Analysis of femtosecond laser ionization/dissociation of polyatomic molecule C_6H_(10)O from one-colour pump-probe measurement

This paper reports that a one-colour fs pump probe measurement has been carried out for studying photoionization/photodissociation of cyclohexanone （C6H10O） in intense laser field. Two of the fragments from eyclohexanone, C2H＋ and C3H3＋, are studied under 800 nm laser pump-probe and the results obtained show similar time evolutions. It proposes a feasible model for analysing the experimental observations of the one-colour fs pump-probe measurement. The results demonstrate that as an intermediate product, the excited molecular parent ions play a very important role in photionization/photodissociation processes in intense laser field.

Limits in Enhancement Factor in Near-Brewster Angle Reflection Pump-Probe Two-Dimensional Infrared Spectroscopy

In this work,we simulated 2D infrared spectroscopy(IR)spectroscopy in both transmission geometry and Brewster-angle reflection geometry.Light dispersion and the leakage of s-polarized light are considered in simulating the enhancement factor of the reflection mode.Our simulation shows that the dispersion in reflection will only alter the 2D IR lineshape slightly and can be corrected.Leaking spolarized light due to imperfectness of IR polarizers in the reflection geometry may limit the enhancement factor,but such limit is above what a typical experiment can reach.In the current experiment,the enhancement factor is mainly limited by the precision of incident angle,for which ordinary rotation stages are probably not adequate enough.Moreover,traditional energy ratio of pump and probe pulses,which is 9:1,may not be ideal and could be changed to 2:1 in the reflection geometry.Considering all the above factors,the enhancement on the order of 1000 is possible in the current experiment.Nevertheless,near-Brewster angle reflection will enhance both the signal and the noise caused by the signal itself,therefore this method only works if the noise is unrelated to the signal,particularly if the noise is caused by the fluctuation in the probe.It cannot improve the signal to noise ratio when the dominate noise is from the signal itself.The theoretical results here agree reasonably well with published experiment results and pave way for realizing even higher enhancement at nearer-Brewster angle.

Development of new diagnostics based on LiF detector for pump-probe experiments

We present new diagnostics for use in optical laser pump-X-ray Free Electron Laser(XFEL)probe experiments to monitor dimensions,intensity profile and focusability of the XFEL beam and to control initial quality and homogeneity of targets to be driven by optical laser pulse.By developing X-ray imaging,based on the use of an LiF crystal detector,we were able to measure the distribution of energy inside a hard X-ray beam with unprecedented high spatial resolution(~1 mm)and across a field of view larger than some millimetres.This diagnostic can be used in situ,provides a very high dynamic range,has an extremely limited cost,and is relatively easy to be implemented in pump-probe experiments.The proposed methods were successfully applied in pump-probe experiments at the SPring-8 Angstrom Compact free electron LAser(SACLA)XFEL facility and its potential was demonstrated for current and future High Energy Density Science experiments.

Ultrafast dynamics of femtosecond laser-induced high spatial frequency periodic structures on silicon surfaces

Femtosecond laser-induced periodic surface structures(LIPSS)have been extensively studied over the past few decades.In particular,the period and groove width of high-spatial-frequency LIPSS(HSFL)is much smaller than the diffraction limit,making it a useful method for efficient nanomanufacturing.However,compared with the low-spatial-frequency LIPSS(LSFL),the structure size of the HSFL is smaller,and it is more easily submerged.Therefore,the formation mechanism of HSFL is complex and has always been a research hotspot in this field.In this study,regular LSFL with a period of 760 nm was fabricated in advance on a silicon surface with two-beam interference using an 800 nm,50 fs femtosecond laser.The ultrafast dynamics of HSFL formation on the silicon surface of prefabricated LSFL under single femtosecond laser pulse irradiation were observed and analyzed for the first time using collinear pump-probe imaging method.In general,the evolution of the surface structure undergoes five sequential stages:the LSFL begins to split,becomes uniform HSFL,degenerates into an irregular LSFL,undergoes secondary splitting into a weakly uniform HSFL,and evolves into an irregular LSFL or is submerged.The results indicate that the local enhancement of the submerged nanocavity,or the nanoplasma,in the prefabricated LSFL ridge led to the splitting of the LSFL,and the thermodynamic effect drove the homogenization of the splitting LSFL,which evolved into HSFL.

Measurement of spatiotemporal characteristics of femtosecond laser pulses by a modified single-shot autocorrelation

To overcome the shortcomings of the single-shot autocorrelation SSA where only one pulse width is obtained when the SSA is applied to measure the pulse width of ultrashort laser pulses a modified SSA for measuring the spatiotemporal characteristics of ultrashort laser pulses at different spatial positions is proposed. The spatiotemporal characteristics of femtosecond laser pulses output from the Ti sapphire regenerative amplifier system are experimentally measured by the proposed method. It was found that the complex spatial characteristics are measured accurately.The pulse widths at different spatial positions are various which obey the Gaussian distribution.The pulse width at the same spatial position becomes narrow with the increase in input average power when femtosecond laser pulses pass through a carbon disulfide CS2 nonlinear medium.The experimental results verify that the proposed method is valid for measuring the spatiotemporal characteristics of ultrashort laser pulses at different spatial positions.

Differential diagnosis of pancreatic cancer by single-shot echo-planar imaging diffusion-weighted imaging

AIM: To investigate the diagnostic ability of single-shot echo-planar imaging(EPI) diffusion-weighted imaging (DWI) to differentiate between malignant and benign pancreatic lesions. METHODS: A computerized search was performed on Pub Med, MEDLINE and EMBASE up to August 2014. Nine studies(10 sets of data) with a total of 304 malignant pancreatic lesions and 188 benign pancreatic lesions were included. The characteristics of each study included the study name, year of publication, magnetic resonance modalities used, patient population, strength of field, pulse time, repetition time, echo time(TE), maximum b factor, mean age, mean body weight, fat suppression, number of benign and malignant lesions, and true positive, true negative, false positive and false negative results. All analyses were performed using Meta-Di Sc and Stata 11.0.RESULTS: The pooled sensitivity and specificity of singleshot EPI DWI were 0.83(95%CI: 0.79-0.87) and 0.77(95%CI: 0.70-0.83), respectively. The positive likelihood ratio and negative likelihood ratio were 5.09(95%CI: 2.19-11.84) and 0.23(95%CI: 0.15-0.36), respectively. The P value for the χ2 heterogeneity for all pooled estimates was < 0.05. From the fitted summary receiver operating characteristic curve, the area under the curve and Q* index were 0.89 and 0.82, respectively. Publication bias was not present(t = 0.58, P = 0.58). Meta-regression analysis indicated that fat suppression, mean age, TE, and maximum b factor were not sources of heterogeneity(all P > 0.05). CONCLUSION: Single-shot EPI DWI is useful to differentiate between malignant and benign pancreatic lesions. Lesion size ≥ 2 cm is the limit for the diagnosis of early lesions.

Detection of the spatiotemporal field of a single-shot terahertz pulse based on spectral holography

According to electro-optical sampling theory, we propose a new method to detect the spatiotemporal field of a single- shot terahertz pulse by spectral holography for the first time. The single-shot terahertz pulse is coupled into a broadened chirped femtosecond pulse according to electro-optical sampling theory in the detecting system. Then the reference wave and the signal wave are split by Dammann grating and spread into the interference band-pass filter. The filtered sub-waves are at different central-frequencies because of the different incident angles. These sub-waves at different central-frequencies interfere to form sub-holograms, which are recorded in a single frame of a charge coupled device （CCD）. The sub-holograms are numerically processed, and the spatiotemporal field distribution of the original terahertz pulse is reconstructed. The computer simulations verify the feasibility of the proposed method.

New terahertz dispersive device for single-shot spectral measurements of terahertz pulse

A new terahertz dispersive device designed for single-shot spectral measurements of broadband terahertz pulses is proposed. With two-dimensional quasi-randomly distributed element design, the device exhibits approximately the dispersive property of single-order diffraction in far field. Its far-field diffraction pattern is experimentally verified employing a continuous terahertz source centered at 2.52 THz and a pyroelectric focal-plane-array camera, which is in good agreement with the numerical result. The device provides a new approach for direct single-shot spectral measurements of broadband terahertz waves.

Single-shot measurement of THz pulses

Terahertz(THz) waves have shown a broad prospect in the analysis of some dielectric materials because of their special properties. For the ultrafast irreversible processes, the THz single-shot measurement is a good choice. In this paper,a single-shot system is investigated, where a pump beam is used to generate THz pulses with high electrical field by optical rectification in LiNbO3, the probe beam with wavefront tilted by a blazed grating is used for single-shot measurement. The time window is up to 90 ps, the signal to noise ratio is 2000 : 1, the spectrum covers from 0.1 THz to about 2.0 THz, and the spectral resolution is 0.011 THz. The single-shot measurement result agrees well with that of a traditional electrical-optic sampling method.

Single-shot grating-based x-ray differential phase contrast imaging with a modified analyzer grating

X-ray grating interferometer has attracted widely attention in the past years due to its capability in achieving x-ray phase contrast imaging with low brilliance source. However, the widely used phase stepping information extraction method reduces system stability and prolongs data acquisition time by several times compared with conventional x-ray absorption- based imaging. The mechanical stepping can be avoided by using a staggered grating, but at the cost of low vertical spatial resolution. In this paper, employing a modified staggered grating and the angular signal radiography, we proposed a single-shot grating-based x-ray differential phase contrast imaging with decent vertical spatial resolution. The theoretical framework was deduced and proved by numerical experiments. Absorption, phase, and scattering computed tomography can be performed without phase stepping. Therefore, we believe this fast and highly stable imaging method with decent resolution would be widely applied in x-ray grating-based phase contrast imaging.

Single-Shot 360-Degree Cranial Deformity Detection System Using Digital Image Correlation

In this paper,a single-shot 360-degree cranial deformity detection system using digital image correlation(DIC)is presented to quickly obtain and detect accurate 3D data of infants’cra-nium.By introducing plane mirrors into a stereo 3D DIC measurement system,a multi-view 3D imaging model is established to convert 3D data from real and virtual perspectives into 360-degree 3D data of the tested infant cranium,achieving single-shot and panoramic 3D measurement.Exper-imental results showed that the performance and measurement accuracy of the proposed system can meet the requirements for cranial deformity detection,which provides a fast,accurate,and low-cost solution medically.

Single-Shot Measurement of Transient Phase Shift Induced by Laser Wake

Based on the frequency-to-time mapping relation of the linearly chirped pulse, the temporal phase shift induced by a laser-excited wake in a helium gas jet is measured using a chirped-pulse spectral interferometry with ～ 140 fs resolution over a temporal region of I ps in a single shot. In this measurement, the image of the wake is obtained with one-dimensional spatial resolution and temporal resolution limited only by the bandwidth and chirp of the pulse. The ＇bubbles＇ feature of the wake structure, along with multiple wakes excited by the main lobe and the side lobe of a laser focal-spot, is captured simultaneously.

Ultrafast Carrier Dynamics in CdSe/CdS/ZnS Quantum Dots

The intra- and inter-band relaxation dynamics of CdSe/CdS/ZnS core/shell/shell quantum dots are investigated with the aid of time-resolved nonlinear transmission spectra which are obtained using femtosecond pump-probe technique. By selectively exciting the core and shell carrier, the dynamics are studied in detail. Carrier relaxation is found faster in the conduction band of the CdS shell （about 130 fs） than that in the conduction band of the CdSe core （about 400 fs）. From the experiments it is distinctly demonstrated the existence of the defect states in the interface between the CdSe core and the CdS shell, indicating that ultrafast spectroscopy might be a suitable tool in studying interface and surface morphology properties in nanosystems.

共振和非共振超快pump-probe偏振光谱理论研究

从相互作用表象Liouville方程出发,得出了任意偏振激光作用下分子系统在时间域内的四阶张量非线性响应函数.处理了分子电子基态核相干运动的pump-probe偏振光谱,给出了在共振、非共振条件下光谱信号的明晰表达式.在基态核转动相干时,利用球张量代数使分子固有响应和激光偏振因素分离。

Attosecond laser station

The attosecond laser station （ALS） at the Synergetic Extreme Condition User Facility （SECUF） is a sophisticated and user-friendly platform for the investigation of the electron dynamics in atoms, molecules, and condensed matter on timescales ranging from tens of femtoseconds to tens of attoseconds. Short and tunable coherent extreme-ultraviolet （XUV） light sources based on high-order harmonic generation in atomic gases are being developed to drive a variety of endstations for inspecting and controlling ultrafast electron dynamics in real time. The combination of such light sources and end-stations offers a route to investigate fundamental physical processes in atoms, molecules, and condensed matter. The ALS consists of four beamlines, each containing a light source designed specifically for application experiments that will be performed in its own end-station. The first beamline will produce broadband XUV light for attosecond photoelectron spectroscopy and attosecond transient absorption spectroscopy. It is also capable of performing attosecond streaking to characterize isolated attosecond pulses and will allow studies on the electron dynamics in atoms, moleculars, and condensed matter. The second XUV beamline will produce narrowband femtoseeond XUV pulses for time-resolved and angle-resolved photoelectron spectroscopy, to study the electronic dynamics on the timescale of fundamental correlations and interactions in solids, especially in superconductors and topological insulators. The third beamline will produce broadband XUV pulses for attosecond coincidence spectroscopy in a cold-target recoil-ion momentum spectrometer, to study the ultrafast dynamics and reactions in atomic and molecular systems. The last beamline produces broadband attosecond XUV pulses designed for time-resolved photoemission electron microscopy, to study the ultrafast dynamics of plasmons in nanostructures and the surfaces of solid materials with high temporal and spatial resolutions simultaneously. The main object of the ALS is to provide domestic and international scientists with unique tools to study fundamental processes in physics, chemistry, biology, and material sciences with ultrafast temporal resolutions on the atomic scale.

基于量子级联激光器的Pump-Probe光路球晶雕刻实验

利用2台中红外量子级联激光器(QCL)组成的泵浦探测(pump-probe)光路通过红外共振吸收对高分子球晶进行选择性熔融进而实现球晶雕刻.当QCL激光频率和分子基团振动频率相同时,会发生共振吸收,产生强烈的热效应,诱导样品快速熔融;QCL激光具有高偏振性,优先诱导振动方向和红外激光偏振方向一致的基团发生共振吸收,因此可以实现选择性熔融;高分子球晶中有沿着各个方向的分子链并且取向方向确定,可以通过pump球晶不同部位来验证球晶雕刻的可行性.一台激光器(pump)对应分子链中基团的强吸收峰,共振加热诱导晶体熔融;另一台激光器(probe)对应分子特征基团(构象)的吸收峰,追踪结构变化;pump光可以选择性定点熔融,pump和probe 2束光均能在线追踪样品熔融程度,是该检测方法的突出优点.选用聚丁烯-1(iPB-1)为研究对象,实验结果显示,球晶熔融程度随基团振动方向与pump光偏振方向夹角的增大而减弱,证明了利用QCL在球晶尺度上进行雕刻是可行的,为原位在线研究快速熔融过程提供了新的研究途径,为定点调控晶型转变及晶体聚集态结构形态提供了思路.

Picosecond time-resolved X-ray ferromagnetic resonance measurements at Shanghai synchrotron radiation facility

An experimental picosecond time-resolved X-ray ferromagnetic resonance(TR-XFMR)apparatus with a time resolution of 13 ps(RMS)or 31 ps(FWHM)was constructed and demonstrated in the 07U and 08U1A soft X-ray beamlines at the Shanghai Synchrotron Radiation Facility(SSRF)using pump-probe detection and X-ray magnetic circular dichroism(XMCD)spectroscopy.Element and time-resolved ferromagnetic resonance was excited by continuous microwave phase-locking of the bunch clock within the photon beam during synchrotron radiation and was characterized by detecting the magnetic circular dichroism signals of the elements of interest in the magnetic films.Using this equipment,we measured the amplitude of the element-specific moment precession during ferromagnetic resonance(FMR)at 2 GHz in a single Ni81Fe19layer.

Rapid and high precision measurement of opto-thermal relaxation with pump-probe method

Opto-thermal relaxation is one of the most important properties of nonlinear optical materials.Rapid and high precision measurement of this parameter is vital in both fundamental research and applications.Current measurement uses either complicated structure with poor precision or high power heating source with low efficiency.Here,we propose a pump-probe method(PPM) to optically measure the thermal relaxation using whispering gallery mode(WGM) microcavities.When the pump laser shines on a microcavity,the materials absorb the input power resonantly and heat up.Then the heat dissipates from the cavities to the surroundings.The opto-thermal effect induces a refractive index change reflected in the signal light transmission spectra.By analyzing the curve character of the transmission spectra of the signal response in the spontaneous relaxation process,the thermal relaxation time can be rapidly measured with high precision.Additionally,we systematically verify the PPM using microtoroids under various pump powers and at various locking points of the signal laser mode.The small rate of refractive index changes($10à8) can be discerned with an input pump power as low as 11.816 l W.Hence,the PPM can be used to detect refractive index perturbation,like gas or liquid sensing,temperature fluctuations with ultra-high sensitivity and be applied to optical materials analysis efficiently.

First commissioning results of the coherent scattering and imaging endstation at the Shanghai soft X-ray free-electron laser facility

The Shanghai soft X-ray free-electron laser(SXFEL)user facility project started in 2016 and is expected to be open to users by 2022.It aims to deliver ultra-intense coherent femtosecond X-ray pulses to five endstations covering a range of 100–620 eV for ultrafast X-ray science.Two undulator lines are designed and constructed,based on different lasing modes:self-amplified spontaneous emission and echo-enabled harmonic generation.The coherent scattering and imaging(CSI)endstation is the first of five endstations to be commissioned online.It focuses on high-resolution single-shot imaging and the study of ultrafast dynamic processes using coherent forward scattering techniques.Both the single-shot holograms and coherent diffraction patterns were recorded and reconstructed for nanoscale imaging,indicating the excellent coherence and high peak power of the SXFEL and the possibility of‘‘diffraction before destruction’’experiments at the CSI endstation.In this study,we report the first commissioning results of the CSI endstation.

The unique magnetic damping enhancement in epitaxial Co2Fe1-xMnxAl films

Uniform precession dynamics and its magnetic damping are investigated in epitaxial Co2Fe1-xMnxAl films by using the time-resolved magneto-optical Kerr effect under out-of-plane configuration.The decay time of uniform precession mode decreases, and thus the magnetic damping increases with the increase of external field.Moreover, the decay time decreases as x decreases, so that the enhancement of magnetic damping occurs in Fe-rich sample.Furthermore, the decay time decreases as the excitation fluence increases, which drops rapidly at low magnetic field comparing with the slow reduction at high magnetic field.This unique magnetic damping enhancement is attributed to the enhancement of homogeneous magnetization.