Single Femtosecond Laser Pulse Research Articles

Highly Nonlinear Light-Nucleus Interaction.

The interaction between light and atomic nuclei is typically weak and confined within the linear and perturbative regime, which limits the achievable nuclear excitation probability and impedes potential applications such as nuclear optical clocks, nuclear lasers, and nuclear energy storage. In this Letter we show that the interaction between hydrogenlike thorium-229 ions (^{229}Th^{89+}) and contemporary intense lasers propels light-nucleus interaction into a highly nonlinear and nonperturbative regime. This interaction unlocks remarkably efficient nuclear excitation: over 10% of the ^{229}Th nuclei can be excited to the isomeric state by a single femtosecond laser pulse. Moreover, the laser-driven ^{229}Th^{89+} ions radiate multiple wavelengths of light that are high-order harmonics of the laser frequency, akin to the high harmonic generation process from laser-driven atoms but with distinct characteristics. These results pioneer a new frontier for exploring light-matter interaction, furnish a powerful method for efficient control over atomic nuclei, and pave a new way of nuclear coherent light emission.

Process simulation and optimization of process parameters of single-pulse femtosecond laser processing Invar 36 alloy

Invar 36 alloy has an extremely low coefficient of thermal expansion and is suitable for preparing a fine metal mask (FMM) for the evaporation of silicon-based organic light emitting display microdisplays. The higher the resolution and the greater the number of pixels, the finer and more delicate the holes required. Femtosecond laser processing technology is an effective technical means for processing Invar 36 alloy FMM due to its characteristics of extremely short pulse width, extremely high pulse energy density, smaller heat-affected zone, and more regular machining edges. The femtosecond laser processing parameters directly affect temperature distribution and then affect the manufacturing quality and efficiency of Invar 36 alloy FMM. At present, femtosecond laser processing of Invar 36 alloy FMM is still in the exploration stage, and the processing mechanism and technology are not clear. In this paper, a simulation model of single-pulse femtosecond laser processing Invar 36 alloy is established based on the two-temperature equation. By comparing the ablation morphology of the simulation output with the experimental measurement results, the validity of the simulation model is verified and the processing mechanism is preliminarily explored. Based on the simulation model, the effects of femtosecond laser energy density, pulse duration, and spot diameter on the electron temperature field, lattice temperature field, and ablation morphology of the craters are explored. The process window of laser processing parameters is determined. A full-factor test is conducted. Take the minimum length of the heat-affected zone, the maximum depth of the ablation crater, and the minimum diameter of the ablation crater as three optimization objectives and obtain Pareto optimal solutions based on genetic algorithm. The optimization of single-pulse femtosecond laser drilling Invar 36 alloy is realized.

Single-pulse ultrafast real-time simultaneous planar imaging of femtosecond laser-nanoparticle dynamics in flames

The creation of carbonaceous nanoparticles and their dynamics in hydrocarbon flames are still debated in environmental, combustion, and material sciences. In this study, we introduce single-pulse femtosecond laser sheet-compressed ultrafast photography (fsLS-CUP), an ultrafast imaging technique specifically designed to shed light on and capture ultrafast dynamics stemming from interactions between femtosecond lasers and nanoparticles in flames in a single-shot. fsLS-CUP enables the first-time real-time billion frames-per-second (Gfps) simultaneous two-dimensional (2D) imaging of laser-induced fluorescence (LIF) and laser-induced heating (LIH) that are originated from polycyclic aromatic hydrocarbons (PAHs) and soot particles, respectively. Furthermore, fsLS-CUP provides the real-time spatiotemporal map of femtosecond laser-soot interaction as elastic light scattering (ELS) at an astonishing 250 Gfps. In contrast to existing single-shot ultrafast imaging approaches, which are limited to millions of frames per second only and require multiple laser pulses, our method employs only a single pulse and captures the entire dynamics of laser-induced signals at hundreds of Gfps. Using a single pulse does not change the optical properties of nanoparticles for a following pulse, thus allowing reliable spatiotemporal mapping. Moreover, we found that particle inception and growth are derived from precursors. In essence, as an imaging modality, fsLS-CUP offers ultrafast 2D diagnostics, contributing to the fundamental understanding of nanoparticle’s inception and broader applications across different fields, such as material science and biomedical engineering.

Pulse-doubling perovskite nanowire lasers enabled by phonon-assisted multistep energy funneling

Laser pulse multiplication from an optical gain medium has shown great potential in miniaturizing integrated optoelectronic devices. Perovskite multiple quantum wells (MQWs) structures have recently been recognized as an effective gain media capable of doubling laser pulses that do not rely on external optical equipment. Although the light amplifications enabled with pulse doubling are reported based on the perovskite MQWs thin films, the micro-nanolasers possessed a specific cavity for laser pulse multiplication and their corresponding intrinsic laser dynamics are still inadequate. Herein, a single-mode double-pulsed nanolaser from self-assembled perovskite MQWs nanowires is realized, exhibiting a pulse duration of 28 ps and pulse interval of 22 ps based on single femtosecond laser pulse excitation. It is established that the continuous energy building up within a certain timescale is essential for the multiple population inversion in the gain medium, which arises from the slowing carrier localization process owning to the stronger exciton–phonon coupling in the smaller-n QWs. Therefore, the double-pulsed lasing is achieved from one fast energy funnel process from the adjacent small-n QWs to gain active region and another slow process from the spatially separated ones. This report may shed new light on the intrinsic energy relaxation mechanism and boost the further development of perovskite multiple-pulse lasers.

Single femtosecond laser pulse–induced valence state conversion in BaFCl: Sm3+ nanocrystals for low-threshold optical storage

Abstract Femtosecond laser-induced valence state conversion (VC) in solid materials has attracted significant research attention due to its potential application in ultra-high density optical storage, boasting advantages such as ultra-high recording speed, easy reading, and high signal-to-noise ratio. However, identifying appropriate materials and technological solutions conducive to efficient single-laser-shot recording remains a pivotal challenge for practical applications. In this work, we report single femtosecond laser pulse–induced VC in BaFCl: Sm3+ nanocrystals utilizing a 4F-configuration optical imaging system comprising two-dimensional scan galvo mirrors. For the first time, we experimentally reveal the luminescence mechanisms and channels of multiphoton absorption-induced Sm2+ ions under both single and multiple 800 nm fs laser pulses. Leveraging the highly efficient single femtosecond laser pulse induced VC, we demonstrate a prototype optical storage experiment by sweeping the recording laser pulse. Remarkably, a threshold pulse energy as low as ∼100 nJ for effective single-laser-shot recording in BaFCl: Sm3+ nanocrystals is obtained under the current experimental conditions. Our investigations offer profound insights into the physical mechanisms underlying femtosecond laser induced VC in solid materials, thereby promoting the prospects of VC based optical storage toward practical applications.

Giant persistent photoconductivity of VO2 device by single-pulse femtosecond laser

The manifestation of giant persistent photoconductivity (GPPC) is demonstrated with a fs (femtosecond) Ti:sapphire laser pulse that has a duration of 40 fs and a central wavelength of 400 nm. The femtosecond laser pulse was irradiated on a two-terminal VO2 device fabricated on a corning glass substrate. Under the applied voltages of 9–12 V, the GPPC takes place within 8.6–15 μs after the laser irradiation. The photocurrent from the GPPC in the VO2 device remains stable with the current decreasing slope of ∼0.003%/minute. With one-dimensional thermal model, the temperature (TIR) of the irradiated area is estimated as a function of time, indicating that TIR is above the insulation-to-metal transition temperature of VO2 thin film prior to the onset of GPPC. The ultrafast onset of GPPC of VO2 device can be utilized for ultrafast optoelectronic switch and memory device.

Single-Shot Laser-Induced Switching of an Exchange Biased Antiferromagnet.

Ultrafast manipulation of magnetic order has challenged the understanding of the fundamental and dynamic properties of magnetic materials. So far single-shot magnetic switching has been limited to ferrimagnetic alloys, multilayers, and designed ferromagnetic (FM) heterostructures. In FM/antiferromagnetic (AFM) bilayers, exchange bias (He) arises from the interfacial exchange coupling between the two layers and reflects the microscopic orientation of the antiferromagnet. Here the possibility of single-shot switching of the antiferromagnet (change of the sign and amplitude of He) with a single femtosecond laser pulse in IrMn/CoGd bilayers is demonstrated. The manipulation is demonstrated in a wide range of fluences for different layer thicknesses and compositions. Atomistic simulations predict ultrafast switching and recovery of the AFM magnetization on a timescale of 2 ps. The results provide the fastest and the most energy-efficient method to set the exchange bias and pave the way to potential applications for ultrafast spintronic devices.

Single femtosecond pulse writing of a bifocal lens.

In this Letter, a method for the fabrication of bifocal lenses is presented by combining surface ablation and bulk modification in a single laser exposure followed by the wet etching processing step. The intensity of a single femtosecond laser pulse was modulated axially into two foci with a designed computer-generated hologram (CGH). Such pulse simultaneously induced an ablation region on the surface and a modified volume inside the fused silica. After etching in hydrofluoric acid (HF), the two exposed regions evolved into a bifocal lens. The area ratio (diameter) of the two lenses can be flexibly adjusted via control of the pulse energy distribution through the CGH. Besides, bifocal lenses with a center offset as well as convex lenses were obtained by a replication technique. This method simplifies the fabrication of micro-optical elements and opens a highly efficient and simple pathway for complex optical surfaces and integrated imaging systems.

Room-temperature sub-100 nm Néel-type skyrmions in non-stoichiometric van der Waals ferromagnet Fe3-xGaTe2 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 Fe3GaTe2 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 Fe3-xGaTe2 using a single femtosecond laser pulse. Our results manifest the Fe3-xGaTe2 as a promising building block for realizing skyrmion-based magneto-optical functionalities.

Unveiling Coherent Control of Halomethane Dissociation Induced by a Single Strong Ultraviolet Pulse.

We present a theoretical investigation into the coherent control of photodissociation reactions in halomethanes, specifically focusing on CH2BrCl by manipulating the spectral phase of a single femtosecond laser pulse. We examine the photodissociation of CH2BrCl under an ultrashort pulse with a quadratic spectral phase and reveal the sensitivity of both the total dissociation probability and the resulting radical products (Br+CH2Cl and Cl+CH2Br) to chirp rates. To gain insights into the underlying mechanism, we calculate the population distributions of excited vibrational states in the ground electronic state, demonstrating the occurrence of resonance Raman scattering (RRS) in the strong-field limit regime. By utilizing chirped pulses, we show that this RRS phenomenon can be suppressed and even eliminated through quantum destructive interference. This highlights the high sensitivity of photodissociation into Cl+CH2Br to the spectral phase, showcasing a phenomenon that goes beyond the traditional one-photon photodissociation of isolated molecules in the weak-field limit regime. These findings emphasize the importance of coherent control in the exploration and utilization of photodissociation in polyatomic molecules, paving the way for new advancements in chemical physics and femtochemistry.

Laser‐Induced Positional and Chemical Lattice Reordering Generating Ferromagnetism

AbstractAtomic scale reordering of lattices can induce local modulations of functional material properties, such as reflectance and ferromagnetism. Pulsed femtosecond laser irradiation enables lattice reordering in the picosecond range. However, the dependence of the phase transitions on the initial lattice order as well as the temporal dynamics of these transitions remain to be understood. This study investigates the laser‐induced atomic reordering and the concomitant onset of ferromagnetism in thin Fe‐based alloy films with vastly differing initial atomic orders. The optical response to single femtosecond laser pulses on selected prototype systems, one that initially possesses positional disorder, Fe60V40, and a second system initially in a chemically ordered state, Fe60Al40, has been tracked with time. Despite the vastly different initial atomic orders the structure in both systems converges to a positionally ordered but chemically disordered state, accompanied by the onset of ferromagnetism. Time‐resolved measurements of the transient reflectance combined with simulations of the electron and phonon temperatures reveal that the reordering processes occur via the formation of a transient molten state with an approximate lifetime of 200 ps. These findings provide insights into the fundamental processes involved in laser‐induced atomic reordering, paving the way for controlling material properties in the picosecond range.

Dielectric breakdown and sub-wavelength patterning of monolayer hexagonal boron nitride using femtosecond pulses

Hexagonal boron nitride (hBN) has emerged as a promising two-dimensional (2D) material for many applications in electronics and photonics. Although its linear and nonlinear optical properties have been extensively studied, the interaction of hBN with high-intensity laser pulses, which is important for realizing high-harmonic generation, creating deterministic defects as quantum emitters, and resist-free patterning in this material, has not been investigated. Here we report the first systematic study of dielectric breakdown in chemical vapor deposition (CVD)-grown hBN monolayers induced by single femtosecond laser pulses. We report a breakdown fluence of 0.7 J cm−2, which is at least 7× higher than that of other monolayer 2D materials. A clean removal of hBN without leaving traces behind or causing lateral damage is demonstrated. The ablation features exhibit excellent fidelity with very small edge roughness, which we attribute to its ultrahigh fracture toughness due to its heterogeneous nature with three-fold symmetry. Moreover, even though defects are known to be abundant in CVD-grown hBN, we show experimentally and theoretically that its nonlinear optical breakdown is nearly intrinsic as defects only marginally lower the breakdown threshold. On top of this, we observe that hBN monolayers have a 4–5× lower breakdown threshold than their bulk equivalent. The last two observations can be understood if the carrier generation in monolayers is intrinsically enhanced due to its 2D nature. Finally, we demonstrate laser patterning of array of holes and lines in hBN with sub-wavelength feature sizes. Our work advances the fundamental knowledge of light-hBN interaction in the strong field regime and firmly establishes femtosecond lasers as novel and promising tools for resist-free patterning of hBN monolayers with high fidelity.

Ultrafast antiferromagnet rearrangement in Co/IrMn/CoGd trilayers

Antiferromagnets offer great potential for high-speed data processing applications, as they can expend spintronic devices from a static storage and gigahertz frequency range to the terahertz range. However, their zero net magnetization makes them difficult to manipulate and detect. In recent years, there has been a lot of attention given to the ultrafast manipulation of magnetic order using ultra-short single laser pulses, but it remains unknown whether a similar scenario can be observed in antiferromagnets. In this work, we demonstrate the manipulation of antiferromagnets with a single femtosecond laser pulse in perpendicular exchange-biased Co/IrMn/CoGd trilayers. We study the dual exchange bias interlayer interaction in quasi-static conditions and competition in ultrafast antiferromagnet rearrangement. Our results show that, compared to conventional ferromagnetic/antiferromagnetic systems, the IrMn antiferromagnet can be ultrafast and efficiently manipulated by the coupled CoGd ferrimagnetic layer, which paves the way for potential energy-efficient spintronic devices.

Numerical simulation and investigation of ultra-short pulse laser ablation on Ti6Al4V and stainless steel

In ultra-short pulse laser machining and micro/surface processing, accurate simulation of laser ablation is important for understanding laser-target interaction and improving ablation performance, but it remains challenging. This work aims to develop a numerical model to improve the accuracy of the ablation depth calculation. A grid deformation scheme is proposed based on energy conservation and considering contributions to instant material removal from both the electron and lattice subsystems. By incorporating this scheme with the two-temperature model (TTM), a reasonable prediction of the instant target surface profile during laser ablation has been achieved. In the case of single-pulse femtosecond laser ablation of Ti6Al4V, the calculated ablation depth ranges from 0.06 to 0.56 μm for laser energy from 1.0 to 10.0 μJ. For single-pulse picosecond laser ablation of stainless steel, as laser energy increases from 6.0 to 18.5 μJ, the predicted ablation crater deepens accordingly from 40 to 87 nm. In addition, for multi-pulse picosecond laser ablation of stainless steel, a linear dependence of the ablation depth on the pulse number is observed up to a depth of about 803 nm at 6.0 μJ and 20 pulses. In all the above-mentioned cases, the calculation results are in better agreement with experimental measurements than conventional TTM or other material removal schemes, validating the accuracy of the proposed model.

Dependence of the Gd concentration range for thermally induced magnetization switching on the intrinsic damping

Ultrafast magnetization switching induced by a single femtosecond laser pulse in the absence of an applied magnetic field has attracted extensive attention due to its great potential for low energy and ultrafast storage applications. However, pulse helicity-independent switching is mainly used for Gd-based materials, and it is now necessary to explore the possibility of further optimization depending on the composition and damping coefficients. For the GdFe alloy with low Gd concentration, we modulate the damping constant for a comparative analysis based on atomic spin simulations. The simulation results show that an appropriate increase in the high damping ratio αFe/αGd not only helps to extend the pulse fluence range for switching but also reduces the minimum Gd concentration requirement for transient ferromagnetic-like state. The results show that the pulse fluence threshold of switching at low Gd concentration is more sensitive to the damping ratio αFe/αGd. On the contrary, modulating the damping ratio αFe/αGd at high Gd concentrations almost does not cause the shift of pulse fluence threshold. The lower Gd concentration for thermally induced magnetization switching is expected to be unlocked by the engineering of element-specific damping.

Two-temperature model for ultrafast melting of Au-based bimetallic films interacting with single-pulse femtosecond laser: Theoretical study of damage threshold

Ultrashort-pulse laser excitation and associated thermal damage of single-layer metallic films have been extensively studied both theoretically as well as experimentally. However, study of ultrafast heat transfer mechanism in bimetallic films, a topic of immense current interest for designing next-generation optical components with better thermal resilience, is limited to a low fluence regime. Moreover, available results for damage threshold (DT) of bimetallic films have several ambiguities. The current work is an attempt towards development of comprehensive theory for the DT of Au-based bimetallic films, analyzing its dependence on associated physical parameters and bridging the gap in existing literature. This has been achieved by developing fully implicit two-temperature model-based Python code. Excellent agreement of the predicted temperature profiles with recently reported [E. L. Gurevich, Y. Levy, S. V. Gurevich, and N. M. Bulgakova, Phys. Rev. B 95, 054305 (2017)] femtosecond laser irradiated Au film validates the code. Subsequently, the code is utilized to investigate the influence of different metallic substrates, $M$ ($M$ = Ni, Cr, Cu) on ultrafast melting damage of $\mathrm{Au}\text{/}M$ films excited by single-pulse femtosecond laser. Simulations carried out for increasing Au layer thickness revealed a nonmonotonic variation of DT for all substrates. This study also brought out an important observation that for every substrate metal, there exists an optimum Au thickness for maximizing the incipient and the complete melting threshold. Maximum achievable enhancement for $\mathrm{Au}\text{/}M$ films over pure Au are found to be 30%, 22%, and 14% with Cu, Ni, and Cr substrates, respectively. The observed distinction in maximum DT among three different $\mathrm{Au}\text{/}M$ targets is explained by developing appropriate thermophysical models. Finally, an empirical function is proposed here for expressing nonmonotonic variation of two-layer DTs. Very good agreement between the substrate-specific peak positions predicted by the proposed function and effective electron diffusion length arising from thermophysical analysis makes the modeling robust and applicable for a wide range of laser wavelengths as well as arbitrary combinations of bimetallic films.

Formation Mechanism of Elemental Te Produced in Tellurite Glass Systems by Femtosecond Laser Irradiation.

The formation of elemental trigonal tellurium (t-Te) on tellurite glass surfaces exposed to femtosecondlaser pulses is discussed. Specifically, the underlying elemental crystallization phenomenon is investigated by altering laser parameters in common tellurite glass compositions under various ambient conditions. Elemental crystallization of t-Te by a single femtosecond laser pulse is unveiled by high-resolution imaging and analysis. The thermal diffusion model reveals the absence of lattice melting upon a single laser pulse, highlighting the complexity of the phase transformation. The typical cross-section displays three different crystal configurations over its depth, in which the overall thickness increases with each subsequent pulse. The effect of various controlled atmospheres shows the suppressing nature of the elemental crystallization, whereas the substrate temperature shows no significant impact on the nucleation of t-Te nanocrystals. This research gives new insight into the elemental crystallization of glass upon femtosecond laser irradiation and shows the potential to fabricate functional transparent electronic micro/nanodevices.

The Experimental and Modeling Study of Femtosecond Laser-Ablated Silicon Surface

In this study, monocrystalline silicon was ablated by a single 1030 nm femtosecond laser pulse. Variable laser fluence (0.16–3.06 J/cm2) was used, and two ablation thresholds (0.8 and 1.67 J/cm2) were determined experimentally. A two-temperature model was established based on the dynamic optical model, the carrier density model, and the phase explosion model for comparison with experimental results. The melting (0.25 J/cm2) and vaporization (0.80 J/cm2) thresholds were determined when the lattice temperature reached melting and boiling points, so as to overcome the latent heat. Finally, the ablation depth was calculated using the phase explosion model, and the ablation threshold was 1.5 J/cm2. The comparisons show that the proposed model can predict the ablation depth obtained by a single femtosecond laser pulse.

Creation of NV centers over a millimeter-sized region by intense single-shot ultrashort laser irradiation

Recently, ultrashort laser processing has attracted attention for creating nitrogen-vacancy (NV) centers because this method can create single NV centers in spatially-controlled positions, which is an advantage for quantum information devices. On the other hand, creating high-density NV centers in a wide region is also important for quantum sensing because the sensitivity is directly enhanced by increasing the number of NV centers. A recent study demonstrated the creation of high-density NV centers by irradiating femtosecond laser pulses, but the created region was limited to micrometer size, and this technique required many laser pulses to avoid graphitization of diamond. Here, we demonstrate the creation of NV centers in a wide region using only an intense single femtosecond laser pulse irradiation. We irradiated a diamond sample with a femtosecond laser with a focal spot size of 41 µm and a laser fluence of up to 54 J/cm2, which is much higher than the typical graphitization threshold in multi-pulse processing. We found that single-pulse irradiation created NV centers without post-annealing for a laser fluence higher than 1.8 J/cm2, and the region containing NV centers expanded with increasing laser fluence. The diameter of the area was larger than the focal spot size and reached over 100 µm at a fluence of 54 J/cm2. Furthermore, we demonstrated the NV centers’ creation in a millimeter-sized region by a single-shot defocused laser pulse over 1100 µm with a fluence of 33 J/cm2. The demonstrated technique will bring interest in the fundamentals and applications of fabricating ultrahigh-sensitivity quantum sensors.

Antireflection microstructures fabricated on the surface of a LiGaSe2 nonlinear crystal.

LiGaSe2 is a propitious material for nonlinear parametric conversion in the mid-infrared (mid-IR) range. Its refractive index of n = 2.25 in the 2-12 µm wavelength range results in significant losses due to Fresnel reflection. However, the conventional method of increasing the transmittance with antireflection coatings (ARCs) significantly reduces the damage threshold of the material. Fabrication of the antireflection microstructures (ARMs) is an alternative approach for increasing the surface transmittance. In this work, ARMs were fabricated on the surface of a LiGaSe2 crystal using a single-pulse femtosecond laser ablation method. An average transmittance of 97.2% in the 2-8 µm spectral range and the maximum transmittance of 98.6% at 4.1 µm were achieved.