The electrocatalytic oxidation of biomass-derived furfural(FF)feedstocks into 2-furoic acid(FA)holds immense industrial potential in optics,cosmetics,polymers,and food.Herein,we fabricated Co O/Ni O/nickel foam(NF)and...The electrocatalytic oxidation of biomass-derived furfural(FF)feedstocks into 2-furoic acid(FA)holds immense industrial potential in optics,cosmetics,polymers,and food.Herein,we fabricated Co O/Ni O/nickel foam(NF)and Cu_(2)O/Ni O/NF electrodes via in situ pulsed laser irradiation in liquids(PLIL)for the bifunctional electrocatalysis of oxygen evolution reaction(OER)and furfural oxidation reaction(FOR),respectively.Simultaneous oxidation of NF surface to NiO and deposition of CoO and/or Cu_(2)O on NF during PLIL offer distinct advantages for enhancing both the OER and FOR.CoO/NiO/NF electrocatalyst provides a consistently low overpotential of~359 m V(OER)at 10 m A/cm^(2),achieving the maximum FA yield(~16.37 m M)with 61.5%selectivity,79.5%carbon balance,and a remarkable Faradaic efficiency of~90.1%during 2 h of FOR at 1.43 V(vs.reversible hydrogen electrode).Mechanistic pathway via in situ electrochemical-Raman spectroscopy on CoO/NiO/NF reveals the involvement of phase transition intermediates(NiOOH and CoOOH)as surface-active centers during electrochemical oxidation.The carbonyl carbon in FF is attacked by hydroxyl groups to form unstable hydrates that subsequently undergo further oxidation to yield FA products.This method holds promise for large-scale applications,enabling simultaneous production of renewable building materials and fuel.展开更多
In order to further improve the propulsion performance of pulsed plasma thrusters for space micro propulsion,a novel laser ablation pulsed plasma thruster is proposed,which separated the laser ablation and electromagn...In order to further improve the propulsion performance of pulsed plasma thrusters for space micro propulsion,a novel laser ablation pulsed plasma thruster is proposed,which separated the laser ablation and electromagnetic acceleration.Optical emission spectroscopy is utilized to investigate the plasma characteristics in the thruster.The spectral lines at different times,positions and discharge intensities are experimentally recorded,and the plasma characteristics in the discharge channel are concluded through analyzing the variation of spectral lines.With the discharge energy of 24 J,laser energy of 0.6 J and the use of aluminum propellant,the specific impulse and thrust efficiency reach 6808 s and 70.6%,respectively.展开更多
Nanosecond pulsed discharges at atmospheric pressure in a pin-to-pin electrode configuration are well reproducible in time and space, which is beneficial to the fundamentals and applications of low-temperature plasmas...Nanosecond pulsed discharges at atmospheric pressure in a pin-to-pin electrode configuration are well reproducible in time and space, which is beneficial to the fundamentals and applications of low-temperature plasmas. In this experiment, the discharges in helium(He) and He with 2.3%water vapor(H_(2)O) are driven by a series of 10 ns overvoltage pulses(~13 k V). Special attention is paid to the spectral characteristics obtained in the center of discharges by time-resolved optical emission spectroscopy. It is found that in helium, the emission of atomic and molecular helium during the afterglow is more intense than that in the active discharge, while in the He+2.3%H_(2)O mixture, helium emission is only observed during the discharge pulse and the molecular helium emission disappears. In addition, the emissions of OH(A-X) and Hα present similar behavior that increases sharply during the falling edge of the voltage pulse as the electrons cool down rapidly. The gas temperature is set to remain low at 540 K by fitting the OH(A-X) band. A comparative study on the emission of radiative species(He, He_(2), OH and H)is performed between these two discharge cases to derive their main production mechanisms. In both cases, the dominant primary ion is He^(+) at the onset of discharges, but their He^(+) charge transfer processes are quite different. Based on these experimental data and a qualitative discussion on the discharge kinetics, with regard to the present discharge conditions, it is shown that the electron-assisted three-body recombination processes appear to be the significant sources of radiative OH and H species in high-density plasmas.展开更多
Interactions between the central nervous system(CNS)and autonomic nervous system(ANS)play a crucial role in modulating perception,cognition,and emotion production.Previous studies on CNS–ANS interactions,or heart–br...Interactions between the central nervous system(CNS)and autonomic nervous system(ANS)play a crucial role in modulating perception,cognition,and emotion production.Previous studies on CNS–ANS interactions,or heart–brain coupling,have often used heart rate variability(HRV)metrics derived from electrocardiography(ECG)recordings as empirical measurements of sympathetic and parasympathetic activities.Functional near-infrared spectroscopy(fNIRS)is a functional brain imaging modality that is increasingly used in brain and cognition studies.The fNIRS signals contain frequency bands representing both neural activity oscillations and heartbeat rhythms.Therefore,fNIRS data acquired in neuroimaging studies can potentially provide a single-modality approach to measure task-induced responses in the brain and ANS synchronously,allowing analysis of CNS–ANS interactions.In this proof-of-concept study,fNIRS was used to record hemodynamic changes from the foreheads of 20 university students as they each played a round of multiplayer online battle arena(MOBA)game.From the fNIRS recordings,neural and heartbeat frequency bands were extracted to assess prefrontal activities and shortterm pulse rate variability(PRV),an approximation for short-term HRV,respectively.Under the experimental conditions used,fNIRS-derived PRV metrics showed good correlations with ECG-derived HRV golden standards,in terms of absolute measurements and video game playing(VGP)-related changes.It was also observed that,similar to previous studies on physical activity and exercise,the PRV metrics closely related to parasympathetic activities recovered slower than the PRV indicators of sympathetic activities after VGP.It is concluded that it is feasible to use fNIRS to monitor concurrent brain and ANS activations during online VGP,facilitating the understanding of VGP-related heart–brain coupling.展开更多
In this study, a stand-off and collinear double pulse laser-induced breakdown spectroscopy (DP LIBS) system was designed, and the magnesium alloy samples at a distance of 2.5 m away from the LIBS system were measure...In this study, a stand-off and collinear double pulse laser-induced breakdown spectroscopy (DP LIBS) system was designed, and the magnesium alloy samples at a distance of 2.5 m away from the LIBS system were measured. The effect of inter-pulse delay on spectra was studied, and the signal enhancement was observed compared to the single pulse LIBS (SP LIBS). The morphology of the ablated crater on the sample indicated a higher efficiency of surface pretreatment in DP LIBS. The calibration curves of Ytterbium (Y) and Zirconium (Zr) were investigated. The square of the correlation coefficient of the calibration curve of element Y reached up to 0.9998.展开更多
We experimentally observe the high resolution direct frequency comb spectroscopy using counter-propagating broadband femtosecond pulses on two-photon transitions in room-temperature ^87 Rb atoms. The Doppler broad- en...We experimentally observe the high resolution direct frequency comb spectroscopy using counter-propagating broadband femtosecond pulses on two-photon transitions in room-temperature ^87 Rb atoms. The Doppler broad- ened background is effectively eliminated with the pulse shaping method and the spectrum modulation technique. The combination of the pulse shaping method and the spectra modulation technique provides a potential approachto reduce background of at least 99%.展开更多
Atmospheric pressure micro-discharges in helium gas with a mixture of 0.5%water vapor between two pin electrodes are generated with nanosecond overvoltage pulses.The temporal and spatial characteristics of the dischar...Atmospheric pressure micro-discharges in helium gas with a mixture of 0.5%water vapor between two pin electrodes are generated with nanosecond overvoltage pulses.The temporal and spatial characteristics of the discharges are investigated by means of time-resolved imaging and optical emission spectroscopy with respect to the discharge morphology,gas temperature,electron density,and excited species.The evolution of micro-discharges is captured by intensified CCD camera and electrical properties.The gas temperature is diagnosed by a two-temperature fit to the ro-vibrational OH(A^(2)Σ^(+)–X^П(2),0–0)emission band and is found to remain low at 425 K during the discharge pulses.The profile of electron density performed by the Stark broadening of Ha 656.1-nm and He I 667.8-nm lines is uniform across the discharge gap at the initial of discharge and reaches as high as 10^(23)m^(-3).The excited species of He,OH,and H show different spatio-temporal behaviors from each other by the measurement of their emission intensities,which are discussed qualitatively in regard of their plasma kinetics.展开更多
Laser-induced plasmas of dual-pulse fiber-optic laser-induced breakdown spectroscopy with different pulse energy ratios are studied by using the optical emission spectroscopy(OES)and fast imaging.The energy of the two...Laser-induced plasmas of dual-pulse fiber-optic laser-induced breakdown spectroscopy with different pulse energy ratios are studied by using the optical emission spectroscopy(OES)and fast imaging.The energy of the two laser pulses is independently adjusted within 0–30 m J with the total energy fixed at 30 m J.The inter-pulse delay remains 450 ns constantly.As the energy share of the first pulse increases,a similar bimodal variation trend of line intensities is observed.The two peaks are obtained at the point where the first pulse is half or twice of the second one,and the maximum spectral enhancement is at the first peak.The bimodal variation trend is induced by the change in the dominated mechanism of dual-pulse excitation with the trough between the two peaks caused by the weak coupling between the two mechanisms.By increasing the first pulse energy,there is a transition from the ablation enhancement dominance near the first peak to the plasma reheating dominance near the second peak.The calculations of plasma temperature and electron number density are consistent with the bimodal trend,which have the values of 17024.47 K,2.75×10^(17)cm;and 12215.93 K,1.17×10^(17)cm;at a time delay of 550 ns.In addition,the difference between the two peaks decreases with time delay.With the increase in the first pulse energy share,the plasma morphology undergoes a transformation from hemispherical to shiny-dot and to oblate-cylinder structure during the second laser irradiation from the recorded images by using an intensified charge-coupled device(ICCD)camera.Correspondingly,the peak expansion distance of the plasma front first decreases significantly from 1.99 mm in the single-pulse case to 1.34 mm at 12/18(dominated by ablation enhancement)and then increases slightly with increasing the plasma reheating effect.The variations in plasma dynamics verify that the change of pulse energy ratios leads to a transformation in the dual-pulse excitation mechanism.展开更多
High-quality superconducting FeSe0.5 Te0.5 films are epitaxiMly grown on different substrates by using the pulsed laser deposition method. By measuring the transport properties and surface morphology of films grown on...High-quality superconducting FeSe0.5 Te0.5 films are epitaxiMly grown on different substrates by using the pulsed laser deposition method. By measuring the transport properties and surface morphology of films grown on single- crystal substrates of Al2O3 (0001), SrTiO3 (001), and MgO (001), as well as monitoring the real-time growth process on MgO substrates with reflection high energy electron diffraction, we find the appropriate parameters for epitaxial growth of high-quality FeSe0.5 Te0.5 thin films suitable for angle-resolved photoemission spectroscopy measurements. We further report the angle-resolved photoemission spectroscopy characterization of the super- conducting films. The clearly resolved Fermi surfaces and the band structure suggest a sample quality that is as good as that of high-quality single-crystals, demonstrating that the pulsed laser deposition method can serve as a promising technique for in situ preparation and manipulation of iron-based superconducting thin films, which may bring new prosperity to angle-resolved photoemission spectroscopy research on iron-based superconductors.展开更多
This paper focuses on the preparation of a new extended set of calibrations of cooling rate(fictive temperature)in fused silica determined by inelastic light scattering and its subsequent use to characterize the local...This paper focuses on the preparation of a new extended set of calibrations of cooling rate(fictive temperature)in fused silica determined by inelastic light scattering and its subsequent use to characterize the local cooling rate distribution in ultra-short pulsed(USP)laser modification.In order to determine the thermal history(e.g.cooling rate and fictive temperature)of fused silica,high-resolution inelastic light-scattering experiments(Raman and Brillouin spectroscopy)were investigated.Calibrations were performed and compared to the existing literature to quantify structural changes due to a change of fictive temperature.Compared to existing calibrations,this paper provides an extension to lower and higher cooling rates.Using this new set of calibrations,we characterized a USP laser modification in fused silica and calculated the local fictive temperature distribution.An equation relating the fictive temperature(Tf)to cooling rates is given.A maximum cooling rate of 3000 K min-1 in the glass transition region around 1200℃ was deduced from the Raman analysis.The Brillouin observations are sensitive to both the thermal history and the residual stress.By comparing the Raman and Brillouin observations,we extracted the local residual stress distribution with high spatial resolution.For the first time,combined Raman and Brillouin inelastic light scattering experiments show the local distribution of cooling rates and residual stresses(detailed behavior of the glass structure)in the interior and the surrounding of an USP laser modified zone.展开更多
Dielectric barrier discharge(DBD) attracts lots of attentions for its great application promises,and the rotational temperature is one of its mostly important parameters.In order to measure the rotational temperature ...Dielectric barrier discharge(DBD) attracts lots of attentions for its great application promises,and the rotational temperature is one of its mostly important parameters.In order to measure the rotational temperature of a pulsed DBD in atmospheric air,the temperature is studied by using optical emission spectroscopy(OES).The discharge is excited by a high voltage pulse with 124 ns rise time and 230 ns full width at half maximum(FWHM) at a repetition rate of a few hundred hertz.The rotational temperatures are studied using different voltages,different repetition rates of the pulse power supply,and different gaps between dielectrics: They are in the range from 390 K to 500 K during the whole discharge.When the gap between dielectrics increases,the rotational temperature initially decreases and then increases.The rotational temperature changes complexly when the pulse repetition rate changes.When the voltage increases,the rotational temperature always decreases,which is not expected.These results allow one to predict the rotational temperature at different supply power parameters and electrode configurations,which is useful for the DBD's industrial application.展开更多
Ultra-short laser pulses possess many advantages for materials processing.Ultrafast laser has a significantly low thermal effect on the areas surrounding the focal point;therefore,it is a promising tool for micro-and ...Ultra-short laser pulses possess many advantages for materials processing.Ultrafast laser has a significantly low thermal effect on the areas surrounding the focal point;therefore,it is a promising tool for micro-and submicro-sized precision processing.In addition,the nonlinear multiphoton absorption phenomenon of focused ultra-short pulses provides a promising method for the fabrication of various structures on transparent material,such as glass and transparent polymers.A laser direct writing process was applied in the fabrication of high-performance three-dimensional(3D)structured multilayer microsupercapacitors(MSCs)on polymer substrates exhibiting a peak specific capacitance of 42.6 mF·cm^-2 at a current density of 0.1 mA·cm^-12.Furthermore,a flexible smart sensor array on a polymer substrate was fabricated for multi-flavor detection.Different surface treatments such as gold plating,reducedgraphene oxide(rGO)coating,and polyaniline(PANI)coating were accomplished for different measurement units.By applying principal component analysis(PCA),this sensing system showed a promising result for flavor detection.In addition,two-dimensional(2D)periodic metal nanostructures inside 3D glass microfluidic channels were developed by all-femtosecond-laser processing for real-time surfaceenhanced Raman spectroscopy(SERS).The processing mechanisms included laser ablation,laser reduction,and laser-induced surface nano-engineering.These works demonstrate the attractive potential of ultra-short pulsed laser for surface precision manufacturing.展开更多
<div style="text-align:justify;"> In this study, a two-dimensional model describing thermal stress on a charge-coupled device (CCD) induced by ms laser pulses was examined. Considering the nonlinearity...<div style="text-align:justify;"> In this study, a two-dimensional model describing thermal stress on a charge-coupled device (CCD) induced by ms laser pulses was examined. Considering the nonlinearity of the CCD’s material parameters and the melting phase transition process of aluminum electrode materials was considered by using equivalent specific heat capacity method, the physical process where a laser pulse irradiating a CCD pixel array was simulated using COMSOL Multiphysics software. The temperature field and thermal stress field were calculated and analyzed. In order to clarify the mechanism producing damage on the CCD detector, Raman spectra from silicon were measured with a micro-Raman spectrometer to determine stress change in the CCD chip. The procedure presented herein illustrates a method for evaluating strain in a CCD after laser irradiation. </div>展开更多
A novel laser-assisted pulsed plasma thruster(LA-PPT)is proposed as an electric propulsion thruster,which separates laser ablation and electromagnetic acceleration.It aims for a higher specific impulse than that achie...A novel laser-assisted pulsed plasma thruster(LA-PPT)is proposed as an electric propulsion thruster,which separates laser ablation and electromagnetic acceleration.It aims for a higher specific impulse than that achieved with conventional LA-PPTs.Owing to the short-time discharge and the novel configuration,the physical mechanism of the discharge is unclear.Time and spatial-resolved optical emission spectroscopy was applied to investigate the variation in the plasma properties in the thruster discharge channel.The plasma species,electron temperature,and electron density were obtained and discussed.Our investigation revealed that there were H_(α),H_(β),H_(γ),H_(ε) atoms,CⅠ,CⅡ,CⅢ,CⅣ,ClⅠ,ClⅡparticles,and a small amount of CH,C_(3),C_(2),H_(2) neutral molecular groups in the plasma.The electron temperature of the discharge channel of the thruster was within 0.6–4.9 e V,and the electron density was within(1.1–3.0)×10^(18)cm^(-3),which shows that the optical emission spectroscopy method is to measure the electron excitation temperature and electron density in heavy particles.But the Langmuir probe method is to measure the temperature and density of free electrons.The use of laser instead of spark plug as the ignition mode significantly changed the plasma distribution in the discharge channel.Unlike the conventional PPT,which has high electron density near the thruster surface,LAPPT showed relatively large electron density at the thruster outlet,which increased the thruster specific impulse.In addition,the change in the ignition mode enabled the electron density in the LA-PPT discharge channel to be higher than that in the conventional PPT.This proves that the ignition mode with laser replacing the spark plug effectively optimised the PPT performance.展开更多
In double-pulse laser-induced breakdown spectroscopy(DP-LIBS), the collinear femtosecond double-pulse laser configuration is experimentally investigated with different initial sample temperatures using a Ti:sapphire l...In double-pulse laser-induced breakdown spectroscopy(DP-LIBS), the collinear femtosecond double-pulse laser configuration is experimentally investigated with different initial sample temperatures using a Ti:sapphire laser. The glass sample is ablated to produce the plasma spectroscopy. During the experiment, the detected spectral lines include two Na(I) lines(589.0 nm and 589.6 nm) and one Ca(I) line at the wavelength of 585.7 nm. The emission lines are measured at room temperature(22 ℃) and three higher initial sample temperatures(T_s?=?100 ℃, 200 ℃, and 250 ℃). The inter-pulse delay time ranges from-250 ps to 250 ps.The inter-pulse delay time and the sample temperature strongly influence the spectral intensity,and the spectral intensity can be significantly enhanced by increasing the sample temperature and selecting the optimized inter-pulse time. For the same inter-pulse time of 0 ps(single-pulse LIBS), the enhancement ratio is approximately 2.5 at T_s?=?200 ℃ compared with that obtained at T_s?=?22 ℃. For the same inter-pulse time of 150 ps, the enhancement ratio can be up to 4 at T_s?=?200 ℃ compared with that obtained at T_s?=?22 ℃. The combined enhancement effects of the different initial sample temperatures and the double-pulse configuration in femtosecond LIBS are much stronger than that of the different initial sample temperatures or the double-pulse configuration only.展开更多
This paper reports that DLC (diamond like carbon)/Ti and DLC films were prepared by using pulsed laser arc deposition. R-ray diffraction, Auger electron spectroscopy, Raman spectroscopy, atomic force microscopy, nan...This paper reports that DLC (diamond like carbon)/Ti and DLC films were prepared by using pulsed laser arc deposition. R-ray diffraction, Auger electron spectroscopy, Raman spectroscopy, atomic force microscopy, nanoindenter, spectroscopic ellipsometer, surface profiler and micro-tribometer were employed to study the structure and tribological properties of DLC/Ti and DLC films. The results show that DLC/Ti film, with I(D)/I(G) 0.28 and corresponding to 76% sp3 content calculated by Raman spectroscopy, uniform chemical composition along depth direction, 98 at% content of carbon, hardness 8.2 GPa and Young's modulus 110.5 GPa, compressive stress 6.579 GPa, thickness 46 nm, coefficient of friction 0.08, and critical load 95mN, exhibits excellent mechanical and tribological properties.展开更多
The emission spectra of excited radicals(OH(A^2E),O(3p^3 P),Hα(3P)) and emissive species(N2^+(B^2∑u^+),N2(C3Πu)) produced by positive pulsed high-voltage needle-plane corona discharges in atmospheri...The emission spectra of excited radicals(OH(A^2E),O(3p^3 P),Hα(3P)) and emissive species(N2^+(B^2∑u^+),N2(C3Πu)) produced by positive pulsed high-voltage needle-plane corona discharges in atmospheric N2 and O2 flows wetted with 10%H2O at 80 ℃ are used to investigate the relative concentrations of the produced radicals.The results indicate that the tendencies of the concentrations of radicals with discharge conditions are similar to each other due to their similar excitation processes by electron collision.The influence of oxygen flow mixed with the nitrogen flow on the emission intensities of O(3p^5P → 3s^5S2^0.),Hα(3P → 2S),N2+(B^2∑u^+ → X^2∑g+0-0),and N2(C^3Πu → B^3Πg 1-0) is presented.When the flow rate of oxygen addition is varied from 0-30 ml min^-1,the emission intensities of O(3p^5P → 3s^5S2^0.),Hα(3P → 2s),and N2^+(B^2∑u^+ →X^2∑g 0-0) increase and reach a maximum.Then,if the oxygen flow rate increases further,the emission intensities tend to decrease.However,the intensity of N2(C^3Πu → B^3Πg1-0) decreases monotonously with the increasing oxygen flow,which indicates that the electron density decreases with the increasing oxygen flow.By the tendencies of the relative intensities to N2(C^3Πu → B^3Πg 1-0),the concentrations of the total produced O,H,and N2^+ are shown to increase with the oxygen flow.Based on the reactions for the production of H and O without and with the addition of O2,the analytic solutions for H and O production are derived in accordance with the experimental results.展开更多
Thin films of PrCoO3 were deposited on LaAlO3 substrates by pulsed laser deposition technique.X-ray diffraction result indicates that films are single phase and c-axis textured.To investigate the spin state transition...Thin films of PrCoO3 were deposited on LaAlO3 substrates by pulsed laser deposition technique.X-ray diffraction result indicates that films are single phase and c-axis textured.To investigate the spin state transition,Raman spectroscopy measurements were performed at different temperatures.The position of the Raman modes is found to increase while full width at half maximum(FWHM) of these modes is found to decrease with the decrease of temperature across spin state transition temperature(220 K) of PrCoO3.展开更多
The present work is devoted to electrical and optical study of a point-plane atmospheric pressure corona discharge reactor in humid air powered by pulsed high voltage supply. The corona current and the injected energy...The present work is devoted to electrical and optical study of a point-plane atmospheric pressure corona discharge reactor in humid air powered by pulsed high voltage supply. The corona current and the injected energy are analyzed as a function of several parameters such as applied voltage and humidity rate. Then, investigations based on emission spectroscopy analysis were used in UV range (from 200 nm to about 400 nm). The main observed excited species were the second positive (SPS), the first negative (FNS) systems and OH(A-X) rotational bands. The latter band was used to simulate the rotational temperature (Tr), whereas the N2+ (FNS) band was used to determine the vibrational temperature (Tv). The electron temperature (Te ) is determined from the ratio of line intensities of the spectral bands of both N2+ FNS at 391.4 nm and N2SPS at 394.4 nm. The rotational, vibrational and electronic temperatures are analyzed as a function of above parameters (applied voltage, frequency and hygrometry rate) near the anodic tip. As well we study the axial variation of electronic temperature for a fixed applied voltage at 6.4 kV, frequency at 10 kHz and 100% of humidity. It is found that the rotational, vibrational and electronic temperatures increased with increasing applied voltage, frequency and humidity rate. The increase of rate hygrometry for an inter-electrode distance fixed at 10 mm causes an increase in both the amplitude of the corona current discharge and the energy injected in corona discharge. This is indicative of more intense reactive plasma while increasing hygrometry rate.展开更多
Resonance enhancement has been increasingly employed in the emergent felntosecond stimu- lated Raman spectroscopy (FSRS) to selectively monitor molecular structure and dynamics with improved spectral and temporal re...Resonance enhancement has been increasingly employed in the emergent felntosecond stimu- lated Raman spectroscopy (FSRS) to selectively monitor molecular structure and dynamics with improved spectral and temporal resolutions and signal-to-noise ratios. Such joint eflforts by the technique- and application-oriented scientists and engineers have laid the foundation for exploiting the tunable FSRS methodology to investigate a great variety of photosensitive systems and elucidate the underlying functional mechanisms on molecular time scales. Dur- ing spectral analysis, peak line shapes remain a major concern with an intricate dependence on resonance conditions. Here, we present a comprehensive study of line shapes by tuning the Rarnan pump wavelength from red to blue side of the ground-state absorption band of the fluorescent dye rhodarnine 6G in solution. Distinct line shape patterns in Stokes and anti-Stokes FSRS as well as from the low to high-frequency modes highlight the competition between multiple third-order and higher-order nonlinear pathways, governed by difl^rent res- onance conditions achieved by Raman pump and probe pulses. In particular, the resonance condition of probe wavelength is revealed to play an important role in generating circular line shape changes through oppositely phased dispersion via hot luminescence (HL) pathways. Meanwhile, on-resonance conditions of the Rarnan pump could promote excited-state vibrational modes which are broadened and red-shifted from the coincident ground-state vibrational modes, posing challenges for spectral analysis. Certain strategies in tuning the Raman pump and probe to characteristic regions across an electronic transition band are discussed to improve the FSRS usability and versatility as a powerful structural dynamics toolset to advance chemical, physical, materials, and biological sciences.展开更多
基金supported by the Korea Basic Science Institute(National research Facilities and Equipment Center)grant funded by the Ministry of Education(2019R1A6C1010042,2021R1A6C103A427)the financial support from the National Research Foundation of Korea(NRF)(2022R1A2C2010686,2022R1A4A3033528,2021R1I1A1A01060380,2021R1C1C2010726,2019H1D3A1A01071209)。
文摘The electrocatalytic oxidation of biomass-derived furfural(FF)feedstocks into 2-furoic acid(FA)holds immense industrial potential in optics,cosmetics,polymers,and food.Herein,we fabricated Co O/Ni O/nickel foam(NF)and Cu_(2)O/Ni O/NF electrodes via in situ pulsed laser irradiation in liquids(PLIL)for the bifunctional electrocatalysis of oxygen evolution reaction(OER)and furfural oxidation reaction(FOR),respectively.Simultaneous oxidation of NF surface to NiO and deposition of CoO and/or Cu_(2)O on NF during PLIL offer distinct advantages for enhancing both the OER and FOR.CoO/NiO/NF electrocatalyst provides a consistently low overpotential of~359 m V(OER)at 10 m A/cm^(2),achieving the maximum FA yield(~16.37 m M)with 61.5%selectivity,79.5%carbon balance,and a remarkable Faradaic efficiency of~90.1%during 2 h of FOR at 1.43 V(vs.reversible hydrogen electrode).Mechanistic pathway via in situ electrochemical-Raman spectroscopy on CoO/NiO/NF reveals the involvement of phase transition intermediates(NiOOH and CoOOH)as surface-active centers during electrochemical oxidation.The carbonyl carbon in FF is attacked by hydroxyl groups to form unstable hydrates that subsequently undergo further oxidation to yield FA products.This method holds promise for large-scale applications,enabling simultaneous production of renewable building materials and fuel.
基金National Natural Science Foundation of China for the financial assistance provided under the grant number 11772354.
文摘In order to further improve the propulsion performance of pulsed plasma thrusters for space micro propulsion,a novel laser ablation pulsed plasma thruster is proposed,which separated the laser ablation and electromagnetic acceleration.Optical emission spectroscopy is utilized to investigate the plasma characteristics in the thruster.The spectral lines at different times,positions and discharge intensities are experimentally recorded,and the plasma characteristics in the discharge channel are concluded through analyzing the variation of spectral lines.With the discharge energy of 24 J,laser energy of 0.6 J and the use of aluminum propellant,the specific impulse and thrust efficiency reach 6808 s and 70.6%,respectively.
基金the funding provided by National Natural Science Foundation of China (No.12065019)Natural Science Foundation of the Jiangsu Higher Education Institutions of China (No. 20KJB140025)+1 种基金the Open Fund of the Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province(No. JBGS032)the Scientific Research Project for the Introduction Talent of Yancheng Institute of Technology(Nos. XJR2020031 and XJR2021069)。
文摘Nanosecond pulsed discharges at atmospheric pressure in a pin-to-pin electrode configuration are well reproducible in time and space, which is beneficial to the fundamentals and applications of low-temperature plasmas. In this experiment, the discharges in helium(He) and He with 2.3%water vapor(H_(2)O) are driven by a series of 10 ns overvoltage pulses(~13 k V). Special attention is paid to the spectral characteristics obtained in the center of discharges by time-resolved optical emission spectroscopy. It is found that in helium, the emission of atomic and molecular helium during the afterglow is more intense than that in the active discharge, while in the He+2.3%H_(2)O mixture, helium emission is only observed during the discharge pulse and the molecular helium emission disappears. In addition, the emissions of OH(A-X) and Hα present similar behavior that increases sharply during the falling edge of the voltage pulse as the electrons cool down rapidly. The gas temperature is set to remain low at 540 K by fitting the OH(A-X) band. A comparative study on the emission of radiative species(He, He_(2), OH and H)is performed between these two discharge cases to derive their main production mechanisms. In both cases, the dominant primary ion is He^(+) at the onset of discharges, but their He^(+) charge transfer processes are quite different. Based on these experimental data and a qualitative discussion on the discharge kinetics, with regard to the present discharge conditions, it is shown that the electron-assisted three-body recombination processes appear to be the significant sources of radiative OH and H species in high-density plasmas.
基金supported by a grant from the National Natural Science Foundation of China(Grant No.21790392).
文摘Interactions between the central nervous system(CNS)and autonomic nervous system(ANS)play a crucial role in modulating perception,cognition,and emotion production.Previous studies on CNS–ANS interactions,or heart–brain coupling,have often used heart rate variability(HRV)metrics derived from electrocardiography(ECG)recordings as empirical measurements of sympathetic and parasympathetic activities.Functional near-infrared spectroscopy(fNIRS)is a functional brain imaging modality that is increasingly used in brain and cognition studies.The fNIRS signals contain frequency bands representing both neural activity oscillations and heartbeat rhythms.Therefore,fNIRS data acquired in neuroimaging studies can potentially provide a single-modality approach to measure task-induced responses in the brain and ANS synchronously,allowing analysis of CNS–ANS interactions.In this proof-of-concept study,fNIRS was used to record hemodynamic changes from the foreheads of 20 university students as they each played a round of multiplayer online battle arena(MOBA)game.From the fNIRS recordings,neural and heartbeat frequency bands were extracted to assess prefrontal activities and shortterm pulse rate variability(PRV),an approximation for short-term HRV,respectively.Under the experimental conditions used,fNIRS-derived PRV metrics showed good correlations with ECG-derived HRV golden standards,in terms of absolute measurements and video game playing(VGP)-related changes.It was also observed that,similar to previous studies on physical activity and exercise,the PRV metrics closely related to parasympathetic activities recovered slower than the PRV indicators of sympathetic activities after VGP.It is concluded that it is feasible to use fNIRS to monitor concurrent brain and ANS activations during online VGP,facilitating the understanding of VGP-related heart–brain coupling.
基金supported by National Natural Science Foundation of China(No.61473279)the National High-Tech Research and Development Program of China(863 Program)(No.2012AA040608)Equipment Development Programs of the Chinese Academy of Sciences(No.YZ201247)
文摘In this study, a stand-off and collinear double pulse laser-induced breakdown spectroscopy (DP LIBS) system was designed, and the magnesium alloy samples at a distance of 2.5 m away from the LIBS system were measured. The effect of inter-pulse delay on spectra was studied, and the signal enhancement was observed compared to the single pulse LIBS (SP LIBS). The morphology of the ablated crater on the sample indicated a higher efficiency of surface pretreatment in DP LIBS. The calibration curves of Ytterbium (Y) and Zirconium (Zr) were investigated. The square of the correlation coefficient of the calibration curve of element Y reached up to 0.9998.
基金Supported by the National Basic Research Program of China under Grant No 2012CB921603the Program for Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China under Grant No IRT13076the National Natural Science Foundation of China under Grant Nos 61378049,10934004,11404198,61575116 and 61505100
文摘We experimentally observe the high resolution direct frequency comb spectroscopy using counter-propagating broadband femtosecond pulses on two-photon transitions in room-temperature ^87 Rb atoms. The Doppler broad- ened background is effectively eliminated with the pulse shaping method and the spectrum modulation technique. The combination of the pulse shaping method and the spectra modulation technique provides a potential approachto reduce background of at least 99%.
基金supported by the National Natural Science Foundation of China(Grant No.51806186)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(Grant No.20KJB140025)+1 种基金the Natural Science Foundation of Jiangsu Province,China(Grant No.BK20181050)the Scientific Research Project for the Introduction Talent of Yancheng Institute of Technology(Grant No.XJR2020)。
文摘Atmospheric pressure micro-discharges in helium gas with a mixture of 0.5%water vapor between two pin electrodes are generated with nanosecond overvoltage pulses.The temporal and spatial characteristics of the discharges are investigated by means of time-resolved imaging and optical emission spectroscopy with respect to the discharge morphology,gas temperature,electron density,and excited species.The evolution of micro-discharges is captured by intensified CCD camera and electrical properties.The gas temperature is diagnosed by a two-temperature fit to the ro-vibrational OH(A^(2)Σ^(+)–X^П(2),0–0)emission band and is found to remain low at 425 K during the discharge pulses.The profile of electron density performed by the Stark broadening of Ha 656.1-nm and He I 667.8-nm lines is uniform across the discharge gap at the initial of discharge and reaches as high as 10^(23)m^(-3).The excited species of He,OH,and H show different spatio-temporal behaviors from each other by the measurement of their emission intensities,which are discussed qualitatively in regard of their plasma kinetics.
基金the Foundation Research Project of Jiangsu Province,China(the Natural Science Fund No.BK20190187)。
文摘Laser-induced plasmas of dual-pulse fiber-optic laser-induced breakdown spectroscopy with different pulse energy ratios are studied by using the optical emission spectroscopy(OES)and fast imaging.The energy of the two laser pulses is independently adjusted within 0–30 m J with the total energy fixed at 30 m J.The inter-pulse delay remains 450 ns constantly.As the energy share of the first pulse increases,a similar bimodal variation trend of line intensities is observed.The two peaks are obtained at the point where the first pulse is half or twice of the second one,and the maximum spectral enhancement is at the first peak.The bimodal variation trend is induced by the change in the dominated mechanism of dual-pulse excitation with the trough between the two peaks caused by the weak coupling between the two mechanisms.By increasing the first pulse energy,there is a transition from the ablation enhancement dominance near the first peak to the plasma reheating dominance near the second peak.The calculations of plasma temperature and electron number density are consistent with the bimodal trend,which have the values of 17024.47 K,2.75×10^(17)cm;and 12215.93 K,1.17×10^(17)cm;at a time delay of 550 ns.In addition,the difference between the two peaks decreases with time delay.With the increase in the first pulse energy share,the plasma morphology undergoes a transformation from hemispherical to shiny-dot and to oblate-cylinder structure during the second laser irradiation from the recorded images by using an intensified charge-coupled device(ICCD)camera.Correspondingly,the peak expansion distance of the plasma front first decreases significantly from 1.99 mm in the single-pulse case to 1.34 mm at 12/18(dominated by ablation enhancement)and then increases slightly with increasing the plasma reheating effect.The variations in plasma dynamics verify that the change of pulse energy ratios leads to a transformation in the dual-pulse excitation mechanism.
基金Supported by the Chinese Academy of Sciences under Grant No 2010Y1JB6the National Basic Research Program of China under Grant No 2010CB923000the National Natural Science Foundation of China under Grant Nos 11234014 and 11227903
文摘High-quality superconducting FeSe0.5 Te0.5 films are epitaxiMly grown on different substrates by using the pulsed laser deposition method. By measuring the transport properties and surface morphology of films grown on single- crystal substrates of Al2O3 (0001), SrTiO3 (001), and MgO (001), as well as monitoring the real-time growth process on MgO substrates with reflection high energy electron diffraction, we find the appropriate parameters for epitaxial growth of high-quality FeSe0.5 Te0.5 thin films suitable for angle-resolved photoemission spectroscopy measurements. We further report the angle-resolved photoemission spectroscopy characterization of the super- conducting films. The clearly resolved Fermi surfaces and the band structure suggest a sample quality that is as good as that of high-quality single-crystals, demonstrating that the pulsed laser deposition method can serve as a promising technique for in situ preparation and manipulation of iron-based superconducting thin films, which may bring new prosperity to angle-resolved photoemission spectroscopy research on iron-based superconductors.
基金The authors gratefully acknowledge support by the Deutsche Forschungsgemeinschaft through the Grant Nos.Ho1691/8-1 I Li2713/4-1 | Schm2115/62-1,the Graduate School in Advanced Optical Technologies(SAOT)of the Friedrich-Alexander-Universitat Erlangen-Nurnberg and the QSIL GmbH Quarzschmelze Ilmenau.
文摘This paper focuses on the preparation of a new extended set of calibrations of cooling rate(fictive temperature)in fused silica determined by inelastic light scattering and its subsequent use to characterize the local cooling rate distribution in ultra-short pulsed(USP)laser modification.In order to determine the thermal history(e.g.cooling rate and fictive temperature)of fused silica,high-resolution inelastic light-scattering experiments(Raman and Brillouin spectroscopy)were investigated.Calibrations were performed and compared to the existing literature to quantify structural changes due to a change of fictive temperature.Compared to existing calibrations,this paper provides an extension to lower and higher cooling rates.Using this new set of calibrations,we characterized a USP laser modification in fused silica and calculated the local fictive temperature distribution.An equation relating the fictive temperature(Tf)to cooling rates is given.A maximum cooling rate of 3000 K min-1 in the glass transition region around 1200℃ was deduced from the Raman analysis.The Brillouin observations are sensitive to both the thermal history and the residual stress.By comparing the Raman and Brillouin observations,we extracted the local residual stress distribution with high spatial resolution.For the first time,combined Raman and Brillouin inelastic light scattering experiments show the local distribution of cooling rates and residual stresses(detailed behavior of the glass structure)in the interior and the surrounding of an USP laser modified zone.
基金Project supported by National Nature Science Foundation of China (11035004), Double Hundred Talent Foundation of CAEP (2009R0102), Key Laboratory of Puised Power of CAEP Science and Technology Development Foundation (2008B040237).
文摘Dielectric barrier discharge(DBD) attracts lots of attentions for its great application promises,and the rotational temperature is one of its mostly important parameters.In order to measure the rotational temperature of a pulsed DBD in atmospheric air,the temperature is studied by using optical emission spectroscopy(OES).The discharge is excited by a high voltage pulse with 124 ns rise time and 230 ns full width at half maximum(FWHM) at a repetition rate of a few hundred hertz.The rotational temperatures are studied using different voltages,different repetition rates of the pulse power supply,and different gaps between dielectrics: They are in the range from 390 K to 500 K during the whole discharge.When the gap between dielectrics increases,the rotational temperature initially decreases and then increases.The rotational temperature changes complexly when the pulse repetition rate changes.When the voltage increases,the rotational temperature always decreases,which is not expected.These results allow one to predict the rotational temperature at different supply power parameters and electrode configurations,which is useful for the DBD's industrial application.
基金the University of Tennessee Research Foundation and a grant from the National Natural Science Foundation of China(51575016).
文摘Ultra-short laser pulses possess many advantages for materials processing.Ultrafast laser has a significantly low thermal effect on the areas surrounding the focal point;therefore,it is a promising tool for micro-and submicro-sized precision processing.In addition,the nonlinear multiphoton absorption phenomenon of focused ultra-short pulses provides a promising method for the fabrication of various structures on transparent material,such as glass and transparent polymers.A laser direct writing process was applied in the fabrication of high-performance three-dimensional(3D)structured multilayer microsupercapacitors(MSCs)on polymer substrates exhibiting a peak specific capacitance of 42.6 mF·cm^-2 at a current density of 0.1 mA·cm^-12.Furthermore,a flexible smart sensor array on a polymer substrate was fabricated for multi-flavor detection.Different surface treatments such as gold plating,reducedgraphene oxide(rGO)coating,and polyaniline(PANI)coating were accomplished for different measurement units.By applying principal component analysis(PCA),this sensing system showed a promising result for flavor detection.In addition,two-dimensional(2D)periodic metal nanostructures inside 3D glass microfluidic channels were developed by all-femtosecond-laser processing for real-time surfaceenhanced Raman spectroscopy(SERS).The processing mechanisms included laser ablation,laser reduction,and laser-induced surface nano-engineering.These works demonstrate the attractive potential of ultra-short pulsed laser for surface precision manufacturing.
文摘<div style="text-align:justify;"> In this study, a two-dimensional model describing thermal stress on a charge-coupled device (CCD) induced by ms laser pulses was examined. Considering the nonlinearity of the CCD’s material parameters and the melting phase transition process of aluminum electrode materials was considered by using equivalent specific heat capacity method, the physical process where a laser pulse irradiating a CCD pixel array was simulated using COMSOL Multiphysics software. The temperature field and thermal stress field were calculated and analyzed. In order to clarify the mechanism producing damage on the CCD detector, Raman spectra from silicon were measured with a micro-Raman spectrometer to determine stress change in the CCD chip. The procedure presented herein illustrates a method for evaluating strain in a CCD after laser irradiation. </div>
基金supported by National Natural Science Foundation of China(No.11772354)。
文摘A novel laser-assisted pulsed plasma thruster(LA-PPT)is proposed as an electric propulsion thruster,which separates laser ablation and electromagnetic acceleration.It aims for a higher specific impulse than that achieved with conventional LA-PPTs.Owing to the short-time discharge and the novel configuration,the physical mechanism of the discharge is unclear.Time and spatial-resolved optical emission spectroscopy was applied to investigate the variation in the plasma properties in the thruster discharge channel.The plasma species,electron temperature,and electron density were obtained and discussed.Our investigation revealed that there were H_(α),H_(β),H_(γ),H_(ε) atoms,CⅠ,CⅡ,CⅢ,CⅣ,ClⅠ,ClⅡparticles,and a small amount of CH,C_(3),C_(2),H_(2) neutral molecular groups in the plasma.The electron temperature of the discharge channel of the thruster was within 0.6–4.9 e V,and the electron density was within(1.1–3.0)×10^(18)cm^(-3),which shows that the optical emission spectroscopy method is to measure the electron excitation temperature and electron density in heavy particles.But the Langmuir probe method is to measure the temperature and density of free electrons.The use of laser instead of spark plug as the ignition mode significantly changed the plasma distribution in the discharge channel.Unlike the conventional PPT,which has high electron density near the thruster surface,LAPPT showed relatively large electron density at the thruster outlet,which increased the thruster specific impulse.In addition,the change in the ignition mode enabled the electron density in the LA-PPT discharge channel to be higher than that in the conventional PPT.This proves that the ignition mode with laser replacing the spark plug effectively optimised the PPT performance.
基金support by National Natural Science Foundation of China (Grant Nos. 11674128, 11504129, and 11674124)Jilin Province Scientific and Technological Development Program, China (Grant No. 20170101063JC)Fundamental Research Project of Chinese State Key Laboratory of Laser Interaction with Matter (Grant No. SKLLIM1605)
文摘In double-pulse laser-induced breakdown spectroscopy(DP-LIBS), the collinear femtosecond double-pulse laser configuration is experimentally investigated with different initial sample temperatures using a Ti:sapphire laser. The glass sample is ablated to produce the plasma spectroscopy. During the experiment, the detected spectral lines include two Na(I) lines(589.0 nm and 589.6 nm) and one Ca(I) line at the wavelength of 585.7 nm. The emission lines are measured at room temperature(22 ℃) and three higher initial sample temperatures(T_s?=?100 ℃, 200 ℃, and 250 ℃). The inter-pulse delay time ranges from-250 ps to 250 ps.The inter-pulse delay time and the sample temperature strongly influence the spectral intensity,and the spectral intensity can be significantly enhanced by increasing the sample temperature and selecting the optimized inter-pulse time. For the same inter-pulse time of 0 ps(single-pulse LIBS), the enhancement ratio is approximately 2.5 at T_s?=?200 ℃ compared with that obtained at T_s?=?22 ℃. For the same inter-pulse time of 150 ps, the enhancement ratio can be up to 4 at T_s?=?200 ℃ compared with that obtained at T_s?=?22 ℃. The combined enhancement effects of the different initial sample temperatures and the double-pulse configuration in femtosecond LIBS are much stronger than that of the different initial sample temperatures or the double-pulse configuration only.
基金Project supported by the National Key Basic Research Program of China (Grant No 2003CB716201) and the National Natural Science Foundation of China (Grant No 50575121) and Electro-Mechmaic Technology Advancing Foundation of NSK Ltd of Japan.
文摘This paper reports that DLC (diamond like carbon)/Ti and DLC films were prepared by using pulsed laser arc deposition. R-ray diffraction, Auger electron spectroscopy, Raman spectroscopy, atomic force microscopy, nanoindenter, spectroscopic ellipsometer, surface profiler and micro-tribometer were employed to study the structure and tribological properties of DLC/Ti and DLC films. The results show that DLC/Ti film, with I(D)/I(G) 0.28 and corresponding to 76% sp3 content calculated by Raman spectroscopy, uniform chemical composition along depth direction, 98 at% content of carbon, hardness 8.2 GPa and Young's modulus 110.5 GPa, compressive stress 6.579 GPa, thickness 46 nm, coefficient of friction 0.08, and critical load 95mN, exhibits excellent mechanical and tribological properties.
基金supported by National Natural Science Foundation of China under Grant No.513377014
文摘The emission spectra of excited radicals(OH(A^2E),O(3p^3 P),Hα(3P)) and emissive species(N2^+(B^2∑u^+),N2(C3Πu)) produced by positive pulsed high-voltage needle-plane corona discharges in atmospheric N2 and O2 flows wetted with 10%H2O at 80 ℃ are used to investigate the relative concentrations of the produced radicals.The results indicate that the tendencies of the concentrations of radicals with discharge conditions are similar to each other due to their similar excitation processes by electron collision.The influence of oxygen flow mixed with the nitrogen flow on the emission intensities of O(3p^5P → 3s^5S2^0.),Hα(3P → 2S),N2+(B^2∑u^+ → X^2∑g+0-0),and N2(C^3Πu → B^3Πg 1-0) is presented.When the flow rate of oxygen addition is varied from 0-30 ml min^-1,the emission intensities of O(3p^5P → 3s^5S2^0.),Hα(3P → 2s),and N2^+(B^2∑u^+ →X^2∑g 0-0) increase and reach a maximum.Then,if the oxygen flow rate increases further,the emission intensities tend to decrease.However,the intensity of N2(C^3Πu → B^3Πg1-0) decreases monotonously with the increasing oxygen flow,which indicates that the electron density decreases with the increasing oxygen flow.By the tendencies of the relative intensities to N2(C^3Πu → B^3Πg 1-0),the concentrations of the total produced O,H,and N2^+ are shown to increase with the oxygen flow.Based on the reactions for the production of H and O without and with the addition of O2,the analytic solutions for H and O production are derived in accordance with the experimental results.
基金Project supported by the Second Stage of Brain Korea 21 Project
文摘Thin films of PrCoO3 were deposited on LaAlO3 substrates by pulsed laser deposition technique.X-ray diffraction result indicates that films are single phase and c-axis textured.To investigate the spin state transition,Raman spectroscopy measurements were performed at different temperatures.The position of the Raman modes is found to increase while full width at half maximum(FWHM) of these modes is found to decrease with the decrease of temperature across spin state transition temperature(220 K) of PrCoO3.
文摘The present work is devoted to electrical and optical study of a point-plane atmospheric pressure corona discharge reactor in humid air powered by pulsed high voltage supply. The corona current and the injected energy are analyzed as a function of several parameters such as applied voltage and humidity rate. Then, investigations based on emission spectroscopy analysis were used in UV range (from 200 nm to about 400 nm). The main observed excited species were the second positive (SPS), the first negative (FNS) systems and OH(A-X) rotational bands. The latter band was used to simulate the rotational temperature (Tr), whereas the N2+ (FNS) band was used to determine the vibrational temperature (Tv). The electron temperature (Te ) is determined from the ratio of line intensities of the spectral bands of both N2+ FNS at 391.4 nm and N2SPS at 394.4 nm. The rotational, vibrational and electronic temperatures are analyzed as a function of above parameters (applied voltage, frequency and hygrometry rate) near the anodic tip. As well we study the axial variation of electronic temperature for a fixed applied voltage at 6.4 kV, frequency at 10 kHz and 100% of humidity. It is found that the rotational, vibrational and electronic temperatures increased with increasing applied voltage, frequency and humidity rate. The increase of rate hygrometry for an inter-electrode distance fixed at 10 mm causes an increase in both the amplitude of the corona current discharge and the energy injected in corona discharge. This is indicative of more intense reactive plasma while increasing hygrometry rate.
基金supported by the U.S.National Science Foundation CAREER grant(CHE-1455353)the Oregon State University(OSU) Research Equipment Reserve Fund(Spring 2014)to C.Fang(USTC9603)the Wei Family Private Foundation in supporting C.Chen(USTC 0903) during his graduate studies at OSU Chemistry
文摘Resonance enhancement has been increasingly employed in the emergent felntosecond stimu- lated Raman spectroscopy (FSRS) to selectively monitor molecular structure and dynamics with improved spectral and temporal resolutions and signal-to-noise ratios. Such joint eflforts by the technique- and application-oriented scientists and engineers have laid the foundation for exploiting the tunable FSRS methodology to investigate a great variety of photosensitive systems and elucidate the underlying functional mechanisms on molecular time scales. Dur- ing spectral analysis, peak line shapes remain a major concern with an intricate dependence on resonance conditions. Here, we present a comprehensive study of line shapes by tuning the Rarnan pump wavelength from red to blue side of the ground-state absorption band of the fluorescent dye rhodarnine 6G in solution. Distinct line shape patterns in Stokes and anti-Stokes FSRS as well as from the low to high-frequency modes highlight the competition between multiple third-order and higher-order nonlinear pathways, governed by difl^rent res- onance conditions achieved by Raman pump and probe pulses. In particular, the resonance condition of probe wavelength is revealed to play an important role in generating circular line shape changes through oppositely phased dispersion via hot luminescence (HL) pathways. Meanwhile, on-resonance conditions of the Rarnan pump could promote excited-state vibrational modes which are broadened and red-shifted from the coincident ground-state vibrational modes, posing challenges for spectral analysis. Certain strategies in tuning the Raman pump and probe to characteristic regions across an electronic transition band are discussed to improve the FSRS usability and versatility as a powerful structural dynamics toolset to advance chemical, physical, materials, and biological sciences.