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Optics and Spectroscopy

Slowing down of the relaxation of high-frequency gas polarization in a constant electric field

Vladimir A. Kukushkin

Published Oct 1, 2001• 0 citations
Publisher

Abstract

It is found that a sufficiently strong electric field can substantially decrease the relaxation rate of high-frequency polarization of a gas corresponding to the resonance dipole-dipole interaction of its molecules. The corresponding decrease in the integrated cross section for intermolecular Weisskopf collisions is calculated using the two-level approximation for the description of quantum dynamics of internal (vibrational) degrees of freedom of molecules, whereas their translational and rotational motions are treated classically. It is shown that the effect is caused by the Stark change of dipole moments of molecules and the ordering of their orientations in a constant electric field. As a result, for a certain magnitude of this field, the contributions of constant and high-frequency dipole moments of a molecule to the change in its density matrix upon a collision are counter-balanced to a considerable extent. The conditions required for the experimental observation of the effect are formulated.

DOI
10.1134/1.1412675

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It is found that a sufficiently strong electric field can substantially decrease the relaxation rate of high-frequency polarization of a gas corresponding to the resonance dipole-dipole interaction of its molecules. The corresponding decrease in the integrated cross section for intermolecular Weisskopf collisions is calculated using the two-level approximation for the description of quantum dynamics of internal (vibrational) degrees of freedom of molecules, whereas their translational and rotational motions are treated classically. It is shown that the effect is caused by the Stark change of dipole moments of molecules and the ordering of their orientations in a constant electric field. As a result, for a certain magnitude of this field, the contributions of constant and high-frequency dipole moments of a molecule to the change in its density matrix upon a collision are counter-balanced to a considerable extent. The conditions required for the experimental observation of the effect are formulated.
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Collisions of polar $^{1}\ensuremath{\Sigma}$ state molecules at ultralow energies are considered, within a model that accounts for long-range dipole-dipole interactions, plus rotation of the molecules. We predict a substantial suppression of dipole-driven inelastic collisions at high values of the applied electric field, namely, field values of several times ${B}_{0}∕\ensuremath{\mu}$. Here B0{B}_{0}B0​ is the rotational constant, and $\ensuremath{\mu}$ is the electric dipole moment of molecules. The sudden large drop in the inelastic cross section is attributed to the onset of degeneracy between molecular rotational levels, which dramatically alters the scattering Hamiltonian. This capability could, in principle, be used to stabilize ultracold gases against collisional losses.
We present a rigorous study of cold and ultracold collisions of $\mathrm{Yb}\mathrm{F}(^{2}\ensuremath{\Sigma})$ molecules with He atoms in external electric and magnetic fields based on an accurate calculation of the interaction potential surface and quantum theory of atom-molecule scattering. We analyze the mechanisms of collisional depolarization of the electron and nuclear spins of YbF and demonstrate that the rate constants for elastic and inelastic collisions of YbF with He are sensitive to the magnitudes of the applied fields. Collisions of heavy polar molecules like YbF may thus be easily manipulated with external electromagnetic fields. We show that collisional spin relaxation of YbF molecules in rotationally excited states is suppressed by electric fields much more significantly than the spin relaxation in the ground rotational state. We explain this by the influence of electric-field-induced Feshbach resonances, which occur at much lower collision energies when the molecule is rotationally excited. Our results suggest that heavy polar molecules may be amenable to magnetic trapping in a buffer gas of He, which could greatly enhance the sensitivity of spectroscopic experiments to measure the electric dipole moment of the electron.
Two elementary models of molecular structure are used to investigate inelastic collisions in cold trapped dipolar gases. A two-state model of a polar molecule (such as one with a Λ-doublet) permits analytic description of the inelastic collision process at energies considerably higher than the gap energy, predicting rate constants and cross sections given by elementary formulae. Alternatively, a three-state model of a rotor molecule in an electric field is investigated, with resultant rate constants and cross sections scaling simply with molecular mass, rotational constant, dipole moment and polarizing field strength. Semiclassical inelastic collision cross sections and rate constants are demonstrated to depend strongly on the model used, especially as regards their dependence on the polarizing field. Inelastic cross sections among doublet dipoles decrease with increasing field strength, while they increase in proportion to the square of the field strength for collisions between rotor dipoles.
An interaction of an atomic/molecular medium with two strong electric fields E L (t) and E M (t) is investigated. The frequency omega L of the first (laser) field E L (t) is close to a transition frequency omega 21 between an upper (2) and a lower (1) atomic levels while the second field E M (t) is of a much lower frequency omega M << omega 21 . The medium is a dipole gas characterized by a nonzero averaged value of electric dipole moment in the states 1 and/or 2. As analytical solution of equations for the density matrix of a dipole atom/molecule interacting with the fields E L (t) and E M (t) is found using the second approximation of the averaging method by Krylov-Bogoliubov-Mitropolskii. The solution obtained is valid in a much broader range of field strengths than an analogous solution that could have been found by the usual time-dependent perturbation theory. Using the solution obtained for the density matrix, polarization of a dipole gas interacting with the fields E L (t) and E M (t) is analytically calculated. This analytical expression for polarization of such media can be utilized for study of various nonlinear optical phenomena. One of the phenomena is a generation of waves at frequencies omega L +or-p omega M and (p+1) omega M (where p=1,2,3,...) in a dipole gas. Another phenomenon is an amplification of the incident wave of the lower frequency omega M due to a stimulated scattering in a dipole gas.
We discuss the influence of collisions on the dynamics of an ultracold gas whose constituents interact via dipolar forces. This dynamics is governed by the elastic scattering cross section of the molecules, which is to some extent under the experimentalist's control. We compare side-by-side several different situations, highlighting their similarities and differences. These situations are collisions between: 1) point dipoles; 2) electric-field-shielded polar molecules; and 3) microwave-shielded polar molecules, including the effect of microwave ellipticity.