飞秒激光与晶体材料相互作用的研究进展

综述了飞秒激光与各种晶体材料作用的现象,如双光子、多光子非线性吸收致上转换发光现象,各类微结构、色心结构等;阐述了飞秒激光与各种晶体的作用机制及在各方面的应用;展望了飞秒激光与晶体材料作用的应用前景.     

The Generation of a Dense Hot Plasma by Intense Subpicosecond Laser Pulses

A simple model is developed for describing the interaction of intense femtosecond laser pulses with solid-state targets which is based on a set of equations of two-temperature hydrodynamics for electrons and ions of a plasma formed upon ionization of the target matter, equations describing the variation of ion composition of plasma upon ionization and the heat energy expenditure on thermal ionization, and equations defining the energy contribution by laser radiation to the target matter. A self-similar solution is suggested which well describes the heating of plasma electrons during the time of effect of a femtosecond laser pulse in a wide range of its parameters. Lagrangian computer codes developed for this purpose are used to derive, in a one-dimensional approximation, a numerical solution for the set of equations for the parameters corresponding to femtosecond experimental facilities under development in Germany and Russia. Profiles of hydrodynamic quantities (electron and ion temperature, plasma pressure and density, mean ion charge) obtained in the numerical solution at different moments of time may be used for preliminary assessment of the results of future experiments with a view to optimizing their parameters.     

Ultra-Short Pulsed Laser Manufacturing and Surface Processing of Microdevices

Ultra-short laser pulses possess many advantages for materials processing. Ultrafast laser has a significantly low thermal effect on the areas surrounding the focal point; therefore, it is a promising tool for micro- and submicro-sized precision processing. In addition, the nonlinear multiphoton absorption phenomenon of focused ultra-short pulses provides a promising method for the fabrication of various structures on transparent material, such as glass and transparent polymers. A laser direct writing process was applied in the fabrication of high-performance three-dimensional (3D) structured multilayer micro-supercapacitors (MSCs) on polymer substrates exhibiting a peak specific capacitance of 42.6 mF·cm⁻² at a current density of 0.1 mA·cm⁻². Furthermore, a flexible smart sensor array on a polymer substrate was fabricated for multi-flavor detection. Different surface treatments such as gold plating, reduced-graphene oxide (rGO) coating, and polyaniline (PANI) coating were accomplished for different measurement units. By applying principal component analysis (PCA), this sensing system showed a promising result for flavor detection. In addition, two-dimensional (2D) periodic metal nanostructures inside 3D glass microfluidic channels were developed by all-femtosecond-laser processing for real-time surface-enhanced Raman spectroscopy (SERS). The processing mechanisms included laser ablation, laser reduction, and laser-induced surface nano-engineering. These works demonstrate the attractive potential of ultra-short pulsed laser for surface precision manufacturing.     

Femtosecond snapshot imaging of propagating light itself

An ultrafast imaging technique has been developed to visualize directly a light pulse that is propagating in a medium. The method, called femtosecond time-resolved optical polarigraphy (FTOP), senses instantaneous changes in the birefringence within the medium that are induced by the propagation of an intense light. A snapshot sequence composed of each femtosecond probing the pulse delay enables ultrafast propagation dynamics of the intense femtosecond laser pulse in the medium, such as gases and liquids, to be visualized directly. Other examples include the filamentation dynamics in CS2 liquid and the propagation dynamics in air related to the interaction with laser breakdown plasma. FTOP can also be used to extract information on the optical Kerr constant and its decay time in media. This method is useful in the monitoring of the intensity distribution in the nonlinear propagation of intense light pulses, which is a frequently studied subject in the field of physics regarding nonlinear optics and laser processing.     

Application of high harmonic radiation in surface science

The development of compact and commercially available table-top, ultra-short pulse laser systems with pulse energies of the order of a few mJ, pulse durations of less then 30 fs and repetition rates of several kHz enables routinely the generation of high harmonic radiation with photon energies up to 100 eV. Thereby many different applications in surface science become possible that benefit from the particular characteristics of this kind of light source. In future, especially time resolved measurements that take advantage of the ultra-short pulses in the femtosecond and attosecond regime will attract considerable attention. Also the access to the whole Brillouin zone will stimulate new, time-resolved experiments. In this paper we will discuss applications of high harmonics to study surface properties using microscopy and photoelectron spectroscopy, and highlight investigations of dynamic processes in the XUV and soft X-ray regime.     

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.     

飞秒激光空间选择性诱导玻璃微结构及应用

利用飞秒激光与玻璃的非线性相互作用，可以对玻璃进行空间选择性微观改性与修饰，赋予新的光功能．本文介绍飞秒激光的持点及其对玻璃微结构的改性，以及近年来利用飞秒激光进行玻璃的缺陷控制、光活性离子(稀土、过渡和重金属离子)价态操作、微晶析出与折射率调控及其在光开关、波分复用、波导型有源器件、光子晶体等微光学器件的制备及光学集成领域应用的进展．     

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.     

Formation of void array inside transparent and absorptive glasses by femtosecond laser irradiation

We demonstrate self-fabrication of void arrays in a fused silica transparent in the visible and a color-filter borosilicate glass strongly absorptive at 800 nm using tightly focused Ti-sapphire femtosecond laser pulses at 1 kHz without scanning. The period, the size, the number of voids, and the length of the aligned void structure were controlled by changing the laser pulse energy, and the position of the focal point inside two materials. The void arrays were observed by an optical microscope and also estimated by an optical diffraction experiment. The void size and period were smaller in the absorptive glass than in the transparent glass. The submicrometer-sized void was observed by a scanning electron microscope. The smaller and clearer void arrays were formed in the color filter than the fused silica glass. With increasing the laser focal depth, the void-array length increased in the fused silica and decreased in the color filter.     

飞秒激光烧蚀MgAl2O4透明陶瓷的实验研究

实验研究了800nm飞秒激光与MgAl2O4透明陶瓷的相互作用，得到其在单脉冲、多脉冲情况下的损伤阈值和损伤面积，用CCD成像技术和扫描电镜观察了烧蚀点的形貌特征，用显微红外光谱仪测试了烧蚀区域的透过光谱．结果表明；单脉冲烧蚀条件下，烧蚀面积与脉冲能量近似为线性关系，而在多脉冲烧蚀条件下，烧蚀面积随着脉冲数量的增加呈近似波尔兹曼（Boltzmann）增大；当激光功率接近损伤阈值时，烧蚀后的区域在波数为2500-7000cm^-1范围内的红外透过率由82％提高到86％，当激光功率超过损伤阈值后，透过率降低20％左右．     

Fabrication of beam shapers in the bulk of fused silica by femtosecond laser pulses

We reported a new approach to the fabrication of three-dimensional refractive-index-modified microstructures inside transparent materials by combining two-dimensional writing by scanning the focus of the femtosecond laser pulse and by forming the long filament in the third dimension. In this way, embedded diffractive beam shapers of grid, square, and ring gratings were obtained in the bulk of fused silica by use of a femtosecond laser with a wavelength of 810 nm and a repetition rate of 1 KHz. These structures and their refractive efficiencies were optimized by selection of the appropriate fabrication parameters, including the pulse energy, grating period, scanning speed, and scanning repetition. The good performance of these devices indicates that, owing to its simple and flexible method for fabricating complex phase elements inside transparent materials, this technique has potential applications to integrated optics.     

Mechanism of fine ripple formation on surfaces of (semi)transparent materials via a half-wavelength cavity feedback

The mechanism of the fine ripples, perpendicular to laser polarization, on the surface of (semi)transparent materials with period smaller than the vacuum wavelength, λ, of the incident radiation is proposed and experimentally validated. The sphere-to-plane transformation of nanoplasma bubbles responsible for the in-bulk ripples accounts for the fine ripples on the surface of dielectrics and semiconductors. The mechanism is demonstrated for 4H:SiC and sapphire surfaces using 800 nm/150 fs and 1030 nm/300 fs laser pulses. The ripples are pinned to the smallest possible standing wave cavity inside material of refractive index n. This defines the corresponding period, Λ = (λ/n)/2, of a light standing wave with intensity, E(2), at the maxima of which surface ablation occurs. The mechanism accounts for the fine ripples at the breakdown conditions. Comparison with ripples recorded on different materials and via other mechanisms using femtosecond pulses is presented and application potential is discussed.     

Controlling spins with light

The interaction of sub-picosecond laser pulses with magnetically ordered materials has developed into an extremely exciting research topic in modern magnetism. From the discovery of sub-picosecond demagnetization over a decade ago to the recent demonstration of magnetization reversal by a single 40?fs laser pulse, the manipulation of spins by ultrashort laser pulses has become a fundamentally challenging topic with a potentially high impact for future spintronics, data storage and manipulation, and quantum computation. We have recently demonstrated that one can generate ultrashort and very strong (teslas) magnetic field pulses via the so-called inverse Faraday effect. Such optically induced magnetic field pulses provide unprecedented means for the generation, manipulation and coherent control of spins on very short time scales. The basic ideas behind these so-called opto-magnetic effects will be discussed and illustrated with recent results, demonstrating the various possibilities of this new field of femto-magnetism.     

Laser‐Directed Assembly of Nanorods of 2D Materials

Herein, the previously unrealized ability to grow nanorods and nanotubes of 2D materials using femtosecond laser irradiation is demonstrated. In as short as 20 min, nanorods of tungsten disulfide, molybdenum disulfide, graphene, and boron nitride are grown in solutions. The technique fragments nanoparticles of the 2D materials from bulk flakes and leverages molecular scale alignment by nonresonant intense laser pulses to direct their assembly into nanorods up to several micrometers in length. The laser treatment process is found to induce phase transformations in some of the materials, and also results in the modification of the nanorods with functional groups from the solvent atoms. Notably, the WS₂ nanoparticles, which are ablated from semiconducting 2H WS₂ crystallographic phase flakes, reassemble into nanorods consisting of the 1T metallic phase. Due to this transition, and the 1D nature of the fabricated nanorods, the WS₂ nanorods display substantial improvements in electrical conductivity and optical transparency when employed as transparent conductors.     

Radiation sources based on laser-plasma interactions

Plasma waves excited by intense laser beams can be harnessed to produce femtosecond duration bunches of electrons with relativistic energies. The very large electrostatic forces of plasma density wakes trailing behind an intense laser pulse provide field potentials capable of accelerating charged particles to high energies over very short distances, as high as 1GeV in a few millimetres. The short length scale of plasma waves provides a means of developing very compact high-energy accelerators, which could form the basis of compact next-generation light sources with unique properties. Tuneable X-ray radiation and particle pulses with durations of the order of or less than 5fs should be possible and would be useful for probing matter on unprecedented time and spatial scales. If developed to fruition this revolutionary technology could reduce the size and cost of light sources by three orders of magnitude and, therefore, provide powerful new tools to a large scientific community. We will discuss how a laser-driven plasma wakefield accelerator can be used to produce radiation with unique characteristics over a very large spectral range.     

Direct characterization of self-guided femtosecond laser filaments in air

High-power femtosecond laser pulses propagating in air form self-guided filaments that can persist for many meters. Characterizing these filaments has always been challenging owing to their high intensity. An apparently novel diagnostic is used to directly measure the fluence distribution of femtosecond laser pulses after they have formed self-guided optical filaments in air. The diagnostic is unique in that the information contained in the filaments is not lost owing to the interaction with the apparatus. This allows filament characteristics such as energy and size to be unambiguously determined for the first time.     

A high-order corrected description of ultra-short and tightly focused laser pulses, and their electron acceleration in vacuum

Field expressions are derived for ultra-short, tightly focused laser pulses up to the second-order temporal correction and seventh-order spatial correction. To evaluate the importance of these corrections, we simulate these fields and investigate the final energy of the accelerated electrons. We vary the order of the corrected expressions, the pulse duration, and the beam waist. We find that electron capture is still an important and generic phenomenon in ultra-short, tightly focused laser pulses. While small differences in the electron acceleration are obtained for various orders of the corrected field equations relative to the paraxial field equations, there is no qualitative difference in the behavior of the electron. Furthermore, the temporal and spatial corrections are found to be correlated.     

仿生超滑表面的飞秒激光微纳制造及应用

仿猪笼草的超滑表面由于可以抵抗多种液体的粘附,具有优异的稳定性与自修复性,受到越来越广泛的关注.而飞秒激光由于其对加工材料的普适性、高精度,以及高可控性,成为仿生超滑表面制备的有力手段.本文以仿猪笼草的超滑表面为背景,以飞秒激光微加工技术为手段.从超滑表面的飞秒激光微纳制备和应用两个方面,概述了超滑表面的微纳制造和应用...     

Long-range detection and length estimation of light filaments using extra-attenuation of terawatt femtosecond laser pulses propagating in air

High-energy femtosecond laser pulses propagating in the atmosphere undergo self-focusing resulting in the appearance of the phenomenon of filamentation. We observed an extra-attenuation of such (terawatt) femtosecond laser pulses propagating in the atmosphere when compared with long pulses (200 ps) with the same energy. This is because, in contrast to the linear propagation of the long pulse, the input femtosecond laser pulse is attenuated owing to either absorption through multiphoton ionization/tunnel ionization or to scattering on the laser-induced plasma; self-phase-modulation and self-steepening further convert partially the energy initially contained in the fundamental bandwidth into the broad side bands of the laser, becoming eventually a white-light laser pulse (supercontinuum). The experimental data allow us to extract an effective extra-attenuation coefficient for an exponential decay of the input pulse energy with the propagation distance. Such a coefficient allows us to estimate an upper bound of the filament length under the experimental conditions used. More generally, our observation leads to a new technique to remotely detect light filaments in the atmosphere.     

Structural changes accompanying color center formation in lithium fluoride exposed to femtosecond laser pulses

This paper examines structural changes produced in crystalline LiF by high-power femtosecond laser pulses and provides some insight into the mechanisms of structural damage to the material. In the region of the onset of multiple femtosecond laser beam filamentation and in the central part of the filaments, we observed partial melting of the material, cracking, and the formation of structural nanodefects that showed up as step pyramids and nanogratings in atomic force microscopy images.