The intrinsic chirp of high-order harmonic generation is an important factor limiting the production of ultrashort attosecond pulses.Based on numerically solving the time-dependent Schrodinger equation,the generation ...The intrinsic chirp of high-order harmonic generation is an important factor limiting the production of ultrashort attosecond pulses.Based on numerically solving the time-dependent Schrodinger equation,the generation process of highorder harmonic from the He atom under the action of orthogonal two-color combined pulse of fundamental frequency and higher intensity second harmonic fields is studied.In this paper,we propose to achieve quasi-chirp-free isolated attosecond pulses by superimposing a higher second-harmonic field on the orthogonal direction of the fundamental frequency field.It is found that the high-energy part of its harmonic emission exhibits small chirp characteristics,which can be used to synthesize isolated attosecond pulses.Through the analysis of the wave packets evolution and the classical motion trajectories of the electron,it is demonstrated that the quasi-chirp-free harmonic can be attributed to the simultaneous return of electrons ionized at different times to the parent particle.The influence of the relative phase of the two pulses on the harmonics is further analyzed,and it is observed that this phenomenon is sensitive to the relative phase,but it can still generate isolated attosecond pulses within a certain phase.展开更多
We conduct an experimental study supported by theoretical analysis of single laser ablating copper to investigate the interactions between laser and material at different sample temperatures,and predict the changes of...We conduct an experimental study supported by theoretical analysis of single laser ablating copper to investigate the interactions between laser and material at different sample temperatures,and predict the changes of ablation morphology and lattice temperature.For investigating the effect of sample temperature on femtosecond laser processing,we conduct experiments on and simulate the thermal behavior of femtosecond laser irradiating copper by using a two-temperature model.The simulation results show that both electron peak temperature and the relaxation time needed to reach equilibrium increase as initial sample temperature rises.When the sample temperature rises from 300 K to 600 K,the maximum lattice temperature of the copper surface increases by about 6500 K under femtosecond laser irradiation,and the ablation depth increases by 20%.The simulated ablation depths follow the same general trend as the experimental values.This work provides some theoretical basis and technical support for developing femtosecond laser processing in the field of metal materials.展开更多
The double ionization process of molecules driven by co-rotating two-color circularly polarized fields is investigated with a three-dimensional classical ensemble model. Numerical results indicate that a considerable ...The double ionization process of molecules driven by co-rotating two-color circularly polarized fields is investigated with a three-dimensional classical ensemble model. Numerical results indicate that a considerable part of the sequential double ionization(DI) events of molecules occur through internal collision double ionization(ICD), and the ICD recollision mechanism is significantly different from that in non-sequential double ionization(NSDI). By analyzing the results of internuclear distances R = 5 a.u. and 2 a.u., these two recollision mechanisms are studied in depth. It is found that the dynamic behaviors of the recollision mechanisms of NSDI and ICD are similar. For NSDI, the motion range of electrons after the ionization is relatively large, and the electrons will return to the core after a period of time. In the ICD process,electrons will rotate around the parent ion before ionization, and the distance of the electron motion is relatively small. After a period of time, the electrons will come back to the core and collide with another electron. Furthermore, the molecular internuclear distance has a significant effect on the electron dynamic behavior of the two ionization mechanisms. This study will help to understand the multi-electron ionization process of complex systems.展开更多
We delve into the phenomenon of high-order harmonic generation within a helium atom under the influence of a plasmon-assisted shaping pulse.Our findings reveal an intriguing manipulation of the frequency peak position...We delve into the phenomenon of high-order harmonic generation within a helium atom under the influence of a plasmon-assisted shaping pulse.Our findings reveal an intriguing manipulation of the frequency peak position in the harmonic emission by adjusting the absolute phase parameter within the frequency domain of the shaping pulse.This phenomenon holds potential significance for experimental setups necessitating precisely tuned single harmonics.Notably,we observe a modulated shift in the created harmonic photon energy,spanning an impressive range of 1.2 eV.This frequency peak shift is rooted in the asymmetry exhibited by the rising and falling edges of the laser pulse,directly influencing the position of the peak frequency emission.Our study quantifies the dependence of this tuning range and the asymmetry of the laser pulse,offering valuable insights into the underlying mechanisms driving this phenomenon.Furthermore,our investigation uncovers the emergence of semi-integer order harmonics as the phase parameter is altered.We attribute this discovery to the intricate interference between harmonics generated by the primary and secondary return cores.This observation introduces an innovative approach for generating semi-integer order harmonics,thus expanding our understanding of high-order harmonic generation.Ultimately,our work contributes to the broader comprehension of complex phenomena in laser-matter interactions and provides a foundation for harnessing these effects in various applications,particularly those involving precise spectral control and the generation of unique harmonic patterns.展开更多
By numerically solving the two-dimensional semiconductor Bloch equation,we study the high-order harmonic emission of a monolayer ZnO under the driving of co-rotating two-color circularly polarized laser pulses.By chan...By numerically solving the two-dimensional semiconductor Bloch equation,we study the high-order harmonic emission of a monolayer ZnO under the driving of co-rotating two-color circularly polarized laser pulses.By changing the relative phase between the fundamental frequency field and the second one,it is found that the harmonic intensity in the platform region can be significantly modulated.In the higher order,the harmonic intensity can be increased by about one order of magnitude.Through time-frequency analysis,it is demonstrated that the emission trajectory of monolayer ZnO can be controlled by the relative phase,and the harmonic enhancement is caused by the second quantum trajectory with the higher emission probability.In addition,near-circularly polarized harmonics can be generated in the co-rotating two-color circularly polarized fields.With the change of the relative phase,the harmonics in the platform region can be altered from left-handed near-circularly polarization to right-handed one.Our results can obtain high-intensity harmonic radiation with an adjustable ellipticity,which provides an opportunity for syntheses of circularly polarized attosecond pulses.展开更多
Spatial confinement can significantly enhance the spectral intensity of laser-induced plasma in air. It is attributed to the compression of plasma plume by the reflected shockwave. In addition,optical emission spectro...Spatial confinement can significantly enhance the spectral intensity of laser-induced plasma in air. It is attributed to the compression of plasma plume by the reflected shockwave. In addition,optical emission spectroscopy of laser-induced plasma can also be affected by the distance between lens and sample surface. In order to obtain the optimized spectral intensity, the distance must be considered. In this work, spatially confined laser-induced silicon plasma by using a Nd:YAG nanosecond laser at different distances between lens and sample surface was investigated.The laser energies were 12 mJ, 16 mJ, 20 mJ, and 24 mJ. All experiments were carried out in an atmospheric environment. The results indicated that the intensity of Si(I) 390.55 nm line firstly rose and then dropped with the increase of lens-to-sample distance. Moreover, the spectral peak intensity with spatial confinement was higher than that without spatial confinement. The enhancement ratio was approximately 2 when laser energy was 24 mJ.展开更多
5f-elements encaged in a gold superatomic cluster are capable of giving rise to unique optical properties due to their hyperactive valence electrons and great radial components of 5f/6d orbitals. Herein, we review our...5f-elements encaged in a gold superatomic cluster are capable of giving rise to unique optical properties due to their hyperactive valence electrons and great radial components of 5f/6d orbitals. Herein, we review our first-principles studies on electronic structures and spectroscopic properties of a series of actinide-embedded gold superatomic clusters with different dimensions. The three-dimensional(3D) and two-dimensional(2D) superatom clusters possess the 18-electron configuration of 1S21P61D10 and 10-electron configuration of 1S21P41D4, respectively. Importantly, their electronic absorption spectra can also be effectively explained by the superatom orbitals. Specifically, the charge transfer(CT) transitions involved in surface-enhance Raman spectroscopy(SERS) spectra for 3D and 2D structures are both from the filled 1D orbitals, providing the enhancement factors of the order of ～ 104 at 488 nm and ～ 105 at 456 nm, respectively. This work implies that the superatomic orbital transitions involved in 5f-elements can not only lead to a remarkable spectroscopic performance, but also a new direction for optical design in the future.展开更多
The photoionization of a hydrogen atom from its ground state with ultra-fast chirped pulses is investigated by numerically solving the time-dependent Schrodinger equation within length,velocity,and Kramers-Henneberger...The photoionization of a hydrogen atom from its ground state with ultra-fast chirped pulses is investigated by numerically solving the time-dependent Schrodinger equation within length,velocity,and Kramers-Henneberger gauges.Converged results for all gauges for chirp-free pulses agree with the prediction of dynamic interference for ground state hydrogen atoms predicted recently by Jiang and Burgdorfer[Opt.Express 26,19921(2018)].In addition,we investigated photoelectron spectra of hydrogen atoms by chirped laser pulses,and showed that dynamic interference effect will be weaken for pulses with increasing linear chirp.Our numerical results can be understood and discussed in terms of an interplay of photoelectron wavepackets from first and second halves of laser enevelop,including the ac Stark energy level shift of the photoelectron final state and atomic stabilization effect at ultra-high intensities.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
In this paper,we present a study on the spatial confinement effect of laser-induced plasma with a cylindrical cavity in laser-induced breakdown spectroscopy(LIBS).The emission intensity with the spatial confinement is...In this paper,we present a study on the spatial confinement effect of laser-induced plasma with a cylindrical cavity in laser-induced breakdown spectroscopy(LIBS).The emission intensity with the spatial confinement is dependent on the height of the confinement cavity.It is found that,by selecting the appropriate height of cylindrical cavity,the signal enhancement can be significantly increased.At the cylindrical cavity(diameter = 2 mm) with a height of 6 mm,the enhancement ratio has the maximum value(approximately 8.3),and the value of the relative standard deviation(RSD)(7.6%) is at a minimum,the repeatability of LIBS signal is best.The results indicate that the height of confinement cavity is very important for LIBS technique to reduce the limit of detection and improve the precision.展开更多
A quasi-classical trajectory(QCT) calculation is used to investigate the vector and scalar properties of the D + Br O → DBr + O reaction based on an ab initio potential energy surface(X1A state) with collision energy...A quasi-classical trajectory(QCT) calculation is used to investigate the vector and scalar properties of the D + Br O → DBr + O reaction based on an ab initio potential energy surface(X1A state) with collision energy ranging from 0.1 kcal/mol to 6 kcal/mol. The reaction probability, the cross section, and the rate constant are studied. The probability and the cross section show decreasing behaviors as the collision energy increases. The distribution of the rate constant indicates that the reaction favorably occurs in a relatively low-temperature region(T < 100 K). Meanwhile, three product angular distributions P(θr), P(φr), and P(θr, φr) are presented, which reflect the positive effect on the rotational angular momentum j' polarization of the DBr product molecule. In addition, two of the polarization-dependent generalized differential cross sections(PDDCSs), PDDCS00 and PDDCS20, are computed as well. Our results demonstrate that both vector and scalar properties have strong energy dependence.展开更多
Spectral intensity,electron temperature and density of laser-induced plasma(LIP) are important parameters for affecting sensitivity of laser-induced breakdown spectroscopy(LIBS).Increasing target temperature is an eas...Spectral intensity,electron temperature and density of laser-induced plasma(LIP) are important parameters for affecting sensitivity of laser-induced breakdown spectroscopy(LIBS).Increasing target temperature is an easy and feasible method to improve the sensitivity.In this paper,a brass target in a temperature range from 25℃ to 200℃ was ablated to generate the LIP using femtosecond pulse.Time-resolved spectral emission of the femtosecond LIBS was measured under different target temperatures.The results showed that,compared with the experimental condition of 25℃,the spectral intensity of the femtosecond LIP was enhanced with more temperature target.In addition,the electron temperature and density were calculated by Boltzmann equation and Stark broadening,indicating that the changes in the electron temperature and density of femtosecond LIP with the increase of the target temperature were different from each other.By increasing the target temperature,the electron temperature increased while the electron density decreased.Therefore,in femtosecond LIBS,a hightemperature and low-density plasma with high emission can be generated by increasing the target temperature.The increase in the target temperature can improve the resolution and sensitivity of femtosecond LIBS.展开更多
Ionizations and fragmentations of benzene, methylbenzene, and chlorobenzene are studied in linearly polarized 50-fs,800-nm and 400-nm strong laser fields using a time-of-flight mass spectrometer. It is shown that at l...Ionizations and fragmentations of benzene, methylbenzene, and chlorobenzene are studied in linearly polarized 50-fs,800-nm and 400-nm strong laser fields using a time-of-flight mass spectrometer. It is shown that at low laser intensity, the parent ions are dominant for any one of the molecules in an 800-nm strong laser field, while extensive fragmentation is observed in a 400-nm laser field, which can be understood by the resonant photon absorption of molecular cations. The ratio of the yield of the parent ion to the yield of the total ion for each molecule is measured as a function of laser intensity in a range from 1.0 × 1013W/cm2 to 4.0 × 1014W/cm2, in either the 800-nm or 400-nm laser field. The results show that the fragmentation of the aromatic molecules increases significantly as the laser intensity is increased. Possible mechanisms for fragmentation in strong laser fields are discussed. Finally, the saturation intensity of ionization of the titled molecules is also determined.展开更多
We propose a scheme to coherently control the field-free orientation of NO molecule whose rotational temperature is above 0 K. It is found that the maximum molecular orientation is affected by two factors: one is the ...We propose a scheme to coherently control the field-free orientation of NO molecule whose rotational temperature is above 0 K. It is found that the maximum molecular orientation is affected by two factors: one is the sum of the population of M = 0 rotational states and the other is their distribution, however, their distribution plays a much more significant role in molecular orientation than the sum of their population. By adopting a series of linearly polarized pulses resonant with the rotational states, the distribution of M = 0 rotational states is well rearranged. Though the number of pulses used is small, a relatively high orientation degree can be obtained. This scheme provides a promising approach to the achievement of a good orientation effect.展开更多
Rydberg state excitations of neutral nitric oxide molecules are studied in strong ultraviolet(UV) and near-infra-red(IR) laser fields using a linear time-of-flight(TOF) mass spectrometer with the pulsed electronic fie...Rydberg state excitations of neutral nitric oxide molecules are studied in strong ultraviolet(UV) and near-infra-red(IR) laser fields using a linear time-of-flight(TOF) mass spectrometer with the pulsed electronic field ionization method.The yield of Rydberg molecules is measured as a function of laser intensity and ellipticity,and the results in UV laser fields are compared with those in near-IR laser fields.The present study provides the first experimental evidence of neutral Rydberg molecules surviving in a strong laser field.The results indicate that a rescattering-after-tunneling process is the main contribution to the formation of Rydberg molecules in strong near-IR laser fields,while multi-photon excitation may play an important role in the strong UV laser fields.展开更多
High level calculations on the ground state of12Mg1 H molecule have been performed using multi-reference configuration interaction(MRCI) method with the Davidson modification. The core–valence correlation and scalar ...High level calculations on the ground state of12Mg1 H molecule have been performed using multi-reference configuration interaction(MRCI) method with the Davidson modification. The core–valence correlation and scalar relativistic corrections are included into the present calculations at the same time. The potential energy curve(PEC) of the ground state, all of the vibrational levels and spectroscopic parameters are fitted. The results show that the levels and spectroscopic parameters are in good agreement with the available experimental data. The analytical potential energy function(APEF) is also deduced from the calculated PEC using the Murrell–Sorbie(M–S) potential function. The present results can provide a helpful reference for the future spectroscopic experiments or dynamical calculations of the molecule.展开更多
In this work, we mainly investigate the NH3 molecular multiphoton ionization process by using the photoelectron velocity map imaging technique. Under the condition of femtosecond laser(wavelength at 800 nm), the photo...In this work, we mainly investigate the NH3 molecular multiphoton ionization process by using the photoelectron velocity map imaging technique. Under the condition of femtosecond laser(wavelength at 800 nm), the photoelectron images are detected. The channel switching and above-threshold ionization(ATI) effect are also confirmed. The kinetic energy spectrum(KES) and the photoelectron angular distributions(PADs) are obtained through the anti-Abel transformation from the original images, and then three ionization channels are confirmed successfully according to the Freeman resonance effect in a relatively low laser intensity region. In the excitation process, the intermediate resonance Rydberg states are C^1 A 1(6 + 2 photons process), B^1 E(6 + 2 photons process) and C^1 A 1(7 + 2 photons process), respectively. At the same time, we also find that the photoelectron angular distributions are independent of laser intensity. In addition, the electrons produced by different processes interfere with each other and they can produce a spider-like structure. We also find ac-Stark movement according to the Stark-shift-induced resonance effect when the laser intensity is relatively high.展开更多
Using the time-dependent pseudo-spectral scheme, we solve the time-dependent Schr ¨odinger equation of a hydrogenlike atom in a strong laser field in momentum space. The intensity-resolved photoelectron energy sp...Using the time-dependent pseudo-spectral scheme, we solve the time-dependent Schr ¨odinger equation of a hydrogenlike atom in a strong laser field in momentum space. The intensity-resolved photoelectron energy spectrum in abovethreshold ionization is obtained and further analyzed. We find that with the increase of the laser intensity, the abovethreshold ionization emission spectrum exhibits periodic resonance structure. By analyzing the population of atomic bound states, we find that it is the multi-photon excitation of bound state that leads to the occurrence of this phenomenon, which is in fairly good agreement with the experimental results.展开更多
基金Project supported by the National Key Research and Development Program of China(Grant No.2019YFA0307700)the National Natural Science Foundation of China(Grant Nos.12074145,11627807,and 11975012)+2 种基金the Research Foundation for Basic Research of Jilin Province,China(Grant No.20220101003JC)the Fundamental Research Funds for the Central Universities of China(Grant No.30916011207)the Outstanding Youth Project of Taizhou University(Grant No.2019JQ002)。
文摘The intrinsic chirp of high-order harmonic generation is an important factor limiting the production of ultrashort attosecond pulses.Based on numerically solving the time-dependent Schrodinger equation,the generation process of highorder harmonic from the He atom under the action of orthogonal two-color combined pulse of fundamental frequency and higher intensity second harmonic fields is studied.In this paper,we propose to achieve quasi-chirp-free isolated attosecond pulses by superimposing a higher second-harmonic field on the orthogonal direction of the fundamental frequency field.It is found that the high-energy part of its harmonic emission exhibits small chirp characteristics,which can be used to synthesize isolated attosecond pulses.Through the analysis of the wave packets evolution and the classical motion trajectories of the electron,it is demonstrated that the quasi-chirp-free harmonic can be attributed to the simultaneous return of electrons ionized at different times to the parent particle.The influence of the relative phase of the two pulses on the harmonics is further analyzed,and it is observed that this phenomenon is sensitive to the relative phase,but it can still generate isolated attosecond pulses within a certain phase.
基金Project supported by the National Key Research and Development Program of China(Grant No.2019YFA0307701)the National Natural Science Foundation of China(Grant Nos.11674128,11674124,and 11974138).
文摘We conduct an experimental study supported by theoretical analysis of single laser ablating copper to investigate the interactions between laser and material at different sample temperatures,and predict the changes of ablation morphology and lattice temperature.For investigating the effect of sample temperature on femtosecond laser processing,we conduct experiments on and simulate the thermal behavior of femtosecond laser irradiating copper by using a two-temperature model.The simulation results show that both electron peak temperature and the relaxation time needed to reach equilibrium increase as initial sample temperature rises.When the sample temperature rises from 300 K to 600 K,the maximum lattice temperature of the copper surface increases by about 6500 K under femtosecond laser irradiation,and the ablation depth increases by 20%.The simulated ablation depths follow the same general trend as the experimental values.This work provides some theoretical basis and technical support for developing femtosecond laser processing in the field of metal materials.
基金the National Key Research and Development Program of China (Grant No.2019YFA0307700)the National Natural Science Foundation of China (Grant Nos.12074145 and 11975012)+1 种基金Jilin Provincial Research Foundation for Basic Research,China (Grant No.20220101003JC)Jilin Provincial Education Department (Grant No.JJKH20230284KJ)。
文摘The double ionization process of molecules driven by co-rotating two-color circularly polarized fields is investigated with a three-dimensional classical ensemble model. Numerical results indicate that a considerable part of the sequential double ionization(DI) events of molecules occur through internal collision double ionization(ICD), and the ICD recollision mechanism is significantly different from that in non-sequential double ionization(NSDI). By analyzing the results of internuclear distances R = 5 a.u. and 2 a.u., these two recollision mechanisms are studied in depth. It is found that the dynamic behaviors of the recollision mechanisms of NSDI and ICD are similar. For NSDI, the motion range of electrons after the ionization is relatively large, and the electrons will return to the core after a period of time. In the ICD process,electrons will rotate around the parent ion before ionization, and the distance of the electron motion is relatively small. After a period of time, the electrons will come back to the core and collide with another electron. Furthermore, the molecular internuclear distance has a significant effect on the electron dynamic behavior of the two ionization mechanisms. This study will help to understand the multi-electron ionization process of complex systems.
基金This project was supported by the National Key Research and Development Program of China(Grant Nos.2022YFE134200 and 2019YFA0307700)the National Natural Science Foundation of China(Grant Nos.11604119,12104177,11904192,12074145,and 11704147)the Fundamental Research Funds for the Central Universities(Grant Nos.GK202207012 and QCYRCXM-2022-241).
文摘We delve into the phenomenon of high-order harmonic generation within a helium atom under the influence of a plasmon-assisted shaping pulse.Our findings reveal an intriguing manipulation of the frequency peak position in the harmonic emission by adjusting the absolute phase parameter within the frequency domain of the shaping pulse.This phenomenon holds potential significance for experimental setups necessitating precisely tuned single harmonics.Notably,we observe a modulated shift in the created harmonic photon energy,spanning an impressive range of 1.2 eV.This frequency peak shift is rooted in the asymmetry exhibited by the rising and falling edges of the laser pulse,directly influencing the position of the peak frequency emission.Our study quantifies the dependence of this tuning range and the asymmetry of the laser pulse,offering valuable insights into the underlying mechanisms driving this phenomenon.Furthermore,our investigation uncovers the emergence of semi-integer order harmonics as the phase parameter is altered.We attribute this discovery to the intricate interference between harmonics generated by the primary and secondary return cores.This observation introduces an innovative approach for generating semi-integer order harmonics,thus expanding our understanding of high-order harmonic generation.Ultimately,our work contributes to the broader comprehension of complex phenomena in laser-matter interactions and provides a foundation for harnessing these effects in various applications,particularly those involving precise spectral control and the generation of unique harmonic patterns.
基金supported by the Zhejiang Provincial Natural Science Foundation of China(Grant Nos.Y23A040001 and LY21F050001)the National Key Research and Development Program of China(Grant No.2019YFA0307700),the National Natural Science Foundation of China(Grant Nos.12074145,11774219,11975012,12374029,12304378,and 12204214)+2 种基金the Jilin Provincial Research Foundation for Basic Research,China(Grant No.20220101003JC)the Foundation of Education Department of Liaoning Province,China(Grant No.LJKMZ20221435)the National College Students Innovation and Entrepreneurship Training Program(Grant No.202310350062).
文摘By numerically solving the two-dimensional semiconductor Bloch equation,we study the high-order harmonic emission of a monolayer ZnO under the driving of co-rotating two-color circularly polarized laser pulses.By changing the relative phase between the fundamental frequency field and the second one,it is found that the harmonic intensity in the platform region can be significantly modulated.In the higher order,the harmonic intensity can be increased by about one order of magnitude.Through time-frequency analysis,it is demonstrated that the emission trajectory of monolayer ZnO can be controlled by the relative phase,and the harmonic enhancement is caused by the second quantum trajectory with the higher emission probability.In addition,near-circularly polarized harmonics can be generated in the co-rotating two-color circularly polarized fields.With the change of the relative phase,the harmonics in the platform region can be altered from left-handed near-circularly polarization to right-handed one.Our results can obtain high-intensity harmonic radiation with an adjustable ellipticity,which provides an opportunity for syntheses of circularly polarized attosecond pulses.
基金support by National Natural Science Foundation of China(Grant Nos.11674128,11504129,and11474129)Jilin Province Scientific and Technological Development Program,China(Grant No.20170101063JC)the Thirteenth Five-Year Scientific and Technological Research Project of the Education Department of Jilin Province,China(2016,No.400)
文摘Spatial confinement can significantly enhance the spectral intensity of laser-induced plasma in air. It is attributed to the compression of plasma plume by the reflected shockwave. In addition,optical emission spectroscopy of laser-induced plasma can also be affected by the distance between lens and sample surface. In order to obtain the optimized spectral intensity, the distance must be considered. In this work, spatially confined laser-induced silicon plasma by using a Nd:YAG nanosecond laser at different distances between lens and sample surface was investigated.The laser energies were 12 mJ, 16 mJ, 20 mJ, and 24 mJ. All experiments were carried out in an atmospheric environment. The results indicated that the intensity of Si(I) 390.55 nm line firstly rose and then dropped with the increase of lens-to-sample distance. Moreover, the spectral peak intensity with spatial confinement was higher than that without spatial confinement. The enhancement ratio was approximately 2 when laser energy was 24 mJ.
基金supported by the National Natural Science Foundation of China(Grant No.11374004)the Science and Technology Development Program of Jilin Province,China(Grant No.20150519021JH)+1 种基金the Fok Ying Tung Education Foundation,China(Grant No.142001)the Support from the High Performance Computing Center(HPCC)of Jilin University,China
文摘5f-elements encaged in a gold superatomic cluster are capable of giving rise to unique optical properties due to their hyperactive valence electrons and great radial components of 5f/6d orbitals. Herein, we review our first-principles studies on electronic structures and spectroscopic properties of a series of actinide-embedded gold superatomic clusters with different dimensions. The three-dimensional(3D) and two-dimensional(2D) superatom clusters possess the 18-electron configuration of 1S21P61D10 and 10-electron configuration of 1S21P41D4, respectively. Importantly, their electronic absorption spectra can also be effectively explained by the superatom orbitals. Specifically, the charge transfer(CT) transitions involved in surface-enhance Raman spectroscopy(SERS) spectra for 3D and 2D structures are both from the filled 1D orbitals, providing the enhancement factors of the order of ～ 104 at 488 nm and ～ 105 at 456 nm, respectively. This work implies that the superatomic orbital transitions involved in 5f-elements can not only lead to a remarkable spectroscopic performance, but also a new direction for optical design in the future.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11774131 and 91850114)
文摘The photoionization of a hydrogen atom from its ground state with ultra-fast chirped pulses is investigated by numerically solving the time-dependent Schrodinger equation within length,velocity,and Kramers-Henneberger gauges.Converged results for all gauges for chirp-free pulses agree with the prediction of dynamic interference for ground state hydrogen atoms predicted recently by Jiang and Burgdorfer[Opt.Express 26,19921(2018)].In addition,we investigated photoelectron spectra of hydrogen atoms by chirped laser pulses,and showed that dynamic interference effect will be weaken for pulses with increasing linear chirp.Our numerical results can be understood and discussed in terms of an interplay of photoelectron wavepackets from first and second halves of laser enevelop,including the ac Stark energy level shift of the photoelectron final state and atomic stabilization effect at ultra-high intensities.
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the support from the Fundamental Research Project of Chinese State Key Laboratory of Laser Interaction with Matter(Grant No.SKLLIM 1502)the National Natural Science Foundation of China(Grant Nos.11674128,11474129 and 11504129)the China Postdoctoral Science Foundation(Grant No.2014M551169)
文摘In this paper,we present a study on the spatial confinement effect of laser-induced plasma with a cylindrical cavity in laser-induced breakdown spectroscopy(LIBS).The emission intensity with the spatial confinement is dependent on the height of the confinement cavity.It is found that,by selecting the appropriate height of cylindrical cavity,the signal enhancement can be significantly increased.At the cylindrical cavity(diameter = 2 mm) with a height of 6 mm,the enhancement ratio has the maximum value(approximately 8.3),and the value of the relative standard deviation(RSD)(7.6%) is at a minimum,the repeatability of LIBS signal is best.The results indicate that the height of confinement cavity is very important for LIBS technique to reduce the limit of detection and improve the precision.
基金supported by the Jilin University,China(Grant No.419080106440)the Chinese National Fusion Project for the International Thermonuclear Experimental Reactor(ITER)(Grant No.2010GB104003)the National Natural Science Foundation of China(Grant No.10974069)
文摘A quasi-classical trajectory(QCT) calculation is used to investigate the vector and scalar properties of the D + Br O → DBr + O reaction based on an ab initio potential energy surface(X1A state) with collision energy ranging from 0.1 kcal/mol to 6 kcal/mol. The reaction probability, the cross section, and the rate constant are studied. The probability and the cross section show decreasing behaviors as the collision energy increases. The distribution of the rate constant indicates that the reaction favorably occurs in a relatively low-temperature region(T < 100 K). Meanwhile, three product angular distributions P(θr), P(φr), and P(θr, φr) are presented, which reflect the positive effect on the rotational angular momentum j' polarization of the DBr product molecule. In addition, two of the polarization-dependent generalized differential cross sections(PDDCSs), PDDCS00 and PDDCS20, are computed as well. Our results demonstrate that both vector and scalar properties have strong energy dependence.
基金Supported by the National Natural Science Foundation of China under Grant No 11404180the Natural Science Foundation of Heilongjiang Province under Grant Nos F201335,A2015010,and A2015011the Postdoctoral Scientific Research Developmental Fund of Heilongjiang Province under Grant No LBH-Q14159
基金support by National Natural Science Foundation of China (Nos. 11674128, 11674124 and 11974138)the Jilin Province Scientific and Technological Development Program, China (No. 20170101063JC)。
文摘Spectral intensity,electron temperature and density of laser-induced plasma(LIP) are important parameters for affecting sensitivity of laser-induced breakdown spectroscopy(LIBS).Increasing target temperature is an easy and feasible method to improve the sensitivity.In this paper,a brass target in a temperature range from 25℃ to 200℃ was ablated to generate the LIP using femtosecond pulse.Time-resolved spectral emission of the femtosecond LIBS was measured under different target temperatures.The results showed that,compared with the experimental condition of 25℃,the spectral intensity of the femtosecond LIP was enhanced with more temperature target.In addition,the electron temperature and density were calculated by Boltzmann equation and Stark broadening,indicating that the changes in the electron temperature and density of femtosecond LIP with the increase of the target temperature were different from each other.By increasing the target temperature,the electron temperature increased while the electron density decreased.Therefore,in femtosecond LIBS,a hightemperature and low-density plasma with high emission can be generated by increasing the target temperature.The increase in the target temperature can improve the resolution and sensitivity of femtosecond LIBS.
基金supported by the National Basic Research Program of China(Grant No.2013CB922200)the National Natural Science Foundation of China(Grant No.11274140)
文摘Ionizations and fragmentations of benzene, methylbenzene, and chlorobenzene are studied in linearly polarized 50-fs,800-nm and 400-nm strong laser fields using a time-of-flight mass spectrometer. It is shown that at low laser intensity, the parent ions are dominant for any one of the molecules in an 800-nm strong laser field, while extensive fragmentation is observed in a 400-nm laser field, which can be understood by the resonant photon absorption of molecular cations. The ratio of the yield of the parent ion to the yield of the total ion for each molecule is measured as a function of laser intensity in a range from 1.0 × 1013W/cm2 to 4.0 × 1014W/cm2, in either the 800-nm or 400-nm laser field. The results show that the fragmentation of the aromatic molecules increases significantly as the laser intensity is increased. Possible mechanisms for fragmentation in strong laser fields are discussed. Finally, the saturation intensity of ionization of the titled molecules is also determined.
基金Project supported by the National Basic Research Program of China(Grant No.2013CB922200)the National Natural Science Foundation of China(Grant Nos.11034003,11474129,11274141,and 11304116)+1 种基金the Research Fund for the Doctoral Program of Higher Education of China(Grant No.20130061110021)the Graduate Innovation Fund of Jilin University(Grant No.2015091)
文摘We propose a scheme to coherently control the field-free orientation of NO molecule whose rotational temperature is above 0 K. It is found that the maximum molecular orientation is affected by two factors: one is the sum of the population of M = 0 rotational states and the other is their distribution, however, their distribution plays a much more significant role in molecular orientation than the sum of their population. By adopting a series of linearly polarized pulses resonant with the rotational states, the distribution of M = 0 rotational states is well rearranged. Though the number of pulses used is small, a relatively high orientation degree can be obtained. This scheme provides a promising approach to the achievement of a good orientation effect.
基金Project supported by the National Basic Research Program of China(Grant No.2013CB922200)the National Natural Science Foundation of China(Grant Nos.11034003 and 11274140)
文摘Rydberg state excitations of neutral nitric oxide molecules are studied in strong ultraviolet(UV) and near-infra-red(IR) laser fields using a linear time-of-flight(TOF) mass spectrometer with the pulsed electronic field ionization method.The yield of Rydberg molecules is measured as a function of laser intensity and ellipticity,and the results in UV laser fields are compared with those in near-IR laser fields.The present study provides the first experimental evidence of neutral Rydberg molecules surviving in a strong laser field.The results indicate that a rescattering-after-tunneling process is the main contribution to the formation of Rydberg molecules in strong near-IR laser fields,while multi-photon excitation may play an important role in the strong UV laser fields.
基金Project supported by the National Natural Science Foundation of China(Grand Nos.11147158,91221301,and 11264020)
文摘High level calculations on the ground state of12Mg1 H molecule have been performed using multi-reference configuration interaction(MRCI) method with the Davidson modification. The core–valence correlation and scalar relativistic corrections are included into the present calculations at the same time. The potential energy curve(PEC) of the ground state, all of the vibrational levels and spectroscopic parameters are fitted. The results show that the levels and spectroscopic parameters are in good agreement with the available experimental data. The analytical potential energy function(APEF) is also deduced from the calculated PEC using the Murrell–Sorbie(M–S) potential function. The present results can provide a helpful reference for the future spectroscopic experiments or dynamical calculations of the molecule.
基金Supported by the National Basic Research Program of China under Grant No 2013CB922200the National Natural Science Foundation of China under Grant Nos 11274141,11304116,11274001 and 11247024the Jilin Provincial Research Foundation for Basic Research under Grant No 20140101168JC
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11574116,11534004,10704028,and 11474123)
文摘In this work, we mainly investigate the NH3 molecular multiphoton ionization process by using the photoelectron velocity map imaging technique. Under the condition of femtosecond laser(wavelength at 800 nm), the photoelectron images are detected. The channel switching and above-threshold ionization(ATI) effect are also confirmed. The kinetic energy spectrum(KES) and the photoelectron angular distributions(PADs) are obtained through the anti-Abel transformation from the original images, and then three ionization channels are confirmed successfully according to the Freeman resonance effect in a relatively low laser intensity region. In the excitation process, the intermediate resonance Rydberg states are C^1 A 1(6 + 2 photons process), B^1 E(6 + 2 photons process) and C^1 A 1(7 + 2 photons process), respectively. At the same time, we also find that the photoelectron angular distributions are independent of laser intensity. In addition, the electrons produced by different processes interfere with each other and they can produce a spider-like structure. We also find ac-Stark movement according to the Stark-shift-induced resonance effect when the laser intensity is relatively high.
基金Project supported by the National Basic Research Program of China(Grant No.2013CB922200)the National Natural Science Foundation of China(Grants Nos.11274141,11034003,11304116,11274001,and 11247024)the Jilin Provincial Research Foundation for Basic Research,China(Grant No.20140101168JC)
文摘Using the time-dependent pseudo-spectral scheme, we solve the time-dependent Schr ¨odinger equation of a hydrogenlike atom in a strong laser field in momentum space. The intensity-resolved photoelectron energy spectrum in abovethreshold ionization is obtained and further analyzed. We find that with the increase of the laser intensity, the abovethreshold ionization emission spectrum exhibits periodic resonance structure. By analyzing the population of atomic bound states, we find that it is the multi-photon excitation of bound state that leads to the occurrence of this phenomenon, which is in fairly good agreement with the experimental results.
