Photodissociation of H2S in the VUV region plays an important role in the atmospheric chemistry and interstellar chemistry.To date,however,few studies have been focused on this topic.In this article,we have described ...Photodissociation of H2S in the VUV region plays an important role in the atmospheric chemistry and interstellar chemistry.To date,however,few studies have been focused on this topic.In this article,we have described a laser dispersion method applied in the apparatus combining the high-n H atom Rydberg tagging time-of-flight technique with the vacuum ultraviolet free electron laser(VUV FEL).The Lyman-αlaser beam(121.6 nm)used in the H-atom detection was generated by the difference frequency four-wave mixing schemes in a Kr/Ar gas cell.After passing through an off-axis biconvex LiF lens,the 121.6 nm beam was dispersed from the 212.6 nm and 845 nm beams due to the different deflection angles experienced by these laser beams at the surfaces of the biconvex lens.This method can eliminate the background signal from the 212.6 nm photolysis.Combined with the VUV FEL,photodissociation of H2S at 122.95 nm was studied successfully.The TOF spectrum was measured and the derived total kinetic energy release spectrum was displayed.The results suggest that the experimental setup is a powerful tool for investigating photodissociation dynamics of molecules in the VUV region which involves the H-atom elimination processes.展开更多
We present the photoelectron momentum distributions(PMDs) and the photoelectron angular distributions(PADs) of He+ ions, aligned H2+ molecules and N2 molecules by intense orthogonally polarized laser pulses. Simulatio...We present the photoelectron momentum distributions(PMDs) and the photoelectron angular distributions(PADs) of He+ ions, aligned H2+ molecules and N2 molecules by intense orthogonally polarized laser pulses. Simulations are performed by numerically solving the corresponding two-dimensional time-dependent Schr?dinger equations(TDSEs) within the single-electron approximation frame. Photoelectron momentum distributions and photoelectron angular distributions present different patterns with the time delays Td, illustrating the dependences of the PMDs and PADs on the time delays by orthogonally polarized laser pulses. The evolution of the electron wavepackets can be employed to describe the intensity of the PADs from the TDSE simulations for N2 molecules.展开更多
We presented an experimental apparatus combining the H-atom Rydberg tagging time-of-flight technique and the laser detonation source for studying crossed beam reactions at hyperthermal collision energies. The prelimin...We presented an experimental apparatus combining the H-atom Rydberg tagging time-of-flight technique and the laser detonation source for studying crossed beam reactions at hyperthermal collision energies. The preliminary study of the F+D2→DF+D reaction at hyperthermal collision energy of 23.84 kJ/mol was performed. Two beam sources were used in this study: one is the hyperthermal F beam source produced by a laser detonation process, and the other is D2 beam source generated by liquid-N2 cooled pulsed valve. Vibrational state-resolved di erential cross sections (DCSs) of product for the title reaction were determined. From the product vibrational state-resolved DCS, it can be concluded that products DF(v'=0, 1, 2, 3) are predominantly distributed in the sideway and backward scattering directions at this collision energy. However, the highest vibrational excited product DF(v'=4), is clearly peaked in the forward direction. The probable dynamical origins for these forward scattering products were analyzed and discussed.展开更多
157 nm photodissociation of jet-cooled CH3OH and C2HsOH was studied using the high-n Rydberg atom time-of-flight （TOF） technique. TOF spectra of nascent H atom products were measured. Simulation of these spectra rev...157 nm photodissociation of jet-cooled CH3OH and C2HsOH was studied using the high-n Rydberg atom time-of-flight （TOF） technique. TOF spectra of nascent H atom products were measured. Simulation of these spectra reveals three different atomic H loss processes： one from hydroxyl H elimination, one from methyl （ethyl） H elimination, and one from secondary dissociation of the methoxy （ethoxy） radical. The relative branching ratio indicates secondary dissociation of ethoxy is less important than that of methoxy. The average angular anisotropy parameter of methanol is negative （with β≈-0.3）, indicating the transition dipole moment is perpendicular to the C-O-H plane. The slightly more negative β value of ethanol （with β≈-0.4） implies that ethanol has a longer rotational period. These experimental results indicate that both systems undergo fast internal conversion to the 3s surface after it is excited to the 3px surface, and then dissociate on the 3s surface. The translational energy distribution of the CH3O＋H products reveals extensive CH3 rocking or CH3 umbrella excitation in the CH30 radical. However the vibrational structures are not resolved in the C2H5O radical.展开更多
The ultrafast photoionization dynamics of N_(2) molecules by x-ray/XUV laser pulses is investigated.The molecular frame photoelectron momentum distributions(MF-PMDs) and the molecular frame photoelectron angular distr...The ultrafast photoionization dynamics of N_(2) molecules by x-ray/XUV laser pulses is investigated.The molecular frame photoelectron momentum distributions(MF-PMDs) and the molecular frame photoelectron angular distributions(MF-PADs) are obtained by numerically solving 2D time-dependent Schrodinger equations within the single-electron approximation(SEA) frame.The results show that the molecular photoionization diffraction appears in 5 nm laser fields.However,when the laser wavelength is 30 nm,the molecular photoionization diffraction disappears and the MF-PMDs show four-lobe pattern.The ultrafast photoionization model can be employed to describe the MF-PMDs and MF-PADs of N_(2) molecules.展开更多
We study the phot odissociation dynamics of CS2 in the ultraviolet region using the time-sliced velocity map ion imaging technique.The S(3 Pj)+CS(X1E+)product channels were observed and identified at four wavelengths ...We study the phot odissociation dynamics of CS2 in the ultraviolet region using the time-sliced velocity map ion imaging technique.The S(3 Pj)+CS(X1E+)product channels were observed and identified at four wavelengths of 201.36,203.10,204.85 and 206.61 nm.In the measured images of S(3Pj=2,1,0),the vibrational states of the CS(X1E+)co-products were partially resolved and the vibrational state distributions were determined.Moreover,the product total kinetic energy releases and the anisotropic parameters were derived.The relatively small anisotropic parameter values indicate that the S(3Pj=2丄0)+CS(X1E+)channels are very likely formed via the indirect predissociation process of CS2.The study of the S(3Pj=2,1;0)+CS(X1E+)channels,which come from the spin-orbit coupling dissociation process of CS2,shows that nonadiabatic process plays a role in the ultraviolet photodissociation of CS2.展开更多
The ultrafast dynamics of water molecules excited to the two F states is studied by combining two-photon excitation and time-resolved photoelectron imaging techniques. The lifetimes of the F1A1 and F1B1 states of H2O ...The ultrafast dynamics of water molecules excited to the two F states is studied by combining two-photon excitation and time-resolved photoelectron imaging techniques. The lifetimes of the F1A1 and F1B1 states of H2O (D2O) were derived to be 1.0±0.3 (1.9±0.4) and 10±3 (30±10) ps, respectively. We propose that the F1A1 state mainly decays through the D state, due to the nonadiabatic coupling between them, while the F1B1 state decays through the F1A1 state via Coriolis interaction.展开更多
Photodissociation dynamics of DNCO+hv→D+NCO at photolysis wavelengths between 200 and 235 nm have been studied using the D-atom Rydberg tagging time-of-flight technique. Product translational energy distributions and...Photodissociation dynamics of DNCO+hv→D+NCO at photolysis wavelengths between 200 and 235 nm have been studied using the D-atom Rydberg tagging time-of-flight technique. Product translational energy distributions and angular distributions have been determined. Nearly statistical distribution of the product translational energy with nearly isotropic angular distribution was observed at 210-235 nm, which may come from the predissociation pathway of internal conversion from S1 to S0 state followed by decomposition on S0 surface. At shorter photolysis wavelengths, in addition to the statistical distribution, another feature with anisotropic angular distribution appears at high translational energy region, which can be attributed to direct dissociation on S1 surface. Compared with HNCO, the direct dissociation pathway for DNCO photodissociation opens at higher excitation energy. According to our assignment of the NCO internal energy distribution, dominantly bending and a little stretching excited NCO was produced via both dissociation pathways.展开更多
Phosphorescent carbon nanodots(CNDs)have various attractive properties and potential applications,but it remains a formidable challenge to achieve large-scale phosphorescent CNDs limited by current methods.Herein,a la...Phosphorescent carbon nanodots(CNDs)have various attractive properties and potential applications,but it remains a formidable challenge to achieve large-scale phosphorescent CNDs limited by current methods.Herein,a large-scale synthesis method for phosphorescent CNDs has been demonstrated via precursors’self-exothermic reaction at room temperature.The as-prepared CNDs show fluorescence and phosphorescence property,which are comparable with that synthesized by solvothermal and microwave method.Experimental and computational studies indicate that exotic atom doped sp^(2) hybridized carbon core works as an emissive center,which facilities the intersystem crossing from singlet state to triplet state.The CNDs show phosphorescence with tunable lifetimes from 193 ms to 1.13 s at different temperatures.The demonstration of large-scale synthesis of phosphorescent CNDs at room temperature opens up a new window for room temperature fabrication phosphorescent CNDs.展开更多
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDB17000000)the National Natural Science Foundation of China (NSFC Center for Chemical Dynamics (No.21688102)+4 种基金the National Natural Science Foundation of China (No.21673232, No.21873099, No.21922306)the International Partnership Program of Chinese Academy of Sci-ences (No.121421KYSB20170012)supported by the National Natural Science Foundation of China (No.21973010)supported by the National Natural Science Foundation of China (No.21773236)supported by the Natural Science Research Project of Education Department of Anhui Province (No.KJ2019A0521).
文摘Photodissociation of H2S in the VUV region plays an important role in the atmospheric chemistry and interstellar chemistry.To date,however,few studies have been focused on this topic.In this article,we have described a laser dispersion method applied in the apparatus combining the high-n H atom Rydberg tagging time-of-flight technique with the vacuum ultraviolet free electron laser(VUV FEL).The Lyman-αlaser beam(121.6 nm)used in the H-atom detection was generated by the difference frequency four-wave mixing schemes in a Kr/Ar gas cell.After passing through an off-axis biconvex LiF lens,the 121.6 nm beam was dispersed from the 212.6 nm and 845 nm beams due to the different deflection angles experienced by these laser beams at the surfaces of the biconvex lens.This method can eliminate the background signal from the 212.6 nm photolysis.Combined with the VUV FEL,photodissociation of H2S at 122.95 nm was studied successfully.The TOF spectrum was measured and the derived total kinetic energy release spectrum was displayed.The results suggest that the experimental setup is a powerful tool for investigating photodissociation dynamics of molecules in the VUV region which involves the H-atom elimination processes.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12074146,21827805,11974007,and 12074142)the Natural Science Foundation of Jilin Province of China(Grant No.20180101225JC)。
文摘We present the photoelectron momentum distributions(PMDs) and the photoelectron angular distributions(PADs) of He+ ions, aligned H2+ molecules and N2 molecules by intense orthogonally polarized laser pulses. Simulations are performed by numerically solving the corresponding two-dimensional time-dependent Schr?dinger equations(TDSEs) within the single-electron approximation frame. Photoelectron momentum distributions and photoelectron angular distributions present different patterns with the time delays Td, illustrating the dependences of the PMDs and PADs on the time delays by orthogonally polarized laser pulses. The evolution of the electron wavepackets can be employed to describe the intensity of the PADs from the TDSE simulations for N2 molecules.
基金supported by the National Natural Science Foundation of China (No.21473015, No.21203016, No.41574101, No.21673232, No.21773213)the Foundation for the Author of National Excellent Doctoral Dissertation of China (No.201222)
文摘We presented an experimental apparatus combining the H-atom Rydberg tagging time-of-flight technique and the laser detonation source for studying crossed beam reactions at hyperthermal collision energies. The preliminary study of the F+D2→DF+D reaction at hyperthermal collision energy of 23.84 kJ/mol was performed. Two beam sources were used in this study: one is the hyperthermal F beam source produced by a laser detonation process, and the other is D2 beam source generated by liquid-N2 cooled pulsed valve. Vibrational state-resolved di erential cross sections (DCSs) of product for the title reaction were determined. From the product vibrational state-resolved DCS, it can be concluded that products DF(v'=0, 1, 2, 3) are predominantly distributed in the sideway and backward scattering directions at this collision energy. However, the highest vibrational excited product DF(v'=4), is clearly peaked in the forward direction. The probable dynamical origins for these forward scattering products were analyzed and discussed.
文摘157 nm photodissociation of jet-cooled CH3OH and C2HsOH was studied using the high-n Rydberg atom time-of-flight （TOF） technique. TOF spectra of nascent H atom products were measured. Simulation of these spectra reveals three different atomic H loss processes： one from hydroxyl H elimination, one from methyl （ethyl） H elimination, and one from secondary dissociation of the methoxy （ethoxy） radical. The relative branching ratio indicates secondary dissociation of ethoxy is less important than that of methoxy. The average angular anisotropy parameter of methanol is negative （with β≈-0.3）, indicating the transition dipole moment is perpendicular to the C-O-H plane. The slightly more negative β value of ethanol （with β≈-0.4） implies that ethanol has a longer rotational period. These experimental results indicate that both systems undergo fast internal conversion to the 3s surface after it is excited to the 3px surface, and then dissociate on the 3s surface. The translational energy distribution of the CH3O＋H products reveals extensive CH3 rocking or CH3 umbrella excitation in the CH30 radical. However the vibrational structures are not resolved in the C2H5O radical.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12074146,11974007,12074142,11904122,91850114,and 11774131)the Natural Science Foundation of Jilin Province of China(Grant No.20180101225JC)。
文摘The ultrafast photoionization dynamics of N_(2) molecules by x-ray/XUV laser pulses is investigated.The molecular frame photoelectron momentum distributions(MF-PMDs) and the molecular frame photoelectron angular distributions(MF-PADs) are obtained by numerically solving 2D time-dependent Schrodinger equations within the single-electron approximation(SEA) frame.The results show that the molecular photoionization diffraction appears in 5 nm laser fields.However,when the laser wavelength is 30 nm,the molecular photoionization diffraction disappears and the MF-PMDs show four-lobe pattern.The ultrafast photoionization model can be employed to describe the MF-PMDs and MF-PADs of N_(2) molecules.
基金This work was supported by the National Key R&D Program of China(No.2017YFF0104500)the National Natural Science Foundation of China(No.21590802 and No.21473173)the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB17000000).
文摘We study the phot odissociation dynamics of CS2 in the ultraviolet region using the time-sliced velocity map ion imaging technique.The S(3 Pj)+CS(X1E+)product channels were observed and identified at four wavelengths of 201.36,203.10,204.85 and 206.61 nm.In the measured images of S(3Pj=2,1,0),the vibrational states of the CS(X1E+)co-products were partially resolved and the vibrational state distributions were determined.Moreover,the product total kinetic energy releases and the anisotropic parameters were derived.The relatively small anisotropic parameter values indicate that the S(3Pj=2丄0)+CS(X1E+)channels are very likely formed via the indirect predissociation process of CS2.The study of the S(3Pj=2,1;0)+CS(X1E+)channels,which come from the spin-orbit coupling dissociation process of CS2,shows that nonadiabatic process plays a role in the ultraviolet photodissociation of CS2.
基金supported by the National Natural Science Foundation of China (No.21573228, No.21833003, No.21673232, and No.21773236)the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDB17000000)
文摘The ultrafast dynamics of water molecules excited to the two F states is studied by combining two-photon excitation and time-resolved photoelectron imaging techniques. The lifetimes of the F1A1 and F1B1 states of H2O (D2O) were derived to be 1.0±0.3 (1.9±0.4) and 10±3 (30±10) ps, respectively. We propose that the F1A1 state mainly decays through the D state, due to the nonadiabatic coupling between them, while the F1B1 state decays through the F1A1 state via Coriolis interaction.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDB17000000)the Chemical Dynamics Research Center (No.21688102)+1 种基金the National Natural Science Foundation of China (No.21873099 and NO.21673232)the Youth Innovation Promotion Association (No.2014160)
文摘Photodissociation dynamics of DNCO+hv→D+NCO at photolysis wavelengths between 200 and 235 nm have been studied using the D-atom Rydberg tagging time-of-flight technique. Product translational energy distributions and angular distributions have been determined. Nearly statistical distribution of the product translational energy with nearly isotropic angular distribution was observed at 210-235 nm, which may come from the predissociation pathway of internal conversion from S1 to S0 state followed by decomposition on S0 surface. At shorter photolysis wavelengths, in addition to the statistical distribution, another feature with anisotropic angular distribution appears at high translational energy region, which can be attributed to direct dissociation on S1 surface. Compared with HNCO, the direct dissociation pathway for DNCO photodissociation opens at higher excitation energy. According to our assignment of the NCO internal energy distribution, dominantly bending and a little stretching excited NCO was produced via both dissociation pathways.
基金This work was supported by the National Natural Science Foundation of China(Nos.11904326,U1804155,and U1604263)China Postdoctoral Science Foundation(Nos.2019TQ0287,and 2019M662510)+1 种基金the Chemical Dynamics Research Center(No.21688102)the Key Technology Team of the Chinese Academy of Sciences(No.GJJSTD20190002).
文摘Phosphorescent carbon nanodots(CNDs)have various attractive properties and potential applications,but it remains a formidable challenge to achieve large-scale phosphorescent CNDs limited by current methods.Herein,a large-scale synthesis method for phosphorescent CNDs has been demonstrated via precursors’self-exothermic reaction at room temperature.The as-prepared CNDs show fluorescence and phosphorescence property,which are comparable with that synthesized by solvothermal and microwave method.Experimental and computational studies indicate that exotic atom doped sp^(2) hybridized carbon core works as an emissive center,which facilities the intersystem crossing from singlet state to triplet state.The CNDs show phosphorescence with tunable lifetimes from 193 ms to 1.13 s at different temperatures.The demonstration of large-scale synthesis of phosphorescent CNDs at room temperature opens up a new window for room temperature fabrication phosphorescent CNDs.
