Near-infrared Femtosecond Laser Research Articles

Rainbow Archimedean spiral emission from optical fibres

We demonstrate a new practical approach for generating multicolour spiral-shaped beams. It makes use of a standard silica optical fibre, combined with a tilted input laser beam. The resulting breaking of the fibre axial symmetry leads to the propagation of a helical beam. The associated output far-field has a spiral shape, independently of the input laser power value. Whereas, with a high-power near-infrared femtosecond laser, a visible supercontinuum spiral emission is generated. With appropriate control of the input laser coupling conditions, the colours of the spiral spatially self-organize in a rainbow distribution. Our method is independent of the laser source wavelength and polarization. Therefore, standard optical fibres may be used for generating spiral beams in many applications, ranging from communications to optical tweezers and quantum optics.

Controlled pDNA Release in Gemini Cationic Lipoplexes by Femtosecond Laser Irradiation of Gold Nanostars.

The design of nanovectors able to overcome biological barriers is one of the main challenges in biomedicine. Gemini cationic lipids are considered potential candidates for gene therapy due to their high biocompatibility and capacity to condense nucleic acids safely in the form of lipoplexes. However, this approach presents difficulties regarding genetic unpacking and, therefore, control over this process becomes crucial to ensure successful transfection. In this work, gemini cationic lipoplexes were prepared in the presence of plasmonic gold nanostars (AuNSs) to afford a nanovector that efficiently releases plasmid DNA (pDNA) upon irradiation with near-infrared femtosecond laser pulses. A critical AuNSs concentration of 50 pM and optimized laser power density of 400 mW led to successful pDNA release, whose efficiency could be further improved by increasing the irradiation time. Agarose gel electrophoresis was used to confirm pDNA release. UV-Vis-NIR spectroscopy and transmission electron microscopy studies were performed to monitor changes in the morphology of the AuNSs and lipoplexes after irradiation. From a physicochemical point of view, this study demonstrates that the use of AuNSs combined with gemini cationic lipoplexes allows control over pDNA release under ultrafast laser irradiation.

Imaging Plasmons with Sub-2 nm Spatial Resolution via Tip-Enhanced Four-Wave Mixing.

Four-wave mixing at plasmonic tip-sample nanojunctions may be used to visualize plasmonic fields with sub-2 nm spatial resolution under ambient laboratory conditions. We illustrate the latter using a gold-coated atomic force microscopy probe irradiated with a pair of near-infrared femtosecond laser pulses and used to image plasmonic gold nanoplates and silver nanocubes. Through diagnostic polarization-dependent tip-only measurements, we illustrate that the four-wave mixing signal is localized to the tip apex. The apex-bound signal is further enhanced when the tip is located at specific locations near plasmonic nanoparticles. Overall, this work paves the way for visualizing chemical transformations as well as coherent electronic and vibrational dynamics with joint femtosecond temporal and few-nanometer spatial resolution under ambient conditions.

Intensity modulation of the population of atomic excited states by using near-infrared femtosecond laser pulses

We have theoretically investigated the modulation structures of the excited-state population of an argon atom exposed to a linearly polarized 800-nm laser pulse in the tunneling region. The numerical result identifies a nearly opposite phase modulation structure between the low-lying n = 4–7 states and over all higher $$n>7$$ states. This phase-dependent alternating population phenomenon is found to be related to the periodic channel-closing effect that results from ac-Stark-shifted multiphoton resonances. Moreover, the angular momentum states attributed to different parities have a similar alternating effect, which confirms a multiphoton process in the tunneling region. We introduce a mechanism of two-photon $$\Lambda $$ -type Raman transitions involving Rydberg and continuum states with a simultaneous redistribution of states to account successfully for this observed out-of-phase angular momentum state population.

Intensity and wavelength dependence of anisotropic nonlinear absorption inside MgO

We report an experimental measurement of nonlinear absorption by using the near-infrared femtosecond laser and a crystalline MgO sample. We show that the nonlinear absorption inside MgO presents a four-fold modulation as a function of the crystal alignment to the laser polarization. In different intensities and wavelengths, we observe that the modulation amplitude is changed. We introduce a model based on the calculation of the carrier density to explain the phenomenon. It shows that the varied modulation is due to the variation of effective electron mass, which is related to the crystal structure. Our work makes a step forward in the application of nonlinear absorption in exploring solid structure.

Ultrafast Electron Dynamics in Gold Films Probed by Near-infrared Femtosecond Laser

Ultrafast Electron Dynamics in Gold Films Probed by Near-infrared Femtosecond Laser

Unique emissive behavior of combustion-derived particles under illumination with femtosecond pulsed near-infrared laser light.

Exposure to combustion-derived particles (CDPs), such as carbonaceous particulate matter (PM), has adverse effects on human health. Hence, selective detection of these particles in biological environments is required to understand their toxicity. The optical detection of carbonaceous PM is possible in biological samples based on white light (WL) emission under illumination with a femtosecond (fs) pulsed near-infrared (NIR) laser. However, it is unclear if common non-CDPs in ambient PM, such as silica and metal oxides, can interfere with CDP detection when illuminated using a fs-pulsed NIR laser. Here, we show that WL emission, when illuminated with a fs-pulsed NIR laser, is observed only for CDPs amongst other common air pollution particles. We report that the intense WL emission from CDPs spanning over the whole visible spectrum is not observed from non-CDPs. This observation is made for four different CDPs and five different, relevant non-CDPs, in wet and dried samples using biologically relevant imaging conditions. This investigation confirms the uniqueness of WL emission as a selective detection mechanism of CDPs using a multiphoton microscopy platform, commonly available in research laboratories. Furthermore, some relevant signatures for the non-CDPs are provided that could potentially lead to the selective monitoring of pollution related nanoparticles (NPs).

Strong-field induced fragmentation and isomerization of toluene probed by ultrafast femtosecond electron diffraction and mass spectrometry.

We investigate the fragmentation and isomerization of toluene molecules induced by strong-field ionization with a femtosecond near-infrared laser pulse. Momentum-resolved coincidence time-of-flight ion mass spectrometry is used to determine the relative yield of different ionic products and fragmentation channels as a function of laser intensity. Ultrafast electron diffraction is used to capture the structure of the ions formed on a picosecond time scale by comparing the diffraction signal with theoretical predictions. Through the combination of the two measurements and theory, we are able to determine the main fragmentation channels and to distinguish between ions with identical mass but different structures. In addition, our diffraction measurements show that the independent atom model, which is widely used to analyze electron diffraction patterns, is not a good approximation for diffraction from ions. We show that the diffraction data is in very good agreement with ab initio scattering calculations.

Suppression of Fragmentation in Mass Spectrometry.

Suppressing fragmentation is a constant challenge in mass spectrometry because a molecular ion can readily be identified and provides information concerning the molecular weight of an analyte. Several techniques such as charge exchange chemical ionization (CECI) and vacuum ultraviolet emission ionization (VUVEI) have been developed to date for achieving this purpose. In this study, we report on the use of tunable ultraviolet (UV) and near-infrared (NIR) femtosecond (fs) lasers (35 fs) for the multiphoton ionization (MPI) of cis- and trans-4-methylcyclohexanols, the reference molecules that are currently used to examine fragmentation suppression. The results obtained here were compared with those obtained by CECI and VUVEI because they were reported as the best techniques for suppressing fragmentation. A molecular ion was strongly enhanced by carefully minimizing the excess energy in the ionic state using tunable UV and NIR fs-lasers. The ratio of the intensities for molecular and fragment ions, [M]+/[M-H2O]+, increased significantly (9.5-fold and 8.5-fold for cis- and trans-isomers, respectively, in UV fs-MPI) compared to the values obtained by CECI and VUVEI, respectively.

Femtosecond laser ablation of metal targets: The physical origin of the power law size distribution of nanoparticles

Near-infrared femtosecond laser is employed to ablate the copper target in vacuum (10−4 Pa). The ejected nanoparticles are collected by a silicon substrate. The 3D profiles of the deposited nanoparticles indicate before resolidification on the substrate they are nanodroplets generated by some phase separation process, such as phase explosion or cavitation. To study the nanoparticles’ generation dynamics and size distribution, the commonly used methods are the molecular dynamics simulation and the Monte Carlo method. However, the former cannot predict the particle size distribution at the final state and the latter cannot provide a clear physical picture. In this paper, taking both the nanoparticles’ generation and ejection into account, an analytical thermodynamic model based on the nanodroplets’ evaporation is proposed. In this model, the nanoparticles’ sizes are redistributed due to the nanodroplets’ evaporation during the flight from the target to the substrate, which provides a clear physical picture and successfully explains the physical origin of the final power law particle size distribution on the substrate. The model bridges the gap between the final size distribution and the thermodynamic generation process of nanoparticles, which will benefit the size control of the ablation-generated nanoparticles.

Selective induction of targeted cell death and elimination by near-infrared femtosecond laser ablation

The techniques for inducing the death of specific cells in tissue has attracted attention as new methodologies for studying cell function and tissue regeneration. In this study, we show that a sequential process of targeted cell death and removal can be triggered by short-term exposure of near-infrared femtosecond laser pulses. Kinetic analysis of the intracellular accumulation of trypan blue and the assay of caspase activity revealed that femtosecond laser pulses induced immediate disturbance of plasma membrane integrity followed by apoptosis-like cell death. Yet, adjacent cells showed no sign of membrane damage and no increased caspase activity. The laser-exposed cells eventually detached from the substrate after a delay of >54 min while adjacent cells remained intact. On the base of in vitro experiments, we applied the same approach to ablate targeted single cardiac cells of a live zebrafish heart. The ability of inducing targeted cell death with femtosecond laser pulses should find broad applications that benefit from precise cellular manipulation at the level of single cells in vivo and in vitro.

Direct Production of CH(A2Δ) Radical from Intense Femtosecond Near-IR Laser Pulses.

CH(A2Δ) radical formation was observed in bromoform and methanol vapor in argon plasma with near-infrared femtosecond laser pulses (43 fs, 1030 nm, 100 kHz, 250 μJ/pulse). The beam was focused with an achromatic lens, creating very high intensity in the plasma that caused Coulomb explosion (calculated intensity was ∼1.1 × 1016 W/cm2 in the focal point). The emitted fluorescence light was measured with high spectral (1-10 cm-1) and temporal resolution (5 ns) with an FT-Vis spectrometer. The step-scan technique allowed the reconstruction of the time-resolved fluorescence spectra from CH(A-X) emission. The emission from atomic lines such as H, Br, C, and O was observed and also from C+ cations and CH and C2 radicals. This indicates that in a significant portion of these organic molecules, all chemical bonds were cleaved in the Coulomb explosion. For both organics, the peak maximum of the CH(A) emission occurred at about 10 ns after excitation by the femtosecond pulse. After the maximum, a rapid emission decay was observed in the case of bromoform (monoexponential decay, t = 10 ns). The fluorescence decay was biexponential when methanol was used as the source for CH(A) generation. It can be assumed that CH(A) generation involved a fast and a slower path with some secondary reactions via the stepwise loss of hydrogen atoms from the CH3 group. The time constants were t1 = 7.8-8.3 ns and t2 = 78-82 ns for the fast and slow components, respectively, and very similar values were obtained at 10 and 25 mbar total pressures. However, in the case of bromoform, the C-Br bonds are significantly weaker; therefore, these atoms can be removed even in a single step via multiphoton absorption. The rotational temperature of CH(A) radicals generated from methanol decreased rapidly in the 30-55 ns time period from 2770 ± 80 to 1530 ± 50 K. The vibrational temperature increased from 3530 ± 450 to 9810 ± 760 K in the 30-80 ns time period and then started to decrease (the average temperatures were Trot = 910 ± 20 K and Tvib = 7490 ± 340 K at 100 ns). This initial increase of Tvib is thought to be the result of electron collision with the CH radicals. The high temperatures of the fragment may indicate the roaming reaction associated with the Coulomb explosion of the parent molecule. We demonstrated that CH(A) radicals can be produced from both organic compounds, and the step-scan technique is ideal for the characterization of their time-resolved spectra using the 100 kHz high repetition rate near-infrared femtosecond laser pulses. The FT/UV-vis step-scan technique can detect neutral species directly with high spectral and time resolution, thus it is a complementary technique to the experiments utilizing ion detection schemes, such as velocity map imaging.

Large ultrafast nonlinear optical response and excellent optical limiting behaviour in pyrene-conjugated zinc(II) phthalocyanines at a near-infrared wavelength

The design and synthesis with full structural utilization of a new type of nonlinear photonic material, Zinc(II) phthalocyanine macrocycle (Pc-pyrene), bearing binary oriented (up/down) pyrene units is reported. The novel pyrene-based macrocycle has been successfully obtained in high yield upon coupling multiple azido pyrene derivatives on a previously fabri-cated alkynyl-substituted macrocyclic platform (Pc1) via multiple tandem Cu(I)-catalysed azide-alkyne cycloaddition (CuAAC) reactions. The ultrafast nonlinear optical characteristics of both Pc1 and Pc-pyrene have been investigated in solution using a near-infrared femtosecond pulsed laser. The femtosecond Z-scan results reveal a low optical limiting threshold and a good set of figures of merit that make these macrocycles feasible for optical limiting as well as switching applications. In a major breakthrough, ultrafast laser-induced deformations in Pc-pyrene-embedded PMMA films results in a very large enhancement of the three-photon absorption coefficient at 800 nm by up to ~105 times that of Pc solutions. Furthermore, the deformed Pc-pyrene PMMA films having the advantage of flexibility and possess an excellent optical limiting threshold (0.0018 J/cm2), much lower than various previously reported values, which enables them to be one of the best optical limiters.

Femtosecond laser writing of plasmonic nanoparticles inside PNIPAM microgels for light-driven 3D soft actuators.

Herein, three-dimensional (3D) incorporation of plasmonic Ag nanoparticles was performed inside temperature-responsive poly(N-isopropylacrylamide) microgels using near-infrared femtosecond laser multi-photon reduction. The nanoparticles, formed by laser writing at lower doses, exhibited intense plasmonic absorption in the gels around 420 nm wavelength. Light-induced local shrinking of up to 86%, under assumption of isotropic shrinkage, in volume was achieved by the efficient photothermal conversion of Ag nanoparticles. Such shrinkages and deformation speeds strongly depended on the geometric design and 3D layout of the laser writing patterns of Ag nanoparticles inside the microgels. In particular, femtosecond laser incorporation enhanced the recovery speed by more than twice in comparison with the gels containing nanoparticles over the entire region. Laser direct incorporation allows for the control of the 3D position and extent and response speeds of gel deformation.

Characterization of soft X-ray FEL pulse duration with two-color photoelectron spectroscopy.

The pulse duration of soft X-ray free-electron laser (FEL) pulses of SACLA BL1 (0.2-0.3 nC per bunch, 0.5-0.8 MeV) were characterized by photoelectron sideband measurements. The intensity of the He 1 s-1 photoelectron sidebands generated by a near-infrared femtosecond laser was measured as a function of the time delay between the two pulses using an arrival time monitor. From the width of the cross-correlation trace thus derived, the FEL pulse duration was evaluated to be 28 ± 5 fs full width at half-maximum in the photon energy range between 40 eV and 120 eV.

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.

Enhancement of terahertz waves from two-color laser-field induced air plasma excited using a third-color femtosecond laser.

This study experimentally demonstrates and theoretically analyzes the enhancement of terahertz (THz) waves from two-color laser-field (consisting of a near-infrared femtosecond laser and its second-harmonic wave) induced air plasma using an additional 800 nm femtosecond laser. The experiments revealed that the additional 800 nm laser increased the THz energy up to 22 times. To understand the enhancement mechanism and reveal the maximum enhancement conditions, the effects of the 800 nm beam's polarization and energy variations of both beams on the THz amplification were studied. With the increase in the 800 nm pulse energy, the THz yield initially increases, and then decreases after reaching an inflection point. The THz increase rate continues to increase with the decrease in energy of the near-infrared two-color fields. The 800 nm beam could efficiently modulate the THz spectral energy distribution by increasing the high-frequency components, while decreasing the low-frequency components.

π-Extended Coumarins Derived with Nonhydrolyzable Iminophosphoranes as Two-Photon-Excited Fluorophores.

Novel coumarin-iminophosphorane (IPP) fluorophores that have stable resonance contributions from aza-ylides were formed by using the nonhydrolysis Staudinger reaction. The N═P formation reaction kinetics obey the conventional Staudinger reaction. The absorption and emission profiles of the coumarin-IPP derivatives can be fine-tuned: an electron-donating group at PPh3 enhances absorption and fluorescence, whereas an electron-withdrawing group at C-3 drives absorption and emission peaks toward blue-light wavelengths. Two-photon adsorption, accompanied by anti-Stokes fluorescence, is achieved under near-infrared femtosecond laser excitation.

Comparison of 1030 nm and 257 nm wavelengths for U-Pb zircon dating by femtosecond laser ablation – Inductively coupled plasma mass spectrometry with support of 3D crater imaging

Femtosecond near-infrared (NIR, 1030 nm) and near-ultraviolet (NUV, 257 nm) laser ablation (fs-LA) were evaluated for U-Pb dating of zircons using inductively coupled plasma mass spectrometry (ICP-MS). The apparent ages are in agreement with the reference ages, within expanded combined uncertainties, at both wavelengths, but NIR fs-LA produces poorer uncertainties and a ≈ 3.5% bias on the reference age of Mudtank and Plešovice zircon. The time resolved 238U signal intensity rises sharply and progressively decreases in NUV, whereas patterns in NIR follow progressive increase and then decrease during ablation. Synchrotron X-ray micro-tomography (XRMT) imaging of an ablated quartz permitted to link the morphology and dimensions of fs-LA craters to the performances of fs-LA-ICP-MS analyses on zircons. Average ablation rates are similar at 3 J.cm-2 for both wavelengths. However, the ablation rate is higher in NIR at 7 J.cm-2 than in NUV at 2 J.cm-2, whereas the fs-LA-ICP-MS yield (in counts.shot-1.ppm-1) is lower in NIR at 7 J.cm-2 than in NUV at 2 J.cm-2. This paradox as well as the biased or imprecise fs-LA-ICP-MS analyses are explained by nonlinear shot-to-shot ablation in NIR compared to NUV, induced by: (i) catastrophic ablation, (ii) incubation effects, and, to a minor extent (iii) preferential ionization of U relative to Pb. Consequently, NIR fs-LA is capable of producing accurate U-Pb ages thanks to the properties of femtosecond laser matter interactions, but with a higher fluence, sample consumption and poorer statistics than those obtained with NUV fs-LA.

Extremely robust femtosecond written fiber Bragg gratings for an ytterbium-doped fiber oscillator with 5 kW output power.

We present highly robust fiber Bragg gratings (FBGs) in passive large-mode-area fibers for kilowatt fiber laser systems. The gratings were inscribed directly through the fiber coating using near-infrared femtosecond laser pulses and then implemented in an all-fiber ytterbium-doped single-mode oscillator setup reaching up to 5 kW signal output power. The untreated cooled FBGs showed thermal coefficients as low as ${1}\;{\rm K}\;{{\rm kW}^{ - 1}}$1KkW-1, proving excellent qualification for the implementation into robust high-power fiber laser setups.