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.     

Characterization of a broadband pulse for phase controlled multiphoton microscopy by single beam SPIDER

We present what we believe to be a new version of spectral phase interferometry for direct electric field reconstruction (SPIDER) using only a single-phase and polarization controlled laser beam. Two narrow pulses and one broadband pulse are selected out of an ultrafast laser pulse by a polarization and phase control technique to generate second harmonic generation (SHG) signals, which are equivalent to a spectral shear interferogram in the conventional SPIDER method. The spectral phase of the broadband laser pulse is extracted analytically with double quadrature spectral interferometry (DQSI). An arbitrary spectral phase can be retrieved with great precision and compensated in situ at the sample position of a microscope. This new method requires no separate reference beam and is suitable for nonlinear optical microscopy with a phase controlled laser pulse.     

Ultrafast laser spectroscopy of semiconductor nanocrystals

A large amount of work has been worldwide directed to understand the properties of semiconductor nanostructures. Ultrafast lasers with pulsewidths of a few femtoseconds allowed the investigation of the dynamics of elementary excitations in semiconductor structures on ultrashort time scales. Recent progress in technology made it possible to fabricate semiconductor nanocrystals (i.e. crystals of nanometer dimensions) of well-defined properties. The purpose of this paper is to review the understanding of carrier relaxation and recombination processes in semiconductor nanocrystals as studied by ultrafast laser spectroscopy. The up-to-date techniques of ultrafast laser spectroscopy as well as the fabrication of semiconductor nanocrystals are discussed in some detail.     

锁模光纤激光器时变动力学

锁模激光器除了可以产生稳定的超短脉冲以外,还可产生一系列重要的非平衡态动力学过程。这些快速变化的动力学过程有助于理解超快激光器和相关非线性系统的动力学,也对超快激光器的稳定性设计有重要指导意义。随着超快探测技术的发展,锁模激光器超快动力学的研究取得了一系列突破。介绍了锁模激光器几个典型的非平衡态动力学过程,包括锁模启动过程,孤子分子动力学,呼吸子超快激光,以及孤子、呼吸子爆炸动力学。这些研究不仅揭示了超快激光器中新的物理机制,也将进一步促进超快激光器、孤子及呼吸子相关理论的发展。     

Imaging Ultrafast Plasmon Dynamics within a Complex Dolmen Nanostructure Using Photoemission Electron Microscopy

We report direct nanoscale imaging of ultrafast plasmon in a gold dolmen nanostructure excited with the 7fs laser pulses by combining the interferometric time-resolved technology with the three-photon photoemission electron microscopy(PEEM).The interferometric time-resolved traces show that the plasmon mode beating pattern appears at the ends of the dimer slabs in the dolmen nanostructure as a result of coherent superposition of multiple localized surface plasmon modes induced by broad bandwidth of the ultrafast laser pulses.The PEEM measurement further discloses that in-phase of the oscillation field of two neighbor defects are surprisingly observed,which is attributed to the plasmon coupling between them.Furthermore,the control of the temporal delay between the pump and probe laser pluses could be utilized for manipulation of the near-field distribution.These findings deepen our understanding of ultrafast plasmon dynamics in a complex nanosystem.     

Polarization-dependent ultrafast carrier dynamics in GaAs with anisotropic response

The transient dynamics of anisotropic properties of GaAs was systematically studied by polarization-dependent ultrafast time-resolved transient absorption. Our findings revealed that the anisotropy of reflectivity was enhanced in both pump-induced and probe-induced processes, suggesting an extraordinary resonance absorption of photon-phonon coupling (PPC) with intrinsic anisotropic characteristic in carrier relaxation, regardless of the concrete crystallinity and orientation of GaAs sample. The results, delivering in-depth cognition about the polarization-dependent ultrafast carrier dynamics, also proved the paramount importance of interaction between polarized laser and semiconductor.     

Femtosecond time-resolved optical polarigraphy: imaging of the propagation dynamics of intense light in a medium

A time-resolved imaging technique for visualizing ultrafast propagation dynamics of intense light pulses in a medium has been demonstrated. The method probes the instantaneous birefringence induced by a pulse in the medium. Through consecutive femtosecond snapshot images of intense femtosecond laser pulses propagating in air, ultrafast temporal changes in the two-dimensional spatial distribution of the optical pulse intensity were clearly seen.     

飞秒脉冲测量技术

随着飞秒激光技术的发展，飞秒激光脉冲的准确测量已成为非常重要的研究内容。文章在简要概述几种常见测量方法的基础上，着重综述了近年来发展起来的光学频率光栅开关法（FROG）及自参考光谱位相相干电场重建法（SPIDER），并介绍了文章作者进行的相关工作。     

Ablation and ultrafast dynamics of zinc selenide under femtosecond laser irradiation

The ablation in zinc selenide (ZnSe) crystal is studied by using 150-fs, 800-nm laser system. The images of the ablation pit measured by scanning electronic microscope (SEM) show no thermal stress and melting dynamics. The threshold fluence is measured to be 0.7 J/cm2. The ultrafast ablation dynamics is studied by using pump and probe method. The result suggests that optical breakdown and ultrafast melting take place in ZnSe irradiated under femtosecond laser pulses.     

饱和功率密度下线性啁啾对交叉偏振波输出特性的影响

交叉偏振波(XPW)技术是一种基于具有各向异性特征的三阶非线性晶体的非线性滤波技术,由于结构简单,稳定可靠,是超强超快激光领域提高时域对比度、压缩脉宽的有效手段之一.在实验中发现,XPW的输出特性受驱动脉冲特性的直接影响,通过理论计算得到了XPW的脉宽和光谱宽度与驱动脉冲的啁啾特性关系,同时利用声光可编程色散滤波器设计实验对理论计算进行了验证.结果表明:实验结果很好地反映了理论计算得出的结论,同时在饱和功率密度条件下,还表现出了一些理论计算没有反映出的新现象,即XPW的光谱展宽突破了驱动脉冲宽度√3倍的限制,最终脉宽也能够压缩至小于入射脉宽的1/√3;此外对于相反线性啁啾的驱动脉冲所产生的XPW信号,其在光谱形状上有明显的偏移差异,同时输出效率也有所不同.最后对这些新现象进行了进一步的分析和理论解释.     

超短脉冲光纤激光器新进展及其应用

超短脉冲光纤激光器是目前激光技术研究领域中最具有活力的研究课题．有着巨大的应用前景。本文介绍超短脉冲光纤激光器的发展概况及最新进展，论述掺稀土超短脉冲光纤激光器原理，对其关键技术及多种新型技术方案做了介绍和比较，分析超短脉冲激光器的应用前景及发展趋势。     

Femtosecond infrared spectroscopy of semiconductors and semiconductor nanostructures

Infrared spectroscopy on ultrafast time scales represents a powerful technique to investigate the nonequilibrium dynamics of elementary excitations in bulk and nanostructured semiconductors. In this article, recent progress in this field is reviewed. After a brief introduction into electronic excitations below the fundamental bandgap and ultrafast processes in semiconductors, infrared pulse generation and the methodology of time-resolved infrared spectroscopy are reviewed. The main part of this paper is devoted to coherent optical polarizations and nonequilibrium excitations of the electronic system in the spectral range below the fundamental band gap. The focus is on the physics of single component plasmas, i.e. electrons or holes. In particular, intraband, inter-valence and intersubband transitions are considered. Processes of phase relaxation, carrier and energy redistribution are analyzed. The potential of ultrafast infrared technology and spectroscopy for future applications is discussed in the final part.     

Ultrafast spin dynamics including spin-orbit interaction in semiconductors

This Letter presents a theoretical investigation of ultrafast spin-dependent carrier dynamics in semiconductors due to strong spin-orbit coupling using holes in bulk GaAs as a model system. By computing the microscopic carrier dynamics in the anisotropic hole-band structure including spin-orbit coupling, we obtain spin-relaxation times in quantitative agreement with measured hole-spin relaxation times [Phys. Rev. Lett. 89, 146601 (2002)10.1103/PhysRevLett.89.146601]. We show that different optical techniques for the measurement of hole-spin dynamics yield different results, in contrast to the case of electron-spin dynamics.     

Modification of carrier dynamics in CdSe nanocrystals by excess Cd in deposition bath

Photoexcited carrier dynamics in thin CdSe nanocrystalline films prepared by chemical bath deposition are strongly dependent on the deposition parameters. In this paper, we show how an increase in concentration of CdSO₄ in deposition bath affects the photoexcited carrier dynamics in nanocrystals. We used ultrafast absorption and photoluminescence laser spectroscopy to compare the carrier dynamics in samples prepared with and without increased CdSO₄ concentration. We have found that in the Cd-rich samples the spectral dependences of both photoluminescence and absorption dynamics are considerably less pronounced and the dynamics are slower. The observed effects were explained by the suppression of surface mediated carrier relaxation due to the passivation of individual nanocrystals by cadmium hydroxide and/or by sulphatocomplexes of Cd²⁺.     

Ultrafast, jitter-free x-ray streak camera that uses single-photon counting

A novel method developed to increase the temporal resolution of x-ray streak cameras is described. The method is analogous to the time-correlated single-photon-counting technique, which is commonly used in atomic physics. By use of short-pulse x-ray radiation from a laser-produced plasma, generated by an ultrafast laser, it is shown that a standard x-ray streak camera with a nominal temporal resolution of >5ps can yield a temporal response of 1.6 ps. The readout technique also removes temporal jitter with respect to the triggering laser. Capabilities and limitations of the technology are discussed.     

Transient surface photoconductivity of GaAs emitter studied by terahertz pump-emission spectroscopy

This paper investigates the ultrafast carrier dynamics and surface photoconductivity of unbiased semi-insulating GaAs in detail by using a terahertz pump-emission technique. Based on theoretical modelling, it finds that transient photoconductivity plays a very important role in the temporal waveform of terahertz radiation pulse. Anomalous enhancement in both terahertz radiation and transient photoconductivity is observed after the excitation of pump pulse and we attribute these phenomena to carrier capture in the EL2 centers. Moreover, the pump power- and temperature-dependent measurements are also performed to verify this trapping model.     

飞秒时间分辨的能谱分析光电子显微镜：异质结超快载流子动力学测量

本文成功搭建了一套集成了能谱分析功能的时间分辨光电子显微镜系统(TR-PEEM),能够对电子密度分布进行时间分辨和能量分辨的成像.这套4D显微镜在空间、时间、能量多维度获取电子动力学信息提供了前所未有的手段.本文使用184 fs的时间分辨、150 meV的能量分辨和优于150 nm的空间分辨对半导体进行了测量,在Si(111)表面的Pb岛上获得了微区光电子能谱和能量分辨的TR-PEEM图像.实验结果表明,这套系统是进行异质结载流子动力学观察的有力工具,有助于在亚微米/纳米空间尺度和超快时间尺度上加深对半导体性质的理解.     

低温生长砷化镓的超快光抽运-太赫兹探测光谱

本文采用光抽运-太赫兹探测技术系统研究了低温生长砷化镓(LT-GaAs)中光生载流子的超快动力学过程.光激发LT-GaAs薄层电导率峰值随抽运光强增加而增加,最后达到饱和,其饱和功率为54μJ/cm~2.当载流子浓度增大时,电子间的库仑相互作用将部分屏蔽缺陷对电子的俘获概率,从而导致LT-GaAs的快速载流子俘获时间随抽运光强增加而变长.光激发薄层电导率的色散关系可以用Cole-Cole Drude模型很好地拟合,结果表明LT-GaAs内部载流子的散射时间随抽运光强增加和延迟时间(产生光和抽运光)变长而增加,主要来源于电子-电子散射以及电子-杂质缺陷散射共同贡献,其中电子-杂质缺陷散射的强度与光激发薄层载流子浓度密切相关,并可由散射时间分布函数α来描述.通过对光激发载流子动力学、光激发薄层电导率以及迁移率变化的研究,我们提出适当增加缺陷浓度,可以进一步降低载流子迁移率和寿命,为研制和设计优良的THz发射器提供了实验依据.     

Single-beam homodyne SPIDER for multiphoton microscopy

We report a new version of spectral phase interferometry for direct electric field reconstruction (SPIDER) requiring only a single phase-shaped laser beam. A narrowband probe pulse is selected out of a broadband ultrafast laser pulse by a phase pulse-shaping technique and mixed with the original broadband pulse to generate a second-harmonic generation (SHG) signal. Using another SHG signal solely generated by the broadband pulse as a local oscillator, the spectral phase of the broadband laser pulse can be analytically retrieved by a combination of double-quadrature spectral interferometry and homodyne optical technique for SPIDER (HOT SPIDER). An arbitrary spectral phase at the sample position of a microscope can be compensated with a precision of 0.05 rad over the FWHM of the laser spectrum. It is readily applicable to a nonlinear microscopy technique with a phase-controlled broadband laser pulse.     

利用一维原子链模型研究薄膜瞬态结构变化

对于晶格结构响应的仿真与实验有助于我们理解激光激发引起的动态过程.利用一维原子链模型研究了激光加热后由于温度分布不均匀性产生的热应力对晶格的影响,该模型的计算结果与使用超快X射线衍射获得的实验结果相符合.该模型为研究光激发金属以及半导体等材料的超快晶格动力学提供了理论分析基础.