Dipolar effects on propagation of ultrashort laser pulse in one-dimensional para-nitroaniline (pNA) molecules

• The dynamic behaviour of ultrashort (femtosecond) laser pulses in a molecular medium is studied by solving the full Maxwell-Bloch equations beyond the limits of the slowly varying envelope approximation and the rotating-wave approximation under the resonant and the non-resonant conditions. A one-dimensional asymmetric charge-transfer molecule, para-nitroaniline, is used as a model molecule whose electronic properties are calculated with the time-dependent hybrid density functional theory. Under the one-photon resonant condition, 4 pi pulse is separated into two sub-pulses. The weight of the second-harmonic component mainly contributed by the two-photon excitation becomes stronger with longer propagation time. Under the two-photon resonant condition, the separation of 4 pi pulse is not induced and many higher-order spectral components beyond the second-harmonic generation occur. Interestingly, when the pulse propagates for long enough, the carrier modification becomes so significant that a continuous spectrum is generated. The Fourier transform of the high-harmonic spectrum demonstrates that an even shorter laser pulse can be produced in both resonant and non-resonant propagations. The effects of permanent dipole moments on the pulse evolution are discussed.

Nyckelord

femtosecond optical pulses

high-harmonic-generation

2-photon absorption

attosecond pulses

2-level medium

light

media

hyperpolarizability

density

moments

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