High-power laser beam shaping using a metasurface for shock excitation and focusing at the microscale.

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.

Biasing the quantum vacuum to control macroscopic probability distributions.

Quantum field theory suggests that electromagnetic fields naturally fluctuate, and these fluctuations can be harnessed as a source of perfect randomness. Many potential applications of randomness rely on controllable probability distributions. We show that vacuum-level bias fields injected into multistable optical systems enable a controllable source of quantum randomness, and we demonstrated this concept in an optical parametric oscillator (OPO). By injecting bias pulses with less than one photon on average, we controlled the probabilities of the two possible OPO output states. The potential of our approach for sensing sub-photon-level fields was demonstrated by reconstructing the temporal shape of fields below the single-photon level. Our results provide a platform to study quantum dynamics in nonlinear driven-dissipative systems and point toward applications in probabilistic computing and weak field sensing.

Photonic flatband resonances for free-electron radiation.

Flatbands have become a cornerstone of contemporary condensed-matter physics and photonics. In electronics, flatbands entail comparable energy bandwidth and Coulomb interaction, leading to correlated phenomena such as the fractional quantum Hall effect and recently those in magic-angle systems. In photonics, they enable properties including slow light1 and lasing2. Notably, flatbands support supercollimation-diffractionless wavepacket propagation-in both systems3,4. Despite these intense parallel efforts, flatbands have never been shown to affect the core interaction between free electrons and photons. Their interaction, pivotal for free-electron lasers5, microscopy and spectroscopy6,7, and particle accelerators8,9, is, in fact, limited by a dimensionality mismatch between localized electrons and extended photons. Here we reveal theoretically that photonic flatbands can overcome this mismatch and thus remarkably boost their interaction. We design flatband resonances in a silicon-on-insulator photonic crystal slab to control and enhance the associated free-electron radiation by tuning their trajectory and velocity. We observe signatures of flatband enhancement, recording a two-order increase from the conventional diffraction-enabled Smith-Purcell radiation. The enhancement enables polarization shaping of free-electron radiation and characterization of photonic bands through electron-beam measurements. Our results support the use of flatbands as test beds for strong light-electron interaction, particularly relevant for efficient and compact free-electron light sources and accelerators.

Nonlinear Optical Absorption in Nanoscale Films Revealed through Ultrafast Acoustics.

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.

A framework for scintillation in nanophotonics.

Bombardment of materials by high-energy particles often leads to light emission in a process known as scintillation. Scintillation has widespread applications in medical imaging, x-ray nondestructive inspection, electron microscopy, and high-energy particle detectors. Most research focuses on finding materials with brighter, faster, and more controlled scintillation. We developed a unified theory of nanophotonic scintillators that accounts for the key aspects of scintillation: energy loss by high-energy particles, and light emission by non-equilibrium electrons in nanostructured optical systems. We then devised an approach based on integrating nanophotonic structures into scintillators to enhance their emission, obtaining nearly an order-of-magnitude enhancement in both electron-induced and x-ray-induced scintillation. Our framework should enable the development of a new class of brighter, faster, and higher-resolution scintillators with tailored and optimized performance.

Enabling Manufacturable Optical Broadband Angular-Range Selective Films.

The ability to control the propagation direction of light has long been a scientific goal. However, the fabrication of large-scale optical angular-range selective films is still a challenge. This paper presents a polymer-enabled large-scale fabrication method for broadband angular-range selective films that perform over the entire visible spectrum. Our approach involves stacking together multiple one-dimensional photonic crystals with various engineered periodicities to enlarge the bandgap across a wide spectral range based on theoretical predictions. Experimental results demonstrate that our method can achieve broadband transparency at a range of incident angles centered around normal incidence and reflectivity at larger viewing angles, doing so at large scale and low cost.

Fullwave Maxwell inverse design of axisymmetric, tunable, and multi-scale multi-wavelength metalenses.

We demonstrate new axisymmetric inverse-design techniques that can solve problems radically different from traditional lenses, including reconfigurable lenses (that shift a multi-frequency focal spot in response to refractive-index changes) and widely separated multi-wavelength lenses (λ = 1 µm and 10 µm). We also present experimental validation for an axisymmetric inverse-designed monochrome lens in the near-infrared fabricated via two-photon polymerization. Axisymmetry allows fullwave Maxwell solvers to be scaled up to structures hundreds or even thousands of wavelengths in diameter before requiring domain-decomposition approximations, while multilayer topology optimization with ∼105 degrees of freedom can tackle challenging design problems even when restricted to axisymmetric structures.

Self-Limiting Electrospray Deposition for the Surface Modification of Additively Manufactured Parts.

Electrospray deposition (ESD) is a spray coating process that utilizes a high voltage to atomize a flowing solution into charged microdroplets. These self-repulsive droplets evaporate as they travel to a target substrate, depositing the solution solids. Our previous research investigated the conditions necessary to minimize charge dissipation and deposit a thickness-limited film that grows in area over time through self-limiting electrospray deposition. Such sprays possess the ability to conformally coat complex three-dimensional (3D) objects without changing the location of the spray needle or orientation of the object. This makes them ideally suited for the postprocessing of materials fabricated through additive manufacturing (AM), opening a paradigm of independent bulk and surface functionality. Having demonstrated 3D coating with film thickness in the range of 1-50 µm on a variety of conductive objects, in this study, we employed model substrates to quantitatively study the technique's limits with regard to geometry and scale. Specifically, we examined the effectiveness of thickness-limited ESD for coating recessed features with gaps ranging from 50 µm to 1 cm, as well as the ability to coat surfaces hidden from the line-of-sight of the spray needle. This was then extended to the coating of hydrogel structures printed by AM, demonstrating that coating could be conducted even into the body of the structures as a means to create hydrophobic surfaces without affecting the absorption-driven humidity response. Further, these coatings were robust enough to create superhydrophobicity in the entire structure, causing it to resist immersion in water.

Multi-frame interferometric imaging with a femtosecond stroboscopic pulse train for observing irreversible phenomena.

We describe a high-speed single-shot multi-frame interferometric imaging technique enabling multiple interferometric images with femtosecond exposure time over a 50 ns event window to be recorded, following a single laser-induced excitation event. The stroboscopic illumination of a framing camera is made possible through the use of a doubling cavity that produces a femtosecond pulse train that is synchronized to the gated exposure windows of the individual frames of the camera. The imaging system utilizes a Michelson interferometer to extract phase and ultimately displacement information. We demonstrate the method by monitoring laser-induced deformation and the propagation of high-amplitude acoustic waves in a silicon nitride membrane. The method is applicable to a wide range of fast irreversible phenomena such as crack branching, shock-induced material damage, cavitation, and dielectric breakdown.

Towards integrated tunable all-silicon free-electron light sources.

Extracting light from silicon is a longstanding challenge in modern engineering and physics. While silicon has underpinned the past 70 years of electronics advancement, a facile tunable and efficient silicon-based light source remains elusive. Here, we experimentally demonstrate the generation of tunable radiation from a one-dimensional, all-silicon nanograting. Light is generated by the spontaneous emission from the interaction of these nanogratings with low-energy free electrons (2-20 keV) and is recorded in the wavelength range of 800-1600 nm, which includes the silicon transparency window. Tunable free-electron-based light generation from nanoscale silicon gratings with efficiencies approaching those from metallic gratings is demonstrated. We theoretically investigate the feasibility of a scalable, compact, all-silicon tunable light source comprised of a silicon Field Emitter Array integrated with a silicon nanograting that emits at telecommunication wavelengths. Our results reveal the prospects of a CMOS-compatible electrically-pumped silicon light source for possible applications in the mid-infrared and telecommunication wavelengths.

Dynamic Strengthening of Carbon Nanotube Fibers under Extreme Mechanical Impulses.

A monofilament fiber spun from individual carbon nanotubes is an arbitrarily long ensemble of weakly interacting, aligned, discrete nanoparticles. Despite the structural resemblance of carbon nanotube monofilament fibers to crystalline polymeric fibers, very little is known about their dynamic collective mechanics, which arise from van der Waals interactions among the individual carbon nanotubes. Using ultrafast stroboscopic microscopy, we study the collective dynamics of carbon nanotube fibers and compare them directly with nylon, Kevlar, and aluminum monofilament fibers under the same supersonic impact conditions. The in situ dynamics and kinetic parameters of the fibers show that the kinetic energy absorption characteristics of the carbon nanotube fibers surpass all other fibers. This study provides insight into the strain-rate-dependent strengthening mechanics of an ensemble of nanomaterials for the development of high-performance fibers used in body armor and other protective nanomaterials possessing exceptional stability in various harsh environments.

Single-Shot Multi-Frame Imaging of Cylindrical Shock Waves in a Multi-Layered Assembly.

We demonstrate single-shot multi-frame imaging of quasi-2D cylindrically converging shock waves as they propagate through a multi-layer target sample assembly. We visualize the shock with sequences of up to 16 images, using a Fabry-Perot cavity to generate a pulse train that can be used in various imaging configurations. We employ multi-frame shadowgraph and dark-field imaging to measure the amplitude and phase of the light transmitted through the shocked target. Single-shot multi-frame imaging tracks geometric distortion and additional features in our images that were not previously resolvable in this experimental geometry. Analysis of our images, in combination with simulations, shows that the additional image features are formed by a coupled wave structure resulting from interface effects in our targets. This technique presents a new capability for tabletop imaging of shock waves that can be extended to experiments at large-scale facilities.

High-velocity micro-particle impact on gelatin and synthetic hydrogel.

The high-velocity impact response of gelatin and synthetic hydrogel samples is investigated using a laser-based microballistic platform for launching and imaging supersonic micro-particles. The micro-particles are monitored during impact and penetration into the gels using a high-speed multi-frame camera that can record up to 16 images with nanosecond time resolution. The trajectories are compared with a Poncelet model for particle penetration, demonstrating good agreement between experiments and the model for impact in gelatin. The model is further validated on a synthetic hydrogel and the applicability of the results is discussed. We find the strength resistance parameter in the Poncelet model to be two orders of magnitude higher than in macroscopic experiments at comparable impact velocities. The results open prospects for testing high-rate behavior of soft materials on the microscale and for guiding the design of drug delivery methods using accelerated microparticles.

Insights into Magneto-Optics of Helical Conjugated Polymers.

Materials with magneto-optic (MO) properties have enabled critical fiber-optic applications and highly sensitive magnetic field sensors. While traditional MO materials are inorganic in nature, new generations of MO materials based on organic semiconducting polymers could allow increased versatility for device architectures, manufacturing options, and flexible mechanics. However, the origin of MO activity in semiconducting polymers is far from understood. In this paper, we report high MO activity observed in a chiral helical poly-3-(alkylsulfone)thiophene (P3AST), which confirms a new design for the creation of a giant Faraday effect with Verdet constants up to (7.63 ± 0.78) × 104 deg T-1 m-1 at 532 nm. We have determined that the sign of the Verdet constant and its magnitude are related to the helicity of the polymer at the measured wavelength. The Faraday rotation and the helical conformation of P3AST are modulated by thermal annealing, which is further supported by DFT calculations and MD simulations. Our results demonstrate that helical polymers exhibit enhanced Verdet constants and expand the previous design space for polythiophene MO materials that was thought to be limited to highly regular lamellar structures. The structure-property studies herein provide insights for the design of next-generation MO materials based upon semiconducting organic polymers.

Corrigendum: Dynamics of supersonic microparticle impact on elastomers revealed by real-time multi-frame imaging.

This corrects the article DOI: 10.1038/srep25577.

Dynamics and extreme plasticity of metallic microparticles in supersonic collisions.

Metallic microparticles can acquire remarkable nanoscale morphologies after experiencing high velocity collisions, but materials science regarding the extreme events has been limited due to a lack of controlled experiments. In this work, collision dynamics and nonlinear material characteristics of aluminum microparticles are investigated through precise single particle collisions with two distinctive substrates, sapphire and aluminum, across a broad range of collision velocities, from 50 to 1,100 m/s. An empirical constitutive model is calibrated based on the experimental results, and is used to investigate the mechanics of particle deformation history. Real-time and post-impact characterizations, as well as model based simulations, show that significant material flow occurs during the impact, especially with the sapphire substrate. A material instability stemming from plasticity-induced heating is identified. The presented methodology, based on the use of controlled single particle impact data and constitutive models, provides an innovative approach for the prediction of extreme material behavior.

Interferometric analysis of laser-driven cylindrically focusing shock waves in a thin liquid layer.

Shock waves in condensed matter are of great importance for many areas of science and technology ranging from inertially confined fusion to planetary science and medicine. In laboratory studies of shock waves, there is a need in developing diagnostic techniques capable of measuring parameters of materials under shock with high spatial resolution. Here, time-resolved interferometric imaging is used to study laser-driven focusing shock waves in a thin liquid layer in an all-optical experiment. Shock waves are generated in a 10 µm-thick layer of water by focusing intense picosecond laser pulses into a ring of 95 µm radius. Using a Mach-Zehnder interferometer and time-delayed femtosecond laser pulses, we obtain a series of images tracing the shock wave as it converges at the center of the ring before reemerging as a diverging shock, resulting in the formation of a cavitation bubble. Through quantitative analysis of the interferograms, density profiles of shocked samples are extracted. The experimental geometry used in our study opens prospects for spatially resolved spectroscopic studies of materials under shock compression.

Dynamics of supersonic microparticle impact on elastomers revealed by real-time multi-frame imaging.

Understanding high-velocity microparticle impact is essential for many fields, from space exploration to medicine and biology. Investigations of microscale impact have hitherto been limited to post-mortem analysis of impacted specimens, which does not provide direct information on the impact dynamics. Here we report real-time multi-frame imaging studies of the impact of 7 µm diameter glass spheres traveling at 700-900 m/s on elastomer polymers. With a poly(urethane urea) (PUU) sample, we observe a hyperelastic impact phenomenon not seen on the macroscale: a microsphere undergoes a full conformal penetration into the specimen followed by a rebound which leaves the specimen unscathed. The results challenge the established interpretation of the behaviour of elastomers under high-velocity impact.

Assembly of a bacteriophage-based template for the organization of materials into nanoporous networks.

M13 bacteriophages are assembled via a covalent layer-by-layer process to form a highly nanoporous network capable of organizing nanoparticles and acting as a scaffold for templating metal-oxides. The morphological and optical properties of the film itself are presented as well as its ability to organize and disperse metal nanoparticles.

Direct-write thermocapillary dewetting of polymer thin films by a laser-induced thermal gradient.

A positive-tone 2D direct-write technique that can achieve sub-wavelength patterning by non-linear overlap effects in a conventional polymer system is described. The technique involves relatively inexpensive free-space optics, skips the usual development step, and promises the possibility of a lithographic method that is solvent-free.