain structure. This allows deterministic switching of the AFM states by thermal or laser heating. Near $T_R$, the domain walls become exceptionally responsive to an applied magnetic field, with the Earth's field sufficient to completely expel them from the crystal. Our findings unlock opportunities to study the mesoscopic AFM behavior of parent cuprates and explore their potential for AFM technologies.