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论文类型：期刊论文

发表时间：2009-12-01

发表刊物：JOURNAL OF THEORETICAL & COMPUTATIONAL CHEMISTRY

收录刊物：SCIE、Scopus

卷号：8

期号：6

页面范围：1197-1215

ISSN号：0219-6336

关键字：Above threshold dissociation (ATD); quantum wave packet; femtosecond laser; molecular alignment

摘要：The above threshold dissociation (ATD) of the HD+ molecular ion in a linearly polarized femtosecond laser field is theoretically studied using three-dimensional time-dependent quantum wave packet method. Based on the Born-Oppenheimer approximation (BOA), calculations are performed on two electronic states, the ground state 1s sigma and the excited state 2p sigma. The energy-dependent distributions of the dissociated fragments, resulting from the ATD, are calculated by using an asymptotic-flow expression in the momentum space. The numerical results demonstrate that, in the laser field of wavelength lambda = 800 nm and full-width at half-maximum (FWHM) tau = 30 fs, only two-photon dissociation is observable at a weaker pulse peak intensity, 5.0 x 10(12) Wcm(-2), while at an intense intensity, 1.5 x 10(15) W cm(-2), the dissociated fragments resulting from four-photon absorption dominates over the photodissociation process. These results are consistent with the experimental observation of Orr et al. [Orr PA et al., Phys Rev Lett 98:163001, 2007]. The ac Stark-shift caused by intense laser field will change the kinetic energies of the fragments. The ATD phenomena are quantitatively interpreted in terms of the concept of light-induced potential. The molecular rotation and alignment have some effects on the kinetic energy spectrum of the dissociated fragments. The molecular rotation reduces the ac Stark-shift and broadens the peaks of kinetic energy spectra of the dissociated fragments. However, the intense laser field can effectively align the molecule and is helpful to increase the ATD probability. The ATD spectrum is related to the initial quantum numbers J(0) and M-0 of the molecule. The ATD spectrum of HD+ is calculated at a limited thermal temperature.