超短激光脉冲对宽带光学物质的微加工

通过讨论超快飞秒激光脉冲和长脉冲宽度的激光脉冲紧导致宽能隙透明电介质的损伤机理和比较超短激光脉冲与长激光脉冲对宽能隙透明电介质的损伤程度，得出超短激光脉冲是一种可对透明宽带电介质进行加工的有效工具的结论。当波长为800nm，脉冲宽度为150fs的激光脉冲紧聚焦到不同的宽能隙透明电介质（K9玻璃和ZK6玻璃）体内时，可制作不同光栅常数的光栅，并在波长为635nm的He-Ne连续激光的垂直照射下，对光栅的远场相对衍射效率和光栅的衍射效率进行了测量。     

Analysis of the nonlinear absorption mechanisms in ablation of transparent materials by high-intensity and ultrashort laser pulses

The mechanisms of nonlinear absorption in transparent materials under irradiation with ultrashort laser pulses are considered theoretically. Nitride semiconductor, sapphire and others transparent dielectrics were investigated. The ablation threshold for these materials is within multi-TW/cm² range. The model was used based on the tunneling absorption under the irradiation by high-intensity ultrashort pulses in terms of the theory of ionization of solid in a field of strong electromagnetic wave. The effect of the energy gap of material on the threshold of laser ablation was adequately explained.     

Mechanisms of femtosecond laser ablation of dielectrics revealed by double pump–probe experiment

We study experimentally the electronic excitation mechanisms involved in the breakdown and ablation of wide band gap dielectrics. A femtosecond pump–probe interferometry technique, with 100 fs temporal resolution, allows measuring the modification of refractive index induced by ultra-short intense laser pulses. To get more information in the complex process of excitation and relaxation mechanisms involved during and after the interaction, we use a sequence of two excitation pulses: a first short pulse at 400 nm excites a controlled density of carriers, and a second one at 800 nm with variable pulse duration, from 50 fs to 10 ps, reaches an excited solid. In Al₂O₃, we show that the total density of carriers never exceeds the sum of the densities excited by the two pulses sent independently. This means that the second pulse deposits further energy in the material by heating the previously excited carriers, and that no electronic multiplication occurs. On the other hand, in SiO₂, it is possible, under specific conditions, to observe an increase of carrier density due to impact ionization. All these results demonstrate that the avalanche process, which is often invoked in the laser breakdown literature, does not play a dominant role in optical breakdown induced by short pulses.     

A three-wavelength Ti:sapphire femtosecond laser for use with the multi-excited photosystem II

We have constructed a three-wavelength Ti:sapphire femtosecond laser with an independent tunable wavelength (λ₁) and two variable central wavelengths (λ₂ and λ₃) for use with the multi-excited photosystem II. Stable sub-40-fs pulses are generated. The λ₁-wavelength pulses can be tuned independently from 750 nm to 850 nm. The center wavelengths λ₂ and λ₃ can be varied from 760 nm to 840 nm. Received: 14 April 2000 / Revised version: 5 September 2000 / Published online: 27 April 2001     

Production of “dichroitic” diffraction gratings in glasses containing silver nanoparticles via particle deformation with ultrashort laser pulses

By repetitive irradiation of pico- or femtosecond laser pulses on glasses containing silver nanoparticles, dichroitic areas can be produced with different optical properties depending on the actual irradiation parameters. This effect, which is nanoscopically caused by permanent deformation of the initially spherical particles to non-spherical shapes and an additional formation of a halo of very small particles, is studied as a function of polarization and number of the applied pulses using two different laser systems (Ti:sapphire, λ=400 nm, t_p=150 fs; Nd:YLF, λ=523.5 nm, t_p=4 ps). A very special diffraction grating produced by this local deformation, which has strongly polarization- and wavelength-dependent features, is introduced and discussed. Received: 20 July 2001 / Published online: 10 October 2001     

Femtosecond laser ablation of silicon–modification thresholds and morphology

We investigated the initial modification and ablation of crystalline silicon with single and multiple Ti:sapphire laser pulses of 5 to 400 fs duration. In accordance with earlier established models, we found the phenomena amorphization, melting, re-crystallization, nucleated vaporization, and ablation to occur with increasing laser fluence down to the shortest pulse durations. We noticed new morphological features (bubbles) as well as familiar ones (ripples, columns). A nearly constant ablation threshold fluence on the order of 0.2 J/cm² for all pulse durations and multiple-pulse irradiation was observed. For a duration of ≈100 fs, significant incubation can be observed, whereas for 5 fs pulses, the ablation threshold does not depend on the pulse number within the experimental error. For micromachining of silicon, a pulse duration of less than 500 fs is not advantageous. Received: 4 December 2000 / Revised version: 29 March 2001 / Published online: 20 June 2001     

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     

Use of saturable absorber dyes for self-starting operation of a self-mode-locked Ti:Al2O3 laser

Extremely stable and self-starting operation of a self-mode-locked Ti:Al₂O₃ laser can be achieved by incorporating a jet of dilute saturable absorber in the laser resonator. We have demonstrated a laser which generates pulses as short as 47 fs, with 700 mW average power near 800 nm when pumped by 7 W from an all-lines argon laser. A mixture of saturable absorber dyes starts the mode-locking process but does not restrict the tuning range of the laser. Pulses less than 100 fs in duration are generated at wavelengths between 700 nm and 900 nm with two sets of optics. Pulses of 100 fs from this laser have been compressed to 26 fs with standard fibre-prism techniques.     

Laser-induced backside wet etching of fluoride and sapphire using picosecond laser pulses

Laser-induced backside wet etching (LIBWE) is a promising process for microstructuring of rigid chemical resistant and inert transparent materials. LIBWE with nanosecond laser pulses has been successfully demonstrated in a number of studies. LIBWE in a time scale of femtosecond and picosecond pulse durations has been investigated only in a few studies and just on fused silica. In the present study LIBWE of fluorides (CaF₂, MgF₂) and sapphire with a mode-locked picosecond (t _p=10 ps) laser at a UV wavelength of λ=355 nm using toluene as absorbing liquid has been demonstrated. The influence of the laser fluence and the pulse number on the etching rate and the achieved surface morphology was investigated. The etching rate grows linearly with the laser fluence in the low and high-fluence ranges with different slopes. The achieved etching rates for CaF₂ and for sapphire were in the same range. Contrary to CaF₂ and sapphire the etching rates of MgF₂ were one magnitude less. For backside etching on sapphire at high fluences smooth surfaces and at low fluences ripples pattern were found, whereas fluoride surfaces showed a trend towards crack formation.     

Growth and properties of KLu(WO4)2, and novel ytterbium and thulium lasers based on this monoclinic crystalline host

High‐quality crystals of monoclinic KLu(WO₄)₂, shortly KLuW, were grown with sizes sufficient for its characterization and substantial progress was achieved in the field of spectroscopy and laser operation with Yb³⁺‐ and Tm³⁺‐doping. We review the growth methodology for bulk KLuW and epitaxial layers, its structural, thermo‐mechanical, and optical properties, the Yb³⁺ and Tm³⁺ spectroscopy, and present laser results obtained in several operational regimes both with Ti:sapphire and direct diode laser pumping using InGaAs and AlGaAs diodes near 980 and 800 nm, respectively. The slope efficiencies with respect to the absorbed pump power achieved with continuous‐wave (CW) bulk and epitaxial Yb:KLuW lasers under Ti:sapphire laser pumping were ≈ 57 and ≈ 66%, respectively. Output powers as high as 3.28 W were obtained with diode pumping in a simple two‐mirror cavity where the slope efficiency with respect to the incident pump power reached ≈ 78%. Passively Q‐switched laser operation of bulk Yb:KLuW was realized with a Cr:YAG saturable absorber resulting in oscillation at ≈ 1031 nm with a repetition rate of 28 kHz and simultaneous Raman conversion to ≈ 1138 nm with maximum energies of 32.4 and 14.4 μJ, respectively. The corresponding pulse durations were 1.41 and 0.71 ns. Passive mode‐locking by a semiconductor saturable absorber mirror (SESAM) produced bandwidth‐limited pulses with duration of 81 fs (1046 nm, 95 MHz) and 114 fs (1030 nm, 101 MHz) for bulk and epitaxial Yb:KLuW lasers, respectively. Slope efficiency as high as 69% with respect to the absorbed power and an output power of 4 W at 1950 nm were achieved with a diode‐pumped Tm:KLuW laser. The slope efficiency reached with an epitaxial Tm:KLuW laser under Ti:sapphire laser pumping was 64 %. The tunability achieved with bulk and epitaxial Tm:KLuW lasers extended from 1800 to 1987 nm and from 1894 to 2039 nm, respectively.     

High resolution patterning of sapphire by F<Subscript>2</Subscript>-laser ablation

The ablation behavior of single crystalline sapphire with nanosecond laser pulses at 157 nm wavelength is investigated. Ablation rates of about 10 to 100 nm/pulse are obtained at fluences ranging from 1 to 9 J/cm². At moderate fluences, incubation behavior is observed, i.e. ablation starts after material modification by a number of laser pulses. The ablation can be utilized to fabricate sapphire micro-optics. The capability of creating lenses or gratings on the tip of sapphire fibers is demonstrated. Multilevel diffractive optical elements and high resolution gratings with 1 μm period are fabricated on planar sapphire substrates.     

Optical field enhancement effects in laser-assisted particle removal

We report on the role of local optical field enhancement in the neighborhood of particles during dry laser cleaning (DLC) of silicon wafer surfaces. Samples covered with spherical colloidal particles (PS, SiO₂) and arbitrarily shaped Al₂O₃ particles with diameters from 320–1700 nm were cleaned using laser pulses with durations from 150 fs to 6.5 ns and wavelengths ranging from 400–800 nm. Cleaned areas were investigated with scanning electron and atomic force microscopy. Holes in the substrate with diameters of 200–400 nm and depths of 10–80 nm, depending on the irradiation conditions, were found at the former positions of the particles. For all pulse durations analyzed (fs, ps, ns), holes are created at laser fluences as small as the threshold fluence. Calculations of the optical field intensities in the particles’ neighbourhood by applying Mie theory suggest that enhancement of the incident laser intensity in the near field of the particles is responsible for these effects. DLC for sub-ns pulses seems to be governed by the local ablation of the substrate rather than by surface acceleration. Received: 31 May 2000 / Accepted: 7 September 2000 / Published online: 22 November 2000     

Flexible gratings fabricated in polymeric plate using femtosecond laser irradiation

Flexible gratings embedded in poly-dimethlysiloxane (PDMS) were fabricated using femtosecond laser pulses. Photo-induced gratings in a flexible PDMS plate were directly written by a high-intensity femtosecond (130 fs) Ti: Sapphire laser (λ_p=800 nm). Refractive index modifications with 4 μm diameters were photo-induced after irradiation of the femtosecond pulses with peak intensities of more than 1×10¹¹ W/cm². The graded refractive index profile was fabricated to be symmetric around the center of the focal point. The diffraction efficiency of the grating samples is measured by an He-Ne laser. The maximum value of refractive index change (Δn) in the laser-modified regions was estimated to be approximately 3.17×10⁻³.     

Ultra-fast laser absorption and ablation dynamics in wide-band-gap dielectrics

The highly nonlinear laser–matter interaction conditions produced by high-intensity amplified ultra-fast laser pulses have proven to be beneficial in the processing of normally transparent wide-band-gap dielectric materials. This article presents experimental studies of the ultra-fast laser absorption process in three wide-band-gap dielectrics: fused silica, calcium fluoride, and sapphire. Time-resolved measurements of the probe transmissivity and reflectivity show both the formation of dense free-electron plasma at the surface due to nonlinear absorption of the laser pulses and rapid structural damage on the order of a few picoseconds. Pump–probe data with intense pump and probe pulses was also correlated to atomic force microscopy measurements of the ablated volume. It was observed that the material removal peaked near zero delay between the pulses and decreased within a temporal separation of about 1 ps. PACS 52.38.Mf; 78.47.+p; 79.20.Ds     

Tunable, low-repetition-rate, cost-efficient femtosecond Ti:sapphire laser for nonlinear microscopy

We report on a broadly tunable, long-cavity Ti:sapphire laser oscillator being mode-locked in the net negative intracavity dispersion regime by Kerr-lens mode-locking, delivering τ _FWHM<300 fs pulses at 22 MHz repetition rate. The wavelength of the laser can be tuned over a 170 nm wide range between 712 nm and 882 nm. Having a typical pump power of 2.6 W, the maximum pulse peak power is 60 kW. Comparison of the reported laser with a standard, 76 MHz Ti:sapphire oscillator regarding two-photon excitation efficiency in a laser scanning microscope shows that the 22 MHz laser generates the same fluorescence signal at considerably, 1.82 times lower average power, which is expected to result in a reduced photothermal damage probability of biological samples. This fact along with the broad tunability and a low pump power requirement makes this cost-effective laser an ideal light source for nonlinear microscopy.     

Laser ablation of polymers using 395 nm and 790 nm femtosecond lasers

We compared a Ti:sapphire fs laser (790 nm) with a second harmonics (395 nm) fs laser, and then mixed them for ablating polyethylene (PE). Compared to the 790 nm fs laser, the 395 nm fs laser harmonics could etch PE faster. However, isolated carbon was formed on the ablated surface, in addition to C=O and C=C-H bonds. When we mixed a faint beam of the 395 nm fs laser harmonics with the 790 nm fs laser, the etching depth became even deeper. Moreover, the chemical composition of the ablated surface remained unchanged. At a total laser fluence of 80 mJ/cm², the most suitable laser fluences for the 395 nm fs laser harmonics and the 790 nm fs laser were found to be approximately 2 and 78 mJ/cm² respectively. PACS 81.65.Cf     

Pulse compression of a high-order harmonic

The fifth harmonic pulses of an intense femtosecond Ti:sapphire laser were experimentally shown to be negatively chirped by using an LiF plate as a positive dispersive medium. The chirp of the harmonic pulse originates from the intensity-dependent atomic dipole phase, which is estimated to be proportional to 25 U_p, where U_p is the ponderomotive energy. Consequently, we have succeeded in compressing the chirped pulses to 13 fs by compensating the intrinsic negative chirp. Chirp effects of the fundamental laser on the pulse width of the fifth harmonic were consistent with the negative chirp of the fifth harmonic.     

Dispersion control in fiber-coupled THz-TDS

To construct a compact THz-TDS system equipped with movable emitter and receiver heads, a specific fiber-delivery system is developed to deliver ultra-short pulses from Ti: sapphire laser through a single-mode fiber. Hence, how to manage the dispersion in fiber-delivery system efficiently becomes one of the most important issues to be solved. In this paper, the theoretical calculation of dispersion in fiber-delivery system was discussed initially. And also, a pair of gratings, which can generate negative group velocity dispersion (GVD), was introduced to compensate the positive dispersion in fiber. A minimum temporal width of pulse about 60 fs was measured at the end of the fiber-delivery system by optimizing the relative position of gratings. The experimental result agreed well to the theoretical calculation and demonstrated the advantages of the fiber-delivery system.     

基于交叉偏振波产生的脉冲净化技术研究与应用

本文利用交叉偏振波产生技术(XPW)对800 nm波段钛宝石飞秒激光器输出的激光脉冲进行时域净化, 提高脉冲时域对比度, 并测量验证了10¹¹对比度的脉冲, 达到测量仪器的动态范围极限, 比初始脉冲时域对比度有三个量级的提高, XPW的效率为22%. 同时发现净化后脉冲光谱宽度也得到一定展宽, 进一步利用啁啾镜对和补偿片对净化后的脉冲进行色散补偿, 得到25 fs脉宽的脉冲. 利用该净化后的激光脉冲作为种子注入已有的太瓦级钛宝石啁啾脉冲放大系统中, 在输出脉冲能量250 mJ, 宽度50 fs, 对应峰值功率5 TW的情况下, 在主脉冲前100 ps以外的范围内测量验证了10¹¹的脉冲对比度.     

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.