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.     

Numerical Simulations of femtosecond-laser-induced dynamic alignment of molecules in the high-frequency off-resonance regime

The motion equation for ? between the molecular axis and laser polarization direction in a high-frequency off-resonance femtosecond laser field is deduced while simultaneously examining the effects of a permanent dipole moment and field-induced polarizability and hyperpolarizability to molecular rotation. Femtosecond-laser-induced dynamic alignment of CO, N₂, and Br₂ molecules are investigated by numerically solving the obtained rotation equation for the angle ?. The effects of the molecular permanent dipole moment and the field-induced polarizability and hyperpolarizability on the degree of alignment are presented at different intensities. Our computational results show that the dynamic alignment of molecules is primarily determined by field-induced polarizability and the second hyperpolarizability for the laser intensity range from 5 × 10¹⁴ to 5 × 10¹⁶ W/cm². The contributions of higher order correction terms to molecular alignment can usually be neglected. The polarizability-field interaction makes the angular distributions of a molecule have a maximum along the polarization axis and a minimum perpendicular to it. The role of the second hyperpolarizability keeps the molecular counts maximum along the laser polarization direction but minimum at an angle of 45° between the molecular axis and the polarization direction. There is also a second maximum of molecular counts perpendicular to the polarization axis. For CO, N₂, and Br₂ molecules, the dependences of laser-induced dynamic alignment on laser intensity exhibit completely different characteristics.     

Laser-induced Alignment and Coulomb Explosion of CO2

实验研究了CO₂分子在飞秒强激光脉冲作用下的动力学过程,包括分子取向,隧穿电离和库仑爆炸,激光强度从1×10¹³W/cm²变化到6×10¹⁴W/cm². 当激光强度小于分子的电离阈值时,CO₂分子的非绝热转动激发形成一个相干转动波包,波包演化导致分子沿激光电场方向取向. 激光脉冲结束后,分子取向可以周期性地再现,利用另一束激光可以对取向结构进一步进行修饰. 当激光强度大于分子     

控制双激光脉冲的宽度提高N2分子的取向

提出了通过控制双激光脉冲宽度的方法来提高N₂分子取向程度. 利用数值方法求解了N₂分子刚性转子模型在双激光脉冲作用下的薛定谔方程,计算了双原子分子N₂在总强度固定的两束激光脉冲作用下,不同脉冲宽度对于N₂分子取向的影响. 研究结果表明,通过调整两束激光脉冲的宽度,选择合适的延迟时间能够有效提高N₂分子的取向程度. 关键词： 双激光脉冲 分子取向 脉冲宽度     

极紫外阿秒脉冲在高次谐波产生过程中引起的非偶极效应

当红外强激光和极紫外(XUV)阿秒脉冲共同作用于原子分子时，电离出去的电子通常会吸收和辐射激光光子而发生能量扩展.讨论了由于XUV阿秒脉冲的短波长与扩展后的电子波包尺度可相比拟时在高次谐波产生过程中引起的非偶极效应.采用H⁺₂作为模型分子，并把分子轴置于激光场的传播方向，通过解二维含时薛定谔方程并比较考虑非偶极效应和采用偶极近似两种方法计算得到的结果，两者相比，前者的谐波强度降低，谐波频率向低级次稍有移动，电子能谱的能带内出现了更多的光电子峰.在相同的光电子能量处，两种方法计算得到的信号强度相差2—5倍.并且这种非偶极效应随着红外基频光光强的增大而增强，随阿秒脉冲波长的增大而减弱. 关键词： 非偶极效应 光场空间不均匀性 阿秒脉冲 高次谐波产生     

Nuclear fusion induced by a super-intense ultrashort laser pulse in a deuterated glass aerogel

A SiO₂ aerogel with absorbed deuterium is proposed as a target for the fusion reaction d + d → He³ + n induced by a superintense ultrashort laser pulse. The multiple inner ionization of oxygen and silicon atoms in the aerogel skeleton occurs in the superintense laser field. All the formed free electrons are heated and removed from the aerogel skeleton by the laser field at the front edge of the laser pulse. The subsequent Coulomb explosion of the deuterated charged aerogel skeleton propels the deuterium ions up to kinetic energies of ten keV and higher. The neutron yield is estimated at up to 10⁵ neutrons per laser pulse for ～200–500 ps if the peak intensity is 10¹⁸ W/cm² and the pulse duration is 35 fs.     

Weak magnetic field behavior of photon echo in a LuLiF4:Er3+ crystal

We report the first observation and study of the photon echo in Er³⁺:LuLiF₄. The energy transition is ⁴ I _15/2 → ⁴ F _9/2 (λ = 6536 Å). The density of ErF₃ is 0.025 wt %. The operation temperature is 1.9 K. Measurements were made at low (up to 1200 Oe) and even zero external magnetic fields. We studied the behavior of the photon echo intensity vs. the magnetic field magnitude and direction about the crystal axis C and vs. the laser pulse separation t ₁₂ and observed an exponential growth and then, after a certain plateau, an exponential decrease in the photon echo intensity as a function of magnetic field upon increasing the magnetic field from zero. The parameters describing the exponential growth and decrease are independent of the direction of magnetic field. The value of the magnetic field (～20–200 Oe) at which the echo intensity is maximal and the value of the maximum itself decrease with increasing pulse separation t ₁₂ and the angle Θ between the magnetic field and crystal axis. The echo intensity decreases exponentially with increasing Θ. The parameter describing the exponential decrease is independent of the magnitude of the field. The echo intensity as a function of pulse separation shows exponential decay. The phase relaxation time depends on the magnitude and direction of the magnetic field. T ₂ is equal to 202 ± 16 ns at zero magnetic field. A phenomenological formula is suggested, which qualitatively presents the mentioned dependences, and the polarization properties of the backward photon echo in this crystal are studied. Because the ion of trivalent erbium is an optimum data carrier, the above results show that fine control of the multichannel transfer of processed optical information may be achieved by weak magnetic fields.     

Rotational quasienergy states and alignment of molecules in a strong laser field

The interaction of a molecule with a strong laser field is investigated. Raman-type transitions between rotational levels of a fixed vibrational state of the ground-state term are taken into account in the “quantum rotator” approximation. An initial problem of the evolution of the state of a molecule interacting with a pulsed field is solved. The dynamics of the degree of alignment of a molecule with respect to the direction of polarization of the field during the pulse is investigated. It is shown that for sufficiently long pulses with a smooth envelope the axis of the molecule adiabatically follows the time-varying field amplitude, and alignment is maximum when the field intensity is maximum. It is shown that alignment of molecules can be substantial only if the second-order composite matrix elements, determining the probability amplitudes of transitions between rotational levels of a molecule, are much greater than the dissociation broadening of the levels. The angular distribution of the dissociation products of a molecule in a strong laser field is investigated. Zh. éksp. Teor. Fiz. 116, 1551–1564 (November 1999)     

Isotope-selective ionization utilizing molecular alignment and non-resonant multiphoton ionization

We demonstrate laser nitrogen isotope separation, which is based on field-free alignment and angular-dependent ionization of ¹⁴N₂ and ¹⁵N₂ isotopologues. A linearly polarized short laser pulse (???~?795?nm, ?????~?60?fs) creates rotational wave packets in the isotopologues, which periodically revive with different revival times as a result of different moments of inertia. Another linearly polarized short laser pulse (???~?795?nm, ?????~?60?fs) ionizes one of the isotopologues selectively as a result of their different angular distributions. In the present experiments, the ion yield ratio R [=I(¹⁵N₂ ⁺)/I(¹⁴N₂ ⁺)] can be changed in the range from 0.85 to 1.22, depending on the time delay between the two laser pulses.     

Possibilities for controlling attosecond x-ray pulse generation during molecular ionization by femtosecond laser radiation

We discuss the role of different factors (molecular sizes and configuration, orientation of the molecular axis with respect to the electric field of a laser pulse, the type of the molecular orbital, etc.), which characterize molecules and their state, in the formation of the nonlinear response of a molecule ionized by a high-power femtosecond laser pulse. In numerical experiments within the framework of a two-dimensional model for the H ₂ ⁺ molecular ion, we study possibilities for controlling the process of nonlinear frequency conversion of femtosecond optical radiation into X-ray radiation of attosecond duration by means of preliminary vibrational or electronic excitation of molecules. We demonstrate the possibilities of using the attosecond pulse generation as a diagnostic tool for probing vibration-rotational dynamics of molecules.     

Femtosecond laser-induced dynamic alignment in Coulomb explosion of CO: Roles of laser wavelength, intensity and pulse duration

Dependences of dynamic alignment of CO molecules induced by intense femtosecond laser fields on laser wavelength, intensity and pulse duration are investigated by numerical simulations. A counting approach and a fourth-order Runge-Kutta algorithm are used to calculate the angular distribution and the time evolution of molecules. A two-step Coulomb explosion model of diatomic molecules in intense laser fields is used to determine the instant that CO molecular dynamic alignment is over. Our calculating results show that the linear polarizability and the damping force play an important role in the angular rotation of CO molecule in conditions of 800 nm laser wavelength and 10¹⁵ W/cm² laser intensity. The contributions of the second-order field-induced dipole moment and the higher-order correction term to molecular rotation acceleration comparing to the linear polarizability and damping force are negligible. The extent of dynamic alignment of CO molecules reduces with the increasing of laser intensity. The dynamic alignment time of CO molecules is tightly connected to the laser pulse duration. The angular distributions of CO molecules as the laser pulse length varied from 50 to 250 fs at laser intensity of 3×10¹⁴ W/cm² are shown and discussed.     

Threshold dependence of the vibrational excitation of molecules on laser radiation intensity

The collisionless vibrational excitation of a polyatomic molecule in an IR laser radiation field has been theoretically studied. It has been shown that (i) the degree of vibrational excitation (namely, number 0000 of vibrational quanta of a molecular mode near-resonant with the IR laser field that are absorbed by the molecule) is low if laser pulse intensity P (energy flux density in the laser beam) is lower than a certain critical value P _cr; (ii) the degree of excitation abruptly increases after crossing the boundary where P = P _cr; (iii) this effect is attributed to two properties inherent in polyatomic molecules, namely, the anharmonicity of the vibrational mode interacting with the laser field and the energy exchange with other modes; and (iv) at P > P _cr, number 00000 is determined only by energy density Φ = Pτ_P, where τ_P is the laser pulse duration, 00000 monotonically increases with increasing Φ. The model is in good agreement with the experimental data.     

Efficient passively Q-switched Nd:YLF TEM00-mode laser at 1053 nm: selection of polarization with birefringence

The natural birefringence of the Nd:YLF crystal is utilized to achieve a reliable TEM₀₀-mode linearly polarized laser at 1053 nm in a compact concave-plano resonator. The efficient selection of the polarization relies on the combined effect of the difference in diffraction angle for ??- and ??-polarization of a wedged laser crystal and the alignment sensitivity of an optical resonator. We further employ a Cr⁴⁺:YAG saturable absorber to perform the passively Q-switched operation. At an incident pump power of 12?W, the maximum average output power is up to 2.3?W with a pulse repetition rate of 8?kHz and a pulse width of 9?ns. The pulse energy and peak power are found to be 288???J and 32?kW, respectively.     

Field-free molecular orientation with chirped laser pulse

We demonstrate theoretically that an efficient field-free molecular orientation driven by the positively chirped laser pulse whose frequency is in the terahertz regime can be achieved, taking the LiH molecule for example. Exact numerical calculations are performed by solving the time-dependent Schrödinger equation including the vibrational and rotational degrees of freedom. The maximal orientation degree of the LiH molecule  |  ? cosθ ?  |  _max  = 0.85 under the action of chirped laser pulse with the peak intensity of 4.78 × 10⁸ W/cm² at T = 0 K, which is larger than  |  ? cosθ ?  |  _max =0.75 driven by the half-cycle laser pulse with the same intensity. The molecular orientation degree decreases with the increase of temperature.     

Influence of collisions and pulse intensity on multiple photon absorption in SF6

Using a pyroelectric detector, the multiple photon absorption (MPA) of the SF₆ molecule in a wide range of pressures (10^-3 -1 torr) has been studied. The significant role of collisions in MPA has been shown. The fraction of molecules excited under essentially collisionless conditions has been defined. It is shown that under collisionless excitation of SF₆ (p < 10^-2 torr) at energy fluences E < 10^-1 J/cm² the intensity of the laser pulse plays the essential role, while in presence of collisions MPA is determined mainly by the energy fluence in the pulse.     

Influence of the shape of the exciting laser pulse on fluorescence saturation in the quantitative analysis of dissolved trace organic substances

Theoretical investigations of the influence of the exciting laser pulse shape on fluorescence saturation in the quantitative analysis of a single-component fluorescing solution, when the Raman signal of the solvent is usedas a reference, are carried out. A quantity α is introduced, responsible for the influence of laser pulse shape on the precision of the analysis. The dependences of α on the exciting radiation photon flux density I_m in the range I_m = 10²² ? 10²⁸ photons/cm²?s and on the duration of the exciting pulses τ_p in the range τ_p = 0.6 ? 60 ns are computed for different pulse shapes in the case of rhodamine 6G dissolved in water. Conditions when α is, in practice, independent of τ_p and of the pulse shape are found. A general analytical expression is found for α, which produces errors not greater than several percent when compared to the computed values of α. An experimental verification of the theoretical results in the case of a rectangular-shaped pulse in the spatial domain and a Gaussian-shaped pulse in the temporal domain is realized.     

The N+2 laser

Results of an experimental investigation of a gas-discharge pulse laser on the transition of the N⁺₂ molecule (λ = 4278 Å) are given. The time and spectral characteristics of the output radiation have been measured.     

Electron-positron pair production by electromagnetic pulses

Electron-positron pair production in vacuum by a single focused laser pulse and by two counter-propagating colliding focused pulses is analyzed. A focused laser pulse is described using a realistic three-dimensional model based on an exact solution of Maxwell’s equations. In particular, this model reproduces an important property of focused beams, namely, the existence of two types of waves with a transverse electric or magnetic vector (e-or h-polarized wave, respectively). The dependence of the number of produced pairs on the radiation intensity and focusing parameter is studied. It has been shown that the number of pairs produced in the field of a single e-polarized pulse is many orders of magnitude larger than that for an h-polarized pulse. The pulse-intensity dependence of the number of pairs produced by a single pulse is so sharp that the total energy of pairs produced by the e-polarized pulse with intensity near the intensity I _S = 4.65 × 10²⁹ W/cm² characteristic of QED is comparable with the energy of the pulse itself. This circumstance imposes a natural physical bound on the maximum attainable intensity of a laser pulse. For the case of two colliding circularly polarized pulses, it is shown that pair production becomes experimentally observable when the intensity of each beam is I ～ 10²⁶ W/cm², which is one to two orders of magnitude lower than that for a single pulse.     

Electron-positron pair creation by powerful laser-ion interaction

Presently available high-power laser pulses of ponderomotive energy U _p ? 2mc ² should permit the fundamental processes of quantum electrodynamics in such fields, in particular, the formation of electron-positron pairs in impacts of laser pulses with highly charged ions, to be observed. We evaluate the highly nonlinear production rates of this process and investigate the most favorable conditions of pair production, in particular, either along the direction of linear polarization or in the propagation direction of the laser pulse. For femtosecond radiation pulses, it is possible to represent the laser beam by a monochromatic and linearly polarized electromagnetic plane wave. This approximation considerably simplifies the calculations required.     

Narrow pulse width and high power passively Q-switched Nd3+:Gd3Ga5O12 laser with Cr4+:YAG saturable absorber

A compact, diode-pumped passively Q-switched Nd³⁺:Gd₃Ga₅O₁₂ (Nd:GGG) laser with Cr⁴⁺:YAG saturable absorber has been successfully demonstrated. Stable Q-switched pulses with pulse energy of 100 ??J and high peak power of 14 kW have been obtained. The pulse width was as short as 7 ns with low repetition rate of 10 kHz. The dependence of pulse width, pulse repetition rate, pulse energy and pulse peak power on pump power have been measured respectively. Experimental results reveal that the Nd:GGG crystal with Cr⁴⁺:YAG saturable absorber is suitable for narrow pulse width and high power passively Q-switched lasers.