Characterization of real-time and ultrafast motions of the complex molecules at surface and interface is critical to understand how interracial molecules function. It requires to develop surface-sensitive, fast-identi...Characterization of real-time and ultrafast motions of the complex molecules at surface and interface is critical to understand how interracial molecules function. It requires to develop surface-sensitive, fast-identification, and time-resolved techniques. In this study, we employ several key technical procedures and successfully develop a highly sensitive femtosecond time-resolved sum frequency generation vibrational spectroscopy （SFG-VS） system. This system is able to measure the spectra with two polarization combinations （ssp and ppp, or psp and ssp） simultaneously. It takes less than several seconds to collect one spectrum. To the best of our knowledge, it is the fastest speed of collecting SFG spectra reported by now. Using the time-resolved measurement, ultrafast vibrational dynamics of the N-H mode of α-helical peptide at water interface is determined. It is found that the membrane environment does not affect the N-H vibrational relaxation dynamics. It is expected that the time-resolved SFG system will play a vital role in the deep understanding of the dynamics and interaction of the complex molecules at surface and interface. Our method may also provide an important technical proposal for the people who plan to develop time-resolved SFG systems with simultaneous measurement of multiple polarization combinations.展开更多
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 ob...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.展开更多
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)...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.展开更多
The photodissociation dynamics of 2-iodotoluene following excitation at 266 nm have been investigated employing femtosecond time-resolved mass spectrometry. The photofragments are detected by multiphoton ionization us...The photodissociation dynamics of 2-iodotoluene following excitation at 266 nm have been investigated employing femtosecond time-resolved mass spectrometry. The photofragments are detected by multiphoton ionization using an intense laser field centered at 800 nm. A dissociation time of 3804-50 fs was measured from the rising time of the co-fragments of toluene radical （C7H7） and iodine atom （I）, which is attributed to the averaged time needed for the C-I bond breaking for the simultaneously excited nσ and ππ＊ states by 266 nm pump light. In addition, a probe light centered at 298.23 nm corresponding to resonance wavelength of ground-state iodine atom is used to selectively ionize ground-state iodine atoms generated from the dissociation of initially populated hσ＊ and ππ＊ states. And a rise time of 4004-50 fs is extracted from the fitting of time-dependent I＋ transient, which is in agreement with the dissociation time obtained by multiphoton ionization with 800 nm, suggesting that the main dissociative products are ground-state iodine atoms.展开更多
The femtosecond time-resolved difference absorption spectra of all-trans-β-Apo-8′-carotenal have been recorded and analyzed by the singular-value decomposition (SVD) method followed by global fitting using a sequent...The femtosecond time-resolved difference absorption spectra of all-trans-β-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-β-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.展开更多
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 l...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.展开更多
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 mater...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.展开更多
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： sapphi...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.展开更多
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 sp...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.展开更多
We demonstrate that the femtosecond time-resolved magneto-optical Kerr rotation oscillates with the direction of polarization of the probe beam when a sample of Al0.25Ga0.75As/GaAs multi-quantum wells is excited by a ...We demonstrate that the femtosecond time-resolved magneto-optical Kerr rotation oscillates with the direction of polarization of the probe beam when a sample of Al0.25Ga0.75As/GaAs multi-quantum wells is excited by a circularly polarized pump and detected by a linearly polarized probe at wavelengths from 800 to 830 nm. Analytical expressions are derived to explain the mechanism, which is in good agreement with the numerical computation and the experimental data. The results suggest that the Kerr signal can be enhanced by choosing an optimal direction of polarization, which is of benefit to the measurement of the weak Kerr rotation.展开更多
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 con...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.展开更多
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-...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 duiing 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.展开更多
We performed a quantitative analysis of time-resolved laser-induced breakdown air plasma spectra to obtain the evolution of temperatures and species relative fractions.The air plasma was generated by focusing a 100 mJ...We performed a quantitative analysis of time-resolved laser-induced breakdown air plasma spectra to obtain the evolution of temperatures and species relative fractions.The air plasma was generated by focusing a 100 mJ Nd:YAG laser pulse,and the time-resolved spectra were recorded by an intensified charge-coupled device camera with incremental delay.The attention was mainly focused on the emission spectra of the first negative system of nitrogen(N_(2)^(+),B^(2)Σ-(u)^(-)-X^(2)Σ^(+)g)and the violet system of carbon nitride(CN,B^(2)Σ^(+)-X^(2)Σ^(+))located at 383-396 nm.A custom-built model was developed to perform the simulation and fitting of the N_(2)^(+)and the CN spectra from the air plasma.The model was verified by comparing to a published model with a 0.9860 Spearman correlation coefficient.With this model,the time-resolved non-equilibrium temperatures and relative fractions of N_(2)^(+)and CN were obtained with a fitting correlation coefficient higher than 0.9108.展开更多
Photoswitchable fluorescent polymeric nanoparticles were widely concerned because of their excellent features including the flexible design,easy preparation and functionalization,and thus exhibited great application p...Photoswitchable fluorescent polymeric nanoparticles were widely concerned because of their excellent features including the flexible design,easy preparation and functionalization,and thus exhibited great application potential in information encryption,anti-counterfeiting,but remained challenging in improving the security.Herein,we described a self-erased time-resolved information encryption via using photoswitchable dual-color fluorescent polymeric nanoparticles(PDFPNs)containing two fluorescence dyes(blue and red)and photochromic spiroxazine derivatives.In view of the different thermo-induced isomerization rates of photochromic spiroxazine derivatives in different flexible substrates,the decoloration rate of PDFPNs can be programmatically tuned by regulating ratio between rigid polymer and flexible polymer.Therefore,after ultraviolet light(UV)irradiation,correct information could only be recognized in preestablished time during the self-erased process.Our results indicated that PDFPNs exhibited fast photo-responsibility(2 min),high fluorescence contrast,well-pleasing photo-reversibility(>20 times),and programmable thermo-responsiveness(24 s-6 h).We thus demonstrated their application in the selferased time-resolved information encryption and anti-counterfeiting with high security.展开更多
Quantum materials have attracted a great deal of attention because of their rich landscape of electronic structures,topological phases,strong correlation effects,and exotic orders.These systems provide a fertile platf...Quantum materials have attracted a great deal of attention because of their rich landscape of electronic structures,topological phases,strong correlation effects,and exotic orders.These systems provide a fertile platform for the exploration of novel quantum phenomena and materials applications.Particularly exciting is the exploration of nonequilibrium dynamics in quantum materials,which has significant research and potential application values.Pump-probe techniques play a key role in revealing the dynamics of quantum materials on remarkably short timescales,providing an attractive yet challenging avenue of research.In this context,time-resolved x-ray as an emerging probe exhibits high time resolution,momentum resolution,and substantial momentum coverage.It can reveal unprecedented transient states,distinguish between entangled ordered states,and has a compelling potential to probe ultrafast dynamics in a wide variety of quantum materials.Despite its unique advantages,time-resolved x-ray scattering still faces several technological and methodological challenges.In this review,we highlight recent advances focusing on the use of time-resolved x-ray scattering to probe dynamic processes in quantum materials.We discuss representative examples across structural,electronic,magnetic,and lattice degrees of freedom,and outline promising directions for future research in this rapidly evolving field.展开更多
Time-resolved flow cytometry(TRFC)was used to measure metabolic differences in estrogen receptor-positive breast cancer cells.This specialty cytometry technique measures fluorescence lifetimes as a single-cell paramet...Time-resolved flow cytometry(TRFC)was used to measure metabolic differences in estrogen receptor-positive breast cancer cells.This specialty cytometry technique measures fluorescence lifetimes as a single-cell parameter thereby providing a unique approach for high-throughput cell counting and screening.Differences in fluorescence lifetime were detected and this was associated with sensitivity to the commonly prescribed therapeutic tamoxifen.Differences in fluorescence lifetime are attributed to the binding states of the autofluorescent metabolite NAD(P)H.The function of NAD(P)H is well described and in general involves cycling from a reduced to oxidized state to facilitate electron transport for the conversion of pyruvate to lactate.NAD(P)H fluorescence lifetimes depend on the bound or unbound state of the metabolite,which also relates to metabolic transitions between oxidative phosphorylation and glycolysis.To determine if fundamental metabolic profiles differ for cells that are sensitive to tamoxifen compared to those that are resistant,large populations of MCF-7 breast cancer cells were screened and fluorescence lifetimes were quantified.Additionally,metabolic differences associated with tamoxifen sensitivity were measured with a Seahorse HS mini metabolic analyzer(Agilent Technologies Inc.Santa Clara,CA)and confocal imaging.Results show that tamoxifen-resistant breast cancer cells have increased utilization of glycolysis for energy production compared to tamoxifen-sensitive breast cancer cells.This work is impacting because it establishes an early step toward developing a reliable screening technology in which large cell censuses can be differentiated for drug sensitivity in a label-free fashion.展开更多
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 ...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.展开更多
Junctions are an important structure that allows charge separation in solar cells and photocatalysts. Here, we studied the charge transfer at an anatase/rutile TiO2 phase junction using time-resolved photoluminescence...Junctions are an important structure that allows charge separation in solar cells and photocatalysts. Here, we studied the charge transfer at an anatase/rutile TiO2 phase junction using time-resolved photoluminescence spectroscopy. Visible （-S00 nm） and near-infrared （NIR, -830 nm） emissions were monitored to give insight into the photoinduced charges of anatase and rutile in the junction, respectively, New fast photoluminescence decay components appeared in the visible emission of futile-phase dominated TiO2 and in the NIR emission of many mixed phase TiO2samples. The fast decays confirmed that the charge separation occurred at the phase junction. The visible emission intensity from the mixed phase TiO2 increased, revealing that charge transfer from rutile to anatase was the main pathway. The charge separation slowed the microsecond time scale photolumines- cence decay rate for charge carriers in both anatase and rutile. However, the millisecond decay of the charge carriers in anatase TiO2 was accelerated, while there was almost no change in the charge carrier dynamics of rutile TiO2. Thus, charge separation at the anatase/rutile phase junction caused an increase in the charge carrier concentration on a microsecond time scale, because of slower electron-hole recombination. The enhanced photocatalytic activity previously observed at ana- tase/rutile phase junctions is likely caused by the improved charge carrier dynamics we report here. These findings may contribute to the development of improved photocatalytic materials.展开更多
The ultrafast dynamics through conical intersections in 2,6-dimethylpyridine has been studied by femtosecond time-resolved photoelectron imaging coupled with time-resolved mass spectroscopy. Upon absorption of 266 nm ...The ultrafast dynamics through conical intersections in 2,6-dimethylpyridine has been studied by femtosecond time-resolved photoelectron imaging coupled with time-resolved mass spectroscopy. Upon absorption of 266 nm pump laser, 2,6-dimethylpyridine is excited to the S2 state with a ππ character from So state. The time evolution of the parent ion signals consists of two exponential decays. One is a fast component on a timescale of 635 fs and the other is a slow component with a timescale of 4.37 ps. Time-dependent photo- electron angular distributions and energy-resolved photoelectron spectroscopy are extracted from time-resolved photoelectron imaging and provide the evolutive information of S2 state. In brief, the ultrafast component is a population transfer from S2 to S1 through the S2/S1 conical intersections, the slow component is attributed to simultaneous IC from the S2 state and the higher vibrational levels of S1 state to So state, which involves the coupling of S2/S0 and S1/So conical intersections. Additionally, the observed ultrafast S2--＋S1 transition occurs only with an 18% branching ratio.展开更多
We report on the theoretical and the experimental investigations of the coherent phonon dynamics in sapphire crystal using the femtosecond time-resolved coherent anti-Stokes Raman scattering （fs-CARS） technique. The...We report on the theoretical and the experimental investigations of the coherent phonon dynamics in sapphire crystal using the femtosecond time-resolved coherent anti-Stokes Raman scattering （fs-CARS） technique. The temporal chirped white-light continuum （WLC） is used for the Stokes pulse, therefore we can perform the selective excitation of the phonon modes without using a complicated laser system. The expected quantum beat phenomenon is clearly observed. The theoretical formulas consist very well with the experimental results. The dephasing times of the excited phonon modes, the wavenumber difference, and the phase shift between the simultaneously excited modes are obtained and discussed. This work opens up a way to study directly high-frequency coherent phonon dynamics in bulk crystals on a femtosecond time scale and is especially helpful for understanding the nature of coherent phonons.展开更多
文摘Characterization of real-time and ultrafast motions of the complex molecules at surface and interface is critical to understand how interracial molecules function. It requires to develop surface-sensitive, fast-identification, and time-resolved techniques. In this study, we employ several key technical procedures and successfully develop a highly sensitive femtosecond time-resolved sum frequency generation vibrational spectroscopy （SFG-VS） system. This system is able to measure the spectra with two polarization combinations （ssp and ppp, or psp and ssp） simultaneously. It takes less than several seconds to collect one spectrum. To the best of our knowledge, it is the fastest speed of collecting SFG spectra reported by now. Using the time-resolved measurement, ultrafast vibrational dynamics of the N-H mode of α-helical peptide at water interface is determined. It is found that the membrane environment does not affect the N-H vibrational relaxation dynamics. It is expected that the time-resolved SFG system will play a vital role in the deep understanding of the dynamics and interaction of the complex molecules at surface and interface. Our method may also provide an important technical proposal for the people who plan to develop time-resolved SFG systems with simultaneous measurement of multiple polarization combinations.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 20573028 and 20973050)
文摘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.
基金This work was supported by the National Natural Science Foundation of China(No.21833003 and No.21773213)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB17000000)Chinese Academy of Sciences(GJJSTD20190002).
文摘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.
基金This work was supported by the National Basic Research Program of China （973 Program） （No.2013CB922200） and the National Natural Science Foundation of China （No.91121006, No.21273274, No.21173256, and No.21303255）.
文摘The photodissociation dynamics of 2-iodotoluene following excitation at 266 nm have been investigated employing femtosecond time-resolved mass spectrometry. The photofragments are detected by multiphoton ionization using an intense laser field centered at 800 nm. A dissociation time of 3804-50 fs was measured from the rising time of the co-fragments of toluene radical （C7H7） and iodine atom （I）, which is attributed to the averaged time needed for the C-I bond breaking for the simultaneously excited nσ and ππ＊ states by 266 nm pump light. In addition, a probe light centered at 298.23 nm corresponding to resonance wavelength of ground-state iodine atom is used to selectively ionize ground-state iodine atoms generated from the dissociation of initially populated hσ＊ and ππ＊ states. And a rise time of 4004-50 fs is extracted from the fitting of time-dependent I＋ transient, which is in agreement with the dissociation time obtained by multiphoton ionization with 800 nm, suggesting that the main dissociative products are ground-state iodine atoms.
文摘The femtosecond time-resolved difference absorption spectra of all-trans-β-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-β-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.
基金supported by the National Natural Science Foundation of China (Grant No.10704083)
文摘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.
基金Project supported by the Science and Technology Development Fund Planning Project for the Universities of Tianjin,China(Grant No.20140902)the Natural Science Foundation of Tianjin City,China(Grant No.16JCQNJC01900)+1 种基金the National Natural Science Foundation of China(Grant Nos.51376136and 61474082)the Science and Technology Achievement Award Project for the Universities of Tianjin,China
文摘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.
基金supported by the Russian Science Foundation(agreement#14-50-00034)(measurements of limit of detection)Russian Foundation for Basic Research(NK 15-32-20878/15)obtained in the frame of "Organization of Scientific Research"in the Far Eastern Federal University supported by Ministry of Education and Science of Russian Federation
文摘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.
基金National Natural Science Foundation of China (Nos. 11674128, and 11674124)Jilin Province Scientific and Technological Development Program, China (No. 20170101063JC).
文摘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.
基金supported by the National Natural Science Foundation of China (Grant Nos. 10821062 and 11074013)
文摘We demonstrate that the femtosecond time-resolved magneto-optical Kerr rotation oscillates with the direction of polarization of the probe beam when a sample of Al0.25Ga0.75As/GaAs multi-quantum wells is excited by a circularly polarized pump and detected by a linearly polarized probe at wavelengths from 800 to 830 nm. Analytical expressions are derived to explain the mechanism, which is in good agreement with the numerical computation and the experimental data. The results suggest that the Kerr signal can be enhanced by choosing an optimal direction of polarization, which is of benefit to the measurement of the weak Kerr rotation.
基金support of National Natural Science Foundation of China(Nos.11674128,11674124 and 11974138)the Scientific and Technological Research Project of the Education Department of Jilin Province,China(No.JJKH20200937KJ)。
文摘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.
基金supported by the National Natural Science Foundation of China (Grant No. 61008023)the Program of Excellent at Harbin Institute of Technology
文摘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 duiing 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.
基金Project supported by the National Natural Science Foundation of China(Grant No.62305087)。
文摘We performed a quantitative analysis of time-resolved laser-induced breakdown air plasma spectra to obtain the evolution of temperatures and species relative fractions.The air plasma was generated by focusing a 100 mJ Nd:YAG laser pulse,and the time-resolved spectra were recorded by an intensified charge-coupled device camera with incremental delay.The attention was mainly focused on the emission spectra of the first negative system of nitrogen(N_(2)^(+),B^(2)Σ-(u)^(-)-X^(2)Σ^(+)g)and the violet system of carbon nitride(CN,B^(2)Σ^(+)-X^(2)Σ^(+))located at 383-396 nm.A custom-built model was developed to perform the simulation and fitting of the N_(2)^(+)and the CN spectra from the air plasma.The model was verified by comparing to a published model with a 0.9860 Spearman correlation coefficient.With this model,the time-resolved non-equilibrium temperatures and relative fractions of N_(2)^(+)and CN were obtained with a fitting correlation coefficient higher than 0.9108.
基金financially supported by the National Key R&D Program of China(Nos.2023YFB3812400,2023YFB3812403)National Natural Foundation of China(Nos.52273206,52350233)+1 种基金Hunan Provincial Natural Science Foundation(No.2021JJ10029)Huxiang High-level Talent Gathering Project(No.2022RC4039).
文摘Photoswitchable fluorescent polymeric nanoparticles were widely concerned because of their excellent features including the flexible design,easy preparation and functionalization,and thus exhibited great application potential in information encryption,anti-counterfeiting,but remained challenging in improving the security.Herein,we described a self-erased time-resolved information encryption via using photoswitchable dual-color fluorescent polymeric nanoparticles(PDFPNs)containing two fluorescence dyes(blue and red)and photochromic spiroxazine derivatives.In view of the different thermo-induced isomerization rates of photochromic spiroxazine derivatives in different flexible substrates,the decoloration rate of PDFPNs can be programmatically tuned by regulating ratio between rigid polymer and flexible polymer.Therefore,after ultraviolet light(UV)irradiation,correct information could only be recognized in preestablished time during the self-erased process.Our results indicated that PDFPNs exhibited fast photo-responsibility(2 min),high fluorescence contrast,well-pleasing photo-reversibility(>20 times),and programmable thermo-responsiveness(24 s-6 h).We thus demonstrated their application in the selferased time-resolved information encryption and anti-counterfeiting with high security.
基金the National Key R&D Program of China(Grants Nos.2024YFA1408702 and 2021YFA1401903)Beijing Natural Science Foundation(Grant No.JQ24001)the National Natural Science Foundation of China(Grant No.12374143)。
文摘Quantum materials have attracted a great deal of attention because of their rich landscape of electronic structures,topological phases,strong correlation effects,and exotic orders.These systems provide a fertile platform for the exploration of novel quantum phenomena and materials applications.Particularly exciting is the exploration of nonequilibrium dynamics in quantum materials,which has significant research and potential application values.Pump-probe techniques play a key role in revealing the dynamics of quantum materials on remarkably short timescales,providing an attractive yet challenging avenue of research.In this context,time-resolved x-ray as an emerging probe exhibits high time resolution,momentum resolution,and substantial momentum coverage.It can reveal unprecedented transient states,distinguish between entangled ordered states,and has a compelling potential to probe ultrafast dynamics in a wide variety of quantum materials.Despite its unique advantages,time-resolved x-ray scattering still faces several technological and methodological challenges.In this review,we highlight recent advances focusing on the use of time-resolved x-ray scattering to probe dynamic processes in quantum materials.We discuss representative examples across structural,electronic,magnetic,and lattice degrees of freedom,and outline promising directions for future research in this rapidly evolving field.
基金the National Institute of Health for supporting this research under grants NIH R35GM152076,NIH 1SC1GM127175-01,NIH T32GM148394.
文摘Time-resolved flow cytometry(TRFC)was used to measure metabolic differences in estrogen receptor-positive breast cancer cells.This specialty cytometry technique measures fluorescence lifetimes as a single-cell parameter thereby providing a unique approach for high-throughput cell counting and screening.Differences in fluorescence lifetime were detected and this was associated with sensitivity to the commonly prescribed therapeutic tamoxifen.Differences in fluorescence lifetime are attributed to the binding states of the autofluorescent metabolite NAD(P)H.The function of NAD(P)H is well described and in general involves cycling from a reduced to oxidized state to facilitate electron transport for the conversion of pyruvate to lactate.NAD(P)H fluorescence lifetimes depend on the bound or unbound state of the metabolite,which also relates to metabolic transitions between oxidative phosphorylation and glycolysis.To determine if fundamental metabolic profiles differ for cells that are sensitive to tamoxifen compared to those that are resistant,large populations of MCF-7 breast cancer cells were screened and fluorescence lifetimes were quantified.Additionally,metabolic differences associated with tamoxifen sensitivity were measured with a Seahorse HS mini metabolic analyzer(Agilent Technologies Inc.Santa Clara,CA)and confocal imaging.Results show that tamoxifen-resistant breast cancer cells have increased utilization of glycolysis for energy production compared to tamoxifen-sensitive breast cancer cells.This work is impacting because it establishes an early step toward developing a reliable screening technology in which large cell censuses can be differentiated for drug sensitivity in a label-free fashion.
基金Project supported by the National Natural Science Foundation of China(Grant No.51705009)the NSAF of China(Grant No.U1530153)
文摘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.
基金supported by the National Natural Science Foundation of China (21203185, 21373209)the National Basic Research Program of China (2014CB239400)
文摘Junctions are an important structure that allows charge separation in solar cells and photocatalysts. Here, we studied the charge transfer at an anatase/rutile TiO2 phase junction using time-resolved photoluminescence spectroscopy. Visible （-S00 nm） and near-infrared （NIR, -830 nm） emissions were monitored to give insight into the photoinduced charges of anatase and rutile in the junction, respectively, New fast photoluminescence decay components appeared in the visible emission of futile-phase dominated TiO2 and in the NIR emission of many mixed phase TiO2samples. The fast decays confirmed that the charge separation occurred at the phase junction. The visible emission intensity from the mixed phase TiO2 increased, revealing that charge transfer from rutile to anatase was the main pathway. The charge separation slowed the microsecond time scale photolumines- cence decay rate for charge carriers in both anatase and rutile. However, the millisecond decay of the charge carriers in anatase TiO2 was accelerated, while there was almost no change in the charge carrier dynamics of rutile TiO2. Thus, charge separation at the anatase/rutile phase junction caused an increase in the charge carrier concentration on a microsecond time scale, because of slower electron-hole recombination. The enhanced photocatalytic activity previously observed at ana- tase/rutile phase junctions is likely caused by the improved charge carrier dynamics we report here. These findings may contribute to the development of improved photocatalytic materials.
基金This work was supported by the National Natural Science Foundation of China （No.10704083）,the Innovation Foundation of Chinese Academyof Sciences （No.KJCX1-YW-N30）, and the Public Science and Technology Program of Shenzhen （No.SY200806260026A）.
文摘The ultrafast dynamics through conical intersections in 2,6-dimethylpyridine has been studied by femtosecond time-resolved photoelectron imaging coupled with time-resolved mass spectroscopy. Upon absorption of 266 nm pump laser, 2,6-dimethylpyridine is excited to the S2 state with a ππ character from So state. The time evolution of the parent ion signals consists of two exponential decays. One is a fast component on a timescale of 635 fs and the other is a slow component with a timescale of 4.37 ps. Time-dependent photo- electron angular distributions and energy-resolved photoelectron spectroscopy are extracted from time-resolved photoelectron imaging and provide the evolutive information of S2 state. In brief, the ultrafast component is a population transfer from S2 to S1 through the S2/S1 conical intersections, the slow component is attributed to simultaneous IC from the S2 state and the higher vibrational levels of S1 state to So state, which involves the coupling of S2/S0 and S1/So conical intersections. Additionally, the observed ultrafast S2--＋S1 transition occurs only with an 18% branching ratio.
基金supported by the National Natural Science Foundation of China (Grant No. 20973050)
文摘We report on the theoretical and the experimental investigations of the coherent phonon dynamics in sapphire crystal using the femtosecond time-resolved coherent anti-Stokes Raman scattering （fs-CARS） technique. The temporal chirped white-light continuum （WLC） is used for the Stokes pulse, therefore we can perform the selective excitation of the phonon modes without using a complicated laser system. The expected quantum beat phenomenon is clearly observed. The theoretical formulas consist very well with the experimental results. The dephasing times of the excited phonon modes, the wavenumber difference, and the phase shift between the simultaneously excited modes are obtained and discussed. This work opens up a way to study directly high-frequency coherent phonon dynamics in bulk crystals on a femtosecond time scale and is especially helpful for understanding the nature of coherent phonons.
