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Demonstration of and future perspective on scaling ultrafast-laser-ablation microstructuring of Li-ion battery electrodes to roll-to-roll production and large-format cells
This work demonstrates integration of an ultrafast laser onto a roll-to-roll machine, the laser structuring of a double-sided, 700 m long roll of graphite battery anode and its subsequent manufacture into 27 Ah prismatic cells. The electrode was ablated with a novel hybrid-microstructure composed of both hexagonally arranged pores for enhanced rate performance and channels for fast electrolyte wetting. Subsequently, this anode and a non-ablated baseline anode are paired with an NMC111 cathode for cell building and electrochemical characterization. Compared to the baseline, laser ablated cells demonstrated a reduction in soaking time of at least 60%, an improvement in fast charge capability with >30% more capacity accepted during 6C charging, and an extension of cycle life of >40% during 0.5C cycling. Further, a perspective is provided on scaling ultrafast laser ablation of battery electrodes to industrial throughputs. Additionally, lessons learned from this pilot-scale demonstration are provided in regards to optical architecture, debris removal, and system control. A techno-economic analysis is used to demonstrate that laser ablation can be integrated into existing electrode manufacturing facilities with only ≈$\$$1.3 per kWh increase (≈2%) in manufacturing cost. Preemptive electrode design for laser ablation is discussed as a further method for enhancing performance. Finally, an analysis of available laser systems and beam-scanning architectures is used to determine design requirements to scale process throughput to a state-of-the-art speed of 50 m min −1 . This analysis demonstrates that laser ablating Li-ion battery electrodes has multiple benefits to manufacturing and battery performance, that the technology already exists to achieve high laser-ablation throughputs, and that integrating ultrafast laser ablation to electrode manufacturing will not create a cost or processing bottleneck.
ULMA Fiber Laser Harnesses for High Intensity Ultrafast Lasers
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Ultrafast laser triggered electron emission from ultrananocrystalline diamond pyramid tip cathode
Nitrogen-incorporated ultrananocrystalline diamond [(N)UNCD] pyramid tip cathode has been considered as a next-generation high peak current electron source for dielectric laser accelerators as well as other high peak current particle accelerator applications. In this work, we study non-linear photoemission from an (N)UNCD pyramid tip cathode using an ultrafast laser with the pulse length of 150 fs with the central wavelength of 800 nm in the peak intensity range of 10 9 –10 10 W/cm 2 . We demonstrated that as the incident laser intensity increases, the current emitted from the nano-tip first increases as a power function with an exponent of about 5 and then starts to roll over to an exponent of 3. This roll over is attributed to the Coulomb interaction between electrons emitted from the tip also known as the space charge. We also measured the photoemission electron energy spectra that show electrons with energies as high as ~10 eV. Based on the shape of the electron energy spectra, we conclude that the high-energy electrons are thermally emitted electrons due to ultrafast laser heating at the tip of the (N)UNCD pyramid tip cathode.
Toward high-power terahertz radiation sources based on ultrafast lasers
A breakthrough to achieve high-power THz sources is needed. This review covers recent advancements in laser-based THz generation, specifically using ultrafast lasers.
Direct reuse of graphite and lithium nickel manganese cobalt oxide (NMC) recovered from ultrafast-laser ablation debris in Li-ion battery electrodes
Here we demonstrate that debris collected from the ultrafast-laser ablation of graphite anodes can be directly reused in a lithium-ion battery with little to no negative effects on electrochemical performance. Further, we show that while post-ablation NMC (LiNi 0.33 Mn 0.33 Co 0.33 O) cathode debris will require additional processing before being incorporated into an electrode, its critical materials (nickel, manganese, and cobalt) are not lost during ablation and can be recovered for recycling. Pre- and post-ablation materials are characterized with a suite of diagnostics, including SEM, TEM, X-ray CT, EDS, and XRD, to study changes in material morphology, composition and crystal structure. Graphite exhibited little to no morphological or compositional changes and a slight annealing of its crystal structure. NMC underwent profound morphological and crystallographic changes, but retained its elemental composition. Finally, post-ablation materials were re-manufactured into electrodes and cycled vs lithium metal. Graphite showed equal or better capacity and Coulombic efficiency compared to pre-ablation electrodes, while the post-ablation NMC exhibited severely reduced electrochemical performance. Furthermore, we discuss the outlook for application of this work to advanced manufacturing lines that produce next-generation, laser-patterned electrodes.
Characterization of ultrafast-laser ablation of micro-structures in Li-ion battery anode and cathode materials: Morphology, rate, and efficiency
Characterization of the rate and quality of ultrafast-laser ablation of Li-ion battery (LIB) electrode materials is presented for a collection of common and next-generation electrodes. Laser ablated micro-structures on the surface of LIB electrodes have been shown to provide dramatic enhancement of high-rate capability and electrode wetting. However, industrial adoption is hampered by a lack of data enabling informed choice of laser parameters and predicting process throughput. Here this work bridges this gap by providing characterization of the ablation process at more laser parameters (laser fluence and number of pulses used) than are currently available in the literature. Further, we expand on previous graphite and lithium iron phosphate (LFP) ablation work by extending ablation characterization to new LIB materials, providing high data resolution and adopting new characterization metrics which are relevant for industrial application of this technology. Ablated pores are characterized by their ablated depth, volume, and how the depth and volume ablation rate changes as a function of pore depth. Finally, we provide a detailed characterization of the morphology of laser ablated micro-structures which informs how material and laser parameters affect the quality of laser-processed electrodes.
Soft x-ray high-harmonic generation in an anti-resonant hollow core fiber driven by a 3 μ m ultrafast laser
High-harmonic upconversion driven by a mid-infrared femtosecond laser can generate coherent soft x-ray beams in a tabletop-scale setup. Here, we report on a compact ytterbium-pumped optical parametric chirped pulse amplifier (OPCPA) laser system seeded by an all-fiber front-end and employing periodically poled lithium niobate (PPLN) nonlinear media operated near the pulse fluence limits of current commercially available PPLN crystals. The OPCPA delivers 3 µm wavelength pulses with 775 µJ energy at 1 kHz repetition rate, with transform-limited 120 fs pulse duration, diffraction-limited beam quality, and ultrahigh 0.33% rms energy stability over >18 h. Using this laser, we generate soft x-ray high harmonics (HHG) in argon gas by focusing into a low-loss, high-pressure gas-filled anti-resonant hollow core fiber (ARHCF), generating coherent light at photon energies up to the argon L-edge (250 eV) and carbon K-edge (284 eV), with high beam quality and ∼1% rms energy stability. This work demonstrates soft x-ray HHG in a high-efficiency guided-wave phase matched geometry, overcoming the high losses inherent to mid-IR propagation in unstructured waveguides, or the short interaction lengths of gas cells or jets. The ARHCF can operate in the long term without damage and with the repetition rate, stability, and robustness required for demanding applications in spectromicroscopy and imaging. Finally, we discuss routes for further optimizing the soft x-ray HHG flux by driving He at higher laser intensities using either the signal (1.5 μm) or idler wavelengths (3 μm).
Proton beam enhancements from ultrafast laser interactions with compound parabolic concentrators
Target normal sheath acceleration (TNSA) is among the most widely studied laser–plasma ion acceleration mechanisms. In this Letter, we report on studies of proton acceleration from flat Cu targets with cone-like focusing structures called compound parabolic concentrators (CPCs) coupled to their front surface. The CPC acts as a non-imaging focusing optic that enhances the laser intensity at the target's front surface by ∼2×, from 9 × 10 18 to 2 × 10 19 W/cm 2 . This effect drives a reduction in the particle source size from the typical laser spot size of 120 μm to the CPC tip size of 65 μm and significant enhancements in the peak energy and temperature (2.6 × increase) of the resulting TNSA proton beam. We also observe increased opening angle of the beam. 2D PIC simulations have been conducted and replicate the experimental behavior. These increases have implications for long focal length facilities that require higher energy proton beams, which now can be achieved without significant infrastructure changes.
Impact of ultrafast laser pulse repetition rate on filament acoustic and emission signatures
Femtosecond filaments formed at standoff distances can be used for interrogating various types of matter, making them of potential interest for remote sensing. However, the physical aspects of the filaments generated at standoff distances are influenced by various environmental and laser properties, including the repetition rate of the laser. In this study, we evaluate the role of the predecessor pulse on the properties of filaments by varying the repetition rate of the laser in the range of 10–1000 Hz and using acoustic and emission signatures to diagnose filament properties. Our results show that filaments are brighter at high repetition rates while they are elongated at low repetition rates. The repetition rate has minimal influence on the downstream edge of the filament generation, while the upstream edge becomes elongated. The shadowgram images showed that the turbulence generated by the predecessor pulse may influence the next pulse when the laser is operating at high repetition rates.
Technology for Ultrafast Lasers at 2-μm Wavelength Final Report
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Room-temperature sub-100 nm Néel-type skyrmions in non-stoichiometric van der Waals ferromagnet Fe 3-$x$ GaTe 2 with ultrafast laser writability
Realizing room-temperature magnetic skyrmions in two-dimensional van der Waals ferromagnets offers unparalleled prospects for future spintronic applications. However, due to the intrinsic spin fluctuations that suppress atomic long-range magnetic order and the inherent inversion crystal symmetry that excludes the presence of the Dzyaloshinskii-Moriya interaction, achieving room-temperature skyrmions in 2D magnets remains a formidable challenge. In this study, we target room-temperature 2D magnet Fe 3 GaTe 2 and unveil that the introduction of iron-deficient into this compound enables spatial inversion symmetry breaking, thus inducing a significant Dzyaloshinskii-Moriya interaction that brings about room-temperature Néel-type skyrmions with unprecedentedly small size. To further enhance the practical applications of this finding, we employ a homemade in-situ optical Lorentz transmission electron microscopy to demonstrate ultrafast writing of skyrmions in Fe 3-$x$ GaTe 2 using a single femtosecond laser pulse. Our results manifest the Fe 3-$x$ GaTe 2 as a promising building block for realizing skyrmion-based magneto-optical functionalities.
Ultrafast Laser Welding and Terahertz Time-domain Spectroscopy of Soda Lime Silicate Glass
Joining and welding techniques of similar and dissimilar materials have reached their limits due to the inflexibility of adapting dielectric materials, e.g., glasses and ceramics, reproducibility for transparent materials, and cycle process time. The ability to join pieces of glasses using laser irradiation allows rapid processing of vacuum insulating glass (VIG) for a widening range of commercial energy-efficient applications. We have used a 1064-nm laser wavelength with 15 picoseconds pulse width and a 155-kHz repetition rate to weld commercial plate glass pieces. The welded samples were characterized via x-ray fluorescence (XRF), time-of-flight secondary ion mass spectrometry (TOF–SIMS), polarimetry, and terahertz time-domain spectroscopy (THz-TDS) to determine the integrity of the weld and chemical changes in the welded areas. Our data shows no significant changes in glass chemistry and structure on average over nano- to micro-scales occurred from the welding process within the limits of the characterization tools. Our results demonstrate successful welding of glass plates without significant changes in the glass chemistry, structure, or properties in the laser-modified region or strains in the bulk glass.
High-throughput homogenization of a quasi-Gaussian ultrafast laser beam using a combined refractive beam shaper and spatial light modulator
Efficiently shaping femtosecond, transverse Gaussian laser beams to flat-top beams with flat wavefronts is critical for large-scale material processing and manufacturing. Existing beam shaping devices fall short either in final beam homogeneity or efficiency. Here, we present an approach that uses refractive optics to perform the majority of the beam shaping and then uses a fine-tune device (spatial light modulator) to refine the intensity profile. For the beam that we selected, circularly asymmetric with intensity fluctuations, our method achieved a uniformity of 0.055 within 90% of the beam area at 92% efficiency. The optimization involved an iterative beam shaping process that converged to optimum within 10 iterations.
Pulse duration dependent effects of ultrafast laser induced damage on a 1030 nm multi-layer dielectric mirror for high repetition rate, high average power laser systems
High repetition rate, high peak, and average power laser systems are crucial for next-generation particle accelerators, inertial confinement fusion, and secondary particle sources. These applications demand durable laser optics, particularly interference coatings on optics lasting millions of shots at high fluence. This study focuses on designing, testing, and simulating multi-layer dielectric (MLD) mirrors for pulse durations of 260 fs, 77 fs, and 25 fs at 1030 nm wavelength and 45-degree incidence angle with p -polarization. S-on-1 laser-induced damage thresholds (LIDT) for varying pulse numbers were determined, with single-shot LIDT values of 0.98 Jcm -2 , 1.63 Jcm -2 , and 2.3 Jcm -2 for 25 fs, 77 fs, and 260 fs respectively. A strong correlation between blister shape and local fluence was observed, implying that the layer expansion in a blister depends on local fluence. We have also examined mechanisms responsible for laser-induced stress generation and energy release rates in blister formation. Damage mechanisms are further explored by finite-difference time-domain (FDTD) simulations, incorporating Keldysh strong field ionization, whose predictions were in excellent agreement with the onset of damage determined experimentally. These findings offer insights for enhancing MLD coating technology, promising more efficient and resilient laser systems for diverse scientific and industrial applications.
Joint Experimental and Computational Characterization of Sum-Frequency Generation between a Continuous Wave Laser and an Ultrafast Frequency Comb Laser for Tunable Laser Development
Ultrafast optical frequency combs allow for both high spectral and temporal resolution in molecular spectroscopy and have become a powerful tool in many areas of chemistry and physics. Ultrafast lasers and frequency combs generated from ultrafast mode-locked lasers often need to be converted to other wavelengths. Commonly used wavelength conversions are optical parametric oscillators, which require an external optical cavity, and supercontinuum generation combined with optical parametric amplifiers. Whether commercial or home-built, these systems are complex and costly. Here, we investigate an alternative, simple, and easy-to-implement approach to tunable frequency comb ultrafast lasers enabled by new continuous-wave laser technology. Sum-frequency generation between an Nd:YAG continuous-wave laser and a Yb:fiber femtosecond frequency comb in a beta-barium borate (BBO) crystal is explored. The resulting sum-frequency beam is a pulsed frequency comb with the same repetition rate as the Yb:fiber source. SNLO simulation software is used to simulate the results and provide benchmarks for designing future systems to achieve wavelength conversion and tunability in otherwise difficult-to-reach spectral regions.
Nanoscale ultrafast lattice modulation with a free-electron laser
Ultrafast optical laser-based techniques have enabled the probing of atomistic processes at their intrinsic temporal scales with femto- and attosecond resolution. However, the long wavelengths of optical lasers have prevented their interrogation and manipulation with nanoscale spatial specificity. Advances in hard X-ray free-electron lasers have enabled progress in developing X-ray transient-grating spectroscopy, a technique that aims to coherently control elementary excitations with nanoscale X-ray standing waves. Thus far, the realization of this technique at the nanoscale has been a challenge. Here we demonstrate X-ray transient-grating spectroscopy with spatial periods of the order of 10 nm via the subfemtosecond synchronization of two hard X-ray pump pulses at a precisely controlled crossing angle. This creates a thermal grating and preferentially excites coherent longitudinal acoustic phonon modes with the transient-grating wavevector. On probing with a third, variably delayed, X-ray pulse with the same photon energy, time-and-wavevector-resolved measurements of the modulation of the induced scattering intensity provide evidence of ballistic thermal transport at nanometre scales. Finally, these results highlight the potential of X-ray transient gratings as a powerful platform for studying nanoscale transport in condensed matter and the coherent control of nanoscale dynamics.
Ultrafast Reactive Laser Sintering of Highly Conductive Garnet-Type LLZTO Solid Electrolytes
Rapid and scalable fabrication of garnet-type solid electrolytes remains a major challenge for the practical deployment of lithium metal batteries. Here, we report reactive laser sintering (RLS) as an ultrafast and potentially scalable strategy for fabricating garnet-type Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) solid electrolytes. RLS of LLZTO enables simultaneous reaction and densification, achieving ∼95% relative density while minimizing lithium loss and suppressing secondary phase formation. Compared to conventional furnace sintering, RLS promotes enhanced grain growth and improved densification, leading to improved ionic conductivity (0.36 ± 0.08 mS cm −1 ) while maintaining comparable activation energies for Li + transport. Structural characterization by X-ray diffraction (XRD), Raman spectroscopy, and solid-state 6 Li/ 7 Li NMR confirms the formation of cubic garnet LLZTO with homogeneous microscale elemental distribution. In addition, nanoindentation measurements demonstrate that RLS preserves the mechanical properties of the garnet framework despite ultrafast localized thermal processing. By integrating simultaneous reaction and densification with tunable microstructural control, reactive laser sintering provides a promising manufacturing pathway for high-performance garnet solid electrolytes toward next-generation solid-state batteries.