Theory of diatomic molecules in an external electromagnetic field from first quantum mechanical principles

The Journal of Physical Chemistry. a
Milan Sindelka, Nimrod Moiseyev

Abstract

We study a general problem of the translational/rotational/vibrational/electronic dynamics of a diatomic molecule exposed to an interaction with an arbitrary external electromagnetic field. The theory developed in this paper is relevant to a variety of specific applications, such as alignment or orientation of molecules by lasers, trapping of ultracold molecules in optical traps, molecular optics and interferometry, rovibrational spectroscopy of molecules in the presence of intense laser light, or generation of high order harmonics from molecules. Starting from the first quantum mechanical principles, we derive an appropriate molecular Hamiltonian suitable for description of the center of mass, rotational, vibrational, and electronic molecular motions driven by the field within the electric dipole approximation. Consequently, the concept of the Born-Oppenheimer separation between the electronic and the nuclear degrees of freedom in the presence of an electromagnetic field is introduced. Special cases of the dc/ac-field limits are then discussed separately. Finally, we consider a perturbative regime of a weak dc/ac field, and obtain simple analytic formulas for the associated Born-Oppenheimer translational/rotational/vibrational...Continue Reading

References

Jun 5, 1995·Physical Review Letters·B Friedrich, D Herschbach
Jan 22, 2002·Physical Review Letters·R A BartelsH C Kapteyn
May 1, 2004·Annual Review of Physical Chemistry·Graham A Worth, Lorenz S Cederbaum
Dec 17, 2004·Physical Review Letters·Kevin F LeeE A Shapiro
Dec 17, 2004·Nature·J ItataniD M Villeneuve

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Citations

Apr 2, 2008·The Journal of Chemical Physics·L S Cederbaum
Nov 8, 2019·Physical Review Letters·Erik UrbanHartmut Haeffner

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