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Journal of Physics B Atomic Molecular and Optical Physics

Time-dependent S-matrix theory of multiphoton ionization: crucial role of the adiabatic hypothesis

K. Unnikrishnan

Published Sep 28, 1990• 6 citations
Publisher

Abstract

It is rigorously proved that, if adiabatic switching off of the interaction is properly implemented, as demanded by formal time-dependent S-matrix theory, even the Keldysh-type theories of multiphoton ionization require energy conservation without allowing for the ponderomotive energy, which only contributes an unobservable phase. The importance of ponderomotive effects in above-threshold ionization therefore needs to be re-examined.

DOI
10.1088/0953-4075/23/18/005

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It is rigorously proved that, if adiabatic switching off of the interaction is properly implemented, as demanded by formal time-dependent S-matrix theory, even the Keldysh-type theories of multiphoton ionization require energy conservation without allowing for the ponderomotive energy, which only contributes an unobservable phase. The importance of ponderomotive effects in above-threshold ionization therefore needs to be re-examined.
The Keldysh-Faisal-Reiss theory of nonresonant multiphoton ionization seems to give reasonably good agreement with experiments for production rates in the above-threshold-ionization peaks. The theory has some conceptual difficulties, since physically equivalent Hamiltonians give radically different results when treated by this method. An alternate form of the S matrix is used here in which approximation must be made upon the exact wave function evolving from the initial state rather than the time-reversed form used in the Keldysh-Reiss treatment. The exact initial state is approximated by an adiabatic form which results in an S matrix that eliminates the conceptual difficulties described above.
A general framework for description of quantum systems in strong external fields is established. The most important application of the theory is concerned with the multiphoton ionization of atoms and molecules. The adiabatic approximation is developed. The Hamiltonian of the system is diagonalized by a time-dependent unitary transformation, which generates an interaction energy vanishing for very slow fields. A general analysis of the photoionization rates is performed. A specific model is considered: one-dimensional motion in the δ-function potential and external harmonic electric field. This model allows the exact solution for time-dependent eigenvalues and eigenfunctions. These solutions are compared with the conventional free electron approach to the ionization states.
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.
Formal time-independent scattering theory is applied to multiphoton ionization of atoms in intense electromagnetic fields. The quantized-field version of the Volkov solution makes this approach possible. With the electron-photon interaction in a monochromatic photon field, it is found that, in the nonrelativistic and large-photon-number limits, the final scattering state exists only in the special case in which the ponderomotive potential per unit photon energy is an integer; otherwise the final state vanishes. In the integer case the corresponding wave function reduces to a single Volkov function, multiplied by an overlap factor. A simple interpretation of this result is given, and some other consequences of this work are discussed.
The Keldysh approximation to treat the multiphoton ionization of atoms is reconsidered. It is shown that, if one consistently uses the hypothesis under which the approximation should be valid (essentially, that of a weak, short-range binding potential), a Keldysh-like term results as an approximation to the first term of a uniformly convergent series in powers of the binding potential. No cancellation occurs when higher-order terms are taken into account. This result allows one to consider the Keldysh approximation as a well-defined theoretical model, without implying, however, that it is adequate to describe multiphoton ionization of real atoms.