One and two-center processes in high-order harmonic generation in diatomic molecules: Influence of the internuclear separation

We analyze the influence of different recombination scenarios, involving one or two centers, on high-order harmonic generation (HHG) in diatomic molecules, for different values of the internuclear separation. We work within the strong-field approximation, and employ modified saddle-point equations, in which the structure of the molecule is incorporated. We find that the two-center interference patterns, attributed to high-order harmonic emission at spatially separated centers, are formed by the quantum interference of the orbits starting at a center C _j and finishing at a different center C _ν in the molecule with those starting and ending at a same center C _j . Within our framework, we also show that contributions starting at different centers exhibit different orders of magnitude, due to the influence of additional potential-energy shifts. This holds even for small internuclear distances. Similar results can also be obtained by considering single-atom saddle-point equations and an adequate choice of molecular prefactors.     

Dramatic enhancement of high-order harmonic generation

We present a dramatic enhancement [Phys. Rev. Lett. 91, 043002 (2003)] of high-order harmonic generation by simultaneous irradiation of booster harmonics. A key feature of our experiment is the use of mixed gases (Xe and He) with different ionization energies. The harmonics from Xe atoms act as a booster to increase the harmonic yield from He by a factor of 4 x 10(3). The dominance of the dramatic enhancement effect is supported by simulation with the time-dependent Schr?dinger equation as well as the observed spatial characteristic of the generated harmonics and dependence on medium conditions.     

Near-threshold high-order harmonic spectroscopy with aligned molecules

We study high-order harmonic generation in aligned molecules close to the ionization threshold. Two distinct contributions to the harmonic signal are observed, which show very different responses to molecular alignment and ellipticity of the driving field. We perform a classical electron trajectory analysis, taking into account the significant influence of the Coulomb potential on the strong-field-driven electron dynamics. The two contributions are related to primary ionization and excitation processes, offering a deeper understanding of the origin of high harmonics near the ionization threshold. This Letter shows that high-harmonic spectroscopy can be extended to the near-threshold spectral range, which is in general spectroscopically rich.     

Ellipticity dependence of high-order above-threshold ionization from aligned diatomic molecules

We investigate high-order above-threshold ionization of the Ar₂ molecule by an elliptically polarized laser field. In order to describe this process we use the modified molecular strong-field approximation. We have found that the differential ionization rate is a very sensitive function of the ellipticity of the laser field and of the molecular orientation. For parallel orientation the rate has the maximum value for linear polarization, independently of the laser intensity. On the other hand, for perpendicular orientation the rate is maximal for a particular value of the ellipticity which is different from zero. Such a behavior can be related to the molecular symmetry. We consider the differential ionization rate of high-energy electrons as a function of the ellipticity for different internuclear distances. We also present, in the electron energy-emission angle plane, our new results for the focal-averaged spectra of electrons ionized by an elliptically polarized laser field. We have found that, in this case, the two-source two-rescattering-centers interference minima are blurred.     

拉伸分子高次谐波产生的阿秒控制

通过数值求解一维含时薛定谔方程,本文研究了高频阿秒脉冲对拉伸双原子分子模型与低频飞秒激光脉冲相互作用产生高次谐波谱的影响.研究表明,若阿秒脉冲在低频脉冲的第二个光学周期截止处注入时,只第二个平台截止位置IP 5.6UP(IP为电离势,UP为有质动力能)附近谐波的效率得到显著提高;若阿秒脉冲的包络峰值处于低频脉冲第三个光学周期T/4(为飞秒激光脉冲的光学周期)附近时,则谐波谱出现了明显的整体抬高现象.对此,本文根据拉伸分子谐波谱的四种产生机制及阿秒脉冲在飞秒激光不同相位注入时的电子电离曲线,对这些谐波谱的结构给出了合理解释.     

Ellipticity dependence of high-order harmonic generation from aligned molecules

We report ellipticity dependence of high-order harmonic generation (HHG) from aligned N2, O2, and CO2 molecules. Experimentally, we find that the ellipticity dependence is sensitive to molecular alignment and to the shape and symmetry of the valence orbitals. It is also found that the destructive interference in the recombination process affects the ellipticity dependence. Theoretically, we extend the original Lewenstein model to a more generalized model, which can be applicable to HHG from molecules, by introducing an electron acceleration parameter xi(theta) and by combining the molecular orbital method. The present observations are successfully explained by our model.     

Polarization state of high-order harmonic emission from aligned molecules

High harmonic emission in isotropic gases is polarized in the same direction as the incident laser polarization. Laser-induced molecular alignment allows us to break the symmetry of the gas medium. By using aligned molecules in high harmonic generation experiments, we show that the polarization of the extreme ultraviolet emission depends strongly on the molecular alignment and the orbital structure. Polarization measurements give insight into the molecular orbital symmetry. Furthermore, molecular alignment will allow us to produce attosecond pulses with time-dependent polarization.     

Iterative procedure for determining high-order corrections to the vibration-rotation spectra of diatomic molecules

The one-dimensional Schrödinger equation is reduced to a system of algebraic equations on the basis of the complex WKB method. As a result, recursion relations are obtained for the numerical calculation of high-order corrections to the vibration-rotation spectra of diatomic molecules. Various nonpolynomial representations of the potential are investigated.V. V. Kuibyshev State University, Tomsk. Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 6, pp. 9–16, June, 1994.     

Probing orbital structure of polyatomic molecules by high-order harmonic generation

The effects of electronic structure and symmetry are observed in laser driven high-order harmonic generation for laser aligned conjugated polyatomic molecular systems. The dependence of the harmonic yield on the angle between the molecular axis and the polarization of the driving laser field is seen to contain the fingerprint of the highest occupied molecular orbitals in acetylene and allene, a good quantitative agreement with calculations employing the strong field approximation was found. These measurements support the extension of the recently proposed molecular orbital imaging techniques beyond simple diatomic molecules to larger molecular systems.     

迭加态原子高次谐波发射的选频提高

本文研究了由体系的基态和较高激发态迭加形成的原子在强激光场作用下的高次谐波发射.观察电离波包的演化过程,阐明了谐波发射效率提高的原因.在给定入射激光条件下,通过选择不同的激发态,可以实现对谐波发射的控制.     

双色激光场中高次谐波转化效率的提高

采用渐近边界条件和辛算法数值求解双色激光场与模型P?schl-Teller势相互作用的含时Schr?dinger方程，计算了电离概率、平均位移、高次谐波以及跃迁概率；数值结果显示添加6倍频光的双色激光场能使高次谐波转化效率明显提高.分析了双色激光场极大地提高高次谐波转化效率的机理，并且通过对产生特定级次谐波的跃迁概率的计算，给出高次谐波转化效率提高的具体数值. 关键词： 渐近边界条件 辛算法 双色激光场 高次谐波     

Generation of non-integer high-order harmonics and significant enhancement of harmonic intensity

High-order harmonics from helium atom in the orthogonally two-color(OTC) laser field are investigated by solving the two-dimensional time-dependent Schrodinger equation.Non-integer high-order harmonics are obtained in some ratio of frequencies of two components.Pure odd and even harmonics from atoms could be separated in two components by adjusting the ratio of frequencies in OTC scheme,and the resolution of harmonics is improved at the same time.The physical mechanism is explained by the periodicity of dipole.With the same intensity of the incident laser,the intensity of the high-order harmonics from the OTC field scheme is improved by three orders of magnitude compared to the monochromatic laser field scheme.A theoretical scheme is provided for experimentally achieving improving energy resolution and separation of pure odd and even harmonics in atoms.Also,we provide a means for improving harmonic intensity.     

Dynamic properties of angle-dependent high-order harmonic generation from coherently rotating molecules

High-order harmonic generation from coherently rotating N2 and O2 molecules has been observed for different alignment angles in a pump and probe experiment using femtosecond laser pulses. The results obtained are in excellent agreement with those calculated using a recently developed theory, which represent the characteristic properties predicted for angle-dependent harmonic generation. It is shown that polarization geometry and alignment distribution play essential roles in potential applications to probe electronic structure and dynamics of molecular systems.     

双色场中高次谐波转化效率提高的数值研究

采用渐近边界条件和辛算法数值求解了双色激光场分别与模型Pschl-Teller势和模型He⁺相互作用的含时Schrdinger方程的无穷空间初值问题,计算了电离概率、电子平均位移、高次谐波与跃迁概率;数值结果显示,添加适当的倍频光的双色激光场使高次谐波转化效率极大提高,并给出定性与定量分析. 关键词： 辛算法 双色激光场 高次谐波 定量分析     

采用适宜靶原子提高高次谐波的转化效率

通过对影响谐波转化效率因素的分析,提出选择适宜的靶原子对象,即选择在高能区具有较强连续态-基态耦合强度的靶原子,可以优化高次谐波的发射条件.本文的数值实验结果表明,利用该方案,可以把平台区尾部谐波的转化效率提高两个数量级.     

强激光场中N2分子高次谐波的干涉效应

在强场近似下,利用Lewenstein模型研究了N2分子在强激光场中发射高次谐波的干涉效应,通过对N2分子产生的高次谐波和分子中单个原子产生高次谐波的比较,表明了干涉效应的存在. 得出随着高次谐波阶数的增加,干涉极小值会随着分子轴与激光偏振方向间夹角的增加而减小,在角度接近900附近时干涉效应消失,与两中心干涉模型预测的趋势一致. 通过分析高次谐波产生的机制和相位随取向角的变化,给出了干涉产生的原因.     

Observation of high-order quantum resonances in the kicked rotor

Quantum resonances in the kicked rotor are characterized by a dramatically increased energy absorption rate, in stark contrast to the momentum localization generally observed. These resonances occur when the scaled Planck's constant Planck's [over ]=r/s 4pi, for any integers r and s. However, only the variant Planck's [over ]=r2pi resonances are easily observable. We have observed high-order quantum resonances (s>2) utilizing a sample of low energy, noncondensed atoms and a pulsed optical standing wave. Resonances are observed for variant Planck's [over ]=r/16 4pi for integers r=2-6. Quantum numerical simulations suggest that our observation of high-order resonances indicate a larger coherence length (i.e., coherence between different wells) than expected from an initially thermal atomic sample.     

通过双色场和静电场的合成来拓宽高次谐波谱

本篇文章提出了一种通过双色激光场和静电场合成来拓宽高次谐波谱平台区域的方案.我们针对氦原子数值求解了一维含时薛定谔方程,并且得到了不同合成激光场条件下的高次谐波谱,并结合了经典电离-回碰动能分布图和时频分布图分析了静电场对高次谐波谱产生过程的影响.计算结果表明,通过在双色激光场上叠加一个静电场,可以有效地拓宽高次谐波谱的平台区域,从而得到一个频带宽度为358eV的超连续谱.     

Nonlinear steady-state sized resonances in diatomic nanostuctural objects

A new solution to modified Bloch equations for a diatomic quantum system consisting of two identical interacting atoms in a field of high-intensity continuous radiation is obtained. On the basis of this solution, the existence of nonlinear sized resonances whose properties strongly depend on the atomic spacing, on the polarization of the external field of radiation, and on the initial inversions of atoms constituting a nanostructural object is shown. Dispersion dependences of induced dipole moments and inversions of atoms of the object are investigated theoretically in the region of sized resonances for various irradiation conditions.