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J P Marangos

Publications and source records attributed to J P Marangos.

4 recordsLinked to original sources

Probing proton dynamics in molecules on an attosecond time scale.

We demonstrate a technique that uses high-order harmonic generation in molecules to probe nuclear dynamics and structural rearrangement on a subfemtosecond time scale. The chirped nature of the electron wavepacket produced by laser ionization in a strong field gives rise to a similar chirp in the photons emitted upon electron-ion recombination. Use of this chirp in the emitted light allows information about nuclear dynamics to be gained with 100-attosecond temporal resolution, from excitation by an 8-femtosecond pulse, in a single laser shot. Measurements on molecular hydrogen and deuterium agreed well with calculations of ultrafast nuclear dynamics in the H2+ molecule, confirming the validity of the method. We then measured harmonic spectra from CH4 and CD4 to demonstrate a few-femtosecond time scale for the onset of proton rearrangement in methane upon ionization.

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Analysis of adiabatic passage by light-induced potentials with chirped laser pulses in three- and four-level diatomic systems.

This paper describes an investigation into the process of adiabatic passage by light-induced potentials (APLIP), which was previously suggested as a method for employing two strong picosecond laser pulses to transfer the population between two electronic states. We have extended earlier numerical studies in order to assess the feasibility of an experimental implementation of the APLIP concept. APLIP has been modeled in a three-level model system based on Na2 with chirped pulses, using laser parameters available from a typical chirped pulse amplified Ti:sapphire laser. The model showed that the APLIP process remains essentially unchanged for chirped pulses of equal magnitude and the opposite, or equal and positive sign of chirp as compared to the transform-limited case. We also examined the case of additional electronic states by introduction of a fourth state that lies close to the "target," i.e., final, state. The investigation showed that there are circumstances in which a significant fraction of the population gets transferred to this state which will disrupt the APLIP process. However, by switching to this fourth state as the target state in an experiment, good transfer efficiency is recovered. The results of the extension of the original APLIP modeling to chirped pulses and additional electronic states indicate that an APLIP experimental realization should be feasible in Na2.

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Controlling two-center interference in molecular high harmonic generation.

We experimentally investigate the process of intramolecular quantum interference in high-order harmonic generation in impulsively aligned CO2 molecules. The recombination interference effect is clearly seen through the order dependence of the harmonic yield in an aligned sample. The experimental results can be well modeled assuming that the effective de Broglie wavelength of the returning electron wave is not significantly altered by the Coulomb field of the molecular ion. We demonstrate that such interference effects can be effectively controlled by changing the ellipticity of the driving laser field.

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Role of the intramolecular phase in high-harmonic generation.

We study numerically the generation of high-order harmonics by two-center molecules for arbitrary angles between the molecular axis and the laser polarization axis. For fixed angle, the harmonic spectrum exhibits a minimum at a frequency which is independent of the laser parameters. The amplitude of each harmonic is strongly angle dependent, and a pronounced minimum is found at the same angle where a sudden jump in the harmonic phase occurs. By calculating the spatial dependence of the harmonic amplitudes and phases, we are able to explain these effects in terms of interfering contributions from various regions within the molecule.

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