Plasma effects and the modulation of white light spectra in the propagation of ultrashort, high-power laser pulses in barium fluoride

We report the results of a study of white light generation in a 7.5 cm long crystal of a high band-gap material, barium fluoride, using ultrashort (<42 fs) laser pulses over a range of values of incident laser power that extend up to more than three orders of magnitude larger than the critical power for self-focusing (P_cr). We explore white light generation and the intensity and spectral distributions within filaments that are formed as a result of the interplay of self-focusing and plasma-induced defocusing. The onset of plasma effects occurs at power levels in excess of 7 GW for ultrashort pulses in BaF₂. For incident power levels that are three orders of magnitude larger than the critical power, blue-shifting of the incident laser wavelength is observed in addition to asymmetric continuum generation. The blue shift enables us to estimate the temporal variation of the electron density in the plasma that is generated within the BaF₂ crystal. PACS 52.38.Hb; 42.65.Jx; 42.65.Tg; 33.80.Wz; 52.35.Mw     

Third-order nonlinear optical response in transparent solids using ultrashort laser pulses

The third-order optical nonlinearity, χ ⁽³⁾, is measured in transparent glasses (BK7 and fused silica) and crystals (BaF₂ and quartz) using 36-fs, 800-nm laser pulses and the optical Kerr gate (OKE) technique; values are found to lie in the range 1.3–1.7×10^-14 esu, in accordance with theoretical estimates. We probe the purely electronic response to the incident ultrashort laser pulse in fused silica and BK7 glass. In BaF₂ and quartz, apart from the electronic response we also observe contribution from the nuclear response to the incident ultrashort pulses. We observe oscillatory modulations that persist for ～400 fs. The response of the media (glasses and crystals) to ultrashort pulses is also measured using two-beam self-diffraction; the diffraction efficiency in the first-order grating is measured to be in the range of 0.06–0.13 %. Third harmonic generation due to self-phase matching in the transient grating geometry is measured as a function of temporal delay between the two incident ultrashort pulses, yielding the autocorrelation signal.     

Depolarization of white light generated by ultrashort laser pulses in optical media

We report measurements of the extinction ratio (ER) of white light generated upon irradiation of BK7 glass by ultrashort (36 fs) laser pulses with incident power approximately 10(3) times larger than the critical power for self-focusing. At low incident powers, the continuum is symmetric about the incident laser wavelength; at high powers it becomes broader and distinctly asymmetric towards the blue side. We observe that ER degrades by 100-fold after the onset of multiphoton-induced free-electron generation (at incident intensity approximately 2 TW cm-2), which also corresponds to the onset of asymmetry in white-light spectra.     

Generation of a variable linear array of phase-coherent supercontinuum sources

We investigate the coherence properties of a linear array of white-light sources produced in bulk media by ultrashort laser pulses. The array is generated out of the spatial interference pattern between two laser pump pulses, so that the number of supercontinuum sources and their separations can be easily manipulated by varying the geometry of the laser beam interaction. We find that all the secondary white-light sources which arise from the generation of filaments in the optical medium are well phase-locked and are thus able to generate stable and high-visibility multiple-beam interference patterns in the far-field. Observations are compared to the results of a simple model which takes into account a clamping of the peak laser intensity inside the filaments and includes intensity-dependent phase shifts among the different sources. PACS 42.65.Jx; 42.65.Ky; 42.65.Re     

Adaptive control of the spatial position of white light filaments in an aqueous solution

We demonstrate control over the spatial coordinates (position and extent) of white light filaments (supercontinuum generation) in an aqueous solution. These are the first experiments to achieve control of filament position through the manipulation of the spectral phase of an ultra-fast (50 fs) 800 nm excitation laser pulse. A closed feedback loop employing a spatial light modulator and a genetic algorithm was used to manipulate the spectral phase of the pulses to achieve a specified filament position and length.     

Spectroscopy and femtosecond laser performance of Yb3+ :Gd0.64Y0.36VO4 crystal

We report for the first time on the efficient continuous-wave and mode-locked laser operation of a diode-pumped Yb:Gd_0.64Y_0.36VO₄ laser. cw output power of 855 mW with a slope efficiency of 45% with respect to the absorbed pump power was demonstrated for the 2.1%-doped crystal. In mode-locked regime with SESAM as passive shutter pulses as short as 100 fs were obtained. PACS 42.55.Xi; 42.65.Re; 42.70.Hj     

Towards observation of sub-diffractive pulse propagation in photonic crystals

It is shown that sub-diffractive (self-collimating) propagation of ultrashort pulses of narrow light beams is possible in two dimensional planar photonic crystal slabs (in particular made with air holes in Si₃N₄ slab) where the sub-diffractive propagation of monochromatic beam of visible light has been demonstrated previously both theoretically and numerically. We found that the sub-diffractive propagations of the pulses of duration of more than 40 fs are indistinguishable from that of monochromatic beams. However, for the pulses with duration less than 40 fs their propagation peculiarities associated with asymmetric spatiotemporal misshaping, spatial and temporal broadening come into play. The effects are pronounced for the pulses of duration less than 20 fs. The phenomena are shown for both TM and TE polarized light by means of numerical integration of 2D Maxwell’s equations with finite-difference time-domain technique.     

Interaction of ultrashort elliptically polarized laser pulses with nonlinear helical photonic metamaterial

The effect of nonlinear properties of a material with a periodic structural cell (three-dimensional spiral) on the specificity of transmission and reflection of elliptically polarized laser pulses normally incident on the metamaterial is studied using the finite-difference time-domain method. An analysis of the hodograph of electric-field strength vector showed that an increase in the peak intensity of a linearly polarized laser pulse incident on a sample leads to an increase in the orthogonal component of the electric-field strength vector in the pulse transmitted through the medium. When pulses containing few electric-field periods are incident on a metamaterial, the latter demonstrates radically different optical properties for right- and left-handed circularly polarized light passing through the medium. It was shown that an increase in the intensity of a right-handed (left-handed) circularly polarized ultrashort pulse, incident on a sample composed of a rather large number of right-handed (left-handed) spirals made of nonlinearmaterial, widens the frequency range within which the incident light is almost entirely reflected from the medium.     

Carrier-envelope phase fluctuations of amplified femtosecond pulses: characterization with a simple spatial interference setup

We demonstrate a direct and versatile scheme to determine the carrier-envelope phase fluctuations of tunable ultrashort optical pulses. The spatial interferogram between the high frequency components and the parametrically amplified and frequency doubled low frequency components of an octave broad white light continuum is measured for every single pulse. It directly reveals the carrier-envelope phase fluctuations of the pump pulses from the regenerative amplifier, as well as of the white light and the tunable pulses generated from it. PACS 42.25.Kb; 42.65.Yj; 42.65.Re     

Probing nonequilibrium dynamics with white-light femtosecond pulses

Femtosecond pulsed lasers have become an invaluable tool for examining ultrafast nonequilibrium dynamics. With pulsewidths of a few hundred femtoseconds (fs) to less than 10 fs, these lasers can clearly provide unprecedented temporal resolution. By amplifying ultrashort laser pulses to sufficient levels of energy per pulse, it is possible to exploit the nonlinear optical properties of certain materials to generate extremely broadband pulses. These pulses retain the time structure of the incident pulse, but contain a spectral bandwidth extending from the infrared to as far as the ultraviolet. By generating white-light pulses, it becomes possible to probe ultrafast nonlinear processes over a large range of energies. In this paper, the process of generating white-light ultrashort pulses will be presented, along with a discussion of different probing techniques and procedures necessary for modeling the transient optical data. Finally, results from pump-probe measurements using a white-light probe on indium phosphide (InP) films will be presented as a demonstration of this technique.     

Enhanced quadratic photocurrent in commercial light emitting diodes for autocorrelation measurement of ultrashort laser pulses

The quadratic photocurrent in commercial light emitting diodes (LEDs) has been studied in reverse bias mode for autocorrelation measurement of ultrashort laser pulses. It is found that the photocurrent can be greatly enhanced by operating the LED biased just below the reverse bias breakdown threshold. The effect of aging of LEDs on laser exposure in this mode of operation is found to be similar to that for the photovoltaic mode. The large internal gain in LED junction has enabled the recording of the second order autocorrelation signal of ∼200 fs laser pulses from 100 MHz laser oscillator with two orders of magnitude smaller average and peak power product compared to the case of the photovoltaic mode. PACS 42.65.Re; 42.50.Hz; 85.60.Jb     

Tunable mid-infrared,high-energy femtosecond laser source for glyco-protein structure analysis

We have developed a 6–12 μm mid-infrared (MIR) femtosecond laser source for glyco-protein structure analysis. The MIR femtosecond laser pulses are generated by a differential frequency generation (DFG) configuration with a combination of Ti:sapphire based regeneratively amplified femtosecond laser pulses (780 nm, 160 fs, 1 mJ) and a β-BaB₂O₄ (BBO) based optical parametric amplifier (OPA). The MIR pulse energy exceeds 4.5 μJ, where a glyco-protein molecule has resonant absorption lines due to the vibrational–rotational transitions. The pulse width is estimated to be less than 1 ps according to the cross correlation measurement between the two OPA output pulses. Using the MIR femtosecond laser pulses, we demonstrated photo-dissociation of the sialyl Lewis X (sLeX) proton added ion, which is the first time to the best of our knowledge. PACS 42.65.Re; 42.62.-b; 42.60.-b; 42.65.-k; 87.50     

Measurement of ultrashort laser pulses using single-crystal films of 4-aminobenzophenone

Single-crystal thin-film of an organic second-order nonlinear optical material, 4-aminobenzophenone (ABP), is used to measure the pulsewidth of a Ti-Sapphire laser producing 45 fs pulses at 1 kHz repetition rate, by the non-collinear second-harmonic generation (SHG) intensity autocorrelation technique. These films are suitable for measurements over a broad wavelength range, down to 780 nm, due to their wide optical transparency. The single-crystal film with thickness (3 μm) less than the coherence length requires no phase-matching for efficient broadband SHG. Pulse walk-off due to group-velocity mismatch (GVM) and temporal broadening of the pulses due to group-velocity dispersion (GVD) are found to be negligible. These effects have been estimated for pulse width down to few-cycle pulses (10 fs), and the analyses show that these films can be used to characterize such ultrashort optical pulses.     

All-fiber design of hybrid Er-doped laser/Yb-doped amplifier system for high-power ultrashort pulse generation

We propose a design of an all-fiber laser system that combines the most advanced Er:fiber laser in the telecommunication range and an efficient Yb-doped amplifier for generation of high-power ultrashort pulses. The system is based on nonlinear wavelength conversion of 1.56 μm ultrashort Er:fiber laser pulses to the 1 μm range in a short pigtail of dispersion-shifted silica fiber with subsequent amplification in the Yb-doped fiber amplifier. Pulses with a duration as short as 85 fs and averaged power of 200 mW are demonstrated.     

在固体透明材料中利用级联四波混频方法获得宽带多色飞秒激光脉冲的研究

飞秒激光光谱学实验研究的深入与拓展对飞秒激光脉冲的要求也越来越高.比如多色抽运探测实验需要同时用到多个不同频率的超短飞秒激光脉冲.本文设计了一个更加简单紧凑的实验装置,对两束不同中心频率的入射光引入相反啁啾,在厚度为0.5 mm的CaF2晶体中利用级联四波混频获得了光谱半高全宽近100nm,支持傅里叶转换极限脉宽小于10 fs的多色飞秒激光脉冲.这一结果将为拓展飞秒激光光谱学研究和应用发挥重要作用.     

57 W, 27 fs pulses from a fiber laser system using nonlinear compression

We report on the generation of 27 fs pulses with an average output power of 57 W and a repetition rate of 78 MHz. The pulses are generated by combining a high average power fiber chirped pulse amplification (FCPA) system with a microstructured large-mode-area fiber for nonlinear compression. The FCPA system delivers 270 fs pulses in a linearly polarized beam with diffraction-limited quality. Nonlinear compression is achieved by launching the pulses into a short (few cm) piece of microstructured fiber and subsequent compression by a pair of chirped mirrors. PACS  42.55.Wd; 42.55.Xi, 42.65.Re     

Tunable second harmonic generation by phase-modulated ultrashort laser pulses

We report on the generation of tunable light around 400?nm by frequency-doubling ultrashort laser pulses whose spectral phase is modulated by a sum of sinusoidal functions. The linewidth of the ultraviolet band produced is narrower than 1?nm, in contrast to the 12?nm linewidth of the non-modulated incident spectrum. The influence of pixellation of the liquid crystal spatial light modulator on the efficiency of the phase-modulated second harmonic generation is discussed.     

Widely tunable ultraviolet sub-30-fs pulses from supercontinuum for transient spectroscopy

Focusing 800-nm pulses of 10–20 fs and ≤0.4 mJ into atmospheric-pressure argon gives rise to a supercontinuum extending down to 250 nm. We show that spectral cuts from this radiation can be shortened by a simple prism compressor down to 30 fs even near the UV cut-off. The resulting pulses have enough energy (several hundred nanojoules) to serve as a simple and rugged broadly tunable pump source in ultra-fast transient spectroscopy. Such an application is demonstrated for the first time, using pulses tuned over 280–320 nm to excite Cr(CO)₆; probing it by intense-field ionization at 800 nm, we determine the lifetime of initially populated states to be as short as 14 fs.PACS 42.65.Jx; 42.65.Ky; 42.65.Re; 42.72.Bj; 82.20.-w; 82.53.-k     

Widely-wavelength-tunable few-cycle optical pulse generation from an all-fiber erbium-doped laser system

A scheme for the construction of fiber laser systems for the generation of tunable ultrashort optical pulses is proposed. The scheme is based on the self-Raman shift of the soliton frequency in dispersion-decreasing fibers with the subsequent spectral broadening owing to the supercontinuum generation in a short highly nonlinear fiber and the compression in the corresponding fiber compressor. An all-fiber laser system for the generation of ultrashort laser pulses in the wavelength range 1.6–2.0 μm is experimentally demonstrated. In particular, the shortest pulses with a duration of 24 fs are generated at wavelengths of 1.8–1.9 μm, which corresponds to less than four optical cycles.     

Spectral and temporal analysis of ultrashort ultraviolet pulses generated by high-intensity laser radiation in the atmosphere

We report direct spectral and temporal characterization of ultrashort ultraviolet (UV) pulses resulting from third-harmonic generation by high-intensity Ti: sapphire laser radiation in the atmosphere. The experimental technique implemented in this work enables the measurement of the pulse width and the chirp of the UV field, as well as the electron density of the plasma produced by laser pulses. The bandwidth of the third harmonic generated in our experiments by laser pulses with an initial pulse width of 45 fs supports transform-limited UV pulses as short as 30 fs.