Degenerate continuum superposition state

In this paper we generalize our previous results and show that direct as well as resonant processes can be controlled via the coherent generation of a degenerate continuum superposition state. Moreover we show that decay via a resonance (predissociation) enhances the probability of full control. The result is a practical way of altering product ratios in chemical (e.g. dissociation and ionization) decay processes using (weak) coherent radiation. 

The essential principle of coherent control in the continuum is to create a linear superposition of degenerate continuum eigenstates out of which the desired process (e.g., dissociation) occurs. If one can alter the coefficients a of the superposition at will, then the probabilities of processes, which derive from squares of amplitudes, will display an interference term whose magnitude depends upon the a,. Thus, varying the coefficients a, allows control over the product properties via quantum interference. This strategy forms the basis for coherent control scenarios in which multiple optical excitation routes are used to dissociate a molecule. It is important to emphasize that interference effects relevant for control over product distributions arise only from energetically degenerate states [7], a feature that is central to the discussion below. 

The system of integral equations [Eq. (66)] is eventually discretized and solved with numerical linear algebra procedures. At each energy, the system (66) must be solved for each of the open channels. A complete set of linearly independent degenerate real (i.e., stationary) continuum solutions if"E is thus obtained. The stationary scattering states xjr E are not orthogonal it can be shown that their superposition is given by... 

Thus the excitation pulse can create a superposition of i), 2) consisting of two states of different reflection symmetry. The resultant superposition possesses no symmetry properties with respect to reflection [78]. We now show that the broken symmetry created by this excitation of nondegenerate bound states translates into a nonsymmetry in the probability of populating the degenerate , n, D ), , n, L ) continuum states upon subsequent excitation. To do so we examine the properties of the bound-free transition matrix elements ( , n, q de,g Ek) that enter into the probability of dissociation. Note first that although the continuum states , n, q ) are nonsymmetric with respect to reflection, we can define symmetric and antisymmetric continuum eigenfunctions , n, s ) and , n, a ) via the relations... 

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