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Important advances have recently been made in the search for materials with complex multi-phase landscapes that host photoinduced metastable collective states with exotic functionalities. In almost all cases so far, the desired phases are accessed by exploiting light-matter interactions via the imaginary part of the dielectric function through above-bandgap or resonant mode excitation. Nonresonant Raman excitation of coherent modes has been experimentally observed and proposed for dynamic material control, but the resulting atomic excursion has been limited to perturbative levels. Here, we demonstrate that it is possible to overcome this challenge by employing nonresonant ultrashort pulses with low photon energies well below the bandgap. Using mid-infrared pulses, we induce ferroelectric reversal in lithium niobate and phase switching in tin selenide and characterize the large-amplitude mode displacements through femtosecond Raman scattering, second harmonic generation, and x-ray diffraction. This approach, validated by first-principle calculations, defines a novel method for synthesizing hidden phases with unique functional properties and manipulating complex energy landscapes at reduced energy consumption and ultrafast speeds., Comment: 5 figures

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.

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.

We demonstrate that the absorption of femtosecond x-ray pulses can excite quasi-spherical high-wavevector coherent acoustic phonon wavepackets using an all x-ray pump and probe scattering experiment. The time- and momentum-resolved diffuse scattering signal is consistent with strain pulses induced by the rapid electron cascade dynamics following photoionization at uncorrelated excitation centers. We quantify key parameters of this process, including the localization size of the strain wavepacket and the energy absorption efficiency, which are determined by the photoelectron and Auger electron cascade dynamics, as well as the electron-phonon interaction. In particular, we obtain the localization size of the observed strain wave packet to be 1.5 and 2.5 nm for bulk SrTiO$_3$ and KTaO$_3$ single crystals, even though there are no nanoscale structures or light-intensity patterns that would ordinarily be required to generate acoustic waves of wavelengths much shorter than the penetration depth. Whereas in GaAs and GaP we do not observe a signal above background. The results provide crucial information on x-ray matter interactions, which sheds light on the mechanism of x-ray energy deposition, and the study of high wavevector acoustic phonons and thermal transport at the nanoscale.

We demonstrate optical pump/THz probe (OPTP) spectroscopy with a variable external magnetic field (0-9 T) in which the time-dependent THz signal is measured by echelon-based single-shot detection at a 1 kHz repetition rate. The method reduces data acquisition times by more than an order of magnitude compared to conventional electro-optic sampling using a scanning delay stage. The approach illustrates the wide applicability of the single-shot measurement approach to nonequilibrium systems that are studied through OPTP spectroscopy, especially in cases where parameters such as magnetic field strength (B) or other experimental parameters are varied. We demonstrate the capabilities of our measurement by performing cyclotron resonance experiments in bulk silicon, where we observe B-field dependent carrier relaxation and distinct relaxation rates for different carrier types. We use a pair of economical linear array detectors to measure 500 time points on each shot, offering equivalent performance to camera-based detection with possibilities for higher repetition rates.

Magnons are quantized collective spin-wave excitations in magnetically ordered materials. Revealing their interactions among these collective modes is crucial for the understanding of fundamental many-body effects in such systems and the development of high-speed information transport and processing devices based on them. Nevertheless, identifying couplings between individual magnon modes remains a long-standing challenge. Here, we demonstrate spectroscopic fingerprints of anharmonic coupling between distinct magnon modes in an antiferromagnet, as evidenced by coherent photon emission at the sum and difference frequencies of the two modes. This discovery is enabled by driving two magnon modes coherently with a pair of tailored terahertz fields and then disentangling a mixture of nonlinear responses with different origins. Our approach provides a route for generating nonlinear magnon-magnon mixing.

Layered hybrid perovskites have attracted much attention in recent years due to their emergent physical properties and exceptional functional performances, but the coexistence of lattice order and structural disorder severely hinders our understanding of these materials. One unsolved problem regards how the lattice dynamics are affected by the dimensional engineering of the inorganic frameworks and the interaction with the molecular moieties. Here, we address this question by using a combination of high-resolution spontaneous Raman scattering, high-field terahertz spectroscopy, and molecular dynamics simulations. This approach enables us to reveal the structural vibrations and disorder in and out of equilibrium and provides surprising observables that differentiate single- and double-layered perovskites. While no distinct vibrational coherence is observed in double-layer perovskites, we discover that an off-resonant terahertz pulse can selectively drive a long-lived coherent phonon mode through a two-photon process in the single-layered system. This difference highlights the dramatic change in the lattice environment as the dimension is reduced. The present findings pave the way for the ultrafast structural engineering of hybrid lattices as well as for developing high-speed optical modulators based on layered perovskites.

Achieving high repeatability and efficiency in laser-induced strong shock wave excitation remains a significant technical challenge, as evidenced by the extensive efforts undertaken at large-scale national laboratories to optimize the compression of light element pellets. In this study, we propose and model a novel optical design for generating strong shocks at a tabletop scale. Our approach leverages the spatial and temporal shaping of multiple laser pulses to form concentric laser rings on condensed matter samples. Each laser ring initiates a two-dimensional focusing shock wave that overlaps and converges with preceding shock waves at a central point within the ring. We present preliminary experimental results for a single ring configuration. To enable high-power laser focusing at the micron scale, we demonstrate experimentally the feasibility of employing dielectric metasurfaces with exceptional damage threshold, experimentally determined to be 1.1 J/cm2, as replacements for conventional optics. These metasurfaces enable the creation of pristine, high-fluence laser rings essential for launching stable shock waves in materials. Herein, we showcase results obtained using a water sample, achieving shock pressures in the gigapascal (GPa) range. Our findings provide a promising pathway towards the application of laser-induced strong shock compression in condensed matter at the microscale., Comment: 8 pages, 4 figures

The laser ultrasonics technique perfectly fits the needs for non-contact, non-invasive, non-destructive mechanical probing of samples of mm to nm sizes. This technique is however limited to the excitation of low-amplitude strains, below the threshold for optical damage of the sample. In the context of strain engineering of materials, alternative optical techniques enabling the excitation of high amplitude strains in a non-destructive optical regime are seeking. We introduce here a non-destructive method for laser-shock wave generation based on additive superposition of multiple laser-excited strain waves. This technique enables strain generation up to mechanical failure of a sample at pump laser fluences below optical ablation or melting thresholds. We demonstrate the ability to generate nonlinear surface acoustic waves (SAWs) in Nb:SrTiO$_3$ substrates, at typically 1 kHz repetition rate, with associated strains in the percent range and pressures close to 100 kbars. This study paves the way for the investigation of a host of high-strength SAW-induced phenomena, including phase transitions in conventional and quantum materials, plasticity and a myriad of material failure modes, chemistry and other effects in bulk samples, thin layers, or two-dimensional materials.

Equilibrium Bose-Einstein condensation of exciton-polaritons, demonstrated with a long-lifetime microcavity [Phys. Rev. Lett. 118, 016602 (2017)], has proven that driven-dissipative systems can undergo thermodynamic phase transitions in the limit where the quasiparticle lifetime exceeds the thermalization time. Here, we identify the role of dimensionality and polariton interactions in determining the degree of thermalization in optically generated traps. To distinguish the effect of trapping from interactions and lifetimes, we measured the polariton distribution under four nonresonant Gaussian pumps in a square geometry and compared it with polariton distributions measured with each pump individually. We found that significant redistribution of polaritons arises by trapping and modification of the density of states. Surprisingly efficient polariton-polariton scattering below the condensation threshold is evidenced by the depletion of the inflection-point polaritons. Our work provides a deeper understanding of polariton distributions and their interactions under various geometries of optically generated potentials.

Tailored light excitation and nonlinear control of lattice vibrations have emerged as powerful strategies to manipulate the properties of quantum materials out of equilibrium. Generalizing the use of coherent phonon-phonon interactions to nonlinear couplings among other types of collective modes would open unprecedented opportunities in the design of novel dynamic functionalities in solids. For example, the collective excitations of magnetic order -- magnons -- can carry information with little energy dissipation, and their coherent and nonlinear control would provide an attractive route to achieve collective-mode-based information processing and storage in forthcoming spintronics and magnonics. Here, we discover that intense terahertz (THz) fields can initiate processes of magnon upconversion mediated by an intermediate magnetic resonance. By using a suite of advanced spectroscopic tools, including a newly demonstrated two-dimensional (2D) THz polarimetry technique enabled by single-shot detection, we unveil the unidirectional nature of coupling between distinct magnon modes of a canted antiferromagnet. Calculations of spin dynamics further suggest that this coupling is a universal feature of antiferromagnets with canted magnetic moments. These results demonstrate a route to inducing desirable energy transfer pathways and THz-induced coupling between coherent magnons in solids and pave the way for a new era in the development of ultrafast control of magnetism.

State-of-the-art hybrid perovskites have demonstrated excellent functionality in photovoltaics and light-emitting applications, and have emerged as a promising candidate for exciton-polariton (polariton) optoelectronics. In the strong coupling regime, polariton formation and Bose-Einstein condensation (BEC) have been demonstrated at room-temperature in several perovskite formulations. Thermodynamically, low-threshold BEC requires efficient scattering to $k_{||}$ = 0, and many applications demand precise control of polariton interactions. Thus far, the primary mechanisms by which polaritons relax in perovskites remains unclear. In this work, we perform temperature-dependent measurements of polaritons in low-dimensional hybrid perovskites with high light-matter coupling strengths ($\hbar \Omega_{Rabi}$ = 260$\pm$5 meV). By embedding the perovskite active layer in a wedged cavity, we are able to tune the Hopfield coefficients and decouple the primary polariton relaxation mechanisms in this material for the first time. We observe the thermal activation of a bottleneck regime, and reveal that this effect can be overcome by harnessing intrinsic scattering mechanisms arising from the interplay between the different excitonic species, such as biexciton-assisted polariton relaxation pathways, and isoenergetic intracavity pumping. We demonstrate the dependence of the bottleneck suppression on cavity detuning, and are able to achieve efficient relaxation to $k_{||}$ = 0 even at cryogenic temperatures. This new understanding contributes to the design of ultra-low-threshold BEC and condensate control by engineering polariton dispersions resonant with efficient relaxation pathways, leveraging intrinsic material scattering mechanisms for next-generation polariton optoelectronics., Comment: *Corresponding authors: danedeq@mit.edu, bulovic@mit.edu

Nonequilibrium hidden states, both transient and long-lived, provide a unique window into thermally inaccessible regimes of strong coupling between microscopic degrees of freedom in quantum materials. Understanding the physical origin of these states is of both fundamental and practical significance, allowing the exploration of far-from-equilibrium thermodynamics and the development of optoelectronic devices with on-demand photoresponses. However, mapping the ultrafast formation of a long-lived hidden phase remains a long-standing challenge in physics since the initial state of the system is not recovered rapidly and conventional pump-probe methods are thus not applicable. Here, using a suite of state-of-the-art single-shot spectroscopy techniques, we present a direct ultrafast visualization of the photoinduced phase transition to both transient and long-lived hidden states in an electronic crystal, 1T-TaS2. Capturing the dynamics of this complex phase transformation in a single-shot fashion demonstrates a commonality in microscopic pathways, driven by the collapse of charge order, that the system undergoes to enter the hidden state and provides unambiguous spectral fingerprints that distinguish such state from thermally accessible phases. We present a theory of fluctuation-dominated process that explains both the dynamics and the nature of the metastable state. Our results settle the debate around the origin of this elusive metastable state and pave the way for the discovery of new quantum phases of matter.

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

Herein we describe a novel spinning pump-probe photoacoustic technique developed to study nonlinear absorption in thin films. As a test case, an organic polycrystalline thin film of quinacridone, a well-known pigment, with a thickness in the tens of nanometers range, is excited by a femtosecond laser pulse which generates a time-domain Brillouin scattering signal. This signal is directly related to the strain wave launched from the film into the substrate and can be used to quantitatively extract the nonlinear optical absorption properties of the film itself. Quinacridone exhibits both quadratic and cubic laser fluence dependence regimes which we show to correspond to two- and three-photon absorption processes. This technique can be broadly applied to materials that are difficult or impossible to characterize with conventional transmittance-based measurements including materials at the nanoscale, prone to laser damage, with very weak nonlinear properties, opaque or highly scattering.

Photoluminescence (PL) intermittency is a ubiquitous phenomenon detrimentally reducing the temporal emission intensity stability of single colloidal quantum dots (CQDs) and the emission quantum yield of their ensembles. Despite efforts for blinking reduction via chemical engineering of the QD architecture and its environment, blinking still poses barriers to the application of QDs, particularly in single-particle tracking in biology or in single-photon sources. Here, we demonstrate the first deterministic all-optical suppression of quantum dot blinking using a compound technique of visible and mid-infrared (MIR) excitation. We show that moderate-field ultrafast MIR pulses (5.5 $\mu$m, 150 fs) can switch the emission from a charged, low quantum yield 'grey' trion state to the 'bright' exciton state in CdSe/CdS core-shell quantum dots resulting in a significant reduction of the QD intensity flicker. Quantum-tunneling simulations suggest that the MIR fields remove the excess charge from trions with reduced emission quantum yield to restore higher brightness exciton emission. Our approach can be integrated with existing single-particle tracking or super-resolution microscopy techniques without any modification to the sample and translates to other emitters presenting charging-induced PL intermittencies, such as single-photon emissive defects in diamond and two-dimensional materials., Comment: 35 pages, 5 figures

Optical-domain Transient Grating (TG) spectroscopy is a versatile background-free four-wave-mixing technique used to probe vibrational, magnetic and electronic degrees of freedom in the time domain. The newly developed coherent X-ray Free Electron Laser sources allow its extension to the X-ray regime. Xrays offer multiple advantages for TG: their large penetration depth allows probing the bulk properties of materials, their element-specificity can address core-excited states, and their short wavelengths create excitation gratings with unprecedented momentum transfer and spatial resolution. We demonstrate for the first time TG excitation in the hard X-ray range at 7.1 keV. In Bismuth Germanate (BGO), the nonresonant TG excitation generates coherent optical phonons detected as a function of time by diffraction of an optical probe pulse. This experiment demonstrates the ability to probe bulk properties of materials and paves the way for ultrafast coherent four-wave-mixing techniques using X-ray probes and involving nanoscale TG spatial periods., Comment: 11 pages, 4 figures

High-velocity microparticle impacts are relevant to many fields from space exploration to additive manufacturing and can be used to help understand the physical and chemical behaviors of materials under extreme dynamic conditions. Recent advances in experimental techniques for single microparticle impacts have allowed fundamental investigations of dynamical responses of wide-ranging samples including soft materials, nano-composites, and metals, under strain rates up to 108 s-1. Here we review experimental methods for high-velocity impacts spanning 15 orders of magnitude in projectile mass and compare method performances. This review aims to present a comprehensive overview of high-velocity microparticle impact techniques to provide a reference for researchers in different materials testing fields and facilitate experimental design in dynamic testing for a wide range of impactor sizes, geometries, and velocities. Next, we review recent studies using the laser-induced particle impact test platform comprising target, projectile, and synergistic target-particle impact response, hence demonstrating the versatility of the method with applications in impact protection and additive manufacturing. We conclude by presenting the future perspectives in the field of high-velocity impact.

Chirality and chiral molecules are key elements in modern chemical and biochemical industries. Individual addressing, and the eventual separation of chiral enantiomers has been and still is an important elusive task in molecular physics and chemistry, and a variety of methods has been introduced over the years to achieve this goal. Here, we theoretically demonstrate that a pair of cross-polarized THz pulses interacting with chiral molecules through their permanent dipole moments induces an enantioselective orientation of these molecules. This orientation persists for a long time, exceeding the duration of the THz pulses by several orders of magnitude, and its dependency on temperature and pulses' parameters is investigated. The persistent orientation may enhance the deflection of the molecules in inhomogeneous electromagnetic fields, potentially leading to viable separation techniques., Comment: 9 pages, 5 figures

The interaction between off-resonant laser pulses and excitons in monolayer transition metal dichalcogenides is attracting increasing interest as a route for the valley-selective coherent control of the exciton properties. Here, we extend the classification of the known off-resonant phenomena by unveiling the impact of a strong THz field on the excitonic resonances of monolayer MoS$_2$. We observe that the THz pump pulse causes a selective modification of the coherence lifetime of the excitons, while keeping their oscillator strength and peak energy unchanged. We rationalize these results theoretically by invoking a hitherto unobserved manifestation of the Franz-Keldysh effect on an exciton resonance. As the modulation depth of the optical absorption reaches values as large as 0.05 dB/nm at room temperature, our findings open the way to the use of semiconducting transition metal dichalcogenides as compact and efficient platforms for high-speed electroabsorption devices., Comment: 40 pages, 11 figures