Ultrafast carrier dynamics in GeSn thin film based on time-resolved terahertz spectroscopy

We measure the time-resolved terahertz spectroscopy of GeSn thin film and studied the ultrafast dynamics of its photo-generated carriers.The experimental results show that there are photo-generated carriers in GeSn under femtosecond laser excitation at 2500 nm,and its pump-induced photoconductivity can be explained by the Drude–Smith model.The carrier recombination process is mainly dominated by defect-assisted Auger processes and defect capture.The firstand second-order recombination rates are obtained by the rate equation fitting,which are(2.6±1.1)×10^(-2)ps^(-1)and(6.6±1.8)×10^(-19)cm^(3)·ps^(-1),respectively.Meanwhile,we also obtain the diffusion length of photo-generated carriers in GeSn,which is about 0.4μm,and it changes with the pump delay time.These results are important for the GeSn-based infrared optoelectronic devices,and demonstrate that Ge Sn materials can be applied to high-speed optoelectronic detectors and other applications.

Time-resolved shadowgraphs and morphology analyses of aluminum ablation with multiple femtosecond laser pulses

Aluminum ablation by multiple femtosecond laser pulses is investigated via time-resolved shadowgraphs and scanning electron microscope （SEM） images of the ablation spot. The spatial distribution of the ejected material and the radius of the shock wave generated during the ablation are found to vary with the increase in the number of pulses. In the initial two pulses, nearly concentric and semicircular stripes within the shock wave front are observed, unlike in subsequent pulses. Ablation by multiple femtosecond pulses exhibits different characteristics compared with the case induced by single femtosecond pulse because of the changes to the aluminum target surface induced by the preceding pulses.

Probing Ultrafast Dissociation Dynamics of Chloroiodomethane in the B Band by Time-Resolved Mass Spectrometry

Ultrafast dissociation dynamics of chloroiodomethane （CH2ICl） in the B band is studied by femtosecond time- resolved time-of-flight （TOF） mass spectrometry. Time-resolved TOF mass signal of parent ion （CH2ICl＋） and main daughter ion （CH2Cl＋） are obtained. The curve for the transient signal of CH2ICl＋ is simple and can be well fitted by an exponential decay convoluted with a Gaussian function. The decay constant determined to be less than 35 fs reflects the lifetime of the B band. Significant substituent effects on photodissociation dynamics of CH2IC1 compared with CH3I are discussed. The dissociation time from the parent ion CH2IC1＋ to the daughter ion CH2Cl＋ is determined in the experiment. The optimized geometry of the ionic state of CH2ICl and the ionization energy are calculated for further analysis of the measurements. In addition, compared with the parent ion, a new decay component with time constant of -596 fs is observed for CH2Cl＋, and reasonable mechanisms are proposed for the explanation.

A Highly Sensitive Femtosecond Time-Resolved Sum Frequency Generation Vibrational Spectroscopy System with Simultaneous Measurement of Multiple Polarization Combinations

Characterization of real-time and ultrafast motions of the complex molecules at surface and interface is critical to understand how interracial molecules function. It requires to develop surface-sensitive, fast-identification, and time-resolved techniques. In this study, we employ several key technical procedures and successfully develop a highly sensitive femtosecond time-resolved sum frequency generation vibrational spectroscopy （SFG-VS） system. This system is able to measure the spectra with two polarization combinations （ssp and ppp, or psp and ssp） simultaneously. It takes less than several seconds to collect one spectrum. To the best of our knowledge, it is the fastest speed of collecting SFG spectra reported by now. Using the time-resolved measurement, ultrafast vibrational dynamics of the N-H mode of α-helical peptide at water interface is determined. It is found that the membrane environment does not affect the N-H vibrational relaxation dynamics. It is expected that the time-resolved SFG system will play a vital role in the deep understanding of the dynamics and interaction of the complex molecules at surface and interface. Our method may also provide an important technical proposal for the people who plan to develop time-resolved SFG systems with simultaneous measurement of multiple polarization combinations.

Polarization Dependent Time-Resolved Infrared Spectroscopy and Its Applications

Polarization dependent time-resolved infrared （TRIR） spectroscopy has proven to be a useful technique to study the structural dynamics in a photochemical process. The angular information of transient species is obtainable in this measurement, which makes it a valuable technique for the investigation of electron distribution, molecular structure, and conformational dynamics. In this review, we briefly introduce the principles and applications of polarization dependent TRIR spectroscopy. We mainly focused on the following topics： （i） an overview of TRIR spectroscopy, （ii） principles of TRIR spectroscopy and its advantages compared to the other ultrafast techniques, （iii） examples that use polarization dependent TRIR spectroscopy to probe a variety of cheinical and dynamical phenomena including protein conformational dynamics, excited state electron localization, and photoisomerization, （iv） the limitations and prospects of TRIR spectroscopy.

纳秒激光诱导损伤熔石英玻璃的动力学过程

采用超快时间分辨阴影成像技术研究了纳秒激光诱导损伤熔石英玻璃前后表面和体内的动力学过程,对比分析了前后表面和体内的损伤差异及损伤机制。在前表面,观察了空气和材料中的等离子体和冲击波的产生与发展过程;亚纳秒激光辐照下,前表面材料内观察到三个应力波,并观察到材料体内的损伤过程。在后表面,除观察到冲击波的产生与发展过程,还观察到表面物质的烧蚀去除与喷发过程。在材料内部,损伤由自聚焦和点缺陷吸收两种机制主导,而且点缺陷吸收诱导材料体内损伤有时间先后顺序。

Development and Application of Ultrafast Circular Dichroism Spectroscopy Techniques

Chirality hold broad applications in life sciences,quantum devices,and various other areas.Traditionally,molecular chirality can be characterized by using steady-state circular dichroism spectroscopy.However,the techniques that can characterize excited state chirality are progressively capturing the public interest as it can provide the dynamic information for chirality generation and transfer.In this review,we focus on the theoretical background and the developmental history of femtosecond time-resolved circular dichroism spectroscopy(TRCD)techniques around the world.Additionally,we provide examples to showcase the utility of these techniques in the analysis of the dynamical molecular chemical structures,the investigation of molecular chirality generation,and the detection of electron spin dynamics in semiconductor quantum dots.

飞秒激光烧蚀典型金属表面产生冲击波膨胀研究

利用时间分辨阴影成像技术进行飞秒激光烧蚀金属表面研究可以直观获取飞秒激光烧蚀金属表面产生冲击波膨胀过程的图像。通过对比飞秒激光烧蚀金属铝、铜、铁靶表面的冲击波膨胀形式发现:金属铜、铁表面的冲击波均以球面波形式传播;由于受到烧蚀物质喷溅的影响,铝靶表面竖直方向的冲击波传播形式由球面波转化为柱面波。

A Surface Femtosecond Two-Photon Photoemission Spectrometer for Excited Electron Dynamics and Time-Dependent Photochemical Kinetics

A surface femtosecond two-photon photoemission （2PPE） spectrometer devoted to the study of ultrafast excited electron dynamics and photochemical kinetics on metal and metal oxide surfaces has been constructed. Low energy photoelectrons are measured using a hemispherical electron energy analyzer with an imaging detector that allows us to detect the energy and the angular distributions of the photoelectrons simultaneously. A Mach-Zehnder interferom- eter was built for the time-resolved 2PPE （TR-2PPE） measurement to study ultrafast surface excited electron dynamics, which was demonstrated on the Cu（111） surface. A scheme for measuring time-dependent 2PPE （TD-2PPE） spectra has also been developed for studies of surface photochemistry. This technique has been applied to a preliminary study on the photochemical kinetics on ethanol/TiO2（110）. We have also shown that the ultrafast dynamics of photoinduced surface excited resonances can be investigated in a reliable way by combining the TR-2PPE and TD-2PPE techniques.

Diffusion effect on the decay of time-resolved photoluminescence under low illumination in lead halide perovskites

Time-resolved photoluminescence(TRPL)has been extensively used to measure the carrier lifetime in lead halide perovskites.The TRPL curves of perovskite materials are usually fitted with a multi-exponential function,instead of a single exponential one.This was considered to be a result of the surface and the bulk recombination or the additional radiative recombination caused by the high excited carrier density.Here,a new model considering the diffusion and the trap-assisted recombination of carriers is proposed to explain the TRPL curves.The expressions of the TRPL curves and the transient absorption(TA)dynamic curves are theoretically derived,demonstrating that the TRPL curve is an infinite exponential series,regardless of the presence of surface recombination or not.Our newly developed highly sensitive nanosecond TA and TRPL were employed to measure the carrier dynamics of the same sample under low illumination in the linear response region of TA,thereby experimentally verifying our model.These results suggest that the decay of the TRPL is not only a consequence of the carrier recombination but also the carrier diffusion.TRPL cannot provide a direct measurement of the carrier lifetime,whereas TA spectroscopy can.Furthermore,the surface and the bulk recombination can be resolved and the average diffusion coefficient(D)can also be correctly obtained by combining TRPL and TA measurements.We also propose an approximate method for calculating the carrier lifetime and diffusion coefficient of high-quality perovskite films.Our model provides not only a new interpretation of the dynamics of the PL decay but also a deep insight into the carrier dynamics in the nanosecond time scale under working condition of perovskites solar cells.

Probing electron and lattice dynamics by ultrafast electron microscopy: Principles and applications

Microscale charge and energy transfer is an ultrafast process that can determine the photoelectrochemical performance of devices.However,nonlinear and nonequilibrium properties hinder our understanding of ultrafast processes;thus,the direct imaging strategy has become an effective means to uncover ultrafast charge and energy transfer processes.Due to diffraction limits of optical imaging,the obtained optical image has insufficient spatial resolution.Therefore,electron beam imaging combined with a pulse laser showing high spatial–temporal resolution has become a popular area of research,and numerous breakthroughs have been achieved in recent years.In this review,we cover three typical ultrafast electron beam imaging techniques,namely,time-resolved photoemission electron microscopy,scanning ultrafast electron microscopy,and ultrafast transmission electron microscopy,in addition to the principles and characteristics of these three techniques.Some outstanding results related to photon–electron interactions,charge carrier transport and relaxation,electron–lattice coupling,and lattice oscillation are also reviewed.In summary,ultrafast electron beam imaging with high spatial–temporal resolution and multidimensional imaging abilities can promote the fundamental under-standing of physics,chemistry,and optics,as well as guide the development of advanced semiconductors and electronics.

Probing the ultrafast dynamics in nanomaterial complex systems by femtosecond transient absorption spectroscopy

Over the past decade the integration of ultrafast spectroscopy with nanoscience has greatly propelled the development of nanoscience, as the key information gleaned from the mechanistic studies with the assistance of ultrafast spectroscopy enables a deeper understanding of the structure–function interplay and various interactions involved in the nanosystems.This mini-review presents an overview of the recent advances achieved in our ultrafast spectroscopy laboratory that address the ultrafast dynamics and related mechanisms in several representative nanomaterial complex systems by means of femtosecond time-resolved transient absorption spectroscopy. We attempt to convey instructive, consistent information regarding the important processes, pathways, dynamics, and interactions involved in the nanomaterial complex systems,most of which exhibit excellent performance in photocatalysis.

高强度飞秒激光脉冲烧蚀固体靶材的超快动力学过程的研究

本文报道了利用超快时间分辨阴影图方法对飞秒激光脉冲烧蚀金属铝的动态物理过程的研究。实验发现在50fs泵浦脉冲轰击靶表面后存在热与非热的烧蚀机制,证明在40J/cm2激光流量下超快激光烧蚀过程是一个涉及到多种不同物理和力学作用的复杂过程。在1—1.5ns延迟的阴影图中清晰地看到被烧蚀物质即将发生相位爆炸时产生的衍射条纹,在4ns和9ns延迟的阴影图中观察到喷射物内部存在由于极强热弹力波的出现而引起的间歇性物质喷射。在硅和玻璃的烧蚀实验中也观察到了类似的物理过程。但对于玻璃样品,没有观察到间歇性物质喷射现象。

多脉冲飞秒激光烧蚀铝靶动态特性研究

利用时间分辨阴影图研究了脉冲能量在200微焦的多脉冲飞秒激光烧蚀铝靶的动态过程、并使用扫描电镜研究了靶材表面烧蚀区域的形貌特征。时间分辨阴影图的记录结果表明,在不同时间延迟条件下,飞秒激光烧蚀铝靶形成的冲击波体积和喷射物的空间分布均随着脉冲个数的增加而发生不同程度的变化,尤其是单脉冲烧蚀情况下在1 ns延时阴影图中观察到的近同心圆条纹会随着脉冲数目增加逐渐变得模糊乃至消失。烧蚀区的电子扫描显微镜图像清楚地揭示出烧蚀过程中伴随有液态铝的产生,其溅射凝固后在靶材表面形成小球和细丝状微纳结构。实验结果进一步证实了由前序脉冲烧蚀导致的铝靶表面结构的改变会对后继脉冲的烧蚀产生显著影响,从而使多脉冲烧蚀表现出明显不同于单脉冲烧蚀的特性。这些结果对飞秒激光脉冲沉积薄膜、直写生成表面微结构等应用的工艺参数优化具有很好的指导意义。

Phyllotaxis-inspired nanosieves with multiplexed orbital angular momentum

Nanophotonic platforms such as metasurfaces,achieving arbitrary phase profiles within ultrathin thickness,emerge as miniaturized,ultracompact and kaleidoscopic optical vortex generators.However,it is often required to segment or interleave independent sub-array metasurfaces to multiplex optical vortices in a single nano-device,which in turn affects the device’s compactness and channel capacity.Here,inspired by phyllotaxis patterns in pine cones and sunflowers,we theoretically prove and experimentally report that multiple optical vortices can be produced in a single compact phyllotaxis nanosieve,both in free space and on a chip,where one meta-atom may contribute to many vortices simultaneously.The time-resolved dynamics of on-chip interference wavefronts between multiple plasmonic vortices was revealed by ultrafast time-resolved photoemission electron microscopy.Our nature-inspired optical vortex generator would facilitate various vortex-related optical applications,including structured wavefront shaping,free-space and plasmonic vortices,and high-capacity information metaphotonics.

Optical spectroscopy study of charge density wave orderOptical spectroscopy study of charge density wave order in Sr_3Rh_4Sn_(13) and (Sr_(0.5)Ca_(0.5))3_Rh_4Sn_(13)

The ultrafast laser-excited magnetization dynamics of ferromagnetic （FM） La0.67Sr0.33MnO3 （LSMO） thin films with BiFeO3 （BFO） coating layers grown by laser molecular beam epitaxy are investigated using the optical pump-probe technique. Uniform magnetization precessions are observed in the films under an applied external magnetic field by measuring the time-resolved magneto-optical Kerr effect. The magnetization precession frequencies of the LSMO thin films with the BFO coating layers are lower than those of uncoated LSMO films, which is attributed to the suppression of the anisotropy field induced by the exchange interaction at the interface between the antiferromagnetic order of BFO and the FM order of LSMO.