The problem of calculating transition probabilities for an atom interacting with an intense radiation field is set up within the context of an effective Hamiltonian formalism. This has the virtue that resonance effects are properly accounted for at the outset; more generally, it provides a convenient framework for approximations. Through the restriction of the class of intermediate states to be included in the construction of the effective potential, a unitary (nonperturbative) model is obtained. A successive approximation procedure for determining the effective potential, which is based on continued-fraction representations, is described. While very likely intractable for the true problem, this successive approximation procedure can be implemented, for the model effective potential, with the aid of a generalized Rayleigh-Ritz procedure described here. The level-shift matrix is constructed from the effective potential; it determines the transition probabilities, linewidths, and energy-level displacements induced by the field. We derive variational expressions of the Kohn type for each of the elements of the model level-shift matrix.
A successive-approximation procedure for calculating multiphoton-transition amplitudes is presented. The theory, designed for use in the strong-field domain where ordinary perturbative methods are unsuitable, provides an extension of previous work along these lines by inclusion of the effects of free-free transitions, i.e., interactions with the field which take the atomic system from one continuum state to another. This approach is based on the introduction of an effective Hamiltonian which operates only in the subspace of states, degenerate or nearly degenerate, among which real transitions can take place. Contributions from virtual intermediate states are included in the structure of the effective potential. This approach provides the framework for the construction of models, defined by the approximations made for the effective potential, which build in the constraints of unitarity and which properly account for the effects of intermediate-state resonances. The present work is focussed on those new features of the problem which arise from the fact that both the electron and the residual atom to which it was originally bound can interact with the field in asymptotic states. To avoid complications associated with long-ranged Coulomb effects, the residual atom is assumed to be neutral. (The initial state is a negative ion.) An approximation procedure is described for calculating the field-modified asymptotic states appropriate for such a system. By way of an illustrative example a low-frequency approximation is given which leads to considerable simplification of the calculational procedure.
The summation of all the higher-order contributions to multiphoton absorption in atoms is presented. The nonperturbative expressions for the transition amplitudes are expressed in terms of continued fractions. They account for the whole perturbation originated by the radiation field on the atom but do not exhibit explicit expression for the level shift. In the case of radiation fields of high intensity the only reliable determination of the level shift involves a careful location of the poles of the resolvent operator. The theory has been tested in considering a two-level atom. An extremely rapid convergence of the continued fractions has been observed, and accurate results concerning high-order resonance shifts have been obtained. The expressions for the transition amplitudes being nonperturbative with regard to the field strength, they can be considered as analytic continuations of the perturbation series. This provides a useful approach to the problem of ultraintense fields.
The construction of physical occupation and transition probabilities in non-Hermitian, effective-Hamiltonian models of coupled near-resonant discrete states which decay to a continuum is analyzed. We consider for definiteness the particular physical example of atomic multiphoton ionization. The possibility of finite duration and arbitrary modulation of this interaction, and of the subsequent ionization and/or decay, in such a system allows us to invoke "adiabatic switching" considerations in conventional
S-matrix theory. The effective Hamiltonian $\stackrel{^}{H}(t)$ is derived for both stationary and time-dependent Schr\"odinger equations. These derivations yield the same effective $\stackrel{^}{H}(t)$, and further reveal that this operator is associated with discrete-state-projected "incoming" scattering states. The Hermitian conjugate operator ${\stackrel{^}{H}}^{\ifmmode\dagger\else\textdagger\fi{}}(t)$ is similarly shown to be associated with discrete-state "outgoing" scattering states. This shows that effective-Hamiltonian theories are intrinsically
S-matrix theories. This fact, in turn, is employed to construct transition amplitudes. The possibility of resonance in the atom-field interaction requires that both the projected incoming states and projected outgoing states be employed in this construction. The projected incoming and outgoing states in the (discrete) bound space are quite conveniently described by effective time-dependent Schr\"odinger equations, supplemented by initial- and final-state boundary conditions. The fact of independent-exponential decay from each mode throughout the history of the interaction, for an arbitrary initial superposition state, in the adiabatic limit, suggests a practical construction for intermediate-time bound-state probabilities. This construction permits the formal definition of individual-state probabilities, which satisfy a generalized adiabatic theorem, and leads to the satisfying result that the total bound-state probability at all intermediate times is the sum of complex-mode probabilities. In marked contrast to the conventional norm-of-state definition of nonionization probability, this sum does not have oscillations at intermediate times, in the limit of adiabatic modulation of the interaction. Superposition-state probabilities, however, exhibit oscillations at intermediate times. The resulting non-Hermitian quantum dynamics is especially suited, and even essential, for an accurate description of near-resonance ionization. Precise matching of the time-dependent $\stackrel{^}{H}(t)$ and ${\stackrel{^}{H}}^{\ifmmode\dagger\else\textdagger\fi{}}(t)$ with bases of their instantaneous eigenstates is required by approximate unitarity in the discrete decaying space, for a consistent theory. We illustrate these considerations in a general way in the context of resolvent-operator techniques. The implementation of the theory in both its time-dependent and stationary-state formulations is presented in an Appendix, for the completely general two-state non-Hermitian Hamiltonian. The results of these formulations are found to agree, in the adiabatic limit, to all orders in the non-Hermitian interaction. The utility of direct diagonalization of the effective $\stackrel{^}{H}(t)$, advocated by Armstrong and Baker, is transparent. The overall context of interpretation of their earlier work is, however, significantly altered. Similar considerations apply for nonswitchable interactions, such as for
K-meson decays. These results represent a practical generalization of quantum mechanics to non-Hermitian systems. The utility, and the necessity, of such a generalization has considerable theoretical interest, and direct experimental implications.
A general perturbation procedure is described for writing down the contributions to any order for the probability of a quantum system described by a time-independent Hamiltonian making a transition from an arbitrary initial state to an arbitrary final state. The results are expressed in terms of certain propagators which involve continued fractions, so that some processes are summed to all orders. The general theory is then applied to a single multilevel atom interacting with any number of modes of the electromagnetic field in the electric dipole approximation. The fundamental theory is considered primarily but a detailed discussion is given of spontaneous and stimulated emission. Expressions for the lineshape are derived incorporating the generalized Lamb shifts and damping constants.
Within the framework of time-dependent perturbation theory, general expressions are derived for the cross section of multiphoton processes induced by radiation acting on a hydrogen atom. Bound-bound transitions involving emission of a single quantum and bound-free transitions are calculated for a wide range of photon energies. In the case of resonance, the transition probability is also discussed. The procedure used to evaluate the sums over intermediate states is described. The numerical computation allows one to compare the results obtained for various competing processes.
The quantum nonperturbative analysis of Kroll and Watson for a two-level system of near-adiabatic atom-atom scattering in an intense laser-field mode is extended to treat a general multilevel system interacting with intense single- or many-field modes. A procedure for rigorously solving the adiabatic eigenvalue problem for the whole charge-field system is given. A new transition-probability formula is derived. Cross sections are calculated for the processes $\mathrm{Li}+\mathrm{H}(X^{1}\ensuremath{\Sigma}^{+})+\ensuremath{\nu}\ensuremath{\hbar}\ensuremath{\omega}\ensuremath{\rightarrow}\mathrm{Li}+\mathrm{H}(A^{1}\ensuremath{\Sigma}^{+} or B^{1}\ensuremath{\Pi})$ where $\ensuremath{\nu}\ensuremath{\ge}1$. Analysis of transition in an atom due to intensity variation of a laser pulse shows that desired transition probability per pulse (e.g., \textonehalf{}) may be achieved by varying the pulse parameters. For this, numerical results of $\mathrm{Na}(3s)+2\ensuremath{\hbar}\ensuremath{\omega}\ensuremath{\rightarrow}\mathrm{Na}(5s)$ and of $\mathrm{Li}(2s)+8\ensuremath{\hbar}\ensuremath{\omega}\ensuremath{\rightarrow}\mathrm{Li}(3s)$ are given.