Combined continuum-atomistic modeling of ultrashort-pulsed laser irradiation of silicon

Ultrafast thermomechanical responses of silicon thin films due to ultrashort-pulsed laser irradiation were investigated using an atomic-level hybrid method coupling the molecular dynamics and the ultrafast two-step energy transport model. The dynamic reflectivity and absorption were considered, and the effects of laser fluence and pulse duration on the thermomechanical response were studied. It was found that both the carrier temperature and number density rapidly increase to their maximum while the lattice temperature rises at a much slower rate. The ultrafast laser heating could induce a strong stress wave in the film, with the maximum compressive and tensile stress occurring near the front and back surfaces, respectively. For laser pulses of the same duration, the higher the laser fluence is, the higher the carrier temperature and density and lattice temperature are induced. For the same laser fluence, a longer pulse generally produces lower carrier density and temperatures and weaker stress shock strength. However, for the fluence of 0.2 J/cm², the lowest lattice temperature was simulated for a 100-fs pulse compared to the 1-ps and 5-ps pulses, due to the increase of reflectivity by high carrier density. It is also shown that the optical properties as functions of lattice temperature usually employed are not suited for modeling ultrafast laser interactions with silicon materials.     

Simulation of thermionic emission optimization in femtosecond laser irradiation metal film by two-layer structure

The thermionic emission of the single-layer gold thin film and the two-layer film was assembled by gold padded with other metals (Ag, Cu, and Ni) and irradiated by the femtosecond laser pulse. Additionally, the emission was simulated by a two-temperature model combined with the Richardson–Dushman equation. It was found that the two-layer metal structure can change the electron temperature of the gold surface and control the thermionic emission compared with the single-layer gold film. With the same laser fluence, the two-layer film structure may shorten the duration of thermionic emission, and the duration of the thermionic emission can be further optimized by changing the proportion of thin film thickness with gold layer in the two-layer structure. The result can be especially beneficial in the context of ultrafast electron emission induced by femtosecond laser.     

数值模拟飞秒激光加热金属的热电子发射

研究了超短超强激光脉冲与薄膜靶相互作用中产生的电子热发射.当超短激光脉冲与薄膜靶相互作用时,首先入射超短脉冲激光对吸收深度内的自由电子进行热激发,接下来热激发电子将能量传递到附近的晶格,再通过电子和晶格二体系的热传导,以及电子晶格间的热耦合,将能量传递到材料的内部.因此,电子在皮秒级甚至更短的时间内不能与晶格进行能量耦合,使电子温度超出晶格温度很多,电子热发射就变得非常明显了.用双温方程联合Richardson-Dushman方程的方法对飞秒脉冲激光照射金属靶的电子热发射进行了研究,结果发现电子热发射对飞     

Formation of nanojets and nanodroplets by an ultrashort laser pulse at focusing in the diffraction limit

A new model has been developed and calculations have been performed for the formation of nanodroplets after action of an ultrashort laser pulse on a thin (10–100 nm) gold film deposited on a glass substrate. The action of a laser results in the melting of the film in the region of a laser spot and in its thermomechanical separation from the substrate. The separated film acquires a dome shape because of a decrease in the temperature in the direction from the center of the laser spot. This theoretical model provides the explanation of the formation of nanodroplets. It has been established that, first, the separation speed of a gold film from glass decreases sharply because the acoustic impedance of gold is much larger than that of glass. Second, nanodroplets are formed owing to the capillary focusing of the substance, which is manifested in the appearance of the drag component directed toward the axis of symmetry of the dome. The surface tension becomes dynamically significant because of the indicated sharp decrease in the separation speed from glass and of the smallness of the diameter of the focal spot (D ～ 1 μm), which is determined by the diffraction limit of optical radiation.     

Spin-flip processes and ultrafast magnetization dynamics in Co: Unifying the microscopic and macroscopic view of femtosecond magnetism

The femtosecond magnetization dynamics of a thin cobalt film excited with ultrashort laser pulses has been studied using two complementary pump-probe techniques, namely, spin-, energy-, and time-resolved photoemission and the time-resolved magneto-optical Kerr effect. Combining the two methods, it is possible to identify the microscopic electron spin-flip mechanisms responsible for the ultrafast macroscopic magnetization dynamics of the cobalt film. In particular, we show that electron-magnon excitation does not affect the overall magnetization even though it is an efficient spin-flip channel on the sub-200 fs time scale. Instead, we find experimental evidence for the relevance of Elliott-Yafet-type spin-flip processes for the ultrafast demagnetization taking place on a time scale of 300 fs.     

Nonlinear absorption of ultrashort laser pulses in thin metal films

Self-consistent simulations of the ultrafast electron dynamics in thin metal films were performed. A regime of nonlinear oscillations was observed that corresponds to ballistic electrons bouncing back and forth against the films' surfaces. When an oscillatory laser field is applied to the film, the field energy is partially absorbed by the electron gas. Maximum absorption occurs when the period of the external field matches the period of the nonlinear oscillations, which, for sodium films, lies in the infrared range. Possible experimental implementations are discussed.     

Formation of an electron beam with a duration shorter than 100 fs during photoemission of electrons by femtosecond laser pulses

Irradiation of a thin metal target by 38-fs laser pulses at a wavelength of 800 nm is shown to generate a beam of photoelectrons that contains a component whose duration is shorter than 100 fs. The ensemble of photoelectrons is formed by photoemission of a gold film about 10 nm thick sputtered on the base of a prism made of fused silica. The laser beam irradiates a dielectric-metal interface and propagates inside the prism at an angle of 45° to a normal to the interface. The photoelectron beam is formed by accelerating photoelectrons in a spatially inhomogeneous electrostatic potential. The ultrashort component of the photoelectron beam is found to be formed under the action of a ponderomotive potential. It is shown that the ultrashort electron component can be separated from the remaining part of the photoelectron beam with the help of an inhomogeneous electrostatic field.     

Theoretical description of ultrafast phenomena in clusters

A theoretical study of different ultrafast nonequilibrium processes taking place during and after ultrashort excitation of clusters is presented. We discuss similarities and differences for several processes involving nonequilibrium ultrafast motion of atoms and electrons. We study ultrashort relaxation of clusters in response to excitations produced by femtosecond laser pulses of different intensities. We show how different relaxation processes, such as bond breaking, melting, fragmentation, emission of atoms, or Coulomb explosion, can be induced, depending on the laser intensity and laser pulse duration. We also discuss processes involving nonequilibrium electron dynamics, such as intraband Auger decay in clusters and ultrafast electronic motion during collisions between clusters and surfaces. We show that this electron dynamics leads to Stückelberg-like oscillations of measurable quantities, such as the electron emission yield. Received: 4 April 2000 / Accepted: 6 November 2000 / Published online: 9 February 2001     

超短脉冲激光辐照硅膜的热弹性

 考虑到热电子崩力的影响,在基于玻耳兹曼理论弛豫时间近似的非线性自相关模型基础上,将晶格温度与应变速率相耦合,建立了超短脉冲激光作用下半导体材料的超快热弹性模型。在单轴应变条件下,利用有限差分法模拟了500 fs脉冲激光作用下2 μm厚硅膜内的载流子温度、晶格温度、载流子数密度、热应力和热电子崩力等的变化情况。结果表明：在低能量密度激光条件下,热弹性效应对半导体材料的影响很小;载流子温度达到峰值的时间比激光强度达到峰值的时间早,随后载流子数密度达到峰值,以及激光脉冲作用5 ps以后硅膜趋于总体热平衡;在脉冲辐照早期,非热平衡阶段形成的热电子崩力在超快损伤过程中起主要作用。     

Plasma dynamics and determination of ablation parameters using the near-target magnified imaging during pulsed laser ablation

A comparative study of the ultrafast dynamics on ZnO thin films deposited on flat Si substrates and on Si micro-cones following ultrashort laser excitation has been carried out using time-resolved optical spectroscopy. By monitoring the transient band gap renormalization induced by nonlinearly excited carriers it is found that fast electron scattering and trapping occurs more efficiently in the micro-cones as compared to the flat films. This enhanced trapping efficiency is attributed to the defects and imperfections that are introduced by the increased surface roughness due to the conical shape.     

Ultrafast optical power limiting in free-standing Pt–polyvinyl alcohol nanocomposite films synthesized in situ

Free-standing platinum–polyvinyl alcohol nanocomposite films have been prepared by a simple in situ method. By thermal annealing, Pt nanoparticles of different sizes and shapes have been obtained. Their optical nonlinearity is measured using ultrafast (100 fs) laser pulses at 404 nm, in the absorption wing region. A strong optical power limiting is found in the films. The timescale of this limiting action is ultrafast, as it happens within the incident laser pulsewidth. Experimental results and numerical simulation indicate that the sign of the nonlinearity can be controlled by varying the film composition and annealing temperature. Use of ultrashort laser pulses in the free-standing film configuration permits a direct and unambiguous determination of the electronic nonlinearity of the material, since accumulative effects occur at later times lying outside the sharp measurement window.     

Energy transport in silicon–aluminum composite thin film during laser short-pulse irradiation

Energy transport in silicon–aluminum composite thin films due to short-pulse laser irradiation is examined. Frequency dependent phonon transport in the silicon film is considered to formulate equivalent equilibrium temperature while modified two-equation model is used in the aluminum film to obtain electron and phonon temperatures. Thermal boundary resistance across the films is incorporated in the analysis. Transmittance, reflectance, and absorption of the incident laser beam are determined using the transfer matrix method. Equivalent equilibrium temperatures resulted from frequency dependent and frequency independent solutions are compared. It is found that phonon temperature increase at the aluminum interface is suppressed by phonon transport to the silicon film, which is more pronounced at low laser pulse intensities. The influence of the ballistic phonons on equivalent equilibrium temperature in the silicon film is found to be significant.     

Cu—Ba—O薄膜在超短激光脉冲作用下的光透射率特性

用泵浦－探测技术测量了金属－介质复合薄膜Ｃｕ－Ｂａ－Ｏ的光学透射率在超短激光脉冲作用下随延迟时间的瞬态变化曲线，获得了薄膜对光的透射率迅速减小并在皮秒时间内恢复原状的实验结果。该现象是由薄膜中金属超微粒子内费米能级附近电子被飞秒激光脉冲激发所产生的非平衡态电子经历瞬态弛豫造成的。本文从理论上给出了薄膜中Ｃｕ超微粒子的电子声子相互作用常数ｇ的修正数值。     

Nonequilibrium phase change in gold films induced by ultrafast laser heating

Ultrafast laser-induced melting in a gold thin film is simulated by an integrated continuum-atomistic method with the extended Drude model for dynamic optical properties. The local order parameter of atoms is used to identify solid and liquid regions. It is shown that the film is superheated in the early nonequilibrium stage and the melted region grows very quickly with a very high rate of melting up to ～13,300 m/s. It is also found that the continuum approach could significantly underestimate the ultrafast phase-change response, and temperature-dependent optical properties should be considered in atomic-level modeling for ultrafast laser heating.     

Melting of Al by ultrafast laser pulses: dynamics at the melting threshold

Using molecular-dynamics simulation, we investigate the melting of a thin Al slab by ultrafast laser irradiation. We employ a laser energy, which is just around the melting threshold. While the equilibrium electron–phonon coupling is well understood, we investigate the influence of the early (i.e., prior to electron thermalization) electron-lattice energy transfer. To this end, as a model study, we vary the fraction of the laser energy, which is directly given to lattice atoms vs. that given to the electronic system. We find that the melting process depends sensitively on the early electron-lattice heating rate. The pressure build-up within the still solid parts of the slab is identified as the main agent which delays the melting transition. The changes in the simulated structure factor data suggest that X-ray measurements of thin films performed just around the melting transition—even if performed long after electron thermalization—may provide information on the early electron-lattice energy coupling process.     

Insight into the thermionic emission regimes under gold film thermal relaxation excited by a femtosecond pulse

We theoretically investigated different thermal relaxation participating in the ultrafast thermionic emission processes on gold film surface with a femtosecond pulse excitation. The thermionic emission regimes under the two temperature relaxation and the thermal diffusion relaxation were demonstrated. The simulations showed that the thermionic emission properties can be defined in the regime under two temperature relaxation by reducing the laser fluence, or widening the pulse duration or increasing the laser wavelength. It was also found that there exists a transition between the two distinct thermionic emission regimes under peculiar laser parameters of laser fluence, pulse duration and laser wavelength. The results were explained as significant intervene of laser irradiation parameters into gold film thermal relaxation processes.     

Laser short pulse heating: Influence of pulse intensity on temperature and stress fields

Laser short-pulse heating of gold surface is considered and the influence of laser pulse intensity on the temperature and stress fields is investigated. Laser step input pulses with different pulse lengths and the same energy content are employed in the simulations. The electron kinetic theory approach employing thermomechanical coupling is introduced to model the non-equilibrium energy transport in the electron and lattice sub-systems. Thermal stress development in the lattice sub-system and temperature rise in the lattice and electron sub-systems are computed. It is found that electron temperature rises rapidly while lattice site temperature rise is gradual in the early heating period, which is more pronounced for high intensity pulses. Thermal stress component in the axial direction is compressive and its magnitude is considerably less than the yielding limit of the substrate material.     

物理参数变化对短脉冲激光激励温度场的影响

 为研究多物理参数（耦合系数、电子热导率、电子热容、晶格热容）同时随温度变化对短脉冲激光辐照金属材料产生温度场分布的影响,基于双温耦合理论,建立了短脉冲激光辐照金属材料金的加热过程的有限元求解模型。在同时考虑脉冲激光的空间、时间分布和多参数同时随温度变化的情况下,得到短脉冲激光辐照金属材料金激励产生的温度场二维瞬态分布,并进一步比较了多物理参数同时随温度变化和采用室温物理参数两种情况下温度场分布的区别。数值结果表明：多物理参数同时随温度变化使电子温度和晶格温度的上升变快,最大值变大,而且使得材料中激光穿透直接辐照到的区域温度变高。     

飞秒激光辐照下硅薄膜的非傅里叶能量输运研究

 在双曲双步输运模型基础上建立数值模型，针对超短脉冲激光作用下硅薄膜的微观能量输运过程展开理论研究。针对电子、晶格超快温升响应过程的数值模拟结果表明，电子作为主要能量载子在几皮秒内主导了能量输运过程。电声子之间的能量耦合系数主要依赖于电子温度，而不是晶格温度。能量耦合过程由于非平衡电子的弹道式输运而呈现非局域性。热波的传播速度与电子能量传播速度有相同量级，而大于硅材料中的声子平均速度。模型预测与相关实验结果吻合。     

光学性质对超快激光辐照下铜膜热响应的影响

在超快激光照射过程中,金属靶材的光学性质是动态变化的。采用双温模型与分子动力学结合法,考虑动态和常数光学性质两种情况,对不同脉宽的超快激光照射下铜薄膜的热响应进行了模拟研究。其中,常数光学性质包括由激光沉积能量相等计算得到的等效平均反射率和室温下的吸收系数。结果表明:两种情况下的电子温度和晶格温度均差别较小,尤其是脉宽远小于电子-晶格弛豫时间的飞秒激光; 而当激光脉宽相当于或大于电子-晶格弛豫时间时,如皮秒激光,光学性质的动态变化对材料的熔化和重凝的影响则比较明显。