Nonintrusive measurement of field-free molecular alignment

A technique was provided to nonintrusively quantify the field-free alignment of molecules by measuring the transient birefringence caused by the aligned molecules. Pure heterodyne alignment signals were obtained from the difference of the signals under an external electric field with opposite polarity and equal magnitude. The results demonstrated that the pure heterodyne alignment signal directly reproduced the revival structure of molecular alignment and its Fourier transform spectroscopy represented the actual populations of the different J states in the rotational wave packet.     

Ionization effects on field-free molecular alignment observed with high-order harmonic generation

In this paper, high-order harmonic generation (HHG) is demonstrated to provide a sensitive way for studying the dynamic process in the field-free molecular alignment. The dependence of the harmonic yield and the degree of alignment on the intensity of aligning pulse is observed in impulsively aligned CO₂ molecules. A good agreement is found between the experimental and calculated results. At low pump intensities, the harmonic yield increases monotonously until the ionization induced refractive index gradient and neutral molecule depletion are significant. The results show that the optimum intensity is around 8.95 × 10¹³ W/cm²; this value is related to the molecular ionization potential.     

Observation of enhanced field-free molecular alignment by two laser pulses

We show experimentally that field-free alignment of iodobenzene molecules, induced by a single, intense, linearly polarized 1.4-ps-long laser pulse, can be strongly enhanced by dividing the pulse into two optimally synchronized pulses of the same duration. For a given total energy of the two-pulse sequence the degree of alignment is maximized with an intensity ratio of 1:3 and by sending the second pulse near the time where the alignment created by the first pulse peaks.     

Control of femtosecond filamentation by field-free revivals of molecular alignment

We show that the filamentation dynamics of a femtosecond laser probe pulse can be readily controlled by properly matching it to the quantum revivals of pre-aligned molecules prepared through impulsive rotational Raman excitation with an advancing ultrashort pump pulse. Several features of the filamentation process including supercontinuum generation, the length of the plasma channel generated in the wake of the filament, the associated secondary radiations and the multiple filamentation pattern are all easily modified by tuning the cross phase modulation induced by the field-free revivals of molecular alignment, through the delay between the pump and the probe pulses. We show that molecular alignment can also be used to generate conical waves with extremely short intensity spike called shocked X-waves and to further tune the frequency of a few-cycle laser pulse in the wake of a self-guided intense filament.     

Nonadiabatic alignment of asymmetric top molecules: field-free alignment of iodobenzene

Nonadiabatic laser alignment of an asymmetric top molecule is studied using the combination of a quantum dynamical theory and time-resolved photofragment imaging experiments. In particular, the degree of alignment of iodobenzene, induced by an intense, linearly polarized picosecond laser pulse, is calculated and measured. Pronounced alignment is obtained under field-free conditions.     

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.     

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.     

Controlling attosecond double ionization dynamics via molecular alignment

We investigate the dynamics of double ionization in aligned nitrogen molecules. An ultrashort, weak laser pulse creates an aligned ensemble of molecules that is ionized with a subsequent, strong probe pulse. We find that the two electrons involved in nonsequential double ionization more likely exit the molecule in the same direction if it is parallel to the probe laser polarization, indicating that they are ejected within a few hundred attoseconds of each other. Double ionization is less probable and takes longer for perpendicular molecules.     

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.     

Strong-field double ionization of Ar below the recollision threshold

Nonsequential double ionization of Ar by 45 fs laser pulses (800 nm) at (4-7)x10;{13} W/cm;{2} was explored in fully differential measurements. Well below the field-modified recollision threshold we enter the multiphoton regime. Strongly correlated back-to-back emission of the electrons along the polarization direction is observed to dominate in striking contrast to all previous data. No effect of Coulomb repulsion can be found, the predicted cutoff in the sum-energy spectra of two emitted electrons is confirmed, and the potential importance of multiple recollisions is discussed.     

S-matrix study on alignment dependence of single ionization of molecular ions with different active orbitals

The orientation-dependent single ionization rate of the diatomic molecular ion H_2^+ with different active orbitals in an intense field is studied by using S-matrix theory. Our results show that the orientation-dependent single ionization probability of H_2^+ is greatly dependent on the symmetry and the electron density distribution of its initial states, and it can be used to identify the excited state of the molecular ion in the dissociation process.     

Strong-field multiphoton ionization of hydrogen. TheS-matrix treatment of the elementary process

Summary A theoretical model is presented to treat the elementary act of strong-field multiphoton ionization of atoms when the electron continuum final-state distribution is important. It is based on theS-matrix formalism and treats the final-state electron-radiation interaction in an essentially nonperturbative way. Selected numerical calculations concern the ionization of hydrogen atoms and include differential and total cross-sections of several multiphoton channels as a function of the laser intensity. Good, qualitative agreement with the experimental observations is found for values of the field intensity which are not critical with respect to the simplifications adopted in constructing the theoretical model. It applies particularly to the use of an ideal model for the laser field. Significant departure from observations is instead found when the implications of the ideal laser model play a critical role, as occurs at channel inversion and suppression. It is concluded that the theoretical treatment to be completely satisfactory needs essentially to incorporate a more realistic laser model such as a multimode one.

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Riassunto Si presenta un modello teorico per il processo elementare della ionizzazione multifotonica di atomi da parte di un forte campo laser quando diventa importante la distribuzione degli stati finali del continuo dell'elettrone. Il modello si fonda sul formalismo della matriceS e tratta l'interazione elettrone-radiazione nello stato finale in modo non perturbativo. I calcoli numerici qui riportati si riferiscono alla ionizzazione di atomi d'idrogeno e includono sezioni d'urto totali e differenziali per diversi canali multifotonici in funzione dell'intensità del laser. Si trova un accordo qualitativo con i dati sperimentali per valori dell'intensità del campo che non sono critici rispetto alle semplificazioni adottate nella costruzione del modello teorico. Un significativo distacco dai dati sperimentali si ha quando le implicazioni del modello di laser ideale giocano un ruolo critico, come si ha per l'inversione e la scomparsa dei canali. Si conclude che il trattamento teorico per essere completamente soddisfacente necessita dell'introduzione di un modello di laser piú realistico, quale, ad esempio, quello a molti modi.

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Резюме Предлагается теоретическая модель для рассмотрения элементарного акта многофотонной ионизации атомов в сильном поле, когда распределение электронных непрерывных конечных состояний является существенным. Подход базируется на формализмеS-матрицы и взаимодействие электронов в конечном состоянии с полем излучения рассматривается непертурбационным образом. Численные вычисления касаются ионизации атомов водорода и включают дифференциальные и полные поперечные сечения для некоторых многофотонных каналов, как функции интенсивности лазерного излучения. Получено хорошее качественное согласие с экспериментальными результатами для значений интенсивности поля, которые не являются критическими по отношению к упрощениям, используемым при конструировании теоретической модели. Используется идеальная модель для лазерного поля. Обнаружено существенное отклонение от экспериментальных результатов в тех случаях, когда имеет место инверсия и подавление каналов. Делается вывод, что теоретический подход становится удовлетворительным, если используется более реалистическая модель лазера, как например, многомодовая модель.

     

Effects of aligning pulse duration on the degree and the slope of nitrogen field-free alignment

Through theoretical analysis,we show how aligning pulse durations affect the degree and the time-rate slope of nitrogen field-free alignment at a fixed pulse intensity.It is found that both the degree and the slope first increase,then saturate,and finally decrease with the increasing pump duration.The optimal durations for the maximum degree and the maximum slope of the alignment are found to be different.Additionally,they are found to mainly depend on the molecular rotational period,and are affected by the temperature and the aligning pump intensities.The mechanism of molecular alignment is also discussed.     

Determination of energy dependent ionization probabilities of sputtered particles

We present a novel method to determine the spectral ionization probability of sputtered species as a function of their emission velocity or energy. The technique is based on detection of neutral and ionic species in a reflectron time-of-flight mass spectrometer under otherwise identical experimental conditions. Using a pulsed ion extraction scheme in combination with sufficiently short primary ion pulses, the spectral ionization probability α⁺(v) can be determined without knowledge of possible energy discrimination effects in instrument transmission. Comparing the measured ionization probability with theoretical predictions, we find that none of the prevailing ionization models is capable of describing the experimental data over the whole velocity range studied.     

Impact-parameter dependence of ionization probabilities of the L sub-shells

Ionization probabilities of the L_I and L_III subshells have been calculated for ⁸²Pb by the impact of protons with in the frame work of binary encounter approximation (BEA) theory. The results obtained have been compared with the probabilities based on semi-classical approximation (SCA) theory.     

On the question of determining molecular electric dipole moments from field-free frequency data

The effective masses in the Hamiltonian of a diatomic molecule with corrections for the breakdown of the Born-Oppenheimer approximation depend on the charge distribution in the molecule, and so the field-free energy levels are possible sources of information on the electric dipole moment of the molecule and other electromagnetic quantities. However, examination of explicit energy formulas and of a general indeterminacy in the effective Hamiltonian shows that this information is inseparable from effects due to the adiabatic correction to the potential. Electric dipole moments and other electromagnetic quantities obtained in this way are therefore not reliable.     

Selective alignment of molecular spin isomers

We experimentally demonstrate field-free, spin-selective alignment of ortho- and para molecular spin isomers at room temperature. By means of two nonresonant, strong, properly delayed femtosecond pulses within a four wave mixing arrangement, we observed selective alignment for homonuclear diatomics composed of spin 1/2 (15N) or spin 1 (14N) atoms. The achieved selective control of the isomers' angular distribution and rotational excitation may find applications to analysis, enrichment, and actual physical separation of molecular spin modifications.     

Strong-field double optical resonance with two kinds of homogeneous broadening

We study the absorption spectrum of a probe field in a two-level atomic system excited by a strong laser field in the presence of both collisional and laser dephasing processes. We show that the effects of these two kinds of homogeneous broadening on the absorption line shape are quite different.     

Positron impact ionization of molecular oxygen

We have carried out distorted wave calculations of positron ionization of molecular oxygen in order to compare with experimental measurements. In this work the oxygen molecule was represented by a Gaussian wave function which includes contributions from alpha and beta electrons. We find that our CPE model produces results which are in good agreement with the combined measurements for total ionization and positronium formation.