184 resultados para photoionization


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Attosecond-pulse extreme-ultraviolet (XUV) photoionization in a two-color laser field is investigated. Attosecond pulse trains with different numbers of pulses are examined, and their strong dependence on photoelectronic spectra is found. Single-color driving-laser-field-assisted attosecond XUV photoionization cannot determine the number of attosecond pulses from the photoelectronic energy spectrum that are detected orthogonally to the beam direction and the electric field vector of the linearly polarized laser field. A two-color-field-assisted XUV photoionization scheme is proposed for directly determining the number of attosecond pulses from a spectrum detected orthogonally. (C) 2005 Optical Society of America.

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By means of the numerical solution of time-dependant Schrodinger equation, we verify a scaling law of photoionization in ultrashort pulses. We find that for a given carrier-envelope phase and duration of the pulse, identical photoionizations are obtained provided that when the central frequency of the pulse is enlarged by k times, the atomic binding potential is enlarged by k times, and the laser intensity is enlarged by k(3) times. The scaling law allows us to reach a significant control over direction of photoemission and offers exciting prospects of reaching similar physical processes in different interacting systems which constitutes a novel kind of coherent control.

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Using an unperturbed scattering theory, the characteristics of H atom photoionization are studied respectively by a linearly- and by a circularly- polarized one-cycle laser pulse sequence. The asymmetry for photoelectrons in two directions opposite to each other is investigated. It is found that the asymmetry degree varies with the carrier-envelope (CE) phase, laser intensity, as well as the kinetic energy of photoelectrons. For the linear polarization, the maximal ionization rate varies with the CE phase, and the asymmetry degree varies with the CE phase in a sine-like pattern. For the circular polarization, the maximal ionization rate keeps constant for various CE phases, but the variation of asymmetry degree is still in a sine-like pattern.

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We theoretically study the influence of Coulomb potential for photoionization of hydrogen atoms in an intense laser field with elliptical polarization. The total ionization rates, photoelectron energy spectra, and photoelectron angular distributions are calculated with the Coulomb-Volkov wave functions in the velocity gauge and compared with those calculated in the length gauge as well as those calculated with the Volkov wave functions. By comparing the results obtained by the Coulomb-Volkov and Volkov wave functions, we find that for linear polarization the influence of Coulomb potential is obvious for low-energy photoelectrons, and as the photoelectron energy and/or the laser intensity increase, its influence becomes smaller. This trend, however, is not so clear for the case of elliptical polarization. We also find that the twofold symmetry in the photoelectron angular distributions for elliptical polarization is caused by the cooperation of Coulomb potential and interference of multiple transition channels. About the gauge issue, we show that the difference in the photoelectron angular distributions obtained by the velocity and length gauges becomes rather obvious for elliptical polarization, while the difference is generally smaller for linear polarization.

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The asymmetric photoionization of atoms irradiated by intense, few-cycle laser pulses is studied numerically. The results show that the pulse intensity affects the asymmetric photoionization in three aspects. First, at higher intensities, the asymmetry becomes distinctive for few-cycle pulses of longer durations. Second, as the laser intensity increases, the maximal asymmetry first decreases then increases after it has reached a minimal value. Last, the value of the carrier-envelope phase corresponding to the maximal asymmetry varies with the pulse intensity. This study reveals that the increasing of pulse intensity is helpful for observing the asymmetric photoionization.

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Photoionization of hydrogen atoms in few-cycle laser pulses is studied numerically. The total ionization probability, the. instantaneous ionization probability; and the partial ionization probabilities in a pair of opposite directions are obtained. The partial ionization probabilities are not always equal to each other which is termed as inversion asymmetry. The variation of asymmetry degree with the CE phase, the pulse duration and the pulse intensity is studied. It is found that the pulse intensity affects the asymmetry degree in many aspects. Firstly, the asymmetry is more distinct at higher intensities than that at lower intensities when the pulse duration exceeds 4 cycles; secondly, the maximal asymmetry in lower intensities varies with the CE phase visibly while at higher intensities riot; thirdly, the partial ionization probabilities equal to each other for some special CE phases. For lower pulse intensities, the corresponding value of CE phase is always 0.5 pi and 1.5 pi, while for higher pulse intensities, the corresponding value varies with the pulse intensity. Similar phenomena were observed in a recent experiment using few-cycle radio-frequency (RF) pulses.

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The photoionization of H atoms irradiated by few-cycle laser pulses is studied numerically. The variations of the total ionization, the partial ionizations in opposite directions, and the corresponding asymmetry with the carrier-envelope phase in several pulse durations are obtained. We find that besides a stronger modulation on the partial ionizations, the change of pulse duration leads to a shift along carrier-envelope (CE) phase in the calculated signals. The phase shift arises from the nonlinear property of ionization and relates closely to the Coulomb attraction of the parent ion to the ionized electron. Our calculations show good agreement with the experimental observation under similar conditions.

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In this paper, a scaling law of photoionization of atoms irradiated by intense, few- cycle laser pulses is established. The scaling law sets a relation to the phase- dependent ionization with the kinetic energy of photoelectrons, the duration and peak intensity of short pulses, and the ionization potential of the target atoms. We find that it will be advantageous to manifest the phase- dependent photoionization by choosing the target atoms with larger ionization potential, using laser with smaller carrier- frequency, and increasing the pulse intensity. (c) 2007 Optical Society of America.

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The disolvated proton, H(OH2)2+ is employed as a chemical reagent in low pressure (˂ 10-5 torr) investigations by ion cyclotron resonance spectroscopy. Since termolecular reactions are absent at low pressure, disolvated protons are not generally observed. However H(OH2)2+ is produced in a sequence of bimolecular reactions in mixtures containing H2O and one of a small number of organohalide precursors. Then a series of hydrated Lewis bases is produced by H3O+ transfer from H(OH2)2+. In Chapter II, the relative stability of hydrated bases containing heteroatoms of both first and second row elements is determined from the preferred direction of H3O+ transfer between BH(OH2)+ complexes. S and P containing bases are shown to bind H3O+ more weakly than O and N bases with comparable proton affinities. A simple model of hydrogen bonding is proposed to account for these observations.

H+ transfer from H(OH2)2+ to several Lewis bases also occurs at low pressure. In Chapter III the relative importance of H3O+ transfer and H+ transfer from H(OH2)2+ to a series of bases is observed to be a function of base strength. Beginning with CH3COOH, the weakest base for which H+ transfer is observed, the importance of H+ transfer increases with increasing proton affinity of the acceptor base. The nature of neutral products formed from H(OH2)2+ by loss of H+ is also considered.

Chapters IV and V deal with thermochemistry of small fluorocarbons determined by photoionization mass spectrometry. The enthalpy of formation of CF2 is considered in Chapter IV. Photoionization of perfluoropropylene, perfluorocyclopropane, and trifluoromethyl benzene yield onsets for ions formed by loss of a CF2 neutral fragment. Earlier determinations of ΔH°f298 (CF2) are reinterpreted using updated thermochemical values and compared with results of this study. The heat of formation of neutral perfluorocyclopropane is also derived. Finally, the energetics of interconversion of perfluoropropylene and perfluorocyclopropane are considered for both the neutrals and their molecular ions.

In Chapter V the heats of formation of CF3+ and CF3I+are derived from photoionization of CF3I. These are considered with respect to ion-molecule reactions observed in CF3I monitored by the techniques of ion cyclotron resonance spectroscopy. Results obtained in previous experiments are also compared.

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The multi-configuration Dirac Fock (MCDF) method is implemented to study doubly excited 2s2p P-1,3(1) resonances of the helium atom and the interference between photoionization and photo excitation autoionization processes. In order to reproduce the total photoionization sprectra, the excited energies from the ground 1s(2) S-1(0) state to the doubly excited 2s2p P-1,3(1) states and the relevant Auger decay rates and widths are calculated in detail. Further more, the interference profile determined by the so-called Fano parameters q and rho(2) is also reproduced. Good agreement is found between the present results and other available theoretical and experimental results. This indeed shows a promising way to investigate the Fano resonances in photoionization of atoms within the MCDF scheme, although there are some discrepancies in the present calculations of the 2s2p P-3(1) state.

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There can be found some notable discrepancies with regard to the resonance structures when R-matrix calculations from the Opacity Project and other sources are compared with recent absolute experimental measurements of Bizau et al [Astron. Astrophts. 439 387 (2005)] for B-like ions N2+, O3+ and F4+. We performed close-coupling calculations based on the R-matrix formalism for the photoionizations of ions mentioned above both for the ground states and first excited states in the near threshold regions. The present results are compared with experimental ones given by Bizau et al and earlier theoretical ones. Excellent agreement is obtained between our theoretical results and the experimental photoionization cross sections. The present calculations show a significant improvement over the previous theoretical results.

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The cross sections of the 18 electron photoionization and corresponding shake-up processes for Li atoms in the ground state 1s(2)2s and excited states 1s(2)2p, 1s(2)3p, 1s(2)3p and 1s(2)3d are calculated using the multi-configuration Dirac-Fock method. The latest experimental photoelectron spectrum at hv = 100 eV [Cubaynes D et al. Phys. Rev. Lett. 99 (2007) 213004] has been reproduced by the present theoretical investigation excellently. The relative intensity of the shake-up satellites shows that the effects of correlation and relaxation become more important for the higher excited states of the lithium atom, which are explained very well by the spatial overlap of the initial and final state wavefunctions. In addition, strong dependence of the cross section on the atomic orbitals of the valence electrons are found, especially near the threshold.

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The photoionization cross sections of the ground level (3s(2) S-1(0)) of atomic Mg have been studied theoretically in the energy region between the Mg+(3s) and Mg+(3p) threshold using the fully relativistic R-matrix method. The positions and widths of resonances have also been obtained and compared with a recent experiment (Wehlitz et al 2007 J. Phys. B 40 2385). Excellent agreement is shown between our theoretical calculations and experimental measurements. In the present calculations, five Rydberg series of doubly excited states have been exhibited, i.e. 3pns P-1, 3pnd P-1, 3pns P-3, 3pnd D-3 and 3pnd P-3, where 3pnd P-3 are confirmed as the fifth series in contrast to the previous theoretical results.