High-order harmonic generation and multi-photon ionization of Na2 in laser fields

In this paper high-order harmonic generation （HHG） spectra and the ionization probabilities of various charge states of small cluster Na2 in the multiphoton regimes are calculated by using time-dependent local density approximation （TDLDA） for one-colour （1064 nm） and two-colour （1064 nm and 532 nm） ultrashort （25 fs） laser pulses. HHG spectra of Na2 have not the large extent of plateaus due to pronounced collective effects of electron dynamics. In addition, the two-colour laser field can result in the breaking of the symmetry and generation of the even order harmonic such as the second order harmonic. The results of ionization probabilities show that a two-colour laser field can increase the ionization probability of higher charge state.     

Size dependence of the maximum energy of protons from Coulomb explosion of methane clusters under intense femtosecond laser irradiation

An investigation of the cluster size dependence of the maximum energy of protons ejected from explosion of methane clusters in an intense femtosecond laser field has been conducted on the basis of the cluster size estimation by Rayleigh scattering measurements. The interaction of a 2×1016-W/cm2 intense laser pulse (790 nm, 60 fs) with the methane clusters revealed that the clusters were Coulomb exploded and the maximum energy (Emax) of the protons produced was linearly proportional to the square of the cluster radius (rc2). In a cluster size range, with the methane cluster radii up to about 3 nm, the established relation of Emax and rc2 was found to be Emax(keV)=3.3 0.75rc2(nm2), in good agreement with the simulation results. This demonstrated that Coulomb explosion of ionic clusters (C 4H4 )n took place following the cluster vertical ionization in the laser-cluster interaction.     

Size dependence of the maximum energy of protons from Coulomb explosion of methane clusters under intense femtosecond laser irradiation

An investigation of the cluster size dependence of the maximum energy of protons ejected from explosion of methane clusters in an intense femtosecond laser field has been conducted on the basis of the cluster size estimation by Rayleigh scattering measurements. The interaction of a 2 × 1016-W/cm2 intense laser pulse (790 nm, 60 fs) with the methane clusters revealed that the clusters were Coulomb exploded and the maximum energy (Emax) of the protons produced was linearly proportional to the square of the cluster radius (r2c). In a cluster size range, with the methane cluster radii up to about 3 nm, the established relation of Emax and rc2 was found to be Emax (keV) = 3.3 + 0.75r2c (nm2), in good agreement with the simulation results. This demonstrated that Coulomb explosion of ionic clusters (C+4H4+)n took place following the cluster vertical ionization in the laser-cluster interaction.     

Structural deformation of nitro group of nitromethane molecule in liquid phase in an intense femtosecond laser field

The structural deformation of NO_2 group induced by an intense femtosecond laser field of liquid nitromethane(NM)molecule is detected by time-and frequency-resolved coherent anti-Stokes Raman spectroscopy(CARS) technique with the intense pump laser. Here, we present the mechanism of molecular alignment and deformation. The CARS spectra and its FFT spectra of liquid NM show that the NO_2 torsional mode couples with the CN symmetric stretching mode and that the NO_2 group undergoes ultrafast structural deformation with a relaxation time of 195 fs. The frequency of the NO_2 torsional mode in liquid NM(50.8±0.3 cm~(-1)) at room temperature is found. Our results prove the structural deformation of two groups in liquid NM molecule occur simultaneously in the intense laser field.     

Photodissociation of sodium iodide and resonant ionization of sodium atom produced

Resonant ionization spectroscopy (RIS) and resonant ionization mass spectroscopy (RIMS) are employed to detect the photodissociation product of sodium iodide molecules in a molecular beam in an intense laser field in the absence of the buffer gases. Time of flight mass spectra is recorded. In particular, the appearances of multiphoton ionization are discussed.     

Ultrafast Optical Response from a Novel Tri-Branched Copolymer

A novel tri-branched copolymer is synthesized to show strong two-photon absorption and intense two-photon absorption induced fluorescence emission under the excitation of the femtosecond laser pulses at wavelength of 80Ohm. The dynamics of the excited state was measured by the pump-probe technique. In a one-colour pump-probe experiment at 800 nm, there was an ultrafast transient absorption, followed by other two relaxation processes. The two-photon absorption process could be one origin for this ultrafast photoabsorption signal, which was further proven by two-colour pump-probe experiments. The other two decaying processes in the transient absorption dynamics have lifetime of about 15ps and 129ps, which reflect the intraband vibrational relaxation and the decay of two-photon excited state, respectively.     

Experimental study of conversion from atomic high—order harmonics to x—ray emissions

There are two physical phenomena in a strong laser intensity. One is the high-order harmonic emission; the other is x-ray emission from optical-field ionized plasmas. The experiment of conversion from high-order harmonics to x-ray emissions was given with a 105fs Ti:sapphire laser by adjusting laser intensities. The ingredient in plasma was investigated by the numerical simulations.Our experimental results suggested that the free electrons have detrimental effects on harmonic generation but are favourable for x-ray emission from optical-field ionized plasmas. If we want to obtain more intense harmonic signals as a coherent light source in the soft x-ray region, we must avoid the production of free electrons in plasmas. At the same time, if we want to observe x-rays for the development of high-repetition-rate table-top soft x-ray lasers, we should strip all atoms in the plasmas to a necessary ionized stage by the optical-field-ionization in the field of a high-intensity laser pulse.     

High-order harmonic generation in a two-color strong laser field with Bohmian trajectory theory

We theoretically study the high-order harmonic generation(HHG) in a two-color laser field using the Bohmian mechanics. Our results show that, for the case of a weak second-color laser field, the simulation of the HHG with only one central Bohmian trajectory is in a good agreement with the ab initio time-dependent Schr o¨dinger equation(TDSE) results.In contrast, with the increase of the amplitude of the second-color laser field, the HHG spectra from the single central Bohmian trajectory deviate from the TDSE results more and more significantly. By analyzing the Bohmian trajectories,we find that the significant deviation is due to the fact that the central Bohmian trajectory leaves the core quickly in the two-color laser field with the breaking of inversion symmetry. Interestingly, we find that another Bohmian trajectory with different initial position, which keeps oscillating around the core, could qualitatively well reproduce the TDSE results. Furthermore, we study the HHG spectrum in a two-color laser field with inversion symmetry and find that the HHG spectrum in TDSE can be still well simulated with the central Bohmian trajectory. These results indicate that, similar to the case of one color laser field, the HHG spectra in a two-color laser field can be also reproduced with a single Bohmian trajectory,although the initial position of the trajectory is dependent on the symmetry of the laser field. Our work thus demonstrates that Bohmian trajectory theory can be used as a promising tool in investigating the HHG process in a two-color laser field.     

Generation of Helical and Axial Magnetic Fields by the Relativistic Laser Pulses in Under—dense Plasma：Three—Dimensional Particle—in—Cell Simulation

The quasi-static magnetic fields created in the interaction of relativistic laser pulses with under-dense plasmas have been investigated by three-dimensional particle-in-cell simulation.The relativistic ponderomotive force can drive and intense electron current in the laser propagation direction,which is responsible for the generation of a helical magnetic field.The axial magnetic field results from a difference bean of wave-wave,which drives a solenoidal current.In particular,the physical significance of the kinetic model for the generation of the axial magnetic field is discussed.     

Experimental study of the time-resolved reflectivity of chromium film

The transient time-resolved reflectivity of chromium film is studied by femtosecond pump-probe technique with a 70-fs laser. Experimental results show that the reflectivity change increases with the power of the pump laser. The fast decrease of the reflectivity occurs between 0-200 fs which is mainly due to the electron-electron interaction. Subsequencely, the slower recovery of the reflectivity between 200-900 fs is mainly due to the electron-phonon coupling process. The reflectivity after 900 fs rises little to a near-constant value for the thermal equilibrium of the system. The experimental results can be explained properly with numerical simulation of the two-temperature model. It is helpful for understanding of the electron ultrafast dynamics in chromium film.     

Molecular ionization of cyclohexanone in femtosecond laser fields: An application of ADK theory

The mechanisms of ionization and dissociation of cyclohexanone (C₆H₁₀O) in a 90 fs, 788 nm linearly polarized laser field ranging from 10¹³ to 10¹⁴ W/cm² by a time-of-flight mass spectrometer (TOF-MS) have been investigated. The ion yields as a function of laser intensity have been measured experimentally. By comparison with the Ammosov-Delone-Krainov (ADK) theory based on a hydrogen-like model, the ionization mechanism of cyclohexanone in this intense femtosecond laser field has been understood. Considering the importance of molecular nuclear motions, we propose that the Franck-Condon (F-C) factor can provide the excess vibrational energy in the molecular ion. This energy is required for the decomposition of the molecular ion which finally results in the observed mass spectrum.     

Electronic photodissociation spectra of the Arn-C4H2 (n=1-4) weakly bound cationic complexes

Electronic spectra of a series of weakly bound clusters consisting of argon (Ar_n, n=1-4) bound to the butadiyne cation, C₄H₂⁺, have been recorded in the visible range from 440 to 520 nm by photodissociation. The C₄H₂⁺ fragment signal was recorded as a function of the laser wavelength during excitation of the A←X electronic transition. The observed transitions were assigned to the band origin of the cationic complexes and to vibronic bands involving excitation of the ν₃ and ν₇ vibrational modes of the C₄H₂⁺ moiety, as well as combination bands of these modes. Comparison of the photodissociation spectra of the various clusters reveals a small blue shift, 25 cm⁻¹ of the band maxima relative to the corresponding transitions reported from gas phase spectra of the bare C₄H₂⁺ cation. The magnitude of the blue shift of each band increases with successive Ar solvation up to n=3. Furthermore, each band becomes increasingly broadened towards the red with the addition of Ar atoms due to an increasing number of unresolved transitions involving excited intermolecular modes.     

DYNAMICS of H+2 in TWO-COLOR ULTRASHORT LASER PULSE

Numerical simulations of ionization and dissociation processes of hydrogen molecular ion H₂⁺ interacting with two-color intense ( 10¹⁴W/cm²-10¹⁵W/cm²) ultrashort (the duration ≈ 22fs) laser pulse are made. The result shows that the ionization and dissociation processes are strongly dependent upon the relative phase between the two color fields. It means that, in the case of ultrashort pulse, the phase coherence control of ionization and dissociation processes can be realized.     

Strong optical fields induce ultrafast rearrangement of H-atoms in ethanol molecules

H-atoms in C₂H₅OH are rearranged by strong optical fields generated by intense, 100 fs long infrared laser pulses to form new bonds that lead to the H ₃ ⁺ molecular ion. This observation appears to be against the expectation that exposure of molecules to intensities of the order of 10¹⁵ W cm^?2 inevitably lead to multiple ionization of molecules followed by instantaneous Coulomb explosion into fragments. The polarization dependence of the H ₃ ⁺ signal and of the energy content of H ₃ ⁺ ions lead to believe that H-atom rear-rangement in ethanol occurs within a single 100 fs pulse.     

工作压强对射频辉光放电H2/C4H8等离子状态的影响

利用辉光放电技术采用等离子体质谱诊断的方法研究了不同工作 压强下H₂/C₄H₈混合气体等离子体中 主要正离子成分及其能量的变化规律, 并分析了压强对H₂/C₄H₈混合气体的离解机理以及主要正离子形成过程的影响. 结果表明: 随着工作压强的增加, 碳氢碎片离子的浓度和能量均逐渐减小. 当工作压强为5 Pa时, H₂/C₄H₈混合气体等离子体中C₃H₅⁺相对浓度最大; 压强为10 Pa时, C₃H₃⁺相对浓度最大; 压强为15, 20 Pa时, C₂H₅⁺相对浓度最大; 压强为25 Pa时, C₄H₉⁺相对浓度最大. 对H₂/C₄H₈等离子体中的主要组分及其能量分布所进行的定性分析, 将为H₂/C₄H₈混合气体辉光放电聚合物涂层的工艺参数优化提供参考技术基础. 关键词： 辉光放电技术 等离子体质谱诊断 工作压强     

Dissociation of molecules in intense laser beam

Dissociation of molecules in the strong laser beam at the intensity of 10¹³–10¹⁴ W/cm² is investigated. Experimentally, the fragmentation of neutral molecules, CH₄, C₂H₄, C₄H₈; and the disintegration of molecular ions, CH ₄ ⁺ are studied by fluorescence spectroscopy and mass spectroscopy respectively. Some new phenomena, the strong dependence on the laser intensity, the universal dissociation, and the thorough fragmentation, are found in the fragmentation, and cannot be explained by the existing theories, as Coulomb Explosion theory or Re-scattering theory. We have suggested two new theories. The Super-excited State (SES) theory interprets the neutral fragmentation of molecules, which is stimulated to the SES by intense laser pulse. The Morse potential energy surface of the SES shows that either direct dissociation or pre-dissociation can take place in the SESs. Another theory, the theory of Field-assisted Dissociation (FAD) interprets the fragmentation of ionic molecules. According to this theory, the electric field of the laser pulse is involved directly to the dissociation process. QCT calculations for the trajectories moving on the dressed PES are performed. The result shows that the chemical bond which is parallel to the laser field vector undergo dissociation spontaneously. The dissociation takes place around 100 fs, which is in agreement with the ultrafast measurement in the pump-probe experiment.     

Ultrafast motion of liquids C2H4Cl2 and C2H4Br2 studied with a femtosecond laser

Transient optical Kerr effect of liquids C₂H₄Cl₂ and C₂H₄Br₂ is investigated, for the first time to our knowledge, with a femtosecond (fs) probe laser delayed with respect to a coherent fs pump laser. Coherent coupling and electronic Kerr signals are observed around zero delay when pump and probe overlap. Persisting after the pump-probe overlap are Kerr signals arising from the torsional and other intramolecular vibrations of the trans and gauche conformations; Kerr signals arising from the intermolecular motion are also observed. Vibrational quantum interference is only observed in liquid C₂H₄Br₂ and the related beats data are fitted with the torsional vibrations, 91 cm⁻¹ (gauche) and 132 cm⁻¹ (trans), and the CCBr angle-bending vibrations, 231 cm⁻¹ (gauche) and 190 cm⁻¹ (trans), with dephasing times, 0.45 ps, 0.45 ps, 2 ps, and 1.5 ps, respectively. These vibrational frequencies agree with those obtained in the frequency-domain. That no vibrational mode is observed for C₂H₄Cl₂ might be attributed to ineffective Raman-pumping. Kerr signals observed after the pump-probe overlap are Fourier transformed to give the spectra of the intermolecular motion and the vibrational spectrum, which agrees with the one observed in the infrared absorption and/or Raman scattering heretofore.     

Ultrafast delocalization of hydrogen atoms in allene in intense laser fields

Ultrafast delocalization of hydrogen atoms in allene (CH₂=C=CH₂) induced by intense laser fields was investigated by the Coulomb explosion coincidence momentum imaging method. On the basis of the kinetic energy distributions of the fragment ions produced through the two three-body Coulomb explosion pathways, C₃H₄³⁺ ? H⁺ + CH⁺ + C₂H₂⁺\mathrm{C}_{3}\mathrm{H}_{4}^{3+} \rightarrow \mathrm{H}^{+} + \mathrm{CH}^{+} + \mathrm{C}_{2}\mathrm{H}_{2}^{+} and C₃H₄³⁺ ? H⁺ + C₂H⁺ +CH₂⁺\mathrm{C}_{3}\mathrm{H}_{4}^{3+} \rightarrow \mathrm{H}^{+} + \mathrm{C}_{2}\mathrm{H}^{+} +\mathrm{CH}_{2}^{+}, and the proton maps for both pathways, it was shown that the decomposition proceeds in a stepwise manner as well as in a concerted manner. The time scale of the hydrogen migration within an allene molecule was estimated to be ∼20 fs.     

三氯乙烯的真空紫外同步辐射光电离和光解离

利用真空紫外(VUV)同步辐射光源和反射式飞行时间质谱仪，在超声冷却条件下对三氯乙烯(C₂HCl₃)进行了光电离研究，通过测量各离子的光电离效率(PIE)曲线，得到了C₂HCl₃的电离势P_I(C₂HCl₃)=9.51±0.05eV，以及C₂HCl₃光解离碎片离子的出现势(P_A)：P_{关键词： 同步辐射光电离 电离势 出现势 三氯乙烯}     

Dissociative photoionization of l-menthone: An experimental and theoretical study

The dissociative photoionization mechanism of l-menthone has been investigated with photoionization mass spectrometry using synchrotron radiation. The adiabatic ionization energy (IE) of l-menthone and the appearance energies (AE) of its major fragment ions C₉H₁₅O⁺, C₉H₁₇⁺, C₈H₁₆⁺, C₇H₁₁O⁺, C₆H₁₀O⁺, C₆H₉O⁺, C₅H₈O⁺, C₅H₁₀⁺, C₄H₆O⁺, C₅H₉⁺, C₄H₈⁺, C₄H₇⁺, C₃H₇⁺, C₃H₆⁺, C₂H₂O⁺, and CH₃⁺ are determined with their photoionization efficiency (PIE) spectra in the photon energy region of ∼8−15.5 eV. Breakdown diagrams identifying the major products are presented. Dissociative photoionization channels for formation of these fragment ions are proposed based on comparison of determined experimental appearance energies and energies predicted with the DFT calculations. According to our results, the experimental dissociation energies are in fair agreement with the theoretical values of the possible photodissociation channels of C₁₀H₁₈O.