High harmonic generation(HHG) driven by intense frequency-comb laser fields can be dramatically enhanced via multiphoton resonance by tuning the carrier-envelope phase(CEP) shift, without increasing the driving in...High harmonic generation(HHG) driven by intense frequency-comb laser fields can be dramatically enhanced via multiphoton resonance by tuning the carrier-envelope phase(CEP) shift, without increasing the driving intensity. However,the multiphoton-resonant enhancement(MRE) factor in the realistic atomic hydrogen is much smaller than that in a twolevel system. To study the deviation, we present a theoretical investigation of the multiphoton resonance dynamics of three-level systems driven by intense frequency-comb laser fields. The many-mode Floquet theorem(MMFT) is employed to provide a nonperturbative and exact treatment of the interaction between the quantum system and the laser fields. The investigations show that the dipole interaction of a two-level system with the third level affects the multiphoton resonance dynamics and enhances the HHG spectra. It is the dipole interaction of the excited level of the two-level system with other levels that results in the smaller MRE factor in the realistic atomic system.展开更多
We investigate experimentally multi-orbital effects in high-order harmonic generation(HHG) from aligned CO2 and N2O molecules by intense femtosecond laser fields with linear and elliptical polarizations.For either of ...We investigate experimentally multi-orbital effects in high-order harmonic generation(HHG) from aligned CO2 and N2O molecules by intense femtosecond laser fields with linear and elliptical polarizations.For either of the aligned molecules, a minimum in the harmonic spectrum is observed, the position of which shifts to lower-order harmonics when decreasing the intensity or increasing the ellipticity of the driving laser.This indicates that the minimum originates from the dynamic interference of different channels, of which the tunneling ionization and recombination are contributed via different molecular orbitals.The results show that both the highest occupied molecular orbital(HOMO) and low-lying HOMO-2 in CO2(or HOMO-1 in N2O) contribute to the molecular HHG in both linearly and elliptically polarized strong laser fields.Our study would pave a way for understanding multi-electron dynamics from polyatomic molecules irradiated by strong laser fields.展开更多
We perform an experimental study of the multi-orbital effect on the high-order harmonic generation(HHG) from aligned N_2 molecules in both linearly and elliptically polarized intense laser fields.Measured by a home-bu...We perform an experimental study of the multi-orbital effect on the high-order harmonic generation(HHG) from aligned N_2 molecules in both linearly and elliptically polarized intense laser fields.Measured by a home-built extreme ultraviolet(XUV) flat grating spectrometer with the pump-probe method, the angular distributions of different orders of HHG are obtained, which show distinctive behaviors for harmonics in the plateau and the cut-off regions.The ellipticity dependence of HHG is investigated by aligning the molecular axis parallel or perpendicular to the laser polarization.Our results indicate that both the highest occupied molecular orbital(HOMO) as well as the lower one(HOMO-1) contribute to the HHG of N2 molecules, in either linearly or elliptically polarized intense laser field.The study paves the way for understanding the ultrafast electron dynamics of molecules exposed to an intense laser field.展开更多
The propagation of optical solitons in fiber amplifiers is discussed by considering a model that includes linear high order dispersion, two photon absorption, nonlinear high order dispersion, self induced Ramam and fi...The propagation of optical solitons in fiber amplifiers is discussed by considering a model that includes linear high order dispersion, two photon absorption, nonlinear high order dispersion, self induced Ramam and five order nonlinear effects. Based on travelling wave method, the solutions of the nonlinear Schr dinger equations, and the influence on soliton propagation as well as high order effect in the fiber amplifier are discussed in detail. It is found that because of existing five order nonlinear effect, the solution is not of secant hyperbola type, but shows high gain state of the fiber amplifier which is very favourable to the propagation of solitons.展开更多
The laser phase effect on the spatial distribution of the molecular high-order harmonic generation(MHHG) spectrum from H_2~+ is theoretically investigated through solving the Non-Bohn-Oppenheimer(NBO) time-depend...The laser phase effect on the spatial distribution of the molecular high-order harmonic generation(MHHG) spectrum from H_2~+ is theoretically investigated through solving the Non-Bohn-Oppenheimer(NBO) time-dependent Schrodinger equation(TDSE).The results are shown as follows,(i) The generated harmonics from the two nuclei each present an asymmetric distribution.Particularly,when the laser phases are chosen from 0.0π to 0.6π and from 1.7π to 2.0π,the contribution from the negative-H plays a main role in harmonic generation.When the laser phases are chosen from 0.7πto 1.6k,the contribution from the positive-H to the harmonic generation is remarkably enhanced and becomes greater than that from the negative-H.The electron localization,the time-frequency analyses of the harmonic spectrum and the time-dependent wave function are shown to explain the asymmetric harmonic distribution in H_2~+,which provides us with a method to control the electron motion in molecules,(ⅱ) As the pulse duration increases,the asymmetric distributions of the MHHG in two H nuclei decrease,(ⅲ) Isotope investigation shows that the asymmetric harmonic distribution can be reduced by introducing the heavy nucleus(i.e.,D_2~+).展开更多
This report investigated the ordering of the alky chain of sphingomyelin (SMs) monolayers induced by cholesterol at the air/water interface using high-resolution broadband sum frequency generation vibrational spectr...This report investigated the ordering of the alky chain of sphingomyelin (SMs) monolayers induced by cholesterol at the air/water interface using high-resolution broadband sum frequency generation vibrational spectroscopy (HR-BB-SFG-VS). The SFG spectra of the three nature sphingomyelin/cholesterol mixture monolayers with two concentrations of the cholesterol at the air/water interface are performed under different polarization combination. A new resolved CH2 symmetric stretching (d+, ~2834 cm-1) and the CH3 symmetric stretching (r+, ~2874 cm-1) mode are applied to characterize the conformational order in the sphingomyelin/cholesterol mixture monolayers. It was found that the cholesterol make the sphingosine backbones more conformational order. During this process, the conformational order of the N-linked acyl chain remains unaltered. Moreover, the sphingosine backbones of SMs have much larger contributions to gauche defects of SMs than one in the N-linked acyl chain. These results presented here not only shed lights on understanding of the interactions of sphingomyelin molecules with cholesterol molecules at interface but also demonstrates the ability of HR-BB-SFG to probe such complicated molecular systems.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11374239,21203144,and 11074199)the Doctoral Fund of Ministry of Education of China(Grant No.20120201120056)the Fundamental Research Funds for the Central Universities,China
文摘High harmonic generation(HHG) driven by intense frequency-comb laser fields can be dramatically enhanced via multiphoton resonance by tuning the carrier-envelope phase(CEP) shift, without increasing the driving intensity. However,the multiphoton-resonant enhancement(MRE) factor in the realistic atomic hydrogen is much smaller than that in a twolevel system. To study the deviation, we present a theoretical investigation of the multiphoton resonance dynamics of three-level systems driven by intense frequency-comb laser fields. The many-mode Floquet theorem(MMFT) is employed to provide a nonperturbative and exact treatment of the interaction between the quantum system and the laser fields. The investigations show that the dipole interaction of a two-level system with the third level affects the multiphoton resonance dynamics and enhances the HHG spectra. It is the dipole interaction of the excited level of the two-level system with other levels that results in the smaller MRE factor in the realistic atomic system.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.91750104,11534004,11874179,11127403,11474130)the Natural Science Foundation of Jilin Province,China(Grant No.20180101289JC)
文摘We investigate experimentally multi-orbital effects in high-order harmonic generation(HHG) from aligned CO2 and N2O molecules by intense femtosecond laser fields with linear and elliptical polarizations.For either of the aligned molecules, a minimum in the harmonic spectrum is observed, the position of which shifts to lower-order harmonics when decreasing the intensity or increasing the ellipticity of the driving laser.This indicates that the minimum originates from the dynamic interference of different channels, of which the tunneling ionization and recombination are contributed via different molecular orbitals.The results show that both the highest occupied molecular orbital(HOMO) and low-lying HOMO-2 in CO2(or HOMO-1 in N2O) contribute to the molecular HHG in both linearly and elliptically polarized strong laser fields.Our study would pave a way for understanding multi-electron dynamics from polyatomic molecules irradiated by strong laser fields.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.91750104,11127403,and 11474130)the Natural Science Foundation of Jilin Province,China(Grant No.20160101332JC)
文摘We perform an experimental study of the multi-orbital effect on the high-order harmonic generation(HHG) from aligned N_2 molecules in both linearly and elliptically polarized intense laser fields.Measured by a home-built extreme ultraviolet(XUV) flat grating spectrometer with the pump-probe method, the angular distributions of different orders of HHG are obtained, which show distinctive behaviors for harmonics in the plateau and the cut-off regions.The ellipticity dependence of HHG is investigated by aligning the molecular axis parallel or perpendicular to the laser polarization.Our results indicate that both the highest occupied molecular orbital(HOMO) as well as the lower one(HOMO-1) contribute to the HHG of N2 molecules, in either linearly or elliptically polarized intense laser field.The study paves the way for understanding the ultrafast electron dynamics of molecules exposed to an intense laser field.
文摘The propagation of optical solitons in fiber amplifiers is discussed by considering a model that includes linear high order dispersion, two photon absorption, nonlinear high order dispersion, self induced Ramam and five order nonlinear effects. Based on travelling wave method, the solutions of the nonlinear Schr dinger equations, and the influence on soliton propagation as well as high order effect in the fiber amplifier are discussed in detail. It is found that because of existing five order nonlinear effect, the solution is not of secant hyperbola type, but shows high gain state of the fiber amplifier which is very favourable to the propagation of solitons.
基金Project supported by the National Natural Science Foundation of China(Grant No.11504151)the Doctoral Scientific Research Foundation of Liaoning Province,China(Grant No.201501123)the Scientific Research Foundation of Liaoning Provincial Education Department,China(Grant No.L2014242)
文摘The laser phase effect on the spatial distribution of the molecular high-order harmonic generation(MHHG) spectrum from H_2~+ is theoretically investigated through solving the Non-Bohn-Oppenheimer(NBO) time-dependent Schrodinger equation(TDSE).The results are shown as follows,(i) The generated harmonics from the two nuclei each present an asymmetric distribution.Particularly,when the laser phases are chosen from 0.0π to 0.6π and from 1.7π to 2.0π,the contribution from the negative-H plays a main role in harmonic generation.When the laser phases are chosen from 0.7πto 1.6k,the contribution from the positive-H to the harmonic generation is remarkably enhanced and becomes greater than that from the negative-H.The electron localization,the time-frequency analyses of the harmonic spectrum and the time-dependent wave function are shown to explain the asymmetric harmonic distribution in H_2~+,which provides us with a method to control the electron motion in molecules,(ⅱ) As the pulse duration increases,the asymmetric distributions of the MHHG in two H nuclei decrease,(ⅲ) Isotope investigation shows that the asymmetric harmonic distribution can be reduced by introducing the heavy nucleus(i.e.,D_2~+).
基金the National Natural Science Foundation of China(No.21227802)the National Natural Science Foundation of China(Nos. 21503235, 21673251)the ICCAS for Start-up Funding
文摘This report investigated the ordering of the alky chain of sphingomyelin (SMs) monolayers induced by cholesterol at the air/water interface using high-resolution broadband sum frequency generation vibrational spectroscopy (HR-BB-SFG-VS). The SFG spectra of the three nature sphingomyelin/cholesterol mixture monolayers with two concentrations of the cholesterol at the air/water interface are performed under different polarization combination. A new resolved CH2 symmetric stretching (d+, ~2834 cm-1) and the CH3 symmetric stretching (r+, ~2874 cm-1) mode are applied to characterize the conformational order in the sphingomyelin/cholesterol mixture monolayers. It was found that the cholesterol make the sphingosine backbones more conformational order. During this process, the conformational order of the N-linked acyl chain remains unaltered. Moreover, the sphingosine backbones of SMs have much larger contributions to gauche defects of SMs than one in the N-linked acyl chain. These results presented here not only shed lights on understanding of the interactions of sphingomyelin molecules with cholesterol molecules at interface but also demonstrates the ability of HR-BB-SFG to probe such complicated molecular systems.