Interference of dissociating wave packets in the I2 molecule driven by femtosecond laser pulses

The interference between two dissociating wave packets of the I2 molecule driven by femtosecond laser pulses is theoretically studied by using the time-dependent quantum wave packet method.Both the internuclear distanceand velocity-dependent density functions are calculated and discussed.It is demonstrated that the interference pattern is determined by the phase difference and the delay time between two pump pulses.With two identical pulses with a delay time of 305 fs and a FWHM of 20 fs,more interference fringes can be observed,while with two pump pulses with a delay time of 80 fs and a FWHM of 20 fs,only a few interference fringes can be observed.     

Role of highest occupied molecular orbitals in molecular field-free alignment by a femtosecond pulse

This paper studies the molecular rotational excitation and field-free spatial alignment in a nonresonant intense laser field numerically and analytically by using the time-dependent Schr?dinger equation. The broad rotational wave packets excited by the femtosecond pulse are defined in conjugate angle space, and their coefficients are obtained by solving a set of coupled linear equations. Both single molecule orientation angles and an ensemble of O₂ and CO molecule angular distributions are calculated in detail. The numerical results show that, for single molecule highest occupied molecular orbital (HOMO) symmetry σ tends to have a molecular orientation along the laser polarization direction and the permanent dipole moment diminishes the mean of the orientation angles; for an ensemble of molecules, angular distributions provide more complex and additional information at times where there are no revivals in the single molecule plot. In particular, at the revival peak instant, with the increase of temperature of the molecular ensemble, the anisotropic angular distributions with respect to the laser polarization direction of the π _g orbital gradually transform to the symmetrical distributions regarding the laser polarization vector and for two HOMO configurations angular distributions of all directions are confined within a smaller angle when the temperature of the molecular ensemble is higher.     

Supercontinuum Generation in Holey Microstructure Fibres with Random Cladding Distribution by Femtosecond Laser Pulses ＊

It is reported that supercontinuum spectrum from 440 to 1050 nm can be generated in holey microstructure fibres (HMFs) with random cladding distribution by Ti:sapphire femtosecond laser pulses with central wavelength of 800 nm. Based on the method of the effective refractive index and the analogy of step-index fibre, we have calculated the effective mode area and the group velocity dispersion (GVD). It is found that the HMFs have specifically ability of localizing light and controlling GVD. The mechanism of supercontinuum generation in the HMFs with random cladding distribution is that the balance between the GVD and the self-phase modulation in the anomalous dispersion region leads to formation of solitons and fission of high order solitons.     

First Principles Study of Adsorption and Reaction of CO on SrTiO3 （100） Surface： the Role of Surface Oxygen Vacancies

The adsorption and reaction of CO on SrTiO3 （100） surface with and without surface oxygen vacancy are investigated by the first-principles calculation based on the density functional theory. The calculated results reveal that the oxygen vacancy site prefers to the activation of the C-O bond. The adsorption energies increase to 1.0855 and 0.3245eV for defect-CO and defect-OC orientations, respectively. Particularly the C-O bond is elongated by about 0.1285 ？ in the defect-OC orientation compared with that in the Ti-OC one without surface oxygen vacancies. There is predominantly a chemisorption mechanism between the CO molecule and the surface in the defect-CO orientation.     

Determination of the temporal structure of femtosecond laser pulses by means of laser-induced air plasma

A new approach is presented to reveal the temporal structure of femtosecond laser pulses by recording the corresponding time-resolved shadowgraphs of the laser-induced air plasma. It is shown that the temporal structures of femtosecond laser pulses, normally not observable by the ordinary intensity autocorrelator, can be detected through intuitively analyzing the ultrafast evolution process of the air plasma induced by the femtosecond laser pulses under examination. With this method, existence of pre- and post-pulses has been clearly unveiled within the time window of ±150 fs in reference with the main 50-fs laser pulses output from a commercial 1-kHz femtosecond laser amplifier. The unique advantage of the proposed method is that it can directly provide valuable information about the pulse temporal structures' effect on the laser-induced ionization or material ablation.     

Natural population inversion in a gaseous molecular filament

We propose a new mechanism/scheme to explain the ultrafast population inversion of molecular ions which takes place in a time scale comparable to the femtosecond laser pulse. The nonlinear pumping process including the pump photons and the self-generated harmonic photons of the pump laser would be responsible for building up population inversion to realize remote molecule lasers in femtosecond laser filaments in gases. It is shown that the remote laser emissions in molecular ions of gases may be a universal process in the femtosecond laser filament.     

Ray-Tracing Simulation on Filamentation of Prefocused and Freely Propagated Laser Pulses in Air

The filamentation mechanisms of prefocused and freely propagated femtosecond laser pulses axe compared using the ray-tracing method. The dynamic spatial replenishment mechanism takes place in the filaments with high electron density, which is generally formed by prefocused laser pulses. The mechanism of long-range filamentation over lOOm distance is analyzed to be the spatiotemporal moving focus.     

Investigation of vortex arms in electron vortices by counter-rotating elliptically polarized attosecond laser pulses

We theoretically investigate the vortex patterns in photoelectron momentum distributions of He⁺driven by counter-rotating elliptically polarized,time delayed attosecond laser pulses by numerically solving the two-dimensional time-dependent Schrodinger equation.It is found that the number of vortex arms is extremely sensitive to the ellipticity and wavelength of counterrotating elliptically polarized laser pulses,which is illustrated by the attosecond perturbation ionization models.In addition,the effect of different time delays between two pulses on the interference patterns is also investigated and the corresponding physical mechanism is demonstrated.Since the wavelength,ellipticity and time delay have a significant effect on the vortex interference patterns,this may be a new method for laser field detection.     

Interaction of intense laser pulses with hydrogen atomic clusters

The interaction between intense femtosecond laser pulses and hydrogen atomic clusters is studied by a simplified Coulomb explosion model. The dependences of average proton kinetic energy on cluster size, pulse duration, laser intensity and wavelength are studied respectively. The calculated results indicate that the irradiation of a femtosecond laser of longer wavelength on hydrogen atomic clusters may be a simple, economical way to produce highly kinetic hydrogen ions. The phenomenon suggests that the irradiation of femtosecond laser of longer wavelength on deuterium atomic clusters may be easier than that of shorter wavelength to drive nuclear fusion reactions. The product of the laser intensity and the squared laser wavelength needed to make proton energy saturated as a function of the squared cluster radius is also investigated. The proton energy distribution calculated is also shown and compared with the experimental data. Our results are in agreement with the experimental results fairly well.     

Generation of third harmonic emission in propagation of femtosecond laser pulses in air

The main characteristics of the third harmonic emission generated by femtosecond laser pulses propagating in air are investigated by numerically solving the coupled nonlinear Schr?dinger equations. Strong third harmonic emission is observed with a maximum conversion efficiency as high as 0.43%. The on-axis phase difference between fundamental beam and third harmonic is investigated. The result is in good agreement with the phase-locking mechanism. Dependence of the conversion of third harmonic emission on focusing conditions is also studied. The results are also compared with those of experiments.     

Field-free molecular orientation enhanced by tuning the intensity ratio of a three-color laser field

We theoretically study the field-free molecular orientation induced by a three-color laser field. The three-color laser field with a large asymmetric degree can effectively enhance the molecular orientation. In particular, when the intensity ratio of the three-color laser field is tuned to a proper value of I_3: I_2: I_1= 0.09 : 0.5 : 1, the molecular orientation can be improved by ～ 20% compared with that of the two-color laser field at intensity ratio I_2: I_1= 1 : 1 for the same total laser intensity of 2×10~(13)W/cm~2. Moreover, we investigate the effect of the carrier-envelope phase(CEP) on the molecular orientation and use the asymmetric degree of the laser field to explain the result. We also show the influences of the laser intensity, rotational temperature, and pulse duration on the molecular orientation. These results are meaningful for the theoretical and experimental studies on the molecular orientation.     

Angular distributions of CH3I fragment ions under the irradiation of a single pulse and trains of ultrashort laser pulses

The angular distribution of CH3I is investigated experimentally using a single Fourier transform-limited laser pulse and a pulse train, where a 90-fs 800-nm linearly polarized laser field with a moderate intensity of 2.8×1013 W/cm2 is used. The dynamic alignment is demonstrated in a single pulse experiment. Moreover, a pulse train is used to optimize the molecular alignment, and the alignment degree is almost identical to that with the single pulse. The results are analysed by using chirped femtosecond laser pulses, and it demonstrates that the structure of pulse train rather than its effective duration is crucial to the molecular alignment.     

Low temperature enhancement of alignment-induced spectral broadening of femtosecond laser pulses

The propagation of femtosecond laser pulses in N2-filled hollow fibers is studied both theoretically and experimentally. The laser pulse aligns the N2 molecules and changes the refractive index, which meanwhile modulates the spectrum of the pulse in turn. The dependence of the spectral modulation on the gas temperature is investigated. We find that both spectral broadening and frequency red-shift are enhanced at low temperature. The degree of enhancement is found to be dependent on the pulse duration. Based on our findings, we propose a method for femtosecond pulse spectral broadening and few-cycle pulse generation via the molecular alignment.     

Coherent control of non-resonant two-photon transition in molecular system

In this paper,we study theoretically and experimentally the coherent control of non-resonant two-photon transition in a molecular system (Perylene dissolved in chloroform solution) by shaping the femtosecond pulses with simple phase patterns (cosinusoidal and π phase step-function shape).The control efficiency of the two-photon transition probability is correlated with both the laser field and the molecular absorption bandwidth.Our results demonstrate that,the two-photon transition probability in a molecular system can be reduced but not completely eliminated by manipulating the laser field,and the control efficiency is minimal when the molecular absorption bandwidth is larger than twice the laser spectral bandwidth.     

Time-dependent density functional theoretical studies on the photo-induced dynamics of an HCI molecule encapsulated in C60 under femtosecond laser pulses

By using first-principles simulations based on time-dependent density functional theory, the chemical reaction of an HCl molecule encapsulated in C60 induced by femtosecond laser pulses is observed. The H atom starts to leave the Cl atom and is reflected by the C60 wall. The coherent nuclear dynamic behaviors of bond breakage and recombination of the HCl molecule occurring in both polarized parallel and perpendicular to the H-Cl bond axis are investigated. The radial oscillation is also found in the two polarization directions of the laser pulse. The relaxation time of the H-Cl bond lengths in transverse polarization is slow in comparison with that in longitudinal polarization. Those results are important for studying the dynamics of the chemical bond at an atomic level.     

Formation of domain reversal by direct irradiation with femtosecond laser in lithium niobate

We propose that domain inversion can be directly induced by femtosecond laser both theoretically and experimentally, which opens a path to achieve three-dimensional （3D） nonlinear crystal with a period in sub-micron-scale. A simulation of domain inversion is modeled by considering the temporal distribution of femtosecond pulses. The calculation results clarify that the domain inversions can happen within or after the interaction with the laser pulse, and the response time of domain inversion is in the picosecond level depending on the intensity and the materials. The domain reversal windows of lithium niobate by femtosecond laser are observed which agrees with theoretical predictions qualitatively.     

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.     

High Resolution Mode-Selective Excitation by Adaptive Femtosecond Pulse Shaping

High resolution mode-selective excitation in the mixture of C6H6 （992 cm^-1） and C6D6 （945 cm^-1） is experimentally achieved by adaptive femtosecond pulse shaping based on the genetic algorithm （GA）, and second harmonic generation frequency-resolved optical gating （SHG-FROG） is adopted to characterize the original and optimal laser pulses, and its mechanism is experimentally validated by tailoring the frequency components of the pump pulses at the Fourier plane. It is indicated that two-pulse coherent mode-selective excitation of the Raman scattering mainly depends on the effective frequency components of the pump pulse related to specific molecular vibrational mode. The experimental results have attractive potential applications in the complicated molecular system.     

Nonadditivity in moments of inertia of high-K multiquasiparticle bands

The experimental high-K 2- and 3-quasiparticle bands of well deformed rare-earth nuclei are analyzed. It is found that there exists significant nonadditivity in moments of inertia (MOIs) for these bands. The microscopic mechanism of the rotational bands is investigated by the particle number conserving (PNC) method in the frame of cranked shell model with pairing, in which the blocking effects are taken care of exactly. The experimental rotational frequency dependence of these bands is well reproduced in PNC calculations. The nonadditivity in MOIs originates from the destructive interference between Pauli blocking effects.     

Time-dependent density functional theoretical studies on the photo-induced dynamics of an HCl molecule encapsulated in C_(60) under femtosecond laser pulses

By using first-principles simulations based on time-dependent density functional theory,the chemical reaction of an HCl molecule encapsulated in C60induced by femtosecond laser pulses is observed.The H atom starts to leave the Cl atom and is reflected by the C60wall.The coherent nuclear dynamic behaviors of bond breakage and recombination of the HCl molecule occurring in both polarized parallel and perpendicular to the H–Cl bond axis are investigated.The radial oscillation is also found in the two polarization directions of the laser pulse.The relaxation time of the H–Cl bond lengths in transverse polarization is slow in comparison with that in longitudinal polarization.Those results are important for studying the dynamics of the chemical bond at an atomic level.