Employing the two-state model and the time-dependent wave packet method, we have investigated the influences of the parameters of the intense femtosecond laser field on the evolution of the wave packet, as well as the...Employing the two-state model and the time-dependent wave packet method, we have investigated the influences of the parameters of the intense femtosecond laser field on the evolution of the wave packet, as well as the population of ground and double-minimum electronic states of the NaRb molecule. For the different laser wavelengths, the evolution of the wave packet of 6{ }^1／Sigma ^ ＋ state with time and internuclear distance is different, and the different laser intensity brings different influences on the population of the electronic states of the NaRb molecule. One can control the evolutions of wave packet and the population in each state by varying the laser parameters appropriately, which will be a benefit for the light manipulation of atomic and molecular processes.展开更多
Using a neutral N2 beam as target, this paper studies the dissociation of N2^＋ in intense femtosecond laser fields （45 fs, ～ 1 × 10^16 W/cm^2） at the laser wavelength of 800 nm based on the time-of-flight mas...Using a neutral N2 beam as target, this paper studies the dissociation of N2^＋ in intense femtosecond laser fields （45 fs, ～ 1 × 10^16 W/cm^2） at the laser wavelength of 800 nm based on the time-of-flight mass spectra of N＋ fragment ions. The angular distributions of N^＋ and the laser power dependence of N^＋ yielded from different dissociation pathways show that the dissociation mechanisms mainly proceed through the couplings between the metastable states （A, B and C） and the upper excited states of N^＋.A coupling model of light-dressed potential energy curves of N2^＋ is used to interpret the kinetic energy release of N^＋.展开更多
Photodissociation of cyclopentanone (C5H8O) and cyclohexanone (C6H10O) was studied with 800nm, 50fs laser pulse at intensities of 5.0 - 13.0x10(13) W/cm(2). A time of flight mass spectrometer was employed to detect th...Photodissociation of cyclopentanone (C5H8O) and cyclohexanone (C6H10O) was studied with 800nm, 50fs laser pulse at intensities of 5.0 - 13.0x10(13) W/cm(2). A time of flight mass spectrometer was employed to detect the ion signals. Parent ions dominated at lower laser intensities. Fragmentation of the parent ions increases with increasing laser intensity and molecular size. The fragmentation mechanism was discussed.展开更多
Ionization and dissociation of nitrosyl chloride CINO were studied using femtosecond laser mass spectra technique. Strong fragmental ions NO^＋ and Cl^＋ were observed with the laser intensity varied from 3.2× 10...Ionization and dissociation of nitrosyl chloride CINO were studied using femtosecond laser mass spectra technique. Strong fragmental ions NO^＋ and Cl^＋ were observed with the laser intensity varied from 3.2× 10^14 to 2.5×10^15 W/cm^2. These fragmental ions were attributed to the direct dissociation of the parent ions. Electronic structure calculations were also carried out with Hartree-Fock, density functional and correlated levels of theory to understand the possible fragmentation pathways. The very low N-Cl bond energy in the parent ion of nitrosyl chloride is a clear reason for the absence of CINO^＋ and CIN^＋ ion peaks from the femtosecond laser mass spectrum.展开更多
We studied the ionization and dissociation of polyatomic molecule methane in an intense femtosecond laser field with wavelength of 810 nm and intensities ranging from 1.4 × 1014 to 2.6× 1015 W/cm2 by mass sp...We studied the ionization and dissociation of polyatomic molecule methane in an intense femtosecond laser field with wavelength of 810 nm and intensities ranging from 1.4 × 1014 to 2.6× 1015 W/cm2 by mass spectroscopy. Abundant fragment ions were observed in addition to the strong parent ion. The effect of frequency chirp was investigated and it was found that the negatively chirped pulses dramatically enhanced the dissociation probability, which might, be used to control the dissociation pathways.展开更多
Methanol was irradiated by 80 fs laser pulse, intensity range of 1013-1014 W/cm2. A TOF-mass spectrometer was coupled to the laser system and used to detect the ions produced. The parent ions CH3OH+ appeared firstly a...Methanol was irradiated by 80 fs laser pulse, intensity range of 1013-1014 W/cm2. A TOF-mass spectrometer was coupled to the laser system and used to detect the ions produced. The parent ions CH3OH+ appeared firstly at the laser intensity of 1.4 ×1013 W/cm2. While the laser intensity was gradually increased, the parent ions were dissociated and the primary ions CH2OH+ were given as verified from the irradiation of deuterated methanol (CH3OD) showing the C-H bond cracking firstly. While the laser intensity was further increased to 2.0 ×1013 W/cm2, the C-O bonds of the parent ions also broke to give CH3+. When the laser intensity was higher, smaller fragment ions like CH+, C+, OH+ and O+ also appeared. Among the fragment ions, only H+ ion yield had anisotropic angular distribution dependence on the laser polarization vector in the dissociation of methanol. All the experimental observations show that the dissociation of methanol proceeds through stepwise mechanism but not Coulomb explosion.展开更多
The laser pulse width effect on the dis- sociation probability of CH4+ irradiated by an ultrafast laser has been investigated experimentally and theoretically. The femtosecond laser at 800 nm with an intensity of 8.0 ...The laser pulse width effect on the dis- sociation probability of CH4+ irradiated by an ultrafast laser has been investigated experimentally and theoretically. The femtosecond laser at 800 nm with an intensity of 8.0 × 1013 W/cm2 was used. The ob- served relative yield of the primary fragment ion CH3+ increases with increasing pulse width and tends to saturate when the pulse width is longer than 120 fs. The field-assisted dissociation (FAD) model and quasi-classical trajectory (QCT) calculation were ap- plied to predicting the dissociation probability of CH4+. The calculated probability is corrected with the mo- lecular orientation effect and the spatial distribution of laser intensity. The modified results show that the dissociation requires at least 23 fs and saturates with long pulse widths (≥100 fs). The result is ap- proximately consistent with the experimental observa- tion.展开更多
Experimental investigations on the dis-sociation and ionization processes of NO2 in intensefields at wavelengths of 810, 405 and 270 nm, arepresented. The ratios of NO +2 /NO + are found to beindependent of the laser ...Experimental investigations on the dis-sociation and ionization processes of NO2 in intensefields at wavelengths of 810, 405 and 270 nm, arepresented. The ratios of NO +2 /NO + are found to beindependent of the laser intensity at these threewavelengths, but show strong dependence on thewavelengths. Longer wavelength produces a largerparent-ion yield in comparison with 405 nm. Peakprofiles of all the fragment ions clearly show little ki-netic energy releasing during the dissociation. Frag-ment ions are suggested to be produced from disso-ciation of the field ionized parent ions. Our resultsindicate that laser pulse wavelengths are the mostimportant parameters in ionization-fragmen- tationprocess of polyatomic molecules in intense field otherthan the laser intensity.展开更多
We present in this paper an investigation of the nonlinear process of above-threshold ionization. The process arises when an atomic or molecular system, exposed to an intense laser pulse, continues to absorb more phot...We present in this paper an investigation of the nonlinear process of above-threshold ionization. The process arises when an atomic or molecular system, exposed to an intense laser pulse, continues to absorb more photons than that needed for the ionization to occur. We trigger this nonlinear process in a simple molecular system by exposing it to an intense transform-limited Gaussian laser pulse of 267-nm wavelength which is the third harmonic of an 800-nm wavelength Tisapphire laser. We explore the characteristics of the process by analyzing the kinetic-energy spectra of the electrons ejected from the molecular system under different laser peak intensities.展开更多
利用强场近似(Strong field approximation,SFA)方法研究氢负离子(H^-)在强激光场中双光子电离的能量谱,所得到的电离谱随角度的变化规律与实验结果符合得很好.进一步的研究表明,H^-离子在强激光场中双光子电离的能量谱与有质动力能有关...利用强场近似(Strong field approximation,SFA)方法研究氢负离子(H^-)在强激光场中双光子电离的能量谱,所得到的电离谱随角度的变化规律与实验结果符合得很好.进一步的研究表明,H^-离子在强激光场中双光子电离的能量谱与有质动力能有关.激光场强度越大,光电子的有质动力能也越大,能量谱向左移动越明显.我们的结果表明,使用强场近似是一种研究负离子在强激光场中电离过程的有效方法.展开更多
基金supported by the National Natural Science Foundation of China (Grant Nos. 10674114 and 10604045)
文摘Employing the two-state model and the time-dependent wave packet method, we have investigated the influences of the parameters of the intense femtosecond laser field on the evolution of the wave packet, as well as the population of ground and double-minimum electronic states of the NaRb molecule. For the different laser wavelengths, the evolution of the wave packet of 6{ }^1／Sigma ^ ＋ state with time and internuclear distance is different, and the different laser intensity brings different influences on the population of the electronic states of the NaRb molecule. One can control the evolutions of wave packet and the population in each state by varying the laser parameters appropriately, which will be a benefit for the light manipulation of atomic and molecular processes.
基金Project supported by the National Natural Science Foundation of China (Grant Nos 10774033,60878018 and 10674036)program for New Century Excellent Talents in University of China (NCET)
文摘Using a neutral N2 beam as target, this paper studies the dissociation of N2^＋ in intense femtosecond laser fields （45 fs, ～ 1 × 10^16 W/cm^2） at the laser wavelength of 800 nm based on the time-of-flight mass spectra of N＋ fragment ions. The angular distributions of N^＋ and the laser power dependence of N^＋ yielded from different dissociation pathways show that the dissociation mechanisms mainly proceed through the couplings between the metastable states （A, B and C） and the upper excited states of N^＋.A coupling model of light-dressed potential energy curves of N2^＋ is used to interpret the kinetic energy release of N^＋.
文摘Photodissociation of cyclopentanone (C5H8O) and cyclohexanone (C6H10O) was studied with 800nm, 50fs laser pulse at intensities of 5.0 - 13.0x10(13) W/cm(2). A time of flight mass spectrometer was employed to detect the ion signals. Parent ions dominated at lower laser intensities. Fragmentation of the parent ions increases with increasing laser intensity and molecular size. The fragmentation mechanism was discussed.
基金Project supported by the Hundred Talent Fund of Chinese Academy of Sciences and the National Natural Science Foundation of China （Nos. 20477047, 20473094）.
文摘Ionization and dissociation of nitrosyl chloride CINO were studied using femtosecond laser mass spectra technique. Strong fragmental ions NO^＋ and Cl^＋ were observed with the laser intensity varied from 3.2× 10^14 to 2.5×10^15 W/cm^2. These fragmental ions were attributed to the direct dissociation of the parent ions. Electronic structure calculations were also carried out with Hartree-Fock, density functional and correlated levels of theory to understand the possible fragmentation pathways. The very low N-Cl bond energy in the parent ion of nitrosyl chloride is a clear reason for the absence of CINO^＋ and CIN^＋ ion peaks from the femtosecond laser mass spectrum.
基金This work was supported by the National Key Basic Research Special Foundation(NKBRSF)under Grant No.G1999075207the National Natural Science Foundation of China under Grant No.19884001,10104003 and 90101027.
文摘We studied the ionization and dissociation of polyatomic molecule methane in an intense femtosecond laser field with wavelength of 810 nm and intensities ranging from 1.4 × 1014 to 2.6× 1015 W/cm2 by mass spectroscopy. Abundant fragment ions were observed in addition to the strong parent ion. The effect of frequency chirp was investigated and it was found that the negatively chirped pulses dramatically enhanced the dissociation probability, which might, be used to control the dissociation pathways.
基金This work was supported by the National Natural Science Foundation of China (Grant No. 29973052) the Ministry of Science & Technology of China.
文摘Methanol was irradiated by 80 fs laser pulse, intensity range of 1013-1014 W/cm2. A TOF-mass spectrometer was coupled to the laser system and used to detect the ions produced. The parent ions CH3OH+ appeared firstly at the laser intensity of 1.4 ×1013 W/cm2. While the laser intensity was gradually increased, the parent ions were dissociated and the primary ions CH2OH+ were given as verified from the irradiation of deuterated methanol (CH3OD) showing the C-H bond cracking firstly. While the laser intensity was further increased to 2.0 ×1013 W/cm2, the C-O bonds of the parent ions also broke to give CH3+. When the laser intensity was higher, smaller fragment ions like CH+, C+, OH+ and O+ also appeared. Among the fragment ions, only H+ ion yield had anisotropic angular distribution dependence on the laser polarization vector in the dissociation of methanol. All the experimental observations show that the dissociation of methanol proceeds through stepwise mechanism but not Coulomb explosion.
文摘The laser pulse width effect on the dis- sociation probability of CH4+ irradiated by an ultrafast laser has been investigated experimentally and theoretically. The femtosecond laser at 800 nm with an intensity of 8.0 × 1013 W/cm2 was used. The ob- served relative yield of the primary fragment ion CH3+ increases with increasing pulse width and tends to saturate when the pulse width is longer than 120 fs. The field-assisted dissociation (FAD) model and quasi-classical trajectory (QCT) calculation were ap- plied to predicting the dissociation probability of CH4+. The calculated probability is corrected with the mo- lecular orientation effect and the spatial distribution of laser intensity. The modified results show that the dissociation requires at least 23 fs and saturates with long pulse widths (≥100 fs). The result is ap- proximately consistent with the experimental observa- tion.
文摘Experimental investigations on the dis-sociation and ionization processes of NO2 in intensefields at wavelengths of 810, 405 and 270 nm, arepresented. The ratios of NO +2 /NO + are found to beindependent of the laser intensity at these threewavelengths, but show strong dependence on thewavelengths. Longer wavelength produces a largerparent-ion yield in comparison with 405 nm. Peakprofiles of all the fragment ions clearly show little ki-netic energy releasing during the dissociation. Frag-ment ions are suggested to be produced from disso-ciation of the field ionized parent ions. Our resultsindicate that laser pulse wavelengths are the mostimportant parameters in ionization-fragmen- tationprocess of polyatomic molecules in intense field otherthan the laser intensity.
文摘We present in this paper an investigation of the nonlinear process of above-threshold ionization. The process arises when an atomic or molecular system, exposed to an intense laser pulse, continues to absorb more photons than that needed for the ionization to occur. We trigger this nonlinear process in a simple molecular system by exposing it to an intense transform-limited Gaussian laser pulse of 267-nm wavelength which is the third harmonic of an 800-nm wavelength Tisapphire laser. We explore the characteristics of the process by analyzing the kinetic-energy spectra of the electrons ejected from the molecular system under different laser peak intensities.
文摘利用强场近似(Strong field approximation,SFA)方法研究氢负离子(H^-)在强激光场中双光子电离的能量谱,所得到的电离谱随角度的变化规律与实验结果符合得很好.进一步的研究表明,H^-离子在强激光场中双光子电离的能量谱与有质动力能有关.激光场强度越大,光电子的有质动力能也越大,能量谱向左移动越明显.我们的结果表明,使用强场近似是一种研究负离子在强激光场中电离过程的有效方法.
