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Physical Review A

Non-Hermitian quantum theory of multiphoton ionization

Howard C. Baker

Published Aug 1, 1984• 61 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.30.773

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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 SSS-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 SSS-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 KKK-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 rigorous and practical time-dependent formulation of quantum decay processes is obtained by converting the Hermitian Schrodinger problem into an equivalent non-Hermitian Schrodinger equation. The properties of the original Hermitian and the reduced non-Hermitian Hamiltonians are compared and the non-Hermitian formulation is shown to be consistent with the theorem of Fock and Krylov for the description of truly decaying states. A self-consistent non-unitary algorithm is developed and used to obtain expressions for the time-dependent transition amplitudes of interest; they automatically preserve the total probability in the sum space at all future times tau >0. The formalism is coded for application to the important problem of ionisation decay of a ground-state hydrogen atom coupled to a strong radiation field with a sub-threshold photon frequency. The first quantitative information on the time dependence of two- and three-photon (resonant and non-resonant) ionisation of the hydrogen atom is obtained.
In the final state of a multiphoton-ionization process the ejected electron may interact simultaneously with the external laser field and with the residual atomic system. A procedure for calculating transition probabilities for such processes is described which incorporates the effects of resonances in the final continuum states of the atom. By using standard methods of scattering theory, it is shown how these resonant states may be separated out leaving a "background" amplitude which is a smooth function of the energy, and which therefore lends itself more readily to numerical evaluation. Such an evaluation may be based on the generalized Lippmann-Schwinger integral equation presented here. The constraint imposed by unitarity on the background amplitude is derived, and it is pointed out how approximations may be set up which satisfy unitarity automatically. A simplified model is described in order to illustrate this and other features of the theory and to make contact with some earlier work on this subject. Finally, a low-frequency approximation is developed in which final-state interaction effects are accounted for in a relatively simple analytical form.
Continuous monitoring can convert a dissipative channel into a resource for accelerating otherwise slow multiphoton transitions. We consider a three-level atom in a ΛΛΛ configuration and condition the evolution on the absence of photon emission through an auxiliary monitored decay channel. The resulting no-jump dynamics is governed by a non-Hermitian Rabi-type Hamiltonian. Using Floquet theory and Brillouin--Wigner projection-operator perturbation method, we derive effective two-state descriptions of odd-multiphoton resonances in the semiclassical and quantum Rabi models. The effective population-transfer rate, defined as the inverse of the time required for the first complete transfer between the atomic states, is maximized at an exceptional point, where its enhancement factor approaches π/2π/2π/2, corresponding to an approximately 57%57\%57% increase over the Hermitian value. Numerical results for three- and five-photon resonances closely reproduce the analytical transition times and yield non-negligible postselection probabilities. By contrast, the complete unconditioned dissipative evolution does not exhibit the same population-transfer enhancement. These results demonstrate a speed--success trade-off for measurement-conditioned multiphoton state transfer.
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.
We establish a quantitative adiabatic estimate for a class of finite-dimensional non-Hermitian Schrödinger dynamics. The original non-Hermitian Hamiltonian is assumed to be diagonalizable with real spectrum and non-crossing eigenvalues. We then construct a dynamically compatible time-dependent metric operator, and its positive square root defines a Dyson map. The associated Dyson-transformed Hamiltonian is Hermitian. When this Dyson-transformed Hamiltonian satisfies the Hermitian adiabatic assumption, the standard resolvent-projection method gives an explicit adiabatic estimate in the Hermitian representation. Pulling this estimate back through the Dyson map gives an approximation in the original non-Hermitian representation. The resulting Dyson-pulled-back projections are then compared with the spectral projections of the original non-Hermitian Hamiltonian by using a contour-resolvent estimate. The final bound contains two contributions: the pulled-back Hermitian adiabatic error and the projection-comparison error. A two-level non-Hermitian model is presented to illustrate the hypotheses of the theorem and the two contributions appearing in the final estimate.
Detailed descriptions of one- and two-photon ionization are presented. We go beyond conventional perturbation theory to investigate the dynamics of both processes for a broad range of field intensities. The general theory of unstable decaying states is applied to the problem of one-photon ionization (the photoeffect). It is found that a non-trivial dependence of the transition dipole moment on the continuum state energy can lead to corrections to exponential decay, and even oscillations in the bound state population. As examples we consider the photoionization of hydrogen and atoms with autoionizing states. Only in the absence of autoionizing states corrections to exponential decay remain inconsequential for any experimentally relevant intensity. Our description of two-photon ionization is formulated in the Heisenberg picture. Besides the usual two-level atom projection operators we introduce explicitly the operators referring to the atomic continuum. By eliminating from the equations of motion the terms related to the electromagnetic self field as well as the terms referring to the continuum, transverse and longitudinal damping corresponding to spontaneous emission and photoionization is obtained. The use of field correlation functions allows us to account for the partial coherence of the applied field. We develop a technique to extract from the equations of motion a unique two-photon ionization rate. Such a characterization of the ionization process is not only instructive because of its simplicity, it is also in many cases completely satisfactory. The resulting general expression for the two-photon ionization rate is the central result of our treatment. From it we recover several familiar results in different limiting cases. In addition, our general rate expression provides the first description of the complete hierarchy of saturation effects that one should expect. We present a number of examples where we calculate the two-photon ionization rate as a function of the detuning, and where we emphasize the saturation and field correlation effects.