Theoretical investigation of laser pulse width dependence in a thermal confinement regime

Previous molecular dynamics (MD) simulations of ultraviolet (UV) laser ablation demonstrate the distinct dependence of material ejection on laser fluence and laser pulse duration. In this paper, we examine the pulse width dependence when the laser pulse widths are appropriate for the thermal confinement regime. We perform MD simulations of laser ablation with a laser pulse duration of 1 ns and compare with a pulse width of 150 ps as in previous simulations. The simulations confirm that the pulse width in thermal confinement regime does not dramatically influence the molecular ejection mechanism. The simulations reveal differentiations, however, in plume composition and the ablation threshold value. PACS 02.70.Ns; 61.80.Az; 79.20.Ap     

Influence factor analysis of field-free molecular orientation

The effects of the characteristics of molecules and external fields on field-free molecular orientation are investigated through the comparison of HBr with LiH driven by the combination of a two-color laser pulse and a time-delayed THz laser pulse. It is shown that the dipole interaction has greater influence on field-free orientation than the hyperpolarizability interaction. In addition to the temperature dependence of orientation degree, the effects of the amplitudes of the two-color laser pulse and THz laser pulse, rising time, and THz laser frequency on molecular orientation are also discussed.     

Angular distributions of CH3I fragment ions under the irradiation of 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.     

Dissociation of vibrationally excited heteronuclear molecules by an intense infrared field

Results of numerical simulations of the vibrational-rotational dynamics of a molecular system in the field of an intense infrared laser pulse are presented. The cases of quasi-monochromatic and ultrashort laser action on the nuclear subsystem are considered. The influence of the coherent repopulation of vibrationally excited molecular states on photodissociation and the peculiarities of photodissociation under the action of an ultrashort laser pulse are discussed. The results obtained for quasi-monochromatic laser action are interpreted in terms of interference stabilization.     

Subfemtosecond pulse generation and multiplicative increase of pulse spacing in high-order stimulated Raman scattering

We demonstrate a technique for multiplicatively increasing the pulse spacing of subfemtosecond pulse trains generated by high-order stimulated Raman scattering, which uses pairs of off-resonant two-photon excitation of a molecular Raman mode to establish strong molecular modulation in the medium. Every laser pair has two single-mode laser beams tuned slightly off two-photon resonance, and the laser pairs have their corresponding carrier frequencies shifted from each other by one half, one third, or one fourth of the selected molecular Raman mode frequency. Theoretical analyses and calculations based on the fundamental vibrational transition of solid hydrogen show that the pulse spacing of the subfemtosecond pulse trains thus generated can readily be doubled, tripled, or even quadrupled.     

Selective excitation of the molecular rotational wave packet by two time-delayed laser pulses

In this paper, we investigate the control of the molecular wave packet of a linear molecule by two femtosecond laser pulses. It is shown that the odd and the even rotational wave packets created by a single laser pulse can be selectively excited by accurately controlling the time delay of another laser pulse. By inserting the peak of the second laser pulse at the position of maximum or minimum value around quarter or three quarter rotational period of the slope curve with odd (or even) rotational wave packet contribution that is created by the first laser pulse, the odd rotational wave packet can be enhanced (or suppressed) while the even rotational wave packet is suppressed (or enhanced). As a result, the molecular alignments around quarter and three quarter rotational periods can be obtained. Moreover, it is also shown that by inserting the second laser pulse around the quarter or three quarter rotational periods, the changes in the maximum degree of the molecular alignment for the odd and the even rotational wave packet contributions are consistent with their corresponding slope curves at these positions.     

Active manipulation of the selective alignment by two laser pulses

This paper solves numerically the full time-dependent Schrdinger equation based on the rigid rotor model, and proposes a novel strategy to determine the optimal time delay of the two laser pulses to manipulate the molecular selective alignment. The results illustrate that the molecular alignment generated by the first pulse can be suppressed or enhanced selectively, the relative populations of even and odd rotational states in the final rotational wave packet can be manipulated selectively by precisely inserting the peak of the second laser pulse at the time when the slope for the alignment parameter by the first laser locates a local maximum for the even rotational states and a local minimum for the odds, and vice versa. The selective alignment can be further optimised by selecting the intensity ratio of the two laser pulses on the condition that the total laser intensity and pulse duration are kept constant.     

Temporal pulsewidth and the wavelength dependences of the product ions obtained by laser ablation of solid C<Subscript>60</Subscript>

By ablating solid C₆₀ with a laser pulse, we observe various processes such as the prompt- and the delayed-ionization of C₆₀, the fragmentation into molecular ions and the formation of cluster ions. We found these processes show distinct dependences on the temporal pulse width, the power and the wavelength of the ablation laser. From the observations, we could confirm efficient coupling of laser energy to C₆₀ through the molecular absorption even with a laser pulse width less than the electron-phonon coupling time of the C₆₀ molecule.     

强光场下非共振双光子跃迁相干控制

利用飞秒激光脉冲相位整形技术,从理论和实验两方面,对强激光场下分子体系苝溶液中非共振双光子跃迁的相干控制进行了研究。通过对飞秒激光脉冲进行相位扫描和余弦相位调制,发现分子体系中非共振双光子的跃迁几率能够被削弱,但不能完全消除。分子体系中非共振双光子跃迁的相干控制受到激光光场的形状和分子吸收谱谱宽的影响;与原子体系相比,分子体系中非共振双光子跃迁相干控制的调制效率降低。     

Generation of an ultrashort optical pulse by four-wave Raman mixing in deuterium cooled at 77 K

When a 100-fs Ti:sapphire laser is focused into molecular deuterium cooled at 77 K, rotational stimulated Raman emission is generated based on four-wave Raman mixing. By phase locking the emission lines, the laser pulsewidth was reduced to 40 fs, when a nearly transform-limited pulse was utilized as a fundamental laser. The pulsewidth was further reduced to 20 fs, when a positively chirped pulse was employed. Computer simulation suggests that the Raman emission is strongly chirped and a train of pulses with lower intensities are formed when a chirp pulse is used as a fundamental laser. PACS 42.65.Dr; 42.55.Ye; 42.50-p     

New results in above-threshold ionization and high-order harmonic generation of atomic and molecular systems

Numerical results obtained applying the strong-field approximation to atomic and molecular processes in intense laser fields are presented. In particular, the forward-backward asymmetry in high-order above-threshold ionization (HATI) of Ar atoms by a few-cycle laser pulse is considered. It is shown that the resonantlike enhancements observed in the focal-averaged spectra disappear with the decreasing laser pulse duration. For HATI and high-order harmonic generation (HHG) by molecular systems, we present new results for diatomic molecules. The choice of gauge and the problem of dressing of the initial bound state are discussed. The appearance of the interference minima in molecular HATI and HHG spectra and their role in the characterization of the molecular structure are considered using the example of the Ar₂ molecule.     

脉冲激光在有机分子材料中的共振传播

利用麦克斯韦-布洛赫耦合方程,研究了激光脉冲在4,4′-二甲氨基二苯乙烯分子材料中的共振传播,探讨了激光脉冲在传播中的时空演化情况.在数值计算中考虑了各种阻尼效应.     

Exact Timing of Returned Molecular Wavepacket

An ionizing wavepacket of electron will re-visit its parent molecular ion during photoionization by strong laser field. This scenario is associated with physical concepts such as molecular re-scattering/collision, interference, diffraction, molecular clock, and generation of XUV light via high-order harmonic generation. On the workbench of a reduced dimensionality model of molecular hydrogen ions irradiated by laser pulse of 0.01-10.0 a.u. intensities, one-cycle pulsewidth, and 800nm wavelength, by deploying a momentum operator on the time-dependent wavefunction of an ionizing wavepacket, we can determine, in a precise manner, the exact time instant for the re-visiting electron to come back to the cation position. The time value is 57.6% of an optical cycle of the exciting laser pulse. This result may be useful in attosecond pump-probe experiments or molecular clock applications.     

Atomistic investigation of ablation of amorphous polystyrene under femtosecond laser pulse

In the present work we elucidate the thermodynamic mechanisms of femtosecond(fs)laser ablation of amorphous polystyrene by means of molecular dynamics(MD)simulations.The effects of extrinsic parameter of laser pulse intensity and intrinsic parameter of molecular architecture on the laser ablation are further studied.Simulation results show that the laser ablation-induced polymeric material removal is achieved by evaporation from the surface and expansion within the bulk.Furthermore,inter-chain sliding and intra-chain change also play important roles in the microscopic deformation of the material.It is found that both the laser pulse intensity and the arrangement of phenyl groups have significant influence on the fs laser ablation of polystyrene.     

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.     

Pulse Duration of Superradiance on Molecular Nitogen Ions in Air Laser Plasma

Russian Physics Journal - The results of a study of pulse duration of superradiance on molecular nitrogen ions in air under different conditions of focusing a femtosecond laser pulse with a...     

THz Radiation Generation via the Interaction of Ultra‐short Laser Pulses with the Molecular Hydrogen Plasma

In this paper, a two dimensional Particle In Cell‐Monte Carlo Collision simulation scheme is used to examine the THz generation via the interaction of high intensity ultra‐short laser pulses with an underdense molecular hydrogen plasma slab. The influences of plasma density, laser pulse duration and its intensity on the induced plasma current density and the subsequent effects on the generated THz signal characteristics are studied. It is observed that the induced current density in the plasma medium and THz spectral intensity are increased at the higher laser pulse intensities, laser pulse durations and plasma densities. Moreover, the generated THz electric field amplitude is reduced at the higher laser pulse durations. A wider frequency range for the generated THz signal is shown at the lower laser pulse durations and higher plasma densities. Additionally, it is found that the induced current density in hydrogen plasma medium is the dominant factor influencing the generation of THz pulse radiation. (© 2016 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Quantum control by ultrafast polarization shaping

We demonstrate that the use of time-dependent light polarization opens a new level of control over quantum systems. With potassium dimer molecules from a supersonic molecular beam, we show that a polarization-shaped laser pulse increases the ionization yield beyond that obtained with an optimally shaped linearly polarized laser pulse. This is due to the different multiphoton ionization pathways in K2 involving dipole transitions which favor different polarization directions of the exciting laser field. This experiment is a qualitative extension of quantum control mechanisms which opens up new directions giving access to the three-dimensional temporal response of molecular systems.     

Double Ionization Dynamics of Molecular Hydrogen in Ultrashort Intense Laser Fields

We experimentally investigate the double ionization of molecular hydrogen subjected to ultrashort intense laser pulses.The total kinetic energy release of the two coincident H~+ ions,which provides a diagnosis of different processes to double ionization of H_2,is measured for two different pulse durations,i.e.,25 and 5fs,and various laser intensities.It is found that,for the long pulse duration(i.e.,25 fs),the double ionization occurs mainly via two processes,i.e.,the charge resonance enhanced ionization and recollision-induced double ionization.Moreover,the contributions from these two processes can be significantly modulated by changing the laser intensity.In contrast,for a few-cycle pulse of 5fs,only the recollsion-induced double ionization survives,and in particular,this process could be solely induced by the first-return recollision at appropriate laser intensities,providing an efficient way to probe the sub-laser-cycle molecular dynamics.     

Pulse polarization splitting in a transient wave plate

We demonstrate propagation of ultrafast laser pulses through a molecular gas acting as a transient wave plate under conditions of strong phase modulation. The resulting decomposition of a linearly polarized laser pulse into two nearly distinct, orthogonally polarized laser pulses is demonstrated with transiently aligned, linear molecules.