In high harmonic generation(HHG),Laguerre–Gaussian(LG) beams are used to generate extreme ultraviolet(XUV)vortices with well-defined orbital angular momentum(OAM),which have potential applications in fields such as m...In high harmonic generation(HHG),Laguerre–Gaussian(LG) beams are used to generate extreme ultraviolet(XUV)vortices with well-defined orbital angular momentum(OAM),which have potential applications in fields such as microscopy and spectroscopy.An experimental study on the HHG driven by vortex and Gaussian beams is conducted in this work.It is found that the intensity of vortex harmonics is positively correlated with the laser energy and gas pressure.The structure and intensity distribution of the vortex harmonics exhibit significant dependence on the relative position between the gas jet and the laser focus.The ring-like structures observed in the vortex harmonics,and the interference of quantum paths provide an explanation for the distinct structural characteristics.Moreover,by adjusting the relative position between the jet and laser focus,it is possible to discern the contributions from different quantum paths.The optimization of the HH vortex field is applicable to the XUV,which opens up a new way for exploiting the potential in optical spin or manipulating electrons by using the photon with tunable orbital angular momentum.展开更多
High-order harmonic generation(HHG) of Ar atom in an elliptically polarized intense laser field is experimentally investigated in this work.Interestingly,the anomalous ellipticity dependence on the laser ellipticity(...High-order harmonic generation(HHG) of Ar atom in an elliptically polarized intense laser field is experimentally investigated in this work.Interestingly,the anomalous ellipticity dependence on the laser ellipticity(ε) in the lower-order harmonics is observed,specifically in the 13rd-order,which displays a maximal harmonic intensity at ε ≈ 0.1,rather than at ε = 0 as expected.This contradicts the general trend of harmonic yield,which typically decreases with the increase of laser ellipticity.In this study,we attribute this phenomenon to the disruption of the symmetry of the wave function by the Coulomb effect,leading to the generation of a harmonic with high ellipticity.This finding provides valuable insights into the behavior of elliptically polarized harmonics and opens up a potential way for exploring new applications in ultrafast spectroscopy and light–matter interactions.展开更多
Ionization and dissociation of linear triatomic molecules, carbon dioxide, are studied in 50-fs 800-nm strong laser fields using time-of-flight mass spectrometer. The yields of double charged ions CO2^2+ and various ...Ionization and dissociation of linear triatomic molecules, carbon dioxide, are studied in 50-fs 800-nm strong laser fields using time-of-flight mass spectrometer. The yields of double charged ions CO2^2+ and various fragment ions(CO^+,O^n+, and C^n+(n = 1, 2)) are measured as a function of ellipticity of laser polarization in the intensity range from 5.0 ×10^13W/cm2 to 6.0 × 10^14W/cm^2. The results demonstrate that non-sequential double ionization, which is induced by laser-driven electron recollision, dominates double ionization of CO2 in the strong IR laser field with intensity lower than2.0 × 10^14W/cm^2. The electron recollision could also have contribution in strong-field multiple ionization and formation of fragments of CO2 molecules. The present study indicates that the intensity and ellipticity dependence of ions yields can be used to probe the complex dynamics of strong-field ionization/dissociation of polyatomic molecules.展开更多
The potential energy curves, spectroscopic constants, and low-lying vibration–rotation levels of ground-state O2 and its cation O2+ and anion O2- were calculated with the explicitly correlated multireference configur...The potential energy curves, spectroscopic constants, and low-lying vibration–rotation levels of ground-state O2 and its cation O2+ and anion O2- were calculated with the explicitly correlated multireference configuration interaction method.The zeroth-order reference wavefunction was treated with the complete active space multiconfigurational self-consistent field method, in which the active space was carefully selected, and an additional molecular orbital πu was added into the full valence active space.The electron correlation of the 1s core in the oxygen atom was considered in the computations.The Davidson correction on molecular energy was considered to account for higher electron excitation.The relativistic effects, including the scalar relativistic effect and spin–orbit coupling, were considered in the computation of potential energy curves.These physical effects on the spectroscopic constants were examined.The low-lying levels of vibration–rotation spectra of O2 and its ions were determined based on the computed potential energy curves.Comparisons with available experiments were made and excellent agreement was obtained for the vibrational and rotational parameters.The spectroscopic constants and vibration–rotation spectrum of O2-, which is sparse in experiments, were provided.Our study will shed some light on further theoretical and experimental studies on these simple but important molecular systems.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
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 accomplish a laboratory facility for producing a femtosecond XUV coherent monochromatic radiation with a broad tunable spectral range of 20 eV-75 eV. It is based on spectral selected single-order harmonics from int...We accomplish a laboratory facility for producing a femtosecond XUV coherent monochromatic radiation with a broad tunable spectral range of 20 eV-75 eV. It is based on spectral selected single-order harmonics from intense laser driven high harmonic generation in gas phase. The time preserving for the selected harmonic radiation is achieved by a Czerny-Turner type monochromator designed with a conical diffraction grating mount for minimizing the time broadening caused by grating diffraction and keeping a relatively high diffraction efficiency. Our measurement shows that the photon flux of the 23-order harmonic(H23) centered at 35.7 eV is 1×10~9 photons/s approximately with a resolving power E/?E ≈ 36.This source provides an ultrashort tunable monochromatic XUV beam for ultrafast studies of electronic and structural dynamics in a large variety of matters.展开更多
We experimentally investigated the high-order harmonic generation(HHG)from aligned O_(2) and N_(2) molecules in a linearly polarized laser field,and presented the dependence of the harmonic spectrum on the driving las...We experimentally investigated the high-order harmonic generation(HHG)from aligned O_(2) and N_(2) molecules in a linearly polarized laser field,and presented the dependence of the harmonic spectrum on the driving laser intensity and molecular alignment angle.The minimum position of HHG of O_(2) varies with changing the laser intensity,which is caused by multi-orbital interference.However,the location of the observed minimum structure in N_(2) harmonic spectrum remained unchanged upon changing the laser intensity.The mechanism of the spectral minimum for N_(2) case is regarded as a Cooperlike minimum in HHG associated with the molecular electronic structure.This work indicates that harmonic spectroscopy can effectively uncover information about molecular structure and electron dynamics.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11974137,92250306,and 12304302)the National Key Program for Science and Technology Research and Development(Grant No.2019YFA0307700)+1 种基金the Natural Science Foundation of Jilin Province,China(Grant Nos.YDZJ202101ZYTS157 and YDZJ202201ZYTS314)the Scientific Research Foundation of Jilin Provincial Education Department,China(Grant No.JJKH20230283KJ)。
文摘In high harmonic generation(HHG),Laguerre–Gaussian(LG) beams are used to generate extreme ultraviolet(XUV)vortices with well-defined orbital angular momentum(OAM),which have potential applications in fields such as microscopy and spectroscopy.An experimental study on the HHG driven by vortex and Gaussian beams is conducted in this work.It is found that the intensity of vortex harmonics is positively correlated with the laser energy and gas pressure.The structure and intensity distribution of the vortex harmonics exhibit significant dependence on the relative position between the gas jet and the laser focus.The ring-like structures observed in the vortex harmonics,and the interference of quantum paths provide an explanation for the distinct structural characteristics.Moreover,by adjusting the relative position between the jet and laser focus,it is possible to discern the contributions from different quantum paths.The optimization of the HH vortex field is applicable to the XUV,which opens up a new way for exploiting the potential in optical spin or manipulating electrons by using the photon with tunable orbital angular momentum.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.92250306,11974137,and 12304302)the National Key Program for Science and Technology Research and Development of China(Grant No.2019YFA0307700)+1 种基金the Natural Science Foundation of Jilin Province,China(Grant Nos.YDZJ202101ZYTS157 and YDZJ202201ZYTS314)the Scientific Research Foundation of the Education Department of Jilin Province,China(Grant No.JJKH20230283KJ)。
文摘High-order harmonic generation(HHG) of Ar atom in an elliptically polarized intense laser field is experimentally investigated in this work.Interestingly,the anomalous ellipticity dependence on the laser ellipticity(ε) in the lower-order harmonics is observed,specifically in the 13rd-order,which displays a maximal harmonic intensity at ε ≈ 0.1,rather than at ε = 0 as expected.This contradicts the general trend of harmonic yield,which typically decreases with the increase of laser ellipticity.In this study,we attribute this phenomenon to the disruption of the symmetry of the wave function by the Coulomb effect,leading to the generation of a harmonic with high ellipticity.This finding provides valuable insights into the behavior of elliptically polarized harmonics and opens up a potential way for exploring new applications in ultrafast spectroscopy and light–matter interactions.
基金supported by the National Natural Science Foundation of China(No.U1532138,No.11474130,and No.91750104)the Natural Science Foundation of Jilin Province,China(No.20180101289JC and No.20160101332JC)
基金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Ionization and dissociation of linear triatomic molecules, carbon dioxide, are studied in 50-fs 800-nm strong laser fields using time-of-flight mass spectrometer. The yields of double charged ions CO2^2+ and various fragment ions(CO^+,O^n+, and C^n+(n = 1, 2)) are measured as a function of ellipticity of laser polarization in the intensity range from 5.0 ×10^13W/cm2 to 6.0 × 10^14W/cm^2. The results demonstrate that non-sequential double ionization, which is induced by laser-driven electron recollision, dominates double ionization of CO2 in the strong IR laser field with intensity lower than2.0 × 10^14W/cm^2. The electron recollision could also have contribution in strong-field multiple ionization and formation of fragments of CO2 molecules. The present study indicates that the intensity and ellipticity dependence of ions yields can be used to probe the complex dynamics of strong-field ionization/dissociation of polyatomic molecules.
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.91750104,11574114,and 11874177)the Natural Science Foundation of Jilin Province,China(Grant No.20160101332JC)
文摘The potential energy curves, spectroscopic constants, and low-lying vibration–rotation levels of ground-state O2 and its cation O2+ and anion O2- were calculated with the explicitly correlated multireference configuration interaction method.The zeroth-order reference wavefunction was treated with the complete active space multiconfigurational self-consistent field method, in which the active space was carefully selected, and an additional molecular orbital πu was added into the full valence active space.The electron correlation of the 1s core in the oxygen atom was considered in the computations.The Davidson correction on molecular energy was considered to account for higher electron excitation.The relativistic effects, including the scalar relativistic effect and spin–orbit coupling, were considered in the computation of potential energy curves.These physical effects on the spectroscopic constants were examined.The low-lying levels of vibration–rotation spectra of O2 and its ions were determined based on the computed potential energy curves.Comparisons with available experiments were made and excellent agreement was obtained for the vibrational and rotational parameters.The spectroscopic constants and vibration–rotation spectrum of O2-, which is sparse in experiments, were provided.Our study will shed some light on further theoretical and experimental studies on these simple but important molecular systems.
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.
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(Grants Nos.11627807,11127403,and 11474130)the National Basic Research Program of China(Grant No.2013CB922200)the Natural Science Foundation of Jilin Province of China(Grant No.20160101332JC)
文摘We accomplish a laboratory facility for producing a femtosecond XUV coherent monochromatic radiation with a broad tunable spectral range of 20 eV-75 eV. It is based on spectral selected single-order harmonics from intense laser driven high harmonic generation in gas phase. The time preserving for the selected harmonic radiation is achieved by a Czerny-Turner type monochromator designed with a conical diffraction grating mount for minimizing the time broadening caused by grating diffraction and keeping a relatively high diffraction efficiency. Our measurement shows that the photon flux of the 23-order harmonic(H23) centered at 35.7 eV is 1×10~9 photons/s approximately with a resolving power E/?E ≈ 36.This source provides an ultrashort tunable monochromatic XUV beam for ultrafast studies of electronic and structural dynamics in a large variety of matters.
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.91750104 and 11974137)the Natural Science Foundation of Jilin Province,China(Grant No.YDZJ202101ZYTS157).
文摘We experimentally investigated the high-order harmonic generation(HHG)from aligned O_(2) and N_(2) molecules in a linearly polarized laser field,and presented the dependence of the harmonic spectrum on the driving laser intensity and molecular alignment angle.The minimum position of HHG of O_(2) varies with changing the laser intensity,which is caused by multi-orbital interference.However,the location of the observed minimum structure in N_(2) harmonic spectrum remained unchanged upon changing the laser intensity.The mechanism of the spectral minimum for N_(2) case is regarded as a Cooperlike minimum in HHG associated with the molecular electronic structure.This work indicates that harmonic spectroscopy can effectively uncover information about molecular structure and electron dynamics.