Generation and detection of incoherent phonons in picosecond ultrasonics

In picosecond ultrasonics experiments the absorption of a femtosecond laser pulse in a thin metallic transducer is used to generate very short acoustic pulses. These pulses are made of coherent longitudinal waves with a frequency spectrum that can reach 100-200 GHz. The laser pulse absorption gives rise to a heating of the film of a few Kelvin within a typical time of 1 ps. Later on, the heat goes in the substrate through an interface thermal resistance and is diffused by thermal conduction. At very low temperature and in pure crystals the thermal phonons emitted by the heated metallic film can propagate ballistically over large distances and produce a so-called heat pulse. We report on the experimental evidence of the coexistence of the coherent acoustic pulse and the incoherent heat pulse generated and detected by laser ultrasonics.     

Thermoelastic wave induced by pulsed laser heating

In this work, a generalized solution for the thermoelastic plane wave in a semi-infinite solid induced by pulsed laser heating is developed. The solution takes into account the non-Fourier effect in heat conduction and the coupling effect between temperature and strain rate, which play significant roles in ultrashort pulsed laser heating. Based on this solution, calculations are conducted to study stress waves induced by nano-, pico-, and femtosecond laser pulses. It is found that with the same maximum surface temperature increase, a shorter pulsed laser induces a much stronger stress wave. The non-Fourier effect causes a higher surface temperature increase, but a weaker stress wave. Also, for the first time, it is found that a second stress wave is formed and propagates with the same speed as the thermal wave. The surface displacement accompanying thermal expansion shows a substantial time delay to the femtosecond laser pulse. On the contrary, surface displacement and heating occur simultaneously in nano- and picosecond laser heating. In femtosecond laser heating, results show that the coupling effect strongly attenuates the stress wave and extends the duration of the stress wave. This may explain the minimal damage in ultrashort laser materials processing. Received: 23 May 2000 / Accepted: 26 May 2000 / Published online: 20 September 2000     

Tuning the shape anisotropy of silver nanoparticles using time-delayed laser pulse pair irradiations

Glass-embedded spherical silver nanoparticles were irradiated by pairs of delayed femtosecond laser pulses. The influence of intensity, relative polarization (parallel or orthogonal) and time delay between the pulses was investigated. We found a delay-dependent reversal of the orientation of prolate nanoparticles produced in the low-intensity regime: at very short time delays up to 10 ps between pulse pairs the polarization direction of the second-hitting pulse defines the particles’ symmetry axes; in an intermediate regime between 10 and 20 ps no optical dichroism is found at all; at more than 20 ps delay between the pulses, finally, the transformed nanoparticles are oriented along the polarization direction of the first-hitting pulse. Also, in the quite different situation of the high-intensity regime using parallel-polarized pulse pairs, where normally oblate particles are created, isotropic spectral changes (i.e., no dichroism) after irradiation were observed at delay times around 20 ps. The possible physical background of this apparently very special inter-pulse delay of around 20 ps is discussed.     

Nonequilibrium magnetization dynamics of gadolinium studied by magnetic linear dichroism in time-resolved 4f core-level photoemission

The magnetic linear dichroism of the gadolinium 4f core level is studied in a time-resolved photoemission experiment employing laser pump- and synchrotron-radiation probe pulses. Upon optical excitation of the 5d6s valence electrons with femtosecond laser pulses, the magnetic order in the 4f spin system is reduced. Remarkably, the linear dichroism remains at 80% of the equilibrium contrast while the lattice temperature reaches the Curie temperature due to electron-phonon scattering. Contrasting itinerant ferromagnets, this shows that equilibration between the lattice and spin subsystems takes in Gd about 80 ps and is established in parallel with heat diffusion.     

Direct observation of the temperature field during ablation of materials by multiple femtosecond laser pulses

We report a direct observation of the temperature field on a steel specimen during ablation by multiple femtosecond laser pulses using an infrared thermography technique. From the experimental results and simulation study of the temperature field, we quantified the deposited thermal power into the specimen during the ablation process. We found that more than two thirds of the incident laser power was deposited in the steel specimen when ablated by multiple femtosecond laser pulses. This result provides further understanding of the heating effect in materials processing by ultrashort laser pulses.     

Thermal characteristics of double-layer thin film target ablated by femtosecond laser pulses

Thermal characteristics of tightly-contacted copper--gold double-layer thin film target under ablation of femtosecond laser pulses are investigated by using a two-temperature theoretical model. Numerical simulation shows that electron heat flux varies significantly on the boundary of copper--gold film with different maximal electron temperature of 1.15×10³ K at 5 ps after ablating laser pulse in gold and copper films, which can reach a balance around 12.6 ps and 8.2 ps for a single and double pulse ablation, respectively, and in the meantime, the lattice temperature difference crossing the gold--copper interface is only about 0.04×10³ K at the same time scale. It is also found that electron--lattice heat relaxation time increases linearly with laser fluence in both single and double pulse ablation, and a sudden change of the relaxation time appears after the laser energy density exceeds the ablation threshold.     

Dynamics of light-induced reflectivity switching in gallium films deposited on silica by pulsed laser ablation

We present what is to our knowledge the first experimental study of light-induced reflectivity changes at an alpha-Ga/Si interface irradiated by femtosecond and picosecond laser pulses. After exposure, the reflectivity can increase from R?0.55 , which is typical for alpha-Ga , to R?0.8 , which is close to that of liquid Ga. The initial step in the reflectivity change of 2-4 ps is resolved with 150-fs laser pulses. The light-induced reflectivity change relaxes during 100ns-10 mus , depending strongly on the background temperature of the Ga mirror and the laser fluence.     

Modeling of the processes of laser-nanoparticle interaction taking into account temperature dependences of parameters

Absorption, electron-phonon coupling and heating of nanoparticles (NPs) under action of short laser pulses on NPs and their cooling after the end of laser action usually has nonlinear character. Nonlinear electron-phonon coupling under action of pico- and femtosecond pulses on metal NPs depends on electron and lattice parameters. Optical (absorption, scattering, extinction) and thermo-physical (coefficient of thermal conductivity, heat capacity, etc.) parameters of different materials of NPs (metals, oxides, semiconductors, etc.) and environments (water, liquids, dielectrics, etc.) depend on temperature and determine nonlinear dynamics of NPs heating and cooling. It is very important to take into account the temperature dependence of optical and thermophysical parameters of NPs and surrounding media under investigation of absorption of laser radiation, electron-phonon coupling, nanoparticle (NP) heating, heat transfer and its cooling after the end of laser pulse action. Theoretical modeling of the processes of laser-NP interaction taking into account temperature dependences of parameters of NPs and environments was carried out. Influence of temperature dependences of these parameters on values and dynamics of the processes is determined.     

Effect of pulse duration on plasmonic enhanced ultrafast laser-induced bubble generation in water

Bubbles generated in water by focusing femtosecond and picosecond laser pulses in the presence of 100 nm gold nanoparticles have been investigated in the fluence range usually used for efficient cell transfection (100–200 mJ/cm²). Since resulting bubbles are at the nanoscale, direct observation using optical microscopy is not possible. An optical in-situ method has been developed to monitor the time-resolved variation in the extinction cross-section of an irradiated nanoparticle solution sample. This method is used to measure the bubbles lifetime and deduce their average diameter. We show that bubbles generated with femtosecond pulses (40–500 fs) last two times longer and are larger in average than those generated with picosecond pulses (0.5–5 ps). Controlling those bubble properties is necessary for optimizing off-resonance plasmonic enhanced ultrafast laser cell transfection.     

Wavelength-independent all-optical synchronization of a Q-switched 100-ps microchip laser to a femtosecond laser reference source

We present a Q-switched microchip laser emitting 1064-nm pulses as short as 100 ps synchronized to a cavity dumped femtosecond laser emitting 800-nm pulses as short as 80 fs. The synchronization is achieved by presaturating the saturable absorber of the microchip laser with femtosecond pulses even though both lasers emit at widely separated wavelengths. The mean timing jitter is 40 ps and thus considerably shorter than the pulse duration of the microchip laser.     

Short-pulse laser ablation of solids: from phase explosion to fragmentation

The mechanisms of laser ablation in silicon are investigated close to the threshold energy for pulse durations of 500 fs and 50 ps. This is achieved using a unique model coupling carrier and atom dynamics within a unified Monte Carlo and molecular-dynamics scheme. Under femtosecond laser irradiation, isochoric heating and rapid adiabatic expansion of the material provide a natural pathway to phase explosion. This is not observed under slower, nonadiabatic cooling with picosecond pulses where fragmentation of the hot metallic fluid is the only relevant ablation mechanism.     

Surface ripple changes during Cr film ablation with a double ultrashort laser pulse

Surface modification is investigated experimentally by varying the time separation of double femtosecond laser radiation and surface ripples by varying the time separation and polarization direction of double pulses train. Nanometer-sized particles are formed during resolidification of the molten region when the second pulse arrives within 10 ps and the molten material is ejected much after 10 ps. The ripple in the outer region remains oblique to the sum of the vector direction of the two pulses when the time delay is zero. With time delay ranging from 0.5 to 10 ps and different polarization directions of the laser radiation, the ripple generally aligned perpendicular to the polarization direction of the electric field with multiple pulses in the vicinity of ablation threshold is effectively eliminated without fragments at the edge. Furthermore, remnant ripples on irradiated area at higher energies with the same polarization direction are removed by irradiation at a lower energy with each different polarization direction of double pulse. Based on morphological observations for different time delays, possible mechanisms of ripple formations and eliminations are suggested.     

Ultrafast relaxation dynamics of electronic excitations in noble-metal clusters

We investigate non-equilibrium relaxation processes in optically excited large gold and silver clusters. Time-resolved pump-probe experiments and model calculations show that optical excitation of the clusters by femtosecond laser pulses results in a heating of the electron system, which is followed by electron cooling via phonon emission. The electron heating leads to an enhanced damping of the surface-plasmon resonance in the clusters. This enhanced damping is caused by an enhancement of the Landau damping and electron scattering rates at high electron temperatures. Furthermore, we find that the rate of electron cooling in the clusters changes with electron temperature; this is a consequence of the temperature-dependent specific heat of the conduction electrons. Finally, pump-probe experiments on ellipsoidal silver clusters show that the thermal expansion of the heated clusters triggers mechanical vibrations at the acoustic eigenfrequencies of the clusters. Received: 6 December 1999 / Published online: 7 August 2000     

超短脉冲激光辐照金属薄膜温升效应的模拟研究

 考虑到材料的质量热容、热导率、驰豫时间等热力学参数随温度非线性变化因素的影响,利用具有人工粘性的、自适应时间步长的前向差分算法,数值求解了电子-晶格双温双曲两步热传导模型,讨论了厚度为50 nm的金膜在0.1 ps脉冲激光辐照下的温升规律。数值结果表明：薄膜前表面自由电子的温度在大约0.27 ps时达到最大值,不同厚度上自由电子达到温度平衡所需的时间大约为1.6 ps,而薄膜温度在整个厚度上达到平衡所需时间为60 ps左右。由电子温度及其温度梯度引起的热电子崩力很可能是造成材料破坏的一个主要因素。     

Laser ablation of silicon in water with nanosecond and femtosecond pulses

We describe laser ablation of Si under water by 5 ns, 355 nm and 100 fs, 800 nm pulses. Compared to that in air, an approximately twofold improvement in the ablation rate is found in water for femtosecond and nanosecond pulses. For higher laser irradiances, the plasma that forms at the water-air interface hampers further improvement of the ablation rate. We investigated the enhanced ablation process in water and found that the cavity-confinement geometry that increases the laser energy coupling to the target and allows more energy to be transferred to the cavity sidewalls plays an important role in the escalated material removal process. In addition, we show that the water layer that effectively reduces the oxidation and redeposition of the ablated debris is also responsible for improvements in the ablation process.     

基于非线性偏振旋转锁模的高功率光子晶体光纤飞秒激光振荡器

为了探索大模场面积光子晶体光纤锁模激光器在全正色散锁模域内的耗散孤子锁模机理, 以获得更大的单脉冲能量和更高的峰值功率, 本文搭建了以掺镱大模场面积光子晶体光纤作为增益介质的耗散孤子锁模激光器. 激光器使用环形腔结构, 利用非线性偏振旋转以及滤光片提供的耗散作用实现了稳定的锁模运转. 实验中, 从激光器振荡级直接获得了平均功率10 W, 重复频率49.09 MHz(对应202 nJ的单脉冲能量), 脉冲宽度为1.03 ps的稳定锁模脉冲输出, 经过腔外色散补偿得到的脉冲宽度为95.5 fs.     

基于飞秒瞬态反射/透射技术的纳米Au半透膜热效应研究

以飞秒激光放大器作为光源联合使用瞬态反射/透射实验技术研究了纳米Au半透明纳米薄膜中非平衡载能粒子的热传导过程. 在相同实验条件下, 发现该薄膜的瞬态透射和反射信号明显不同并且延迟时间在5.0–7.5 ps时瞬态透射信号的符号发生改变. 对纳米薄膜的透射和反射信号进行了对比分析, 分别使用双温模型和Crude近似进行数据模拟并拟合, 分析认为沿膜厚方向的温度梯度变化和界面热阻效应引起介电函数的变化不同, 从而引起了瞬态透射信号和反射信号的不同. 对于半透明金属纳米薄膜需要同时考虑其瞬态透射和反射影响才能得到准确的瞬态吸收结果. 随着抽运脉冲能量的增加, 可以看到上升时间约为1.0 ps, 电子-晶格弛豫时间增加.     

Simulation of laser ablation in aluminum: the effectivity of double pulses

Lasers are becoming a more and more important tool in cutting and shaping materials. Improving precision and effectivity is an ongoing demand in science and industry. One possibility is double pulses. Here, we study laser ablation of aluminum by the two-temperature model. There the laser is modeled as a source in a continuum heat conduction equation for the electrons, whose temperature then is transferred to a molecular dynamics particle model by an electron–phonon coupling term. The melting and ablation effectivity is investigated depending on the relative intensity and the time delay between two Gaussian shaped laser pulses. It turns out that at least for aluminum the optimal pulse shapes are standard Gaussian pulses. For double pulses with delay times up to 200 ps, we find a behavior as observed in experiment: The ablation depth decreases beyond a delay of 10 ps even if one does not account for the weakening at the second pulse due to laser–plasma interaction.     

Mechanisms of femtosecond laser nanosurgery of cells and tissues

We review recent advances in laser cell surgery, and investigate the working mechanisms of femtosecond laser nanoprocessing in biomaterials with oscillator pulses of 80-MHz repetition rate and with amplified pulses of 1-kHz repetition rate. Plasma formation in water, the evolution of the temperature distribution, thermoelastic stress generation, and stress-induced bubble formation are numerically simulated for NA=1.3, and the outcome is compared to experimental results. Mechanisms and the spatial resolution of femtosecond laser surgery are then compared to the features of continuous-wave (cw) microbeams. We find that free electrons are produced in a fairly large irradiance range below the optical breakdown threshold, with a deterministic relationship between free-electron density and irradiance. This provides a large ‘tuning range’ for the creation of spatially extremely confined chemical, thermal, and mechanical effects via free-electron generation. Dissection at 80-MHz repetition rate is performed in the low-density plasma regime at pulse energies well below the optical breakdown threshold and only slightly higher than used for nonlinear imaging. It is mediated by free-electron-induced chemical decomposition (bond breaking) in conjunction with multiphoton-induced chemistry, and hardly related to heating or thermoelastic stresses. When the energy is raised, accumulative heating occurs and long-lasting bubbles are produced by tissue dissociation into volatile fragments, which is usually unwanted. By contrast, dissection at 1-kHz repetition rate is performed using more than 10-fold larger pulse energies and relies on thermoelastically induced formation of minute transient cavities with lifetimes <100 ns. Both modes of femtosecond laser nanoprocessing can achieve a 2–3 fold better precision than cell surgery using cw irradiation, and enable manipulation at arbitrary locations. PACS 42.62.Be; 72.20.Jv     

On the nature of “coherent artifact”

The coherent interaction of femtosecond laser pulses in the pump-probe regime has been experimentally studied in the time domain by monitoring light reflection from a tellurium single crystal. The optical response of the probed medium exhibits periodic variations at a frequency equal to that of the exciting laser radiation. Experimental dependences of the observed “coherent artifact” on the pump/probe intensity ratio, the number of accumulated pulses, and the mutual orientation of the polarization vectors of electromagnetic fields and the crystallographic axes are well described by the proposed phenomenological model.