Intense Femtosecond Laser Pulses Research Articles

Understanding the Seeding Pulse-Induced Optical Amplification in N 2 + Pumped by 800 NM Femtosecond Laser Pulses

Nitrogen ions pumped by intense femtosecond laser pulses present an optical gain at 391.4 nm, evident by energy amplification of an injected resonant seeding pulse. We report a time-resolved measurement of the amplification process with seeding pulses having varying intensities. It is found that the amplification factor depends on the intensity of the seeding pulse and the effective temporal window for the optical gain becomes longer by applying more intense seeding pulses. These two features are in sharp contrast with classic pump-probe experiments, pinpointing the crucial role of macroscopic coherence and its dynamics during the lasing process. We further measure the temporal profile of the amplified emission for seeding pulse injected at different time delays. A complicated temporal behavior is observed, which highlights the nature of the superfluorescence.

Nondestructive Femtosecond Laser Lithography of Ni Nanocavities by Controlled Thermo-Mechanical Spallation at the Nanoscale.

We present a new approach to femtosecond direct laser writing lithography to pattern nanocavities in ferromagnetic thin films. To demonstrate the concept, we irradiated 300 nm thin nickel films by single intense femtosecond laser pulses through glass substrate. Using a fluence above the ablation threshold, the process is destructive, leading to the formation of an ablation crater. By progressively lowering the laser fluence, the formation of closed spallation cavities below the ablation threshold is achieved. Systematic studies by the electron and optical interferometric microscopies, supported by molecular dynamics simulations, enabled us to gain an understanding of the thermo-mechanical spallation mechanism at the solid-molten interface. We achieved the fabrication of periodic arrangements of closed spallation nanocavities. Due to their topology, closed magnetic nanocavities can support unique couplings of multiple excitations (magnetic, optical, acoustic, spintronic). Thereby, they offer a unique physics playground for emerging fields in magnetism, magneto-photonic, and magneto-acoustic applications.

Ionization of carbon monoxide in intense infrared femtosecond laser pulses

Using the time-dependent Hartree-Fock method, the CO ionization in intense femtosecond laser pulses at infrared wavelengths has been investigated. We have considered a laser intensity domain (4 × 1013–1.4 × 1014 W/cm2) in which the tunneling ionization mechanism plays an important role in the intense field ionization of CO. A dominant contribution of the highest occupied molecular orbital was found.

Formation Mechanism of Excited Neutral Nitrogen Molecules Pumped by Intense Femtosecond Laser Pulses

Backward amplified spontaneous emission of neutral nitrogen molecules has been reported from laser-induced plasma filaments. The cavity-free UV emission has great potential applications in remote atmospheric sensing. However, the formation mechanism for the excited nitrogen molecules inside filaments remains controversial. Here we study the formation mechanism of excited nitrogen molecules pumped by intense femtosecond laser pulses. After modification of the electron energy distribution by inclusion of the recollision between the electron and its parent ion as well as modification of the electron collision cross section by inclusion of the secondary electron contribution, the theoretical calculations reproduce the experimental observations very well. The results clearly demonstrate that excited nitrogen molecules are generated through collisions between energetic electrons and neutral nitrogen molecules.

Giant Enhancement of Air Lasing by Complete Population Inversion in N_{2}^{+}.

A fine manipulation of population transfer among molecular quantum levels is a key technology for control of molecular processes. When a light field intensity is increased to the TW-PW cm^{-2} level, it becomes possible to transfer a population to specific excited levels through nonlinear light-molecule interaction, but it has been a challenge to control the extent of the population transfer. We deplete the population in the X^{2}Σ_{g}^{+}(v=0) state of N_{2}^{+} almost completely by focusing a dual-color (800nm and 1.6 μm) intense femtosecond laser pulse in a nitrogen gas, and make the intensity of N_{2}^{+} lasing at 391nm enhanced by 5-6 orders of magnitude. By solving a time-dependent Schrödinger equation describing the population transfer among the three lowest electronic states of N_{2}^{+}, we reveal that the X^{2}Σ_{g}^{+}(v=0) population is depleted by the vibrational Raman excitation followed by the electronic excitation A^{2}Π_{u}(v=2,3,4)←X^{2}Σ_{g}^{+}(v=1)←X^{2}Σ_{g}^{+}(v=0), resulting in the excessive population inversion between the B^{2}Σ_{u}^{+}(v=0) and X^{2}Σ_{g}^{+}(v=0) states. Our results offer a promising route to efficient population transfer among vibrational and electronic levels of molecules by a precisely designed intense laser field.

Evidence of noncollisional femtosecond laser energy deposition in dielectric materials

Electron dynamics in the bulk of large band gap dielectric crystals induced by intense femtosecond laser pulses at 800 nm is studied. With laser intensities under the ablation threshold (a few 10 TW/cm\textsuperscript{2}), electrons with unexpected energies in excess of 40-50 eV are observed by using the photoemission spectroscopy. A theoretical approach based on the Boltzmann kinetic equation including state-of-the-art modeling for various particles interactions is developed to interpret these experimental observations. A direct comparison shows that both electron heating in the bulk and a further laser field acceleration after ejection from the material contribute equivalently to the final electron energy gain. The electron heating in the bulk is shown to be significantly driven by a non-collisional process, i.e. direct multiphoton transitions between sub-bands of the conduction band. This work also sheds light on the contribution of the standard electron excitation/relaxation collisional processes, providing a new baseline to study the electron dynamics in dielectric materials and associated applications as laser material structuring.

Blueshifts of high-order harmonic generation in crystalline silicon subjected to intense femtosecond near-infrared laser pulse

We present the generation of high order harmonics in crystalline silicon subjected to intense near-infrared 30fs laser pulses. The harmonic spectrum extends from the near infrared to the extreme ultraviolet spectral region. Depending on the pulsed laser intensity, we distinguish two regimes of harmonic generation: (i) perturbative regime: electron-hole pairs born during each half-cycle of the laser pulse via multiphoton and tunnel transitions are accelerated in the laser electric field and gain kinetic energy; the electron-hole pairs then recombine in the ground state by emitting a single high-energy photon. The resultant high harmonic spectrum consists of sharp peaks at odd harmonic orders. (ii) non-perturbative regime: the intensity of the harmonics increases, their spectral width broadens and the position of harmonics shifts to shorter wavelengths. The blueshifts of high harmonics in silicon are independent on the harmonic order which may be helpful in the design of continuously tunable XUV sources.

Towards full surface Brillouin zone mapping by coherent multi-photon photoemission

We report a novel approach for coherent multi-photon photoemission in the entire Brillouin zone with infrared light that is readily implemented in a laboratory setting. We excite a solid state material, Ag(110), with intense femtosecond laser pulses to excite higher-order multi-photon photoemission; angle-resolved electron spectroscopic acquisition records photoemission at large in-plane momenta involving optical transitions from the occupied to unoccupied bands of the sample that otherwise might remain hidden by the photoemission horizon. We propose this as a complementary ultrafast method to time- and angle-resolved two-color, e.g. infrared pump and extreme ultraviolet probe, photoemission spectroscopy, with the advantage of being able to measure and control the coherent electron dynamics.

Photoinjection of fluorescent nanoparticles into intact plant cells using femtosecond laser amplifier

The introduction of nanoparticles to intact plant cells is promising as a transporting technique of a wide range of functional molecules. Among various molecular delivery methods, femtosecond laser photoinjection possesses target selectivity at a single cell level and is potentially applicable for many types of materials. However, for plant cells, the vacuoles’ turgor pressure and the thick cell wall limit the application of photoinjection to only small objects. In this work, we overcome these limitations by employing a single pulse irradiation from a femtosecond laser amplifier. After laser irradiation on intact tobacco BY-2 cells, 80 nm fluorescent nanoparticles dispersed in a cell culture medium were successfully injected into their cytoplasm. This breakthrough would lead to a vast utilization of nanoparticles containing functional molecules for single cell manipulation in plant physiological study and genetic engineering. Such an injection was observed even when the laser pulse was focused neither on the cell wall nor on the cell membrane, but beside the cells. With these results, we suggest pore formation on the cell membrane by instantaneous deformation induced by an intense femtosecond laser pulse as an injection mechanism of nanoparticles. Reported photomechanical effects of the amplified femtosecond laser on the permeability of the biological membrane would offer new perspectives in biophotonics.

Rotational quantum beat lasing without inversion

In standard lasers, light amplification requires population inversion between an upper and a lower state to break the reciprocity between absorption and stimulated emission. However, in a medium prepared in a specific superposition state, quantum interference may fully suppress absorption while leaving stimulated emission intact, opening the possibility of lasing without inversion. Here we show that lasing without inversion arises naturally during propagation of intense femtosecond laser pulses in air. It is triggered by the combination of molecular ionization and molecular alignment, both unavoidable in intense light fields. The effect could enable inversionless amplification of broadband radiation in many molecular gases, opening unusual opportunities for remote sensing.

Mechanism of Nickel Phyllosilicate Formation by Laser Ablation in Liquid

One-step synthesis of nickel-phyllosilicate (Ni-PS) nanocomposites was achieved using a femtosecond-reactive laser ablation in liquid (fs-RLAL) technique. The focusing of intense femtosecond laser pulses onto a silicon wafer immersed in aqueous nickel nitrate generated Ni-PS with high Ni loading in excess of 20 wt % under alkaline pH conditions. Analysis of the dissolved species in solution present after laser processing revealed that silicic acid was the key dissolved ablation product that reacted with the nickel nitrate to form the Ni-PS under alkaline conditions. When the solution was below pH 7, no silicic acid was generated from ablation, and consequently, no Ni-PS was formed in the dried product. The mechanism of Ni-PS formation from fs-RLAL of a silicon wafer immersed in aqueous nickel nitrate solutions is discussed. On the basis of this mechanism, it is expected that the fs-RLAL method will be capable of generating a variety of metal-phyllosilicates from different metal salt precursors.

Comparative study of strong-field ionization of alkaline-earth-metal atoms

We report on a comparative study of strong-field ionization of alkaline-earth-metal atoms by intense femtosecond laser pulses from near-infrared to midinfrared wavelengths. By collecting the ionization signals only produced within the central portion of the laser focus, the focus volume effect is largely reduced and the saturation intensities for different alkaline-earth-metal atoms are reliably determined, which permits us to directly test the strong-field-ionization theories. We demonstrate that the Perelomov-Popov-Terent'ev model accurately predicts the experimental ionization yields and saturation intensities in general for arbitrary values of the Keldysh parameter, while the Ammosov-Delone-Krainov simulations agree with the experiments for the tunneling-ionization regime and also for the regime when the Keldysh parameter is around 1. Our work presents benchmark data for strong-field ionization of alkaline-earth metals over a broad range of laser parameters and confirms the validity of Keldysh's picture for such atoms.

Femtosecond soft X-ray absorption spectroscopy of warm dense matter at the PAL-XFEL.

Free-electron laser pulse-based X-ray absorption spectroscopy measurements on warm dense copper are presented. The incident X-ray pulse energies were measured with a detector assembly consisting of a photocathode membrane andmicrochannel plates, and the transmitted energies were measured simultaneously with a photodiode detector. The precision of the absorption measurements was evaluated. For a warm dense copper foil irradiated by an intense femtosecond laser pulse, the enhanced X-ray absorption below the L3-edge, followed by the rapid evolution of highly excited Fermi liquid within apicosecond, were successfully measured. This result demonstrates a unique capability to study femtosecond non-equilibrium electron-hole dynamics in extreme states of matter.

Giant Optical Nonlinearities of Photonic Minibands in Metal–Dielectric Multilayers

The giant nonlinear optical responses of photonic minibands of (Ag/SiO2)4 metal–dielectric multilayers are reported using high intense femtosecond laser pulses. Ag and SiO2 alternative stack of layers form a series of coupled Fabry–Pérot resonators (Ag–SiO2–Ag) and the cavity modes are split into transmission minibands in the metal reflective spectral region. The strong saturation of two‐photon absorption associated with multiphoton absorption (MPA) is observed at photonic miniband minimum (≈700 nm), whereas MPA is the strong dominant nonlinearity at peak maximum (≈725 nm). The metal‐cavity induced manifold enhancement (>103 times) in the Ag intrinsic nonlinearity follows wide miniband spectral (700–765 nm) trend. Results are discussed with respect to single (Ag/SiO2)1 and bare Ag thin film results. The broad origin of giant nonlinearity is ascribed to the strong local cavity field enhanced metal interband transitions initiated by multiphoton absorption processes. The strong confinement of optical field and energy dissipation within these metal–dielectric coupled resonators are further evidenced by transfer matrix method simulations. The giant multiphoton absorptive type nonlinearities with very high laser‐damage threshold (≈50 GW cm−2) from these composite transparent metals are potentially beneficial for novel nonlinear optical limiters, optical Bragg coatings, and saturable optical absorbers for extremely high‐power ultrafast lasers operation.

Polarization-dependent micro-structure fabrication with direct femtosecond laser writing on plastic polarizer films.

Iodine-doped polyvinyl alcohol (IDPVA) film has been widely used as a plastic polarizer due to its great linear dichroism. We found that the anisotropic character of the plastic polarizer can be permanently damaged upon exposure of high intensity femtosecond laser pulses. This process is a two-photon-induced chemical reaction and denominated as two-photon-induced isotropy (TPII). The TPII effect can form a high polarization contrast on the base of the original IDPVA films. With this property, polarization-sensitive diffractive optical elements are fabricated in IDPVA films. The low cost of the IDPVA film and the high polarization contrast of TPII make it a promising new candidate for femtosecond laser fabrication of polarization-selective optical elements.

Remote Detection of Uranium Using Self-Focusing Intense Femtosecond Laser Pulses

Optical measurement techniques can address certain important challenges associated with nuclear safety and security. Detection of uranium over long distances presents one such challenge that is difficult to realize with traditional ionizing radiation detection, but may benefit from the use of techniques based on intense femtosecond laser pulses. When a high-power laser pulse propagates in air, it experiences collapse and confinement into filaments over an extended distance even without external focusing. In our experiments, we varied the initial pulse chirp to optimize the emission signal from the laser-produced uranium plasma at an extended distance. While the ablation efficiency of filaments formed by self-focusing is known to be significantly lower when compared to filaments produced by external focusing, we show that filaments formed by self-focusing can still generate luminous spectroscopic signatures of uranium detectable within seconds over a 10-m range. The intensity of uranium emission varies periodically with laser chirp, which is attributed to the interplay among self-focusing, defocusing, and multi-filament fragmentation along the beam propagation axis. Grouping of multi-filaments incident on target is found to be correlated with the uranium emission intensity. The results show promise towards long-range detection, advancing the diagnostics and analytical capabilities in ultrafast laser-based spectroscopy of high-Z elements.

Above-threshold multiphoton photoemission from noble metal surfaces

Exciting solids with intense femtosecond laser pulses prompts electrons of the interrogated material to respond in a highly nonlinear manner, as is evident in the emission of high-order harmonic radiation and photoelectrons with kinetic energies well above that of the driving photons. Such high-field interactions can be resolved, for example, in above-threshold multiphoton photoemission (ATP) spectroscopy. In this work, we interrogate the nonlinear photoelectric responses of the pristine copper, silver, and gold noble metal surfaces in (111) and (100) crystal orientations in the perturbative regime. Using multiphoton photoemission spectroscopy (mPP) excited by finely tuned optical fields, we characterize enhancement of the mPP and ATP yields from (111) surfaces in selected ${k}_{||}$-momentum ranges when the occupied Shockley surface (SS) states are (near-)resonantly coupled by multiphoton transitions to image potential (IP) intermediate states in the excitation process. The ATP signal from the IP states of (111) surfaces is largely defined by their formation through polarization of SS electrons; this observation is contrasted with ATP experiments from the Ag(100) surface, for which the SS becomes an unoccupied resonance and the IP states can only be excited from bands with significantly more bulk character. In addition, based on the optical power and nonlinear order-dependent mPP spectra, we provide evidence for ATP being a one-step, rather than a sequential process, as previously postulated.

Strong-field control of H3 + production from methanol dications: Selecting between local and extended formation mechanisms.

Using the CD3OH isotopologue of methanol, the ratio of D2H+ to D3 + formation is manipulated by changing the characteristics of the intense femtosecond laser pulse. Detection of D2H+ indicates a formation process involving two hydrogen atoms from the methyl side of the molecule and a proton from the hydroxyl side, while detection of D3 + indicates local formation involving only the methyl group. Both mechanisms are thought to involve a neutral D2 moiety. An adaptive control strategy that employs image-based feedback to guide the learning algorithm results in an enhancement of the D2H+/D3 + ratio by a factor of approximately two. The optimized pulses have secondary structures 110-210 fs after the main pulse and result in photofragments that have different kinetic energy release distributions than those produced from near transform limited pulses. Systematic changes to the linear chirp and higher order dispersion terms of the laser pulse are compared to the results obtained with the optimized pulse shapes.

Guiding performance of 6 GHz electromagnetic wave by single laser plasma filament

The guiding of a 6 GHz electromagnetic (EM) wave along a plasma filament produced by intense femtosecond laser pulses is investigated with the electromagnetic simulation software XFDTD. The results confirm that the plasma filament can guide the EM wave over a long distance, with low attenuation relative to freely propagating the signal. Furthermore, the filament can change the phase wavelength of the signal in the waveguide. Also notable is that the power density of the wave along the filament monotonically decreases with increasing EM wave propagation length. The wavelength of the EM wave along the plasma filament is about 4.98 cm, which is slightly less than that of the incident 6 GHz signal, i.e., the wave velocity along the filament is less than the speed of light.

Optimization of N2+ lasing through population depletion in the X2Σg+ state using elliptically modulated ultrashort intense laser fields

The authors generate air lasing by elliptically-modulated intense femtosecond laser pulses and show that the lasing intensities of N${}_{2}$${}^{+}$ at 391 and 428 nm can be manipulated by adjusting the temporal separation between the two polarization components in the elliptically-modulated laser pulse and their relative amplitudes. The authors interpret this characteristic ellipticity dependence in terms of the post-ionization coupling occurring in the later part of the laser pulse, which depletes efficiently the population in the X${}_{2}$ ${\mathrm{\ensuremath{\Sigma}}}_{g}^{+}$ (v'' = 0) state.