Two-photon fluorescence excitation spectroscopy by pulse shaping ultrabroad-bandwidth femtosecond laser pulses

A fast and automated approach to measuring two-photon fluorescence excitation (TPE) spectra of fluorophores with high resolution (~2 nm) by pulse shaping ultrabroad-bandwidth femtosecond laser pulses is demonstrated. Selective excitation in the range of 675-990 nm was achieved by imposing a series of specially designed phase and amplitude masks on the excitation pulses using a pulse shaper. The method eliminates the need for laser tuning and is, thus, suitable for non-laser-expert use. The TPE spectrum of Fluorescein was compared with independent measurements and the spectra of the pH-sensitive dye 8-hydroxypyrene-1,3,6-trisulfonic acid (HPTS) in acidic and basic environments were measured for the first time using this approach.     

Inducing and probing non-thermal transitions in semiconductors using femtosecond laser pulses

Soon after it was discovered that intense laser pulses of nanosecond duration from a ruby laser could anneal the lattice of silicon, it was established that this so-called pulsed laser annealing is a thermal process. Although the radiation energy is transferred to the electrons, the electrons transfer their energy to the lattice on the timescale of the excitation. The electrons and the lattice remain in equilibrium and the laser simply 'heats' the solid to the melting temperature within the duration of the laser pulse. For ultrashort laser pulses in the femtosecond regime, however, thermal processes (which take several picoseconds) and equilibrium thermodynamics cannot account for the experimental data. On excitation with femtosecond laser pulses, the electrons and the lattice are driven far out of equilibrium and disordering of the lattice can occur because the interatomic forces are modified due to the excitation of a large (10% or more) fraction of the valence electrons to the conduction band. This review focuses on the nature of the non-thermal transitions in semiconductors under femtosecond laser excitation.     

Two- and three-photon absorption and frequency upconverted emission of silicon quantum dots

In this communication, we present the experimental results of two- and three-photon excitation studies on silicon quantum dots (QDs) in chloroform (as well as in water) by using femtosecond laser pulses with wavelengths of 778 and 1335 nm and a pulse duration approximately 160 fs. The photoluminescence spectral distributions are nearly the same upon one-, two-, and three-photon excitation. With one- and two-photon excitation, the temporal relaxation measurements of photoluminescence emission manifest the same multiexponential decay behavior in the time range from 0.05 ns to 15 mus, characterized by three successive decay constants: 0.75 ns, 300 ns, and 5 mus, respectively. Finally, the two-photon absorption spectrum in the spectral range of 650-900 nm and the three-photon absorption spectrum in the spectral range of 1150-1400 nm have been measured.     

Carbon Nanotubes as an Ultrafast Emitter with a Narrow Energy Spread at Optical Frequency

Ultrafast electron pulses, combined with laser‐pump and electron‐probe technologies, allow ultrafast dynamics to be characterized in materials. However, the pursuit of simultaneous ultimate spatial and temporal resolution of microscopy and spectroscopy is largely subdued by the low monochromaticity of the electron pulses and their poor phase synchronization to the optical excitation pulses. Field‐driven photoemission from metal tips provides high light‐phase synchronization, but suffers large electron energy spreads (3–100 eV) as driven by a long wavelength laser (>800 nm). Here, ultrafast electron emission from carbon nanotubes (≈1 nm radius) excited by a 410 nm femtosecond laser is realized in the field‐driven regime. In addition, the emitted electrons have great monochromaticity with energy spread as low as 0.25 eV. This great performance benefits from the extraordinarily high field enhancement and great stability of carbon nanotubes, superior to metal tips. The new nanotube‐based ultrafast electron source opens exciting prospects for extending current characterization to sub‐femtosecond temporal resolution as well as sub‐nanometer spatial resolution.     

High-density optical data storage with one-photon and two-photon near-field fluorescence microscopy

A spatially localized photochemical reaction induced by near-field femtosecond laser pulses is demonstrated on a nanometer scale and used for high-density optical data storage. Recorded domains down to 120 and 70 nm are obtained with one-photon and two-photon excitation, respectively. It is shown that the local-field confinement that is due to the quadratic dependence of two-photon excitation on light intensity has the potential to increase the near-field optical storage density.     

Application of femtosecond-laser induced nanostructures in optical memory

The femtosecond laser induced micro- and nanostructures for the application to the three-dimensional optical data storage are investigated. We have observed the increase of refractive index due to local densification and atomic defect generation, and demonstrated the real time observation of photothermal effect after the femtosecond laser irradiation inside a glass by the transient lens (TrL) method. The TrL signal showed a damped oscillation with about an 800 ps period. The essential feature of the oscillation can be reproduced by the pressure wave creation and propagation to the outward direction from the irradiated region. The simulation based on elastodynamics has shown that a large thermoelastic stress is relaxed by the generation of the pressure wave. In the case of soda-lime glass, the velocity of the pressure wave is almost same as the longitudinal sound velocity at room temperature (5.8 microm/ns). We have also observed the localized photo-reduction of Sm3+ to Sm2+ inside a transparent and colorless Sm(3+)-doped borate glass. Photoluminescence spectra showed that some the Sm3+ ions in the focal spot within the glass sample were reduced to Sm2+ ions after femtosecond laser irradiation. A photo-reduction bit of 200 nm in three-dimensions can be recorded with a femtosecond laser and readout clearly by detecting the fluorescence excited by Ar+ laser (lambda = 488 nm). A photo-reduction bit can be also erased by photo-oxidation with a cw Ar+ laser (lambda = 514.5 nm). Since photo-reduction bits can be spaced 150 nm apart in a layer within glass, a memory capacity of as high as 1 Tbit can be achieved in a glass piece with dimensions of 10 mm x 10 mm x 1 mm. We have also demonstrated the first observation of the polarization-dependent periodic nanostructure formation by the interference between femtosecond laser light and electron acoustic waves. The observed nanostructures are the smallest embedded structures ever created by light. The period of self-organized nanostructures can be controlled from approximately 140 to 320 nm by the pulse energy and the number of irradiated pulses. Furthermore, we have also observed the self-assembled sub-wavelength periodic structures created in silica glass by femtosecond pulses on the plane of the propagation of light.     

Non-linear optical properties of zinc oxide nanowires

High quality zinc oxide (ZnO) nanowires were grown on n-type Si (100) using vapor-liquid-solid process. We obtained the photoluminescence spectra of ZnO nanowires based on nonlinear optical process using an ultrashort wavelength femtosecond laser as a pumping source. The spectra shows the second harmonic generation phenomenon, as well as the exciton-exciton collision peak at 388 nm and the green emission peak at 515 nm caused by oxygen vacancy. A laser emission peak near 392 nm was observed when pump intensity surpassed 52 mJ/cm2 and a sharp peak about 0.5 nm wide emerged when the energy intensity reached 700 mJ/cm2. We attribute this excitation process to a two-photon absorption process enhanced by Rabi oscillation.     

Limitations arising from two-photon absorption of solvent in pulsed-laser thermal lens detection: determination of the two-photon absorption coefficient of ethanol at 266 nm

Two-photon absorption of the solvent under pulsed-laser excitation at 266 nm produces a high background thermal lens signal interfering with the analyte signal. Discrimination of both solvent and analyte signals along with calibration of the photothermal response has allowed the determination of the two-photon absorption coefficient of ethanol. The obtained value, 3.0x10(-10) cm W-1, is close to the literature values obtained from transmittance measurements using picosecond or femtosecond laser pulses.     

Femtosecond laser assisted hatching: Dependence of <Emphasis Type="Italic">zona pellucida</Emphasis> drilling efficiency and embryo development on laser wavelength and pulse energy

Ultrashort laser pulses have enabled highly precise and delicate processing of biological specimens. We present the results of using femtosecond laser pulses for dissection of zona pellucida (ZP) in mouse embryos during assisted hatching procedure. We studied the effects of application of femtosecond laser radiation in the infrared (1028 nm) and visible (514 nm) wavelength ranges. Laser irradiation parameters were optimized so as not to compromise the viability of the treated embryos. We have demonstrated that application of femtosecond laser pulses with the energies in the range of 250–320 nJ (for the wavelength of 1028 nm) and 47–112 nJ (for 514 nm) resulted in efficient ZP dissection. Femtosecond laser-assisted ZP drilling does not slow down the development of pre-implantation embryos and leads to 90–95% frequency of complete hatching. The thermal effects can be significantly lower when femtosecond lasers are used as compared to continuous wave or long-pulse lasers. It is crucial when dealing with living cells or organisms. By optimizing femtosecond laser radiation parameters assisted hatching as well as a wide range of embryo-surgical procedures can be efficiently performed, thus creating a great potential of using femtosecond lasers as a multi-purpose “tool of choice” for specialists in the fields of embryology and developmental biology.     

Energy dependent saturable and reverse saturable absorption in cube-like polyaniline/polymethyl methacrylate film

Solid films of cube-like polyaniline synthesized by inverse microemulsion polymerization method have been fabricated in a transparent PMMA host by an in situ free radical polymerization technique, and are characterized by spectroscopic and microscopic techniques. The nonlinear optical properties are studied by open aperture Z-scan technique employing 5 ns (532 nm) and 100 fs (800 nm) laser pulses. At the relatively lower laser pulse energy of 5 μJ, the film shows saturable absorption both in the nanosecond and femtosecond excitation domains. An interesting switchover from saturable absorption to reverse saturable absorption is observed at 532 nm when the energy of the nanosecond laser pulses is increased. The nonlinear absorption coefficient increases with increase in polyaniline concentration, with low optical limiting threshold, as required for a good optical limiter.     

Glass formation and third-order optical nonlinear characteristics of bismuthate glasses within Bi2O3–GeO2–TiO2 pseudo-ternary system

Glass-forming region of Bi₂O₃–GeO₂–TiO₂ (BGT) pseudo-ternary system was determined by using melt-quench method. A series of high transparent glass samples were selected and their structural characteristics were investigated by FT-IR and Raman spectra. By employing Z-scan and optical Kerr shutter techniques with femtosecond laser pulses as excitation source, third-order optical nonlinearities (TON) of the BGT glasses as well as the TON response time were investigated at wavelength of 800 nm. The ultrafast nonlinear response and high figure of merit suggest great potentials of BGT glasses in applications of all-optical switching or related optical devices.     

Scanning force microscopic investigations of the femtosecond laser pulse irradiation of indium phosphide in air

Laser ablation of single-crystalline indium phosphide (InP) was performed in air by means of linearly polarized Ti : sapphire femtosecond pulses (800 nm, 130 fs, 10 Hz). As a result of the irradiation with a variable number of laser pulses per spot (N /spl les/ 5), several morphological changes (crater formation, rim formation, ripple structures, and cones) were observed. These effects were explored using force modulation microscopy (FMM), a technique based on scanning force microscopy, allowing the simultaneous imaging of both topography and local stiffness at a high lateral resolution. The first laser pulse induces the formation of a protruding rim (height < 20 nm, width /spl ap/ 300 nm) bordering the ablated crater. A Fourier analysis of the multipulse generated topographies reveals the formation of wavelength-sized periodic ripples (modulation depth < 100 nm) with an orientation perpendicular to that of the electric field vector of the laser radiation. Besides these morphological alterations, material modifications were also observed in the irradiated regions by means of the FMM technique. Within the ablated craters, local stiffness variations were found revealing an inhomogeneous material composition/structure as a consequence of the femtosecond pulse laser treatment.     

Intracavity frequency-doubled femtosecond cr(4+):forsterite laser

The generation of femtosecond optical pulses centered at ~620 nm directly from an all-solid-state laser oscillator is reported. Red pulses with pulse widths of the order of 170 fs were obtained with 24-mW average power at an 81-MHz repetition rate. They were achieved by intracavity frequency doubling of a mode-locked Cr(4+):forsterite laser with a 1-mm-thick beta-BaB(2)O(4) crystal. The process of laser mode locking was modified by surface coating the doubling crystal.     

Ultrafast optical phase modulation with metallic nanoparticles in ion-implanted bilayer silica

The nonlinear optical response of metallic-nanoparticle-containing composites was studied with picosecond and femtosecond pulses. Two different types of nanocomposites were prepared by an ion-implantation process, one containing Au nanoparticles (NPs) and the other Ag NPs. In order to measure the optical nonlinearities, we used a picosecond self-diffraction experiment and the femtosecond time-resolved optical Kerr gate technique. In both cases, electronic polarization and saturated absorption were identified as the physical mechanisms responsible for the picosecond third-order nonlinear response for a near-resonant 532 nm excitation. In contrast, a purely electronic nonlinearity was detected at 830 nm with non-resonant 80 fs pulses. Regarding the nonlinear optical refractive behavior, the Au nanocomposite presented a self-defocusing effect, while the Ag one presented the opposite, that is, a self-focusing response. But, when evaluating the simultaneous contributions when the samples are tested as a multilayer sample (silica-Au NPs-silica-Ag NPs-silica), we were able to obtain optical phase modulation of ultra-short laser pulses, as a result of a significant optical Kerr effect present in these nanocomposites. This allowed us to implement an ultrafast all-optical phase modulator device by using a combination of two different metallic ion-implanted silica samples. This control of the optical phase is a consequence of the separate excitation of the nonlinear refracting phenomena exhibited by the separate Au and Ag nanocomposites.     

Modification of the structure and hydrogen content of amorphous hydrogenated silicon films under conditions of femtosecond laser-induced crystallization

We have studied the Raman spectra of initially amorphous hydrogenated silicon (a-Si:H) films upon their exposure to femtosecond laser-radiation pulses with the fluence varied within 30–155 mJ/cm². The distribution of the volume fraction of a crystalline phase over the surface of processed films is determined for the first time and a correlation is established between changes in this value and the hydrogen content in a-Si:H films upon the crystallization induced by femtosecond laser radiation.     

Optically controlled thermal management on the nanometer length scale

The manipulation of polymers and biological molecules or the control of chemical reactions on a nanometer scale by means of laser pulses shows great promise for applications in modern nanotechnology, biotechnology, molecular medicine or chemistry. A controllable, parallel, highly efficient and very local heat conversion of the incident laser light into metal nanoparticles without ablation or fragmentation provides the means for a tool like a 'nanoreactor', a 'nanowelder', a 'nanocrystallizer' or a 'nanodesorber'. In this paper we explain theoretically and show experimentally the interaction of laser radiation with gold nanoparticles on a polymethylmethacrylate (PMMA) layer (one-photon excitation) by means of different laser pulse lengths, wavelengths and pulse repetition rates. To the best of our knowledge this is the first report showing the possibility of highly local (in a 40?nm range) regulated heat insertion into the nanoparticle and its surroundings without ablation of the gold nanoparticles. In an earlier paper we showed that near-infrared femtosecond irradiation can cut labeled DNA sequences in metaphase chromosomes below the diffraction-limited spot size. Now, we use gold as well as silver-enhanced gold nanoparticles on DNA (also within chromosomes) as energy coupling objects for femtosecond laser irradiation with single-and two-photon excitation. We show the results of highly localized destruction effects on DNA that occur only nearby the nanoparticles.     

Magnetooptical Kerr effect measurements of ultrafast spin dynamics in cobalt nanodots

We present our magnetooptical Kerr effect (MOKE) studies on picosecond spin dynamics in closely spaced rectangular Co dots with sizes ranging from 2/spl times/6 /spl mu/m/sup 2/ down to 100 /spl times/ 300 nm/sup 2/ under in-plane, picosecond, magnetic pulse excitation. A low-temperature-grown GaAs photoconductive switch, excited by femtosecond laser pulses, was used to produce /spl sim/25-ps-long magnetic transients along the surface of the coplanar-waveguide centerline, which contained arrays of patterned Co dots. The resulting spin dynamics in the dots was detected by a time-synchronized train of femtosecond optical probe pulses employing the time-resolved MOKE. Our experimental technique allowed us to measure the initial picosecond dynamics of spins in Co nanodots, followed by damped oscillations. We ascribe the observed results to the small-angle coherent spin precession and show that it depends on the size of magnetic dots.     

Three-photon absorption induced whispering gallery mode lasing in ZnO twin-rods microstructure

The ZnO twin-rods microstructure synthesized by hydrothermal method was employed as a whispering gallery mode lasing microcavity. The growth mechanism of the ZnO twin-rods single crystal was analyzed. Three-photon absorption induced whispering gallery mode lasing with low threshold was observed under the excitation of femtosecond pulses at 800 nm. The spectra from the individual branch and the connection part were investigated, and the whispering gallery mode lasing mechanism was discussed.     

飞秒激光与金膜作用的脉冲累积效应

采用1kHz飞秒激光（脉宽148fs,中心波长775nm）对石英衬底的金膜的烧蚀过程进行了研究．单脉冲与多脉冲的烧蚀阈值可以通过烧蚀点的直径平方与所用的激光能流的关系曲线获得．通过累积能流和烧蚀脉冲数的关系,可以得到金膜的脉冲累积因子．采用飞秒激光加工材料的一些特点可以合理解释单脉冲阈值附近获得的一些实验现象．     

Polarized Fluorescence in NADH Two-Photon Excited by Femtosecond Laser Pulses in the Wavelength Range of 720–780 nm

Technical Physics Letters - The decay of polarized fluorescence in coenzyme NADH in aqueous-methanol solution under two-photon excitation by femtosecond laser pulses within the spectral range of...