4.6 Article

Quantum-beat imaging of the nuclear dynamics in D2+: Dependence of bond softening and bond hardening on laser intensity, wavelength, and pulse duration

Journal

PHYSICAL REVIEW A
Volume 79, Issue 3, Pages -

Publisher

AMER PHYSICAL SOC
DOI: 10.1103/PhysRevA.79.033410

Keywords

deuterium; Fourier transforms; photoionisation; quantum optics; positive ions; quantum beat spectra; quantum optics; vibrational states

Funding

  1. NSF
  2. Division of Chemical Sciences, Office of Basic Energy Sciences, Office of Science, U.S. DOE

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Based on a quantum-mechanical model, we calculate the time evolution of an initial nuclear vibrational wave packet in D-2(+) generated by the rapid ionization of D-2 in an ultrashort pump-laser pulse. By Fourier transformation of the nuclear probability density with respect to the time delay between the pump pulse and the instant destructive Coulomb-explosion imaging of the wave packet at the high-intensity spike of an intense probe-laser pulse, we provide two-dimensional internuclear-distance-dependent power spectra that serve as a tool for visualizing and analyzing the nuclear dynamics in D-2(+) in an intermittent external laser field. The external field models the pedestal to the central ultrashort spike of a realistic probe pulse. Variation in the intensity, wavelength, and duration of this probe-pulse pedestal (i) allows us to identify the optimal laser parameters for the observation of field-induced bond softening and bond hardening in D-2(+) and (ii) suggests a scheme for quantitatively testing the validity of the Floquet picture that is commonly used for the interpretation of short-pulse laser-molecule interactions, despite its implicit continuum wave (infinite pulse length) assumption.

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