Thermal Analysis of Gold Nanorods Heated with Femtosecond Laser Pulses

We present an axisymmetric computational model to study the heating processes of gold nanoparticles, specifically nanorods, in aqueous medium by femtosecond laser pulses. We use a two-temperature model for the particle, a heat diffusion equation for the surrounding water to describe the heat transfer processes occurring in the system, and a thermal interface conductance to describe the coupling efficiency at the particle/water interface. We investigate the characteristic time scales of various fundamental processes, including lattice heating and thermal equilibration at the particle/surroundings interface, the effects of multiple laser pulses, and the influence of nanorod orientation relative to the beam polarization on energy absorption. Our results indicate that the thermal equilibration at the particle/water interface takes approximately 500 ps, while the electron-lattice coupling is achieved at approximately 50 ps when a 48×14 nm gold nanorod is heated to a maximum temperature of 1270 K with the application of a laser pulse having 4.70 J/m(2) average fluence. Irradiation by multiple pulses arriving at 12.5 ns time intervals (80 MHz repetition rate) causes a temperature increase of no more than 3 degrees during the first few pulses with no substantial changes during the subsequent pulses. We also analyze the degree of the nanorods' heating as a function of their orientation with respect to the polarization of the incident light. Lastly, it is shown that the temperature change of a nanorod can be modeled using its volume equivalent sphere for femtosecond laser heating within 5-15% accuracy.     

Simulation of the acceleration mechanism by light-propulsion for the powder particles at laser direct material deposition

The results of the numerical analysis of heat- and mass-transfer processes at powder particles' motion in a gas flow and laser beam by light-propulsion force during the laser cladding and direct material deposition are presented. Under consideration were the stainless steel particles, the radiation power range of the CO₂ laser were 1000, 3000 and 5000 W. Finally, the particles of 45 μm in diameter reach the maximum velocity of about 80, 220, 280 m/s. It is shown that as particles are heated by the laser up to the temperature approaching the boiling point, the particles' velocity in the light field by the vapor recoil pressure may increase significantly. The radius of the particles slightly varies due to the evaporation; the losses in the clad material mass are negligibly small. Comparisons of numerical results with known experimental data on light-propulsion acceleration of single particles (aluminum, aluminum oxide and graphite) under the influence of pulse laser radiation are also presented. Particle acceleration resulting from the laser evaporation depends on the particle diameter, powder material properties, focusing degree and attenuation laser beam intensity by the direction of its propagation.     

激光等离子体去除微纳颗粒的热力学研究

微杂质污染一直是影响精密器件制造质量和使用寿命的关键因素之一.对于微纳米杂质颗粒用传统的清洗方式(超声清洗等)难以去除,而激光等离子体冲击波具有高压特性,可以实现纳米量级杂质颗粒的去除,具有很大的应用潜力.本文主要研究了激光等离子体去除微纳米颗粒过程中的热力学效应:实验研究了激光等离子体在不同脉冲数下对Si基底上Al颗粒去除后的颗粒形貌变化,发现大颗粒会发生破碎而转变成小颗粒,一些颗粒达到熔点后发生相变形成光滑球体,这源于等离子体的热力学效应共同作用的结果.为了研究微粒物态转化过程,基于冲击波传播理论研究,得到冲击波压强与温度特性的演化规律;同时,利用有限元模拟方式研究激光等离子冲击波压强和温度对微粒作用规律,得到了颗粒内随时间变化的应力分布和温度分布,并在此基础上得到等离子体对颗粒的热力学作用机制.     

Experimental mathematical model of nanosecond laser interaction with material

Interaction of nanosecond pulsed lasers with material was studied from thermal point of view using experimental techniques and theoretical approach of dimensional analysis. Experimental data of laser heating, melting and plasma formation on metallic samples and silicon, presented mainly in previous publication and partly in this paper, were used for formation of experimental mathematical model in the form of criteria equations of laser-material interaction process. Four different criteria equations were created: for maximum surface temperature increase, melting threshold, melting duration and plasma formation threshold. Two equations account for changes of thermal properties with temperature. The value of latent heat of fusion was found to have almost no influence on melting duration. The presented model showed good agreement with the measured results. The criteria equations can be used for approximate prediction of laser pulse effects on materials without creating an exact mathematical or numerical model and for control of technological processes.     

高温电离气体中微细颗粒的加热

本文分析表明，自由分子流区高温电离气体中颗粒的团相加热、熔化、液相加热与强烈蒸发等加热阶段所需的时间，均正比于颗粒半径，其中蒸发阶段需时最长．颗粒表面温度高于约４０００Ｋ时，热电子发射开始显著影响颗粒的加热速率，辐射则在低得多的温度下（如２０００Ｋ）开始影响颗粒的加热．     

Mechanism of pulse laser interaction with colloidal nanoparticles

The laser is a very powerful and very useful instrument in modern nanoscience and nanotechnology. The knowledge of the interaction mechanism of the laser beam with nanoparticles is needed to control the laser processing of different nano‐objects. It was shown that the particle heating–melting–evaporation model can be successfully applied for many phenomena arising when colloidal nanoparticle interact with pulsed laser beams. The general approach of this model is discussed in detail. The two main components of the model, light absorption by particles, and the thermodynamics of phase transitions in particulate material are considered. Special attention is devoted to the correct estimation of the possible heat losses. The way in which the phase diagrams, where the different phase conditions of particle material are presented in laser fluence−particle diameter coordinates, were produced is demonstrated. It is shown how this model can be applied for understanding the mechanism of such complicated processes as particle‐size reduction and submicrometer spherical particle growth, as well as other processes that occur when colloidal particles are irradiated by a pulsed laser.     

Features and Limiting Characteristics of the Heating of a Substance by a Laser-Accelerated Fast Electron Beam

The features of plasma formation in a substance heated by a laser-accelerated fast electron beam have been studied. These features are related to the ratio of the heating rate to the rate of energy loss because of radiation processes and electronic thermal conductivity, which are governed by the dependence of the energy of the heating beam particles on the beam intensity, which is characteristic of laser-driven electron acceleration. It has been shown that energy losses increase with the beam intensity and significantly limit the maximum temperature of the formed plasma. The possibility of generating an intense γ-radiation pulse of a nonnuclear origin because of the bremsstrahlung of laser-accelerated electrons has been discussed.

     

基于分子运动对流换热和热辐射下煤粉颗粒群粒子的加热分析

本文建立了在烟气对流加热和辐射状态下的煤粉颗粒群加热模型,通过数值模拟,模拟研究了不同锅炉炉膛尺寸下不同煤粉粒子粒径的煤粉群粒子加热时间以及粒子温升的关系,对对流换热和辐射换热在着火热源中所占比重进行了分析,模型很好的模拟了粒子的升温,能够较好的反映出煤粉粒子加热升温机理,为煤粉射流微元加热及着火提供了计算方法。     

Effects of particle size and laser wavelength on heating of silver nanoparticles under laser irradiation in liquid

Laser energy absorption results in significant heating of metallic nanoparticles and controlling the heating of nanoparticles is one of the essential stages of selective cell targeting. It is necessary to note that the laser action should be done by laser pulses with a wavelength that is strongly absorbed by the particles and it is important to select wavelengths that are not absorbed by the medium. Laser pulse duration must be chosen sufficiently short to minimize heat flow emitted from absorbing particles. Numerical calculations based on Mie theory were used to obtain the effect of laser wavelength and particle size on absorption factor for colloidal silver nanoparticles with radii between 5 and 50 nm. Calculations for acquiring temperatures under irradiations of pulsed KrF laser and pulsed Nd:YAG laser were performed. We showed that for low wavelengths of the laser, smaller nanoparticles have larger absorption efficiency compared to larger nanoparticles and in high wavelengths, temperature of all particles increased in the same way.     

Laser melting of carbide tool surface: Model and experimental studies

Laser controlled melting is one of the methods to achieve structural integrity in the surface region of the carbide tools. In the present study, laser heating of carbide cutting tool and temperature distribution in the irradiated region are examined. The phase change process during the heating is modeled using the enthalpy–porosity method. The influence of laser pulse intensity distribution across the irradiated surface (β) on temperature distribution and melt formation is investigated. An experiment is carried out and the microstructural changes due to laser consecutive pulse heating is examined using the scanning electron microscope (SEM). It is found that melt depth predicted agrees with the experimental results. The maximum depth of the melt layer moves away from the symmetry axis with increasing β.     

Simulation of elastic displacement of surface during laser short pulse heating of gold

The laser short pulse heating initiates nonequilibrium heating of the substrate material, which in turn results in the thermal stresses developing in the region below the surface. The surface temperature can be measured possibly through the monitoring of the resulting surface displacement. This requires in detail investigation into the surface displacement and surface temperature rises across the heated spot during the laser short pulse heating process. In the present study, the laser short pulse heating of gold surface is considered and the temperature rise at the surface and elastic displacement of the surface are investigated. The spatial and temporal distributions of surface displacement and surface temperature are predicted and the elastic response of the substrate material due to temperature rise is explored. It is found that the temporal and spatial distributions of the surface displacement do not follow the temperature rise at the surface. Consequently, care should be taken when measuring the temperature rise at the surface by means of monitoring the surface displacement during a laser short pulse heating process.     

Effect of the wavelength dependence of the emissivity on inferred soot temperatures measured by spectrally resolved laser-induced incandescence

Flame-generated soot was heated using a pulsed laser, and temperatures of the irradiated soot were inferred by fitting the Planck function to spectrally resolved laser-induced incandescence with the temperature as an adjustable parameter. The effect of the wavelength dependence of the emissivity on the inferred temperatures of the irradiated soot was studied using selected expressions for the soot emissivity in the fit. Depending upon the choice of the functional form of the emissivity, the maximum temperature reached by the soot during the laser pulse was calculated to span a range of 341 K (3475–3816 K) at a 1064-nm laser fluence of 0.1 J/cm² and 456 K (4115–4571 K) at a 1064-nm laser fluence of 0.4 J/cm² with a 1σ standard deviation about the mean of ∼25 K. Comparison of the present results with temperature measurements from previous studies suggests that the emissivity may depend on flame conditions and that further investigation on the subject is needed. The use of two-color or spectrally resolved LII to infer the soot temperature during or after laser heating requires a careful characterization of the wavelength dependence of the emissivity. The spread in temperature leads to large uncertainties regarding the physico-chemical processes occurring at the surface of the soot during the laser heating.     

A multi-step reaction model for ignition of fully-dense Al-CuO nanocomposite powders

A multi-step reaction model is developed to describe heterogeneous processes occurring upon heating of an Al-CuO nanocomposite material prepared by arrested reactive milling. The reaction model couples a previously derived Cabrera-Mott oxidation mechanism describing initial, low temperature processes and an aluminium oxidation model including formation of different alumina polymorphs at increased film thicknesses and higher temperatures. The reaction model is tuned using traces measured by differential scanning calorimetry. Ignition is studied for thin powder layers and individual particles using respectively the heated filament (heating rates of 10³–10⁴ K s^?1) and laser ignition (heating rate ～10⁶ K s^?1) experiments. The developed heterogeneous reaction model predicts a sharp temperature increase, which can be associated with ignition when the laser power approaches the experimental ignition threshold. In experiments, particles ignited by the laser beam are observed to explode, indicating a substantial gas release accompanying ignition. For the heated filament experiments, the model predicts exothermic reactions at the temperatures, at which ignition is observed experimentally; however, strong thermal contact between the metal filament and powder prevents the model from predicting the thermal runaway. It is suggested that oxygen gas release from decomposing CuO, as observed from particles exploding upon ignition in the laser beam, disrupts the thermal contact of the powder and filament; this phenomenon must be included in the filament ignition model to enable prediction of the temperature runaway.     

杂质诱导熔石英激光的损伤机理

发展了355 nm纳秒激光下亚波长杂质粒子引起熔石英损伤的基本模型。通过Mie散射理论和热传导方程,计算了粒子与熔石英边界处的温度随粒子尺寸的变化关系,并分析了达到临界温度时,不同粒子诱导损伤所需的关键能量密度,讨论了各粒子最易引起熔石英损伤的尺寸。实验采用355 nm纳秒激光脉冲作用熔石英及其HF刻蚀样品,测得两者的损伤概率。研究表明:粒子吸收激光能量,随着粒子半径的增加,其边缘温度先增大后减小,一定尺寸范围内的粒子才会引起熔石英的损伤;关键能量密度所对应的粒子半径为最易引起熔石英损伤的关键粒子半径;经刻蚀后,熔石英样品表面杂质数密度降低,损伤概率降低,损伤阈值提高。     

Experimental study of laser-induced processes on the surfaces of carbonaceous materials with simultaneous measuring of their temperatures

Results are presented from experiments on monitoring laser-induced processes (heating, melting, and ablation) on surfaces of carbonaceous materials (glassy carbon, pyrocarbon) using a laser display and according to the brightness temperature determined during these processes with a high-temperature pyrometer. The melting brightness temperature of glassy carbon (2720 ± 15 K) is determined using a continuouswave fiber laser. Some wave structures are revealed. No melting of pyrocarbon was observed over the range of powers and temperatures. The surfaces ablated after heating.     

Processes underlying the laser photochromic effect in colloidal plasmonic nanoparticle aggregates

We have studied the dynamic and static processes occurring in disordered multiparticle colloidal Ag aggregates with natural structure and affecting their plasmonic absorption spectra under pico-and nanosecond pulsed laser radiations, as well as the physical origin responsible for these processes. We have shown that depending on the duration of the laser pulse,the mechanisms of laser modification of such aggregates can be associated both with changes in the resonant properties of the particles due to their heating and melting(picosecond irradiation mode) and with the particle shifts in the resonant domains of the aggregates(nanosecond pulses) which depend on the wavelength, intensity, and polarization of the radiation.These mechanisms result in formation of a narrow dip in the plasmonic absorption spectrum of the aggregates near the laser radiation wavelength and affect the shape and position of the dip. The effect of polydispersity of nanoparticle aggregates on laser photochromic reaction has been studied.     

Thermal processes of a powder particle in coaxial laser cladding

This paper presents a numerical analysis of the heating, melting and evaporation processes of a single spherical powder particle when irradiated by a CO₂ laser beam in coaxial laser cladding. The power particle has a size ranging from 20 to 200 μm and the intensity of the laser has been varied from 500 to 3000 W. The laser energy, initial powder velocity and size have been shown to have important effects on the temperature profile of the powder stream. It has also been shown that high powder evaporation due to high power laser radiation may induce significant loss in the powder particle mass, to as much as 25% of the initial size at certain conditions in the simulation.     

强激光加热旋转薄柱壳的参量选择分析

为了把激光加热静止圆柱壳的实验测量结果应用到旋转圆柱壳的激光参量估计中,研究了旋转圆柱壳的激光加热效率。用积分变换法得到了旋转圆柱壳的温度分布,分析了最大温升点相对激光峰值强度点的滞后现象。基于静止圆柱壳和薄壳假设,导出了旋转圆柱壳激光加热效率及估计辐照时间的表达式。对于旋转金属圆柱壳,最大温升点相对激光峰值强度点的滞后角和激光加热效率取决于无量纲参量DR(柱壳半径R与束斑半径r0之比)、DL(横向热扩散尺度4ατL与束斑半径r0之比)及DM(加热时间τL与柱壳旋转频率fR的乘积)。达到相同的最大温升时,旋转圆柱壳的激光辐照时间和静止圆柱壳的激光辐照时间之间存在与激光功率无关的非线性关系,而激光功率决定了所需的绝对激光辐照时间。     

Comparison of LII derived soot temperature measurements with LII model predictions for soot in a laminar diffusion flame

Laser-induced incandescence (LII) was used to derive temperatures of pulsed laser heated soot particles from their thermal emission intensities detected at two wavelengths in a laminar ethylene/air co-annular diffusion flame. The results are compared to those of a numerical nanoscale heat and mass transfer model. Both aggregate and primary particle soot size distributions were measured using transmission electron microscopy (TEM). The model predictions were numerically averaged over these experimentally derived size distributions. The excitation laser wavelength was 532 nm, and the LII signal was detected at 445 nm and 780 nm. A wide range of laser fluence from very low to moderate (0.13 to 1.56 mJ/mm²) was used in the experiments. A large part of the temporal decay curve, beginning 12–15 nsec after the peak of the laser excitation pulse, is successfully described by the model, resulting in the determination of accommodation coefficients, which varies somewhat with soot temperature and is in the range of 0.36 to 0.46. However, in the soot evaporative regime, the model greatly overpredicts the cooling rate shortly after the laser pulse. At lower fluences, where evaporation is negligible, the initial experimental cooling rates, immediately following the laser pulse, are anomalously high. Potential physical processes that could account for these effects are discussed. From the present data the soot absorption function, E(m), of 0.4 at 532 nm is obtained. A procedure for correcting the measured signals for the flame radiation is presented. It is further shown that accounting for the local gas temperature increase due to heat transfer from soot particles to the gas significantly improves the agreement in the temperature dependence of soot cooling rates between model and experiments over a large range of laser fluences.