Ultrafast dynamics control on ablation of Cu using shaped femtosecond pulse trains

The ablation processes of Cu film are investigated using temporal shaped femtosecond pulse trains. The depth is modulated by changing the number and interval of the sub-pulses. The underlying ultrafast dynamic processes are discussed based on plasma shielding and electron multiple heating mechanisms. When the sub-pulse interval is less than 0.4 ps electron multiple heating is the dominant mechanism, while the plasma shielding dominates the subsequent ablation processes when the sub-pulse interval is larger than 0.4 ps. The curve of depth obtained by three pulse trains shows more significant oscillation as the function of sub-pulse interval under the low-fluence. We propose that the oscillation of depth is due to the coherent phonon oscillation excited by the pulse train. The study provides a basis for giving insight into the ultrafast dynamics for improving micromachining and nano-fabrications using shaped femtosecond pulse trains.     

Coherent structural dynamics and electronic correlations during an ultrafast insulator-to-metal phase transition in VO2

We directly trace the multi-THz conductivity of VO2 during an insulator-metal transition triggered by a 12-fs light pulse. The femtosecond dynamics of lattice and electronic degrees of freedom are spectrally discriminated. A coherent wave packet motion of V-V dimers at 6 THz modulates the lattice polarizability for approximately 1 ps. In contrast, the electronic conductivity settles to a constant value already after one V-V oscillation cycle. Based on our findings, we propose a qualitative model for the nonthermal phase transition.     

Ultrafast dynamics process of platinum nanoparticles under femtosecond laser

The energy relaxation dynamics process of Pt nanoparticles with a diameter of 25 nm after a 400-nm femtosecond laser excitation was investigated using pump-probe technology with 130 fs laser pulse. Experimental results show that the process includes a fast decay with time constant of 850 fs and a slow decay with time constant of 9 ps. Theoretical discussion indicates that the former results from electron-phonon coupling process, while the latter is from phonon-phonon coupling process.     

Fe/Si薄膜中相干声学声子的光激发研究

本文通过抽运-探测技术, 利用飞秒激光脉冲激发并探测了Fe/Si薄膜中的高频相干声学声子. 通过经典的阻尼谐振函数, 对声学声子的动力学行为进行了拟合. 实验及拟合结果表明, 该声学声子的共振频率约为0.25 THz, 其退相时间约为12 ps, 且都与激发光的波长和能量密度无关. 声学声子的振幅随着激发光能量密度的增加而线性地增强. 临界参数12_τe-ph/T约为0.6, 表明相干声学声子的驱动力主要来源于电子热应力的贡献. 最后, 结合薄膜的厚度和质量密度, 可以得到室温下垂直于该Fe/Si薄膜表面(out of plane) 的弹性常数C_⊥约为283 GPa.     

Ultra-Fast Decay Process of Electrons in LiNbO3 Crystal Induced by Femtosecond Pulse

Temporal evolution of absorption induced by single femtosecond pulse （13Ors, 800nm） with high intensity in LiNbO3 is obtained using the probe shadow imaging technique in order to investigate light-induced electron relaxation processes. By saturating the polaron density with a high intensity laser pulse, ultra-fast decay process on picosecond time scale is observed. The decay time constant is about 141 ps and it is attributed to the direct interband electron-hole recombination process.     

晶格振动的超快光谱调控

采用飞秒激光抽运脉冲激发了Bi_2Te_3薄膜频率为1.856 THz的声子相干振动,并用探测光测量得到了其阻尼振动信号.结合Raman光谱,确定该振动为A~1_(1g)对称振动模式的相干光学声子.为了实现该模式振动的调控,在抽运光路上安装了脉冲整形器,进而控制生成具有不同时间间隔和能量比的两束脉冲激光.研究表明,当两束脉冲的间隔时间为相干光学声子振动半周期的奇数倍时,调整两束脉冲的能量比值,可以实现A~1_(1g)模式振动的完全消除.继而将两束脉冲的能量比值保持不变,得到了振幅随间隔时间的变化曲线,与理论分析符合.结果进一步证实了用超快光谱调控特定晶格振动的可行性,从而为研究材料内部超快能量传递过程提供了有效手段.     

Femtosecond time-resolved laser-induced desorption of positive ions from MgO

We have used the pump-probe technique to measure the photostimulated positive ion yield as a function of time delay between two sub-threshold femtosecond laser pulses. We find that the ion yield from UV femtosecond irradiated MgO depends critically on the laser pulse delay, (t, in two-pulse experiments. In single-pulse experiments, excitation of MgO produces a variety of ions including Mg⁺, MgO⁺, and a significant yield of H⁺. In contrast, if the femtosecond laser pulse is split into two sub-threshold beams and then recombined with a variable time delay, the ion yield may be drastically altered depending on the delay between pulses. The Mg⁺ desorption yield displays three distinct lifetimes and persists for laser delays of over 100 ps. A pulse delay of only (t=500 fs nearly eliminates ion desorption except for Mg⁺. The use of a pair of delayed femtosecond laser pulses can thus control the species of the desorbed ion. The mechanism for femtosecond laser desorption is clearly different from nanosecond laser desorption. We hypothesize that the creation of electron-hole pairs by nonresonant two-photon excitation contributes to the ultrafast desorption mechanism.     

超短超强激光对比度的测量研究

 为了准确地确定飞秒激光对比度的信息，基于两束不同激光的互相关原理，利用非线性晶体对激光强度变化十分敏感的特性，研制了一台三阶相关仪，并用其对钛宝石激光放大系统输出的飞秒激光脉冲进行了测量，得到了有关该系统的强度对比度的信息。结果显示：该系统输出的激光对比度在10⁶左右，在脉冲的前沿和后沿有很强的ASE辐射，并且延续了很长的一段时间；种子脉冲的对比度在10⁵左右，而且在主脉冲前约2ps的位置上，有一个强度很低的小脉冲，在主脉冲的两翼各有一个非常小的台阶。     

Ultrafast magnetization reversal dynamics investigated by time domain imaging

Spatiotemporal magnetization reversal dynamics in a Ni(80)Fe(20) microstructure is studied using ps time scale scanning Kerr microscopy. Time domain images reveal a striking change in the reversal associated with the reduction in switching time when a transverse bias field is applied. Magnetization oscillations subsequent to reversal are observed at two resonance frequencies, which sensitively depend on the bias field strength. The oscillation at f = 2 GHz is caused by the damped precession of M, while the lower frequency approximately 0.8 GHz mode is interpreted in terms of domain wall oscillation.     

Oscillation of the refractive index at the focal region of a femtosecond laser pulse inside a glass

The temporal evolution of refractive-index change produced by a tightly focused femtosecond (fs) laser pulse inside a soda-lime glass plate was investigated by use of a transient lens method with subpicosecond time resolution. An oscillating behavior of the light intensity in the central region of the probe beam was observed 0-1500 ps after irradiation of the plate. The oscillation was interpreted in terms of a rapid temperature increase and the ensuing propagation of the pressure wave. This study is to our knowledge the first real-time observation of refractive-index change inside a glass induced by a fs laser pulse.     

Large transverse motion and micro-bunching of trapped electrons in a wakefield accelerator driven by temporally-asymmetric laser pulses

The transverse oscillatory motion of trapped electrons under the influence of the laser fields trailing the temporally-asymmetric driving laser pulse was investigated with a theoretical model of the quasi-steady state solution of trapped electron dynamics in the cavity. Our studies show that the transverse oscillation of electrons accelerated in the ion cavity can increase drastically due to the resonance with the laser field of the tail of the temporally-asymmetric pulse. The motion of the accelerated electrons can be represented by a forced harmonic oscillation and it was confirmed by 2D particle-in-cell simulations. These transverse oscillations of beams lead to micro-bunching as well, which can be used for generation of femtosecond coherent radiations of keV range photon energies.     

无展宽器的高重复率钛宝石啁啾飞秒脉冲再生放大器的研究

通过优化放大腔结构参数和采用高光束质量的泵浦激光,依靠放大器腔内各个元件的色散展宽种子脉冲, 用钛宝石作为增益介质, 在低泵浦能量下, 实现了高光束质量,高稳定的中等能量的高重复率飞秒脉冲再生放大. 将钛宝石晶体离焦放置,有效的避免了光学损伤. 在1.1 mJ的绿光泵浦下, 获得了2 ps, 120 μJ, 重复频率为1 KHz, 光谱带宽7.8 nm的放大脉冲, 用石英棱镜对压缩可得到130 fs的激光脉冲.     

Probing molecular dynamics at attosecond resolution with femtosecond laser pulses

The kinetic energy distribution of D+ ions resulting from the interaction of a femtosecond laser pulse with D2 molecules is calculated based on the rescattering model. From analyzing the molecular dynamics, it is shown that the recollision time between the ionized electron and the D+2 ion can be read from the D+ kinetic energy peaks to attosecond accuracy. We further suggest that a more precise reading of the clock can be achieved by using shorter fs laser pulses (about 15 fs).     

高等植物外周捕光天线LHCⅡ中的超快光动力学过程

利用飞秒抽运探测技术及时间分辨荧光(TRPL)等光谱技术对高等植物LHCⅡ中的超快光动力学过程进行了研究。在其时间分辨荧光光谱中表现出了明显的各向异性特性。实验上观察了LHCⅡ中色素间的能量传递过程,由飞秒动力学发现,单体内Chlb到邻近的Chla之间的能量传递在200～300fs的时间尺度,Chla激子带间的能量弛豫发生在几百飞秒,不同单体Chla分子间能量分布过程在几个皮秒。而时间分辨荧光和飞秒动力学过程中上百皮秒的慢过程归属于不同聚集体间的能量平衡过程或分子构象变化。     

Time-wavelength two-dimensional femtosecond fluorescence imaging

We report a new femtosecond time-resolved fluorescence spectrometer that enables us to observe fluorescence intensity as a time-wavelength two-dimensional image in a single measurement. This method utilizes a time-to-space conversion technique and fluorescence sum-frequency mixing with a femtosecond gate pulse. It provides a fluorescence image covering temporal and spectral spans of approximately 2 ps and approximately 60 nm, respectively. Calibration of the time and intensity axes of the image is made by use of a long-lived dye fluorescence. The two-dimensional fluorescence image of beta-carotene obtained demonstrates the high potential of this method for quantitative studies of ultrafast excited-state dynamics.     

Investigation of ultrafast processes in photoexcited bismuth by broadband probing in the wavelength range 0.4–0.9 μm

The decay of the photoexcited state of a bismuth single crystal is investigated in the wavelength range from 400 to 900 nm by means of femtosecond laser reflection spectroscopy. Oscillations produced by coherent fully symmetric A _1g phonons have been detected in the photoinduced response, along with a relaxation component. The dynamics of the electronic subsystem of the crystal is shown to be characterized by three values of the decay time: 1 ps, 7 ps, and ∼1 ns. The spectral dependence of the reflectivity oscillation amplitude has been measured; the possible cause of the shape of the derived curve is described.     

Femtosecond electron and spin dynamics in Ni/W(110) films

The collapse of the magnetic exchange splitting in 7 monolayer thick epitaxial Ni/W(110) films following a femtosecond laser pulse was measured using time-resolved photoemission spectroscopy. Ultrafast demagnetization during the laser induced hot electron cascade proceeds via spin-flip excitations with a relaxation time constant of 300+/-70 fs. At longer times the electronic system cools down and the magnetization is finally reestablished with a time constant of 3.2+/-0.2 ps.     

Real-time measurement of the orientational dynamics of aqueous solvation shells in bulk liquid water

We present a study of the orientational dynamics of aqueous solvation shells of halogenic anions in bulk water solution with femtosecond two-color midinfrared spectroscopy. These orientational dynamics have time constants between 2.5 and 12 ps, depending on the type of anion and the temperature. We find that the solvation shell of the larger ion I- shows faster dynamics than that of the smaller ions Cl- and Br-.     

光谱扫描滤波法提升飞秒激光信噪比的理论分析

在时间--频率域中,啁啾脉冲被淹没在放大自发辐射等噪声中,且其瞬时频率线性分布,基于此,提出采用光谱扫描滤波的办法来提升高功率飞秒激光系统的信噪比,并以法布里--珀罗干涉仪作为光谱扫描滤波器,对该法提升信噪比的效果进行了详细的理论分析.采用短时傅里叶变换方法,研究了光谱扫描滤波器对自发辐射放大(ASE)的滤波效果,数值分析表明,在时间抖动为-2 ps到2 ps之间、光谱扫描滤波器的通带宽度为0.4 nm条件下,该法能将飞秒激光系统的信噪比提升2个量级,而啁啾信号光以超过90%的透光率通过光谱扫描滤波器;级联光谱扫描滤波方式能进一步提升飞秒激光信噪比.     

变像管皮秒分幅和飞秒扫描相机的实验研究

本文将描述两种变像管皮秒分幅相机和一种飞秒扫描相机的设计特点、动态测试方法和实验结果。第一种变像管皮秒分幅相机采用了交叉点扫描多光栏分幅的方法,其变像管具有长加速电极和短阳极的静电弱聚焦系统与偏转灵敏度高、偏转像质好的偏转群体结构;其超快速控制电路只需一个光电开关斜坡电压脉冲发生器和一个特殊设计的脉冲成形网络即可送出具有合适时间关联的4对正负极性三角波和一对正负极性的单台阶液电压脉冲。实验表明,该相机在提供6幅分幅图像的情况下,每幅图像全曝光时间为80ps,除 3～4幅图像间的时间间隔为680ps外,其余均为160ps,动态空间分辨率达到5.51p/mm。第二种变像管皮秒分幅相机采用快门式分幅方法;其变像管采用行波偏转系统,内增强MCP做成带状线结构,并具有输入输出阻抗变换器,其三台阶波和快门脉冲序列均由光电开关电路和脉冲成形网络产生。该相机在提供三幅分幅图像的情况下,每幅图像全曝光时间为660ps,画幅之间的时间间隔均为4ns,动态空间分辨率为5.5lp/mm。飞秒扫描相机采用MCP内增强飞秒扫描变像管、具有负时间畸变的中继透镜和无触发晃动的光电开关扫描电路。实验证明,该相机在时间分辨率为500fs时,其动态范围为30;当时间分辨率为1.2ps时,其动态范围可达500;无扫描图像弯曲现象,触发晃动为±2ps.