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     

Theory for the ultrafast dynamics of excited clusters: interplay between elementary excitations and atomic structure

We present a theoretical study of the short-time relaxation of clusters in response to ultrafast excitations using femtosecond laser pulses. We analyze the excitation of different types of clusters (Hg_n, Ag_n, Si_n, C₆₀ and Xe_n) and classify the relaxation dynamics in three different regimes, depending on the intensity of the exciting laser pulse. For low-intensity pulses (I<10¹² W/cm²) we determine the time-dependent structural changes of clusters upon ultrashort ionization and photodetachment. We also study the laser-induced non-equilibrium fragmentation and melting of Si_n and C₆₀ clusters, which occurs for moderate laser intensities, as a function of the pulse duration and energy. As an example for the case of high intensities (I>10¹⁵ W/cm²), the explosion of clusters under the action of very intense ultrashort laser fields is described. Received: 26 November 1999 / Published online: 2 August 2000     

Molecular dynamics simulations of laser-induced damage of nanostructures and solids

A theoretical approach to treat laser induced femtosecond structural changes in covalently bonded nanostructures and solids is described. Our approach consists in molecular dynamic simulations performed on the basis of time-dependent, many-body potential energy surfaces derived from tight-binding Hamiltonians. The shape and spectral composition of the laser pulse is explicitly taking into account in a non-perturbative way. We show a few examples of the application of this approach to describe the laser damage and healing of defects in carbon nanotubes with different chiralities and the ultrafast nonequilibrium melting of bulk germanium, initiated by the laser-induced softening and destabilization of transversal acoustic phonon modes.     

飞秒激光热反射系统测量金属薄膜中的热波

金属材料中的热波现象可以利用包含电子弛豫时间影响的双曲两步模型进行理论分析.通过飞秒激光热反射实验系统对金属薄膜材料进行了测量.利用偏振分光棱镜将飞秒激光分成抽运光和探测光,其中较强的抽运光用于加热金属薄膜而较弱的探测光用于探测薄膜表面反射率随时间的变化,两束光之间的光程差通过步进电机进行精确控制.利用金属薄膜反射率和电子温度的正比例关系就可以得到电子温度随时间的变化规律.实验发现在加热激光脉冲过后的电子温度下降区间会出现另一个较弱的电子温度波峰,并利用相同厚度的两块金属薄膜样品重复测量对实验结果进行了验证.理论上这一现象可以解释为金属薄膜中热波在背面反射的结果,并且实验结果和双曲两步模型给出的热波理论计算结果相符合.根据实验结果计算出热波传递速度约为5×105m/s,对应的电子弛豫时间为60fs.     

Laser-induced nonthermal fragmentation of C60 studied by semiclassical dynamics simulation

Photofragmentation of the C₆₀ fullerene induced by ultrafast laser pulses is studied by semiclassical dynamics simulation. The simulation study is focused on the excitation below the continuum levels. A laser pulse of 40 fs (FWHM) with an effective photon energy of 2.0 eV and different intensities was selected to interact with the C₆₀ fullerene. The simulation results show that averaged fragmentation size distribution over groups of initial geometries selected at random exhibits a power law pattern with the peak at C₂ at high laser pulse intensities. The threshold for the C₆₀ fragmentation was determined. The simulation finds that as many as 55 electrons are excited from the occupied molecular orbitals to unoccupied molecular orbitals upon the laser irradiation and that the number of the fragments significantly depends on the number of electrons excited. Finally, the temperature examination seems to suggest that the nonthermal effect may play a significant role in laser fragmentation of the C₆₀ fullerene.     

Optical properties in nonequilibrium phase transitions

An open question about the dynamical behavior of materials is how phase transition occurs in highly nonequilibrium systems. One important class of study is the excitation of a solid by an ultrafast, intense laser. The preferential heating of electrons by the laser field gives rise to initial states dominated by hot electrons in a cold lattice. Using a femtosecond laser pump-probe approach, we have followed the temporal evolution of the optical properties of such a system. The results show interesting correlation to nonthermal melting and lattice disordering processes. They also reveal a liquid-plasma transition when the lattice energy density reaches a critical value.     

Observation of Sub-femtosecond Polarization Beats Using Twin Noisy Driving Fields

We study the phase-conjugate polarization interference in a V-type three-level system and obtain an analytic closed form for the second-order stochastic correlation of sum-frequency polarization beat. In our Na vapour atomic system pumped by laser pulse of nano-second timescale duration, we experimentally demonstrate an ultrafast modulation of the four-wave mixing signal intensity with a sub-femtosecond timescale period, corre- sponding to the sum-frequency of the resonant transitions from 3S1/2 to 3Pl/2 and 3P3/2.     

Laser-induced graphitization on a diamond (111) surface

We report an atomistic simulation study of laser-induced graphitization on the diamond (111) surface. Our simulation results show that the diamond to graphite transition occurs along different pathways depending on the length of the laser pulse being used. Under nanosecond or longer laser pulses, graphitization propagates vertically into bulk layers, leading to the formation of diamond-graphite interfaces after the laser treatment. By contrast, with femtosecond (0.2-0.5 ps) laser pulses, graphitization of the surface occurs layer by layer, resulting in a clean diamond surface after the ablation. This atomistic picture provides an explanation of recent experimental observations.     

Modeling of Nonthermal Solid‐to‐Solid Phase Transition in Diamond Irradiated with Femtosecond x‐ray FEL Pulse

In this contribution we review in detail our recently developed hybrid model able to trace simultaneously nonequilibrium electron kinetics, evolution of an electronic structure, and eventually nonthermal phase transition in solids irradiated with femtosecond free‐electron laser pulses. Diamond irradiated with an ultrashort intense x‐ray pulse serves as an example to show how an irradiated material undergoes an ultrafast phase transition on sub‐picosecond timescales. The transition of diamond into graphite is induced by an excitation of electrons from the valence band into the conduction band, which, in turn, induces a rapid change of the interatomic potential. Our theoretical model incorporates: a Monte‐Carlo method for tracing high‐energy electrons and K‐shell holes in diamond; a temperature equation for the valence‐band and low‐energy conduction‐band electrons; a tight binding method for calculation of the evolving electronic structure of the material and potential energy surfaces; and molecular dynamics propagating atomic trajectories. This unified approach predicts the damage threshold of diamond in a good agreement with experimentally measured values. It reveals a multi‐step nature of nonthermal phase transition being an interplay between electronic excitation, changes of the band structure, and atomic reordering. An effect of pulse parameters, such as photon energy and temporal pulse shape, on the phase transition is discussed in detail. (© 2015 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

基于瞬态光栅频率分辨光学开关法测量飞秒脉冲的研究

超宽光谱的飞秒脉冲测量一直是超快激光领域的重要研究方向之一.常规的飞秒脉冲自相关方法是通过测量自相关倍频信号来获得,而倍频信号具有波长选择性,不同中心波长的飞秒脉冲测量需要更换不同的倍频晶体,十分不方便.因此,提出了一种改进型的瞬态光栅频率分辨光学开关(TG-FROG)方法用于测量飞秒脉冲.该方法结合四波混频和频率分辨光学开关方法,其基本过程是将待测脉冲分为三束,其中两束脉冲经过精密的延时控制并聚焦在光学介质上达到时空重合,利用三阶非线性效应产生稳定的瞬态光栅作为开关光;另一束脉冲作为探测光与产生的瞬态光栅进行相互作用产生一个信号光,使用光谱仪对该信号光的光谱与延迟时间进行测量,并通过反演迭代算法处理而获取待测飞秒脉冲的光谱与电场信息.该方法只需要待测光的功率密度达到三阶非线性效应就可以实现测量,因此可以应用于任意中心波长的飞秒脉冲测量.利用该方法对中心波长分别为800 nm, 400 nm的飞秒脉冲,以及超连续亚10 fs的周期量级超宽光谱飞秒脉冲进行了测量,并与常规的干涉自相关仪器测量结果进行了比较,所得测量结果基本一致.实验结果表明,建立的基于TG-FROG方法对不同中心波长,不同脉冲宽度的飞秒脉冲测量是十分有效的.     

Features of femtosecond laser pulse reflection from a sharp boundary of relativistic laser plasma

The features of femtosecond laser pulse reflection from a plasma target of near-critical density were analytically and numerically studied in a wide range of laser pulse intensities and durations. Based on analytical calculations, it is shown that the pulse reflectance at a constant intensity decreases with decreasing pulse duration. Based of numerical simulation results, it is shown that, as a superintense femtosecond laser pulse is incident on a plasma layer with a concentration close to the critical one, a quasi-periodic electron-density structure is formed in the plasma bulk, which can both increase and decrease the the laser pulse reflectance.     

富勒烯有机-无机杂化材料的非共珍三阶非线性光学特性

采用中心波长800 nm、脉宽30 fs的超短激光脉冲,通过飞秒光开关技术（Optical Kerr Shutter,OKS）对富勒烯有机-无机杂化材料的飞秒超快非线性特性进行了实验研究.获得270 fs的开关时间,所得的富勒烯有机-无机杂化材料的三阶非线性系数χ(3)约为4.5×10－14 esu,比C60分子的三阶非线性系数χ(3)高一个数量级.通过实验测定的光克尔信号强度与激发光和探测光偏振方向夹角的依赖关系表明：30 fs的超短激光脉冲激发富勒烯有机-无机杂化材料的克尔信号主要是源于光诱导双折射效应,而非用200 fs的超短激光脉冲时来自瞬态栅的自衍射效应.     

First-principles electron dynamics control simulation of diamond under femtosecond laser pulse train irradiation

A real-time and real-space time-dependent density functional is applied to simulate the nonlinear electron-photon interactions during shaped femtosecond laser pulse train ablation of diamond. Effects of the key pulse train parameters such as the pulse separation, spatial/temporal pulse energy distribution and pulse number per train on the electron excitation and energy absorption are discussed. The calculations show that photon-electron interactions and transient localized electron dynamics can be controlled including photon absorption, electron excitation, electron density, and free electron distribution by the ultrafast laser pulse train.     

Influence of a nanosecond pulsed laser on aluminium alloys: Distribution of oxygen

Nanosecond laser pulses may produce both thermal melting (as femtosecond and picosecond pulses) or ultrafast nonthermal melting depending on the pulse fluence. This was demonstrated experimentally by Sokolowski-Tinten et al. [1], who found that the transformation of GaAs into its liquid state occurs within several tens of picoseconds at fluences close to the melt threshold due to thermal melting under highly superheated conditions or within several hundred femtoseconds via carrier excitation for very high fluences. The processes occurring under high energetic fs pulse irradiation could be described more precisely with the help of the theoretical work of Stampfli et al. In this work, a nanosecond pulsed laser (Nd:Yag) is used to irradiate an aluminum alloy sample. The oxygen distribution is studied as a function of distance in order to get an idea about the temperature distribution.     

Femtosecond dynamics of the collinear-to-spiral antiferromagnetic phase transition in CuO

We report on the ultrafast dynamics of magnetic order in a single crystal of CuO at a temperature of 207 K in response to strong optical excitation using femtosecond resonant x-ray diffraction. In the experiment, a femtosecond laser pulse induces a sudden, nonequilibrium increase in magnetic disorder. After a short delay ranging from 400 fs to 2 ps, we observe changes in the relative intensity of the magnetic ordering diffraction peaks that indicate a shift from a collinear commensurate phase to a spiral incommensurate phase. These results indicate that the ultimate speed for this antiferromagnetic reorientation transition in CuO is limited by the long-wavelength magnetic excitation connecting the two phases.     

Timescales in the response of materials to femtosecond laser excitation

The interaction of ultrashort laser pulses with materials involves a number of special features that are different from laser–matter interaction for longer pulse durations. For femtosecond laser excitation the fundamental physical processes such as energy deposition, melting, and ablation are separated in time. By choosing proper time windows, the various processes can be investigated separately. We present selected examples of theoretical studies of free electron excitation in metals, timescales of different melting processes, and peculiarities of near-threshold ablation. Depending on the timescales and intensity ranges, the discussed processes are combined in an overall picture of possible pathways of the material from excitation to ablation. PACS 61.80.-x; 64.70.-p     

Femtosecond mid-infrared spectroscopy of low-energy excitations in solids

Recent progress in the generation and spectroscopic application of femtosecond pulses in the wavelength range between 3 and 25 m has led to new insight into low-energy excitations of solids, in particular semiconductors, semiconductor nanostructures, and high-T_C superconductors. The ultrafast nonequilibrium dynamics of such excitations has been observed in real-time and the underlying microscopic interactions have been analyzed. This article gives a brief overview of this exciting field of ultrafast science with the main emphasis on pulse generation and applications in semiconductor research where femtosecond intersubband Rabi flopping in quantum wells and quantum coherent electron transport in quantum cascade devices have been observed. PACS 78.67.De; 73.21.Fg; 07.57.Hm; 42.65.Re     

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。     

富勒烯有机-无机杂化材料的非共珍三阶非线性光学特性

采用中心波长800 nm、脉宽30 fs的超短激光脉冲,通过飞秒光开关技术(Optical Kerr Shutter,OKS)对富勒烯有机-无机杂化材料的飞秒超快非线性特性进行了实验研究.获得270 fs的开关时间,所得的富勒烯有机-无机杂化材料的三阶非线性系数X~(3)约为4.5×10~(-4) esu,比C_(60)分子的三阶非线性系数X~(3)高一个数量级.通过实验测定的光克尔信号强度与激发光和探测光偏振方向夹角的依赖关系表明:30 fs的超短激光脉冲激发富勒烯有机-无机杂化材料的克尔信号主要是源于光诱导双折射效应,而非用200 fs的超短激光脉冲时来自瞬态栅的自衍射效应.     

New approach of semiconductor laser related technologies for ultrafast photonics

Ultrashort laser pulses offer new jump in information and communication technology. Especially semiconductor laser based ultrafast photonic devices and systems are promising. We review our new approaches for femtosecond pulse generation, and thin film technology for broad band semiconductor optical amplifiers.