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
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
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 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
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
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
First-principle calculations reveal that the configuration system of hexagonal boron nitride(h-BN) monolayer with triangular vacancy can induce obvious magnetism, contrary to that of the nonmagnetic pristine boron nit...First-principle calculations reveal that the configuration system of hexagonal boron nitride(h-BN) monolayer with triangular vacancy can induce obvious magnetism, contrary to that of the nonmagnetic pristine boron nitride monolayer.Interestingly, the h-BN with boron atom vacancy(VB-BN) displays metallic behavior with a total magnetic moment being 0.46μ_B per cell, while the h-BN with nitrogen atom vacancy(VN-BN) presents a half-metallic characteristic with a total magnetic moment being 1.0μ_B per cell. Remarkably, piezoelectric stress coefficient e_(11) of the VN-BN is about 1.5 times larger than that of pristine h-BN. Furthermore, piezoelectric strain coefficient d_(11)(12.42 pm/V) of the VN-BN is 20 times larger than that of pristine h-BN and also one order of magnitude larger than the value for the h-MoS_2 monolayer, which is mainly due to the spin-down electronic state in the V_N-BN system. Our study demonstrates that the nitrogen atom vacancies can be an efficient route to tailoring the magnetic and piezoelectric properties of h-BN monolayer, which have promising performances for potential applications in nano-electromechanical systems(NEMS) and nanoscale electronics devices.展开更多
We simultaneously investigate variations of a low order harmonic and photoelectron emission with an incident laser intensity by solving the time-dependent Schr o¨dinger equation in a momentum space. It can be fou...We simultaneously investigate variations of a low order harmonic and photoelectron emission with an incident laser intensity by solving the time-dependent Schr o¨dinger equation in a momentum space. It can be found that, the intensity of low order harmonic and photoelectron are gradually enhanced with the increase of the laser intensity, when the laser frequency is not in resonance with the transition frequency between the laser-induced high excited states and the ground state. If the resonance occurs, the intensity of the lower order harmonic is reduced and the interference can be observed in the lower order photoelectron spectra.展开更多
We simulate the dynamic response of H^(+)_(2) in a linearly polarized laser field by numerically solving the time-dependent Schr?dinger equation.The elliptically polarized high-order harmonics generated by H^(+)_(2)ir...We simulate the dynamic response of H^(+)_(2) in a linearly polarized laser field by numerically solving the time-dependent Schr?dinger equation.The elliptically polarized high-order harmonics generated by H^(+)_(2)irradiated by the linearly polarized laser field are systematically investigated.The result shows that the amplitude and rotation of the ellipticity of harmonics are affected by the alignment angle and internuclear distance of the molecule.Analyzing the change in forces acted on the ionized electrons and the trajectories of the electrons,the phenomena are found to be due to the change in the direction of the total Coulomb forces from the two nuclei felt by the recollided ionized electrons in the direction perpendicular to the laser polarization direction.Based on the influence law,we can select the harmonics with a specific frequency band under different alignment angles and then synthesize the isolated attosecond pulses with different rotations,which can be continuously converted from right-handed circular polarization,linear polarization,and left-handed circular polarization by changing the alignment angle.This study provides a new possible approach to the real-time detection of molecular states by using attosecond pulses and obtaining more optimized harmonics with molecular properties.展开更多
Since roaming was found as a new but common reaction path of isomerization, many of its properties, especially those of roaming transition state(TS_R), have been studied on many systems. However, the mechanism of roam...Since roaming was found as a new but common reaction path of isomerization, many of its properties, especially those of roaming transition state(TS_R), have been studied on many systems. However, the mechanism of roaming is still not clear at an atomic level. In this work, we use first-principles calculations to illustrate the detailed structure of TS_R in an internal isomerization process of nitrobenzene. The calculations distinctively show its nature of antiferromagnetic coupling between two roaming fragments. Moreover, the effect of dispersion is also revealed as an important issue for the stability of the TS_R. Our work provides a new insight into the TS_R from the view of electronic structure and contributes to the basic understanding of the roaming systems.展开更多
We investigated the ionization of an atom with different orbital angular momenta in a high-frequency laser field by solving the time-dependent Schr¨odinger equation.The results showed that the ionization stabiliz...We investigated the ionization of an atom with different orbital angular momenta in a high-frequency laser field by solving the time-dependent Schr¨odinger equation.The results showed that the ionization stabilization features changed with the relative direction between the angular momentum of the initial state and the vector field of the laser pulse.The ionization mechanism of the atom irradiated by a high frequency was explained by calculating the transition matrix and evolution of the time-dependent wave packet.This study can provide comprehensive understanding to improve atomic nonadiabatic ionization.展开更多
In this paper, we investigated the influence of sample temperature on the expansion dynamics and the optical emission spectroscopy of laser-induced plasma, and Ge was selected as the test sample. The target was heated...In this paper, we investigated the influence of sample temperature on the expansion dynamics and the optical emission spectroscopy of laser-induced plasma, and Ge was selected as the test sample. The target was heated from room temperature(22 °C) to 300 °C, and excited in atmospheric environment by using a Q-Switched Nd:YAG pulse laser with the wavelength of 1064 nm. To study the plasma expansion dynamics, we observed the plasma plume at different laser energies(5.0, 7.4 and 9.4 mJ)and different sample temperatures by using time-resolved image. We found that the heated target temperature could accelerate the expansion of plasma plume. Moreover, we also measured the effect of target temperature on the optical emission spectroscopy and signal-to-noise ratio.展开更多
We investigated the dependence of laser-induced breakdown spectral intensity on the focusing position of a lens at different sample temperatures(room temperature to 300 ℃) in atmosphere.A Q-switched Nd:YAG nanosecond...We investigated the dependence of laser-induced breakdown spectral intensity on the focusing position of a lens at different sample temperatures(room temperature to 300 ℃) in atmosphere.A Q-switched Nd:YAG nanosecond pulsed laser with 1064 nm wavelength and 10 ns pulse width was used to ablate silicon to produce plasma. It was confirmed that the increase in the sample's initial temperature could improve spectral line intensity. In addition, when the distance from the target surface to the focal point increased, the intensity firstly rose, and then dropped.The trend of change with distance was more obvious at higher sample temperatures. By observing the distribution of the normalized ratio of Si atomic spectral line intensity and Si ionic spectral line intensity as functions of distance and temperature, the maximum value of normalized ratio appeared at the longer distance as the initial temperature was higher, while the maximum ratio appeared at the shorter distance as the sample temperature was lower.展开更多
We macroscopically investigate the effect of the laser intensity and gas density on quantum trajectories in the highorder harmonic generation of Ne atoms irradiated by few-cycle, 800-nm laser pulses. The time–frequen...We macroscopically investigate the effect of the laser intensity and gas density on quantum trajectories in the highorder harmonic generation of Ne atoms irradiated by few-cycle, 800-nm laser pulses. The time–frequency profile of the harmonics shows that the long quantum trajectory is dominant at both lower and higher gas densities for a low laser intensity. At high laser intensities, the long quantum trajectory plays an important role for lower gas densities, while the short quantum trajectory is dominant at higher gas densities. An analysis of the phase mismatch for high-order harmonic generation shows that the primary emission of the quantum trajectories is determined by dynamic changes in the laser electric field during the propagation process.展开更多
High-level ab initio calculations of aluminum monoiodide(AlI) molecule are performed by utilizing the multireference configuration interaction plus Davidson correction(MRCI+Q) method. The core-valence correlation(CV) ...High-level ab initio calculations of aluminum monoiodide(AlI) molecule are performed by utilizing the multireference configuration interaction plus Davidson correction(MRCI+Q) method. The core-valence correlation(CV) and spin–orbit coupling(SOC) effect are considered. The adiabatic potential energy curves(PECs) of a total of 13 Λ–S states and 24 ? states are computed. The spectroscopic constants of bound states are determined, which are in accordance with the results of the available experimental and theoretical studies. The interactions between the Λ–S states are analyzed with the aid of the spin–orbit matrix elements. Finally, the transition properties including transition dipole moment(TDM),Frank–Condon factors(FCF) and radiative lifetime are obtained based on the computed PEC. Our study sheds light on the electronic structure and spectroscopy of low-lying electronic states of the AlI molecule.展开更多
Cd F molecule, which plays an important role in a great variety of research fields, has long been subject to numerous researchers. Due to the unstable nature and heavy atom Cd containing in the Cd F molecule, electron...Cd F molecule, which plays an important role in a great variety of research fields, has long been subject to numerous researchers. Due to the unstable nature and heavy atom Cd containing in the Cd F molecule, electronic states of the molecule have not been well studied. In this paper, high accurate ab initio calculations on the Cd F molecule have been performed at the multi-reference configuration interaction level including Davidson correction(MRCI + Q). Adiabatic potential energy curves(PECs) of the 14 low-lying Λ–S states correlating with the two lowest dissociation limits Cd(~1S_g) + F(~2P_u) and Cd(~3P_u) + F(~2P_u) have been constructed. For the bound Λ–S and ? states, the dominant electronic configurations and spectroscopic constants are obtained,and the calculated spectroscopic constants of bound states are consistent with previous experimental results. The dipole moments(DMs) of 2 Σ+ and 2Π are determined, and the spin–orbit(SO) matrix elements between each pair of X2Σ+, 22Σ+, 12Π, and 22Π are obtained. The results indicate that the sudden changes of DMs and SO matrix elements arise from the variation of the electronic configurations around the avoided crossing region. Moreover,the Franck–Condon factors(FCFs), the transition dipole moments(TDMs), and radiative lifetimes of low-lying states-the ground state X2Σ+are determined. Finally, the transitional properties of 22Π–X2Σ+and 22Σ+–X2Σ+are studied. Based on our computed spectroscopic information of Cd F, the feasibility and challenge for laser cooling of Cd F molecule are discussed.展开更多
In double-pulse laser-induced breakdown spectroscopy(DP-LIBS), the collinear femtosecond double-pulse laser configuration is experimentally investigated with different initial sample temperatures using a Ti:sapphire l...In double-pulse laser-induced breakdown spectroscopy(DP-LIBS), the collinear femtosecond double-pulse laser configuration is experimentally investigated with different initial sample temperatures using a Ti:sapphire laser. The glass sample is ablated to produce the plasma spectroscopy. During the experiment, the detected spectral lines include two Na(I) lines(589.0 nm and 589.6 nm) and one Ca(I) line at the wavelength of 585.7 nm. The emission lines are measured at room temperature(22 ℃) and three higher initial sample temperatures(T_s?=?100 ℃, 200 ℃, and 250 ℃). The inter-pulse delay time ranges from-250 ps to 250 ps.The inter-pulse delay time and the sample temperature strongly influence the spectral intensity,and the spectral intensity can be significantly enhanced by increasing the sample temperature and selecting the optimized inter-pulse time. For the same inter-pulse time of 0 ps(single-pulse LIBS), the enhancement ratio is approximately 2.5 at T_s?=?200 ℃ compared with that obtained at T_s?=?22 ℃. For the same inter-pulse time of 150 ps, the enhancement ratio can be up to 4 at T_s?=?200 ℃ compared with that obtained at T_s?=?22 ℃. The combined enhancement effects of the different initial sample temperatures and the double-pulse configuration in femtosecond LIBS are much stronger than that of the different initial sample temperatures or the double-pulse configuration only.展开更多
We theoretically investigate the photoelectron emission from an atom irradiated by an amplitude modulated sinusoidally phase-modulated pulse through solving the time-dependent Schr¨odinger equation in the momentu...We theoretically investigate the photoelectron emission from an atom irradiated by an amplitude modulated sinusoidally phase-modulated pulse through solving the time-dependent Schr¨odinger equation in the momentum space. By controlling the phase amplitude of the pulse in the frequency domain, it can be found that the photoelectron spectra appear as explicit interference phenomena, which originated from the interference between the directly ionized electron and the ionization of the pre-excited atom from different subpulses.展开更多
We present a parallel numerical method of simulating the interaction of atoms with a strong laser field by solving the time-depending Schrodinger equation(TDSE)in spherical coordinates.This method is realized by combi...We present a parallel numerical method of simulating the interaction of atoms with a strong laser field by solving the time-depending Schrodinger equation(TDSE)in spherical coordinates.This method is realized by combining constructing block diagonal matrices through using the real space product formula(RSPF)with splitting out diagonal sub-matrices for short iterative Lanczos(SIL)propagator.The numerical implementation of the solver guarantees efficient parallel computing for the simulation of real physical problems such as high harmonic generation(HHG)in these interaction systems.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(Grant No.11474123)the Natural Science Foundation of Jilin Province,China(Grant No.20170101154JC)
文摘First-principle calculations reveal that the configuration system of hexagonal boron nitride(h-BN) monolayer with triangular vacancy can induce obvious magnetism, contrary to that of the nonmagnetic pristine boron nitride monolayer.Interestingly, the h-BN with boron atom vacancy(VB-BN) displays metallic behavior with a total magnetic moment being 0.46μ_B per cell, while the h-BN with nitrogen atom vacancy(VN-BN) presents a half-metallic characteristic with a total magnetic moment being 1.0μ_B per cell. Remarkably, piezoelectric stress coefficient e_(11) of the VN-BN is about 1.5 times larger than that of pristine h-BN. Furthermore, piezoelectric strain coefficient d_(11)(12.42 pm/V) of the VN-BN is 20 times larger than that of pristine h-BN and also one order of magnitude larger than the value for the h-MoS_2 monolayer, which is mainly due to the spin-down electronic state in the V_N-BN system. Our study demonstrates that the nitrogen atom vacancies can be an efficient route to tailoring the magnetic and piezoelectric properties of h-BN monolayer, which have promising performances for potential applications in nano-electromechanical systems(NEMS) and nanoscale electronics devices.
基金Project supported by the National Key Research and Development Program of China(Grant No.2017YFA0403300)the National Natural Science Foundation of China(Grant Nos.11774129,11274141,11627807,11604119,and 11534004)the Jilin Provincial Research Foundation for Basic Research,China(Grant No.20170101153JC)
文摘We simultaneously investigate variations of a low order harmonic and photoelectron emission with an incident laser intensity by solving the time-dependent Schr o¨dinger equation in a momentum space. It can be found that, the intensity of low order harmonic and photoelectron are gradually enhanced with the increase of the laser intensity, when the laser frequency is not in resonance with the transition frequency between the laser-induced high excited states and the ground state. If the resonance occurs, the intensity of the lower order harmonic is reduced and the interference can be observed in the lower order photoelectron spectra.
基金Project supported by the National Key Research and Development Program of China(Grant No.2019YFA0307700)the Science Foundation of China(Grant Nos.11627807,11774129,and 12074145)+1 种基金the High Performance Computing Center of Jilin University for supercomputer timethe high performance computing cluster Tiger@IAMP。
文摘We simulate the dynamic response of H^(+)_(2) in a linearly polarized laser field by numerically solving the time-dependent Schr?dinger equation.The elliptically polarized high-order harmonics generated by H^(+)_(2)irradiated by the linearly polarized laser field are systematically investigated.The result shows that the amplitude and rotation of the ellipticity of harmonics are affected by the alignment angle and internuclear distance of the molecule.Analyzing the change in forces acted on the ionized electrons and the trajectories of the electrons,the phenomena are found to be due to the change in the direction of the total Coulomb forces from the two nuclei felt by the recollided ionized electrons in the direction perpendicular to the laser polarization direction.Based on the influence law,we can select the harmonics with a specific frequency band under different alignment angles and then synthesize the isolated attosecond pulses with different rotations,which can be continuously converted from right-handed circular polarization,linear polarization,and left-handed circular polarization by changing the alignment angle.This study provides a new possible approach to the real-time detection of molecular states by using attosecond pulses and obtaining more optimized harmonics with molecular properties.
基金Project supported by the Science Challenging Program,China(Grant No.JCKY2016212A501)the National Natural Science Foundation of China(Grant No.11374004)
文摘Since roaming was found as a new but common reaction path of isomerization, many of its properties, especially those of roaming transition state(TS_R), have been studied on many systems. However, the mechanism of roaming is still not clear at an atomic level. In this work, we use first-principles calculations to illustrate the detailed structure of TS_R in an internal isomerization process of nitrobenzene. The calculations distinctively show its nature of antiferromagnetic coupling between two roaming fragments. Moreover, the effect of dispersion is also revealed as an important issue for the stability of the TS_R. Our work provides a new insight into the TS_R from the view of electronic structure and contributes to the basic understanding of the roaming systems.
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.12074145,11627807,11774175,11534004,11774129,11604119,and 11975012)Fundamental Research Funds for the Central Universities of China(Grant No.30916011207)。
文摘We investigated the ionization of an atom with different orbital angular momenta in a high-frequency laser field by solving the time-dependent Schr¨odinger equation.The results showed that the ionization stabilization features changed with the relative direction between the angular momentum of the initial state and the vector field of the laser pulse.The ionization mechanism of the atom irradiated by a high frequency was explained by calculating the transition matrix and evolution of the time-dependent wave packet.This study can provide comprehensive understanding to improve atomic nonadiabatic ionization.
基金support by National Natural Science Foundation of China(Grant Nos.11674128,11504129,and 11474129)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In this paper, we investigated the influence of sample temperature on the expansion dynamics and the optical emission spectroscopy of laser-induced plasma, and Ge was selected as the test sample. The target was heated from room temperature(22 °C) to 300 °C, and excited in atmospheric environment by using a Q-Switched Nd:YAG pulse laser with the wavelength of 1064 nm. To study the plasma expansion dynamics, we observed the plasma plume at different laser energies(5.0, 7.4 and 9.4 mJ)and different sample temperatures by using time-resolved image. We found that the heated target temperature could accelerate the expansion of plasma plume. Moreover, we also measured the effect of target temperature on the optical emission spectroscopy and signal-to-noise ratio.
基金support by National Natural Science Foundation of China (Grant Nos. 11674128, 11504129, and 11474129)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We investigated the dependence of laser-induced breakdown spectral intensity on the focusing position of a lens at different sample temperatures(room temperature to 300 ℃) in atmosphere.A Q-switched Nd:YAG nanosecond pulsed laser with 1064 nm wavelength and 10 ns pulse width was used to ablate silicon to produce plasma. It was confirmed that the increase in the sample's initial temperature could improve spectral line intensity. In addition, when the distance from the target surface to the focal point increased, the intensity firstly rose, and then dropped.The trend of change with distance was more obvious at higher sample temperatures. By observing the distribution of the normalized ratio of Si atomic spectral line intensity and Si ionic spectral line intensity as functions of distance and temperature, the maximum value of normalized ratio appeared at the longer distance as the initial temperature was higher, while the maximum ratio appeared at the shorter distance as the sample temperature was lower.
基金Project supported by the National Key Research and Development Program of China(Grant No.2017YFA0403300)the National Natural Science Foundation of China(Grant Nos.11627807,11774175,11534004,11774129,and 11604119)+2 种基金the Fundamental Research Funds for the Central Universities of China(Grant No.30916011207)the Jilin Provincial Research Foundation for Basic Research,China(Grant No.20170101153JC)the Science and Technology Project of the Jilin Provincial Education Department,China(Grant No.JJKH20190183KJ)
文摘We macroscopically investigate the effect of the laser intensity and gas density on quantum trajectories in the highorder harmonic generation of Ne atoms irradiated by few-cycle, 800-nm laser pulses. The time–frequency profile of the harmonics shows that the long quantum trajectory is dominant at both lower and higher gas densities for a low laser intensity. At high laser intensities, the long quantum trajectory plays an important role for lower gas densities, while the short quantum trajectory is dominant at higher gas densities. An analysis of the phase mismatch for high-order harmonic generation shows that the primary emission of the quantum trajectories is determined by dynamic changes in the laser electric field during the propagation process.
基金Project supported by the National Key Research and Development Program of China(Grant No.2017YFA0403300)the National Natural Science Foundation of China(Grant Nos.11874179,11574114,and 11874177)the Natural Science Foundation of Jilin Province,China(Grant Nos.20180101289JC)
文摘High-level ab initio calculations of aluminum monoiodide(AlI) molecule are performed by utilizing the multireference configuration interaction plus Davidson correction(MRCI+Q) method. The core-valence correlation(CV) and spin–orbit coupling(SOC) effect are considered. The adiabatic potential energy curves(PECs) of a total of 13 Λ–S states and 24 ? states are computed. The spectroscopic constants of bound states are determined, which are in accordance with the results of the available experimental and theoretical studies. The interactions between the Λ–S states are analyzed with the aid of the spin–orbit matrix elements. Finally, the transition properties including transition dipole moment(TDM),Frank–Condon factors(FCF) and radiative lifetime are obtained based on the computed PEC. Our study sheds light on the electronic structure and spectroscopy of low-lying electronic states of the AlI molecule.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11604052,11404180,and 11574114)the Natural Science Foundation of Heilongjiang Province,China(Grant No.A2015010)+3 种基金the Natural Science Foundation of Anhui Province,China(Grant No.1608085MA10)the International Science&Technology Cooperation Program of Anhui Province,China(Grant No.1403062027)the University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province,China(Grant No.2015095)the Natural Science Foundation of Jilin Province,China(Grant No.20150101003JC)
文摘Cd F molecule, which plays an important role in a great variety of research fields, has long been subject to numerous researchers. Due to the unstable nature and heavy atom Cd containing in the Cd F molecule, electronic states of the molecule have not been well studied. In this paper, high accurate ab initio calculations on the Cd F molecule have been performed at the multi-reference configuration interaction level including Davidson correction(MRCI + Q). Adiabatic potential energy curves(PECs) of the 14 low-lying Λ–S states correlating with the two lowest dissociation limits Cd(~1S_g) + F(~2P_u) and Cd(~3P_u) + F(~2P_u) have been constructed. For the bound Λ–S and ? states, the dominant electronic configurations and spectroscopic constants are obtained,and the calculated spectroscopic constants of bound states are consistent with previous experimental results. The dipole moments(DMs) of 2 Σ+ and 2Π are determined, and the spin–orbit(SO) matrix elements between each pair of X2Σ+, 22Σ+, 12Π, and 22Π are obtained. The results indicate that the sudden changes of DMs and SO matrix elements arise from the variation of the electronic configurations around the avoided crossing region. Moreover,the Franck–Condon factors(FCFs), the transition dipole moments(TDMs), and radiative lifetimes of low-lying states-the ground state X2Σ+are determined. Finally, the transitional properties of 22Π–X2Σ+and 22Σ+–X2Σ+are studied. Based on our computed spectroscopic information of Cd F, the feasibility and challenge for laser cooling of Cd F molecule are discussed.
基金support by National Natural Science Foundation of China (Grant Nos. 11674128, 11504129, and 11674124)Jilin Province Scientific and Technological Development Program, China (Grant No. 20170101063JC)Fundamental Research Project of Chinese State Key Laboratory of Laser Interaction with Matter (Grant No. SKLLIM1605)
文摘In double-pulse laser-induced breakdown spectroscopy(DP-LIBS), the collinear femtosecond double-pulse laser configuration is experimentally investigated with different initial sample temperatures using a Ti:sapphire laser. The glass sample is ablated to produce the plasma spectroscopy. During the experiment, the detected spectral lines include two Na(I) lines(589.0 nm and 589.6 nm) and one Ca(I) line at the wavelength of 585.7 nm. The emission lines are measured at room temperature(22 ℃) and three higher initial sample temperatures(T_s?=?100 ℃, 200 ℃, and 250 ℃). The inter-pulse delay time ranges from-250 ps to 250 ps.The inter-pulse delay time and the sample temperature strongly influence the spectral intensity,and the spectral intensity can be significantly enhanced by increasing the sample temperature and selecting the optimized inter-pulse time. For the same inter-pulse time of 0 ps(single-pulse LIBS), the enhancement ratio is approximately 2.5 at T_s?=?200 ℃ compared with that obtained at T_s?=?22 ℃. For the same inter-pulse time of 150 ps, the enhancement ratio can be up to 4 at T_s?=?200 ℃ compared with that obtained at T_s?=?22 ℃. The combined enhancement effects of the different initial sample temperatures and the double-pulse configuration in femtosecond LIBS are much stronger than that of the different initial sample temperatures or the double-pulse configuration only.
基金Project supported by the National Key Research and Development Program of China(Grant No.2017YFA0403300)the National Natural Science Foundation of China(Grants Nos.11774129,11274141,11627807,11604119,and 11534004)the Jilin Provincial Research Foundation for Basic Research,China(Grant No.20170101153JC)
文摘We theoretically investigate the photoelectron emission from an atom irradiated by an amplitude modulated sinusoidally phase-modulated pulse through solving the time-dependent Schr¨odinger equation in the momentum space. By controlling the phase amplitude of the pulse in the frequency domain, it can be found that the photoelectron spectra appear as explicit interference phenomena, which originated from the interference between the directly ionized electron and the ionization of the pre-excited atom from different subpulses.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11534004,11627807,11774131,and 11774130)the Scientific and Technological Project of Jilin Provincial Education Department in the Thirteenth Five-Year Plan,China(Grant No.JJKH20170538KJ)
文摘We present a parallel numerical method of simulating the interaction of atoms with a strong laser field by solving the time-depending Schrodinger equation(TDSE)in spherical coordinates.This method is realized by combining constructing block diagonal matrices through using the real space product formula(RSPF)with splitting out diagonal sub-matrices for short iterative Lanczos(SIL)propagator.The numerical implementation of the solver guarantees efficient parallel computing for the simulation of real physical problems such as high harmonic generation(HHG)in these interaction systems.
