Coherent coupling between vibrational modes of C-H bonds at different positions studied by femtosecond time-resolved coherent anti-Stokes Raman scattering

We performed femtosecond time-resolved coherent anti-Stokes Raman scattering （fs-CARS） measurements on liquid toluene and PVK film. For both samples, we selectively excited the CH stretching vibrational modes and observed the expected quantum beat signals. The frequency of the well-defined beats is in good agreement with the energy difference between the two simultaneously excited modes, which demonstrates that a coherent coupling between the vibrational modes of the C H chemical bonds exists at the different positions of the molecules. The dephasing times of the excited modes are obtained simultaneously.

Ultrafast Decay Dynamics of N-Ethylpyrrole Excited to the S_(1)Electronic State:A Femtosecond Time-Resolved Photoelectron Imaging Study

N-ethylpyrrole is one of ethylsubstituted derivatives of pyrrole and its excited-state decay dynamics has never been explored.In this work,we investigate ultrafast decay dynamics of N-ethylpyrrole excited to the S_(1)electronic state using a femtosecond time-resolved photoelectron imaging method.Two pump wavelengths of 241.9 and 237.7 nm are employed.At 241.9 nm,three time constants,5.0±0.7 ps,66.4±15.6 ps and 1.3±0.1 ns,are derived.For 237.7 nm,two time constants of 2.1±0.1 ps and 13.1±1.2 ps are derived.We assign all these time constants to be associated with different vibrational states in the S_(1)state.The possible decay mechanisms of different S_(1)vibrational states are briefly discussed.

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 characteristics of a nanosecond pulsed multi-hollow needle plate packed bed dielectric barrier discharge

In this paper,self-designed multi-hollow needle electrodes are used as a high-voltage electrode in a packed bed dielectric barrier discharge reactor to facilitate fast gas flow through the active discharge area and achieve large-volume stable discharge.The dynamic characteristics of the plasma,the generated active species,and the energy transfer mechanisms in both positive discharge(PD)and negative discharge(ND)are investigated by using fast-exposure intensified charge coupled device(ICCD)images and time-resolved optical emission spectra.The experimental results show that the discharge intensity,number of discharge channels,and discharge volume are obviously enhanced when the multi-needle electrode is replaced by a multihollow needle electrode.During a single voltage pulse period,PD mainly develops in a streamer mode,which results in a stronger discharge current,luminous intensity,and E/N compared with the diffuse mode observed in ND.In PD,as the gap between dielectric beads changes from 0 to250μm,the discharge between the dielectric bead gap changes from a partial discharge to a standing filamentary micro-discharge,which allows the plasma to leave the local area and is conducive to the propagation of surface streamers.In ND,the discharge only appears as a diffusionlike mode between the gap of dielectric beads,regardless of whether there is a discharge gap.Moreover,the generation of excited states N_(2)^(+)(B^(2)∑_(u)^(+))and N2(C^(3)Π_(u))is mainly observed in PD,which is attributed to the higher E/N in PD than that in ND.However,the generation of the OH(A^(2)∑^(+))radical in ND is higher than in PD.It is not directly dominated by E/N,but mainly by the resonant energy transfer process between metastable N_(2)(A^(3)∑_(u)^(+))and OH(X^(2)Π).Furthermore,both PD and ND demonstrate obvious energy relaxation processes of electron-to-vibration and vibration-to-vibration,and no vibration-to-rotation energy relaxation process is observed.

Ultrafast dynamics of o-fluorophenol studied with femtosecond time-resolved photoelectron and photoion spectroscopy

The ultrafast dynamics of o-fluorophenol via the excited states has been studied by femtosecond time-resolved photoelectron imaging. The photoion and photoelectron spectra taken with a time delay between 267 nm pump laser and 800 nm probe laser provide a longer-lived S1 electronic state of about ns timescale. In comparison,the spectra obtained by exciting the S2 state with femtosecond laser pulses at 400 nm and ionizing with pulses at 800 nm suggest that the S2 state has an ultrashort lifetime about 102 fs and reflects the internal conversion dynamics of the S2 state to the S1 state.

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.

Determination of Iron in Water Solution by Time-Resolved Femtosecond Laser-Induced Breakdown Spectroscopy

The influence of the energy of femtosecond laser pulses on the intensity of Fe I （371.99 nm） emission line and the continuous spectrum of the plasma generated on the surface of Fe^3＋ water solution by a Ti： sapphire laser radiation with pulse duration 〈45 fs and energies up to 7 mJ is determined. A calibration curve was obtained for Fe3＋ concentration range from 0.5 g/L to the limit of detection in water solution, and its saturation was detected for concentrations above 0.25 g/L, which is ascribed to self-absorption. The 3σ- limit of detection obtained for Fe in water solution is 2.6 mg/L in the case of 7 mJ laser pulse energy. It is found that an increase of laser pulse energy insignificantly affects on LOD in the time-resolved LIBS and leads to a slight improvement of the limit of detection.

Time-resolved spectroscopy of femtosecond laser-induced Cu plasma with spark discharge

The combination of spark discharge and laser-induced breakdown spectroscopy (LIBS) is called spark discharge assisted LIBS.It works under laser-plasma triggered spark discharge mode,and shows its ability to enhance spectral emission intensity.This work uses a femtosecond laser as the light souuce,since femtosecond laser has many advantages in laser-induced plasma compared with nanosecond laser,meanwhile,the study on femtosecond LIBS with spark discharge is rare.Time-resolved spectroscopy of spark discharge assisted femtosecond LIBS was investigated under different discharge voltages and laser energies.The results showed that the spectral intensity was significantly enhanced by using spark discharge compared with LIBS alone.And,the spectral emission intensity using spark discharge assisted LIBS increased with the increase in the laser energy.In addition,at low laser energy,there was an obvious delay on the discharge time compared with high laser energy,and the discharge time with positive voltage was different from that with negative voltage.

Time-resolved K-shell x-ray spectra of nanosecond laser-produced titanium tracer in gold plasmas

A study of a nanosecond laser irradiation on the titanium-layer-buried gold planar target is presented. The timeresolved x-ray emission spectra of titanium tracer are measured by a streaked crystal spectrometer. By comparing the simulated spectra obtained by using the FLYCHK code with the measured titanium spectra, the temporal plasma states, i.e.,the electron temperatures and densities, are deduced. To evaluate the feasibility of using the method for the characterization of Au plasma states, the deduced plasma states from the measured titanium spectra are compared with the Multi-1D hydrodynamic simulations of laser-produced Au plasmas. By comparing the measured and simulated results, an overall agreement for the electron temperatures is found, whereas there are deviations in the electron densities. The experiment–theory discrepancy may suggest that the plasma state could not be well reproduced by the Multi-1D hydrodynamic simulation, in which the radial gradient is not taken into account. Further investigations on the spectral characterization and hydrodynamic simulations of the plasma states are needed. All the measured and FLYCHK simulated spectra are given in this paper as datasets. The datasets are openly available at http://www.doi.org/10.57760/sciencedb.j00113.00032.

Femtosecond time-resolved difference absorption spectroscopy of all-trans-β-Apo-8′-carotenal

The femtosecond time-resolved difference absorption spectra of all-trans-b- Apo-8′-carotenal have been recorded and analyzed by the singular-value decomposition (SVD) method followed by global fitting using a sequential model for the excited-state energy relaxation. With this model, we have obtained the excited-state absorption spectra and the lifetimes of the corresponding excited states both in nonpolar solvent n-hexane and polar solvent methanol. Three excited states, namely S3(170fs), S2(2.32ps) and S1(26ps) in n-hexane, and two excited states S2 (190fs) and S1(9.4ps) in methanol have been observed. The excited-state absorption spectra of all-trans-b-Apo-8′-carotenal in methanol display a red shift and broadeness, while the lifetime of S1 state becomes shorter. It is proposed that these effects are related to the presence of a carbonyl functional group that leads to the solvent effect on the excited-state energy level. At the same time, it is shown that the SVD method is a useful tool in resolving the time-resolved absorption spectra.

High-performance liquid metal electromagnetic actuator fabricated by femtosecond laser

Small-scale electromagnetic soft actuators are characterized by a fast response and simplecontrol,holding prospects in the field of soft and miniaturized robotics.The use of liquid metal(LM)to replace a rigid conductor inside soft actuators can reduce the rigidity and enhance the actuation performance and robustness.Despite research efforts,challenges persist in the flexible fabrication of LM soft actuators and in the improvement of actuation performance.To address these challenges,we developed a fast and robust electromagnetic soft microplate actuator based on a laser-induced selective adhesion transfer method.Equipped with unprecedentedly thin LM circuit and customized low Young’s modulus silicone rubber(1.03 kPa),our actuator exhibits an excellent deformation angle(265.25?)and actuation bending angular velocity(284.66 rad·s^(-1)).Furthermore,multiple actuators have been combined to build an artificial gripper with a wide range of functionalities.Our actuator presents new possibilities for designing small-scaleartificial machines and supports advancements in ultrafast soft and miniaturized robotics.

Effect of sample temperature on femtosecond laser ablation of copper

We conduct an experimental study supported by theoretical analysis of single laser ablating copper to investigate the interactions between laser and material at different sample temperatures,and predict the changes of ablation morphology and lattice temperature.For investigating the effect of sample temperature on femtosecond laser processing,we conduct experiments on and simulate the thermal behavior of femtosecond laser irradiating copper by using a two-temperature model.The simulation results show that both electron peak temperature and the relaxation time needed to reach equilibrium increase as initial sample temperature rises.When the sample temperature rises from 300 K to 600 K,the maximum lattice temperature of the copper surface increases by about 6500 K under femtosecond laser irradiation,and the ablation depth increases by 20%.The simulated ablation depths follow the same general trend as the experimental values.This work provides some theoretical basis and technical support for developing femtosecond laser processing in the field of metal materials.

Triboelectric‘electrostatic tweezers'for manipulating droplets on lubricated slippery surfaces prepared by femtosecond laser processing

The use of‘Electrostatic tweezers'is a promising tool for droplet manipulation,but it faces many limitations in manipulating droplets on superhydrophobic surfaces.Here,we achieve noncontact and multifunctional droplet manipulation on Nepenthes-inspired lubricated slippery surfaces via triboelectric electrostatic tweezers(TETs).The TET manipulation of droplets on a slippery surface has many advantages over electrostatic droplet manipulation on a superhydrophobic surface.The electrostatic field induces the redistribution of the charges inside the neutral droplet,which causes the triboelectric charged rod to drive the droplet to move forward under the electrostatic force.Positively or negatively charged droplets can also be driven by TET based on electrostatic attraction and repulsion.TET enables us to manipulate droplets under diverse conditions,including anti-gravity climb,suspended droplets,corrosive liquids,low-surface-tension liquids(e.g.ethanol with a surface tension of 22.3 mN·m^(-1)),different droplet volumes(from 100 nl to 0.5 ml),passing through narrow slits,sliding over damaged areas,on various solid substrates,and even droplets in an enclosed system.Various droplet-related applications,such as motion guidance,motion switching,droplet-based microreactions,surface cleaning,surface defogging,liquid sorting,and cell labeling,can be easily achieved with TETs.

Self-propelled Leidenfrost droplets on femtosecond-laser-induced surface with periodic hydrophobicity gradient

The controllable transfer of droplets on the surface of objects has a wide application prospect in the fields of microfluidic devices,fog collection and so on.The Leidenfrost effect can be utilized to significantly reduce motion resistance.However,the use of 3D structures limits the widespread application of self-propulsion based on Leidenfrost droplets in microelectromechanical system.To manipulate Leidenfrost droplets,it is necessary to create 2D or quasi-2D geometries.In this study,femtosecond laser is applied to fabricate a surface with periodic hydrophobicity gradient(SPHG),enabling directional self-propulsion of Leidenfrost droplets.Flow field analysis within the Leidenfrost droplets reveals that the vapor layer between the droplets and the hot surface can be modulated by the SPHG,resulting in directional propulsion of the inner gas.The viscous force between the gas and liquid then drives the droplet to move.

Femtosecond laser fabrication of 3D vertically aligned micro-pore network on thick-film Li_(4)Ti_(5)O_(12)electrode for high-performance lithium storage

The development of energy storage devices with high energy density relies heavily on thick film electrodes,but it is challenging due to the limited ion transport kinetics inherent in thick electrodes.Here,we report on the preparation of a directional vertical array of micro-porous transport networks on LTO electrodes using a femtosecond laser processing strategy,enabling directional ion rapid transport and achieving good electrochemical performance in thick film electrodes.Various three-dimensional(3D)vertically aligned micro-pore networks are innovatively designed,and the structure,kinetics characteristics,and electrochemical performance of the prepared ion transport channels are analyzed and discussed by multiple characterization and testing methods.Furthermore,the rational mechanisms of electrode performance improvement are studied experimentally and simulated from two aspects of structural mechanics and transmission kinetics.The ion diffusion coefficient,rate performance at 60 C,and electrode interface area of the laser-optimized 60-15%micro-porous transport network electrodes increase by 25.2 times,2.2 times,and 2.15 times,respectively than those of untreated electrodes.Therefore,the preparation of 3D micro-porous transport networks by femtosecond laser on ultra-thick electrodes is a feasible way to develop high-energy batteries.In addition,the unique micro-porous transport network structure can be widely extended to design and explore other high-performance energy materials.

Clinical efficacy of femtosecond laser-assisted phacoemulsification in diabetic cataract patients

BACKGROUND Diabetic patients with cataracts encounter specific difficulties during cataract surgery due to alterations in microcirculation,blood supply,metabolism,and the microenvironment.Traditional phacoemulsification may not fully tackle these issues,especially in instances with substantial preoperative astigmatism.The utilization of femtosecond laser-assisted phacoemulsification,in conjunction with Toric intraocular lens(IOL)implantation,offers a potentially more efficient strategy.This research seeks to evaluate the efficacy and possible complications of this approach in diabetic cataract patients.AIM To investigate the clinical efficacy and complications of femtosecond laser-assisted phacoemulsification combined with Toric IOL implantation in diabetic cataract patients,comparing it with traditional phacoemulsification methods.METHODS This retrospective study enrolled 120 patients with diabetes cataract from May 2019 to May 2021.The patients were divided into two groups:the control group underwent traditional phacoemulsification and Toric IOL implantation,while the treatment group received Len Sx femtosecond laser-assisted treatment.Outcome measures included naked eye vision,astigmatism,high-level ocular phase difference detection,clinical efficacy,and complication.RESULTS There were no significant preoperative differences in astigmatism or naked eyesight between the two groups.However,postoperative improvements were observed in both groups,with the treatment group showing greater enhancements in naked eye vision and astigmatism six months after the procedure.High-level corneal phase difference tests also indicated significant differences in favor of the treatment group.CONCLUSION This study suggests that femtosecond laser-assisted phacoemulsification combined with Toric IOL implantation appears to be more effective in enhancing postoperative vision in diabetic cataract patients compared to traditional methods offering valuable insights for clinical practice.

Time-resolved spectroscopy for 5s^('4)D_(7/2) state transitions undergoing electron–ion recombination in femtosecond laser-produced copper plasma

In the femtosecond laser-produced Cu-plasma, the transient transition dynamics that the excited state 5s4D7/2 via electron-ion recombination transfers to 4p4F9/20 （465.11 nm, Λ1 line） and 4p4D7/20 （529.25 nm, Λ2 line） states are investigated by using the time-resolved spectroscopy. The occupation number and relevant lifetime of the excited state 5s4D7/2, the temporal evolutions of spectral intensities for Λ1 line and Λ2 line emissions are demonstrated to be in direct proportion to the employed laser intensity, which reveals the transient features of transition dynamics clearly differing from that resulted in the traditional collision excitation. Furthermore, some unique characteristics for Λ1 and Λ2 transitions stemming from electron-ion recombination are examined in detail.

High performance micromachining of sapphire by laser induced plasma assisted ablation(LIPAA)using GHz burst mode femtosecond pulses

GHz burst-mode femtosecond(fs)laser,which emits a series of pulse trains with extremely short intervals of several hundred picoseconds,provides distinct characteristics in materials processing as compared with the conventional irradiation scheme of fs laser(single-pulse mode).In this paper,we take advantage of the moderate pulse interval of 205 ps(4.88 GHz)in the burst pulse for high-quality and high-efficiency micromachining of single crystalline sapphire by laser induced plasma assisted ablation(LIPAA).Specifically,the preceding pulses in the burst generate plasma by ablation of copper placed behind the sapphire substrate,which interacts with the subsequent pulses to induce ablation at the rear surface of sapphire substrates.As a result,not only the ablation quality but also the ablation efficiency and the fabrication resolution are greatly improved compared to the other schemes including single-pulse mode fs laser direct ablation,single-pulse mode fs-LIPAA,and nanosecond-LIPAA.

Time-resolved spectroscopy of collinear femtosecond and nanosecond dual-pulse laser-induced Cu plasmas

In this paper,we investigate the time-resolved spectroscopy of collinear femtosecond(fs)and nanosecond(ns)dual-pulse(DP)laser-induced plasmas.A copper target was used as an experimental sample,and the fs laser was considered as the time zero reference point.The interpulse delay between fs and ns laser beams was 3μs.First,we compared the time-resolved peak intensities of Cu(I)lines from Cu plasmas induced by fs+ns and ns+fs DP lasers with collinear configuration.The results showed that compared with the ns+fs DP,the fs+ns DP laser-induced Cu plasmas had stronger peak intensities and longer lifetimes.Second,we calculated time-resolved plasma temperatures using the Boltzmann plot with three spectral lines at Cu(I)510.55,515.32 and 521.82 nm.In addition,time-resolved electron densities were calculated based on Stark broadening with Cu(I)line at 521.82 nm.It was found that compared with ns+fs DP,the plasma temperatures and electron densities of the Cu plasmas induced by fs+ns DP laser were higher.Finally,we observed images of ablation craters under the two experimental conditions and found that the fs+ns DP laser-produced stronger ablation,which corresponded to stronger plasma emission.

Measurements of the concentration of organic solutions by femtosecond time-resolved ERE-CARS

A variant of all-resonant CARS named electronic-resonant enhancement CARS(ERE-CARS) is applied to measure the methanol-water solution concentration at room temperature.The measurements are performed using the ERE-CARS signal of the Raman vibrations near the C-H stretching modes(at 2835 and 2942 cm 1) in methanol.By changing the timing(t>0) of the laser pulses of this non-degenerate four wave mixing technique,the concentration information based on the vibrational dynamics of the C-H bonds can be successfully detected as the frequency-spread dephasing rate during the first few hundred fs in the ERE-CARS signal with high sensitivity and accuracy.Femtosecond time-resolved ERE-CARS technique is applied to the concentration analysis of a mixture of the organic solution.This investigation indicates that femtosecond time-resolved ERE-CARS technique might be a powerful tool for real-time detection for solution concentration of different liquids.