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Journal of the Optical Society of America B

Diagrammatic many-body theory for atoms in high-intensity laser fields Part I

Lars Jönsson, Goran P. Wendin

Published May 1, 1992• 7 citations
Publisher

Abstract

Diagrammatic many-body theory has been used extensively in the treatment of electron–electron correlations in atomic photoionization at low intensities. We discuss how it can be used at high intensities also. The standard diagrammatic formalism is derived for time-independent interactions by using adiabatic switching. This formalism can be formally derived for harmonic fields also but leads to unphysical results for strong fields. If the amplitude function of the laser field is an exponential function, however, the standard derivation still applies. If the adiabatic limit is not taken, this time-dependent formalism can be used for any intensity. In practice one is still limited to slow turn-on, but, assuming slow turn-on, we show that for a discrete system the linked expansion, when summed to infinite order, gives the Floquet state that is adiabatically connected to the ground state. When continua are included, we find that qualitatively correct results are obtained only if one uses an expansion of the time derivative of the wave function instead of an expansion of the wave function itself. We also show that the imaginary part of the self-energies must be excluded from the energy denominators, since they otherwise lead to unphysical results. These results are found by treating model systems for which the exact solutions are known and for which the diagrams can be evaluated to any order.

DOI
10.1364/josab.9.000627

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Introduction

Isaiah Shavitt, Rodney J. Bartlett

Scope The book focuses primarily on many-body (or better, many-electron) methods for electron correlation. These include Rayleigh–Schrödinger perturbation theory (RSPT) , particularly in its diagrammatic representation (referred to as many-body perturbation theory , or MBPT ), and coupled-cluster (CC) theory; their relationship to configuration interaction (CI) is included. Further extensions address properties other than the energy, and also excited states and multireference CC and MBPT methods. The many-body algebraic and diagrammatic methods used in electronic structure theory have their origin in quantum field theory and in the study of nuclear matter and nuclear structure. The second-quantization formalism was first introduced in a treatment of quantized fields by Dirac (1927) and was extended to fermion systems by Jordan and Klein (1927) and by Jordan and Wigner (1928). This formalism is particularly useful in field theory, in scattering problems and in the study of infinite systems because it easily handles problems involving infinite, indefinite or variable numbers of particles. The diagrammatic approach was introduced into field theory by Feynman (1949a,b) and applied to many-body systems by Hugenholtz (1957) and by Goldstone (1957). Many-body perturbation theory and its linked-diagram formalism were first introduced by Brueckner and Levinson (1955) and by Brueckner (1955), and were formalized by Goldstone (1957). Other important contributions to the methodology, first in field theory and then in the theory of nuclear structure, are due to Dyson (1949a,b), Wick (1950), Hubbard (1957, 1958a,b) and Frantz and Mills (1960). Applications to the electronic structure of atoms and molecules began with the work of Kelly (1963, 1964a,b, 1968), and molecular applications using finite analytical basis sets appeared in the work of Bartlett and Silver (1974a, b).

Cambridge University Press eBooks•Aug 6, 2009•26 citations
Diagrammatic many-body theory has been used extensively in the treatment of electron–electron correlations in atomic photoionization at low intensities. We discuss how it can be used at high intensities also. The standard diagrammatic formalism is derived for time-independent interactions by using adiabatic switching. This formalism can be formally derived for harmonic fields also but leads to unphysical results for strong fields. If the amplitude function of the laser field is an exponential function, however, the standard derivation still applies. If the adiabatic limit is not taken, this time-dependent formalism can be used for any intensity. In practice one is still limited to slow turn-on, but, assuming slow turn-on, we show that for a discrete system the linked expansion, when summed to infinite order, gives the Floquet state that is adiabatically connected to the ground state. When continua are included, we find that qualitatively correct results are obtained only if one uses an expansion of the time derivative of the wave function instead of an expansion of the wave function itself. We also show that the imaginary part of the self-energies must be excluded from the energy denominators, since they otherwise lead to unphysical results. These results are found by treating model systems for which the exact solutions are known and for which the diagrams can be evaluated to any order.
Starting from first principles, I derive a time-dependent diagrammatic many-body formalism that can be used for strong harmonic fields. My aim has been to treat many-electron effects in an atom interacting with an intense laser field. The formalism derived describes the atom in terms of a damped many-body Floquet state. The diagrammatic expansion is similar to the ordinary time-independent atomic many-body theory, but some important changes have been made: The energy denominators contain time-dependent self-energies and the exact ground-state shift; the intermediate levels are dressed atomic states, for which each harmonic of a given atomic state is counted as a separate level; and the ground-state energy shift is given by a time-dependent Brillouin–Wigner-type energy equation, which in general must be solved numerically. The formalism is not linked but contains no divergences in the adiabatic limit of the electron–electron interaction. For weak fields the formalism reduces to the ordinary linked expansion. For a two-level system all diagrams can be summed, and the result is equivalent to the usual continued-fraction solution. I also derive the exact diagrammatic solution for a single level interacting with a continuum.
The diagrammatic solution to a (sequentially coupled) one-electron three-level system in an intense laser field is derived. The solution is in the form of a continued-fraction expansion and is equal to the Floquet state that is adiabatically connected to the ground state. The formalism used is a recently presented diagrammatic many-body theory by Jonsson that can be used for non-perturbative calculations in strong fields. The purpose of the calculation is to demonstrate how a non-trivial one-electron problem can be solved exactly within the formalism.
In order to properly describe the dynamics of a many-particle system in strong, time-dependent fields, a nonperturbative treatment of all constituents and of their correlation is needed. An ab initio solution of the time-dependent many-body Schrödinger equation is only feasible for simple systems. Hence, for many-electron systems in intense laser fields practicable methods for solving the quantum-mechanical many-body problem are required. An formally exact approach is the time-dependent density functional theory. In this work a mathematically rigorous formulation of the foundations of this theory is given. Further the non-locality in time of the exchange-correlation functionals is examined, and we formally define the notion of "quantum memory". We investigate the fundamental process of Rabi oscillations from a density-functional point of view and find the few-level approximation to be in conflict with the basis of time-dependent density functional theory. Finally, we apply the theory to calculate the electron dynamics of C60 in intense laser pulses. Although the laser light is far off-resonant with respect to the collective modes of the C60 the multi-electron dynamics strongly influences the harmonic spectra. The efficiency of this multi-particle recollision process with respect to the usual single active electron approximation of high-order harmonic generation is estimated by two analytical models.
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 multiple-linear-time-scale method is used to construct a perturbation theory for NNN-level quantum systems subjected to time-dependent perturbations. The secular and small-denominator terms which plague conventional time-dependent perturbation theory are avoided; consequently, the theory is useful for treating long-term behavior and resonant interactions. The introduction of a self-energy operator allows the shifts in energy levels to be displayed explicitly. When the perturbation is the dipole interaction with an electromagnetic field, the successive approximations yield the well-known rotating-wave approximation, corrections due to counter rotating terms, and the Bloch-Siegert frequency shift. The formalism is applicable to arbitrary pulse shapes, provided that $\ensuremath{\parallel}{H}_{1}\ensuremath{\parallel}\ensuremath{\ll}\ensuremath{\hbar}\overline{\ensuremath{\omega}}$, where $\ensuremath{\parallel}{H}_{1}\ensuremath{\parallel}$ represents the inter-action strength and $\overline{\ensuremath{\omega}}$ is a characteristic frequency of the field. Rabi oscillations induced by multiphoton resonances are automatically included, and this effect is demonstrated in the case of a square pulse with frequency approximately one half the resonance frequency for a transition between two vibrational levels of a molecule. These calculations are compared to an exact numerical solution in order to find the limits of validity of the approximation. Even at high intensities ($I\ensuremath{\sim}{10}^{14}$ W/cm2{\mathrm{cm}}^{2}cm2) the shifted resonance frequency is quite accurate; however, the approximate and exact solutions are slightly out of phase, so that the approximate solution can only be trusted for a few Rabi cycles. For much lower intensities ($I\ensuremath{\sim}{10}^{10}$ W/cm2{\mathrm{cm}}^{2}cm2), the approximate solution is valid for many thousands of Rabi cycles.
Scope The book focuses primarily on many-body (or better, many-electron) methods for electron correlation. These include Rayleigh–Schrödinger perturbation theory (RSPT) , particularly in its diagrammatic representation (referred to as many-body perturbation theory , or MBPT ), and coupled-cluster (CC) theory; their relationship to configuration interaction (CI) is included. Further extensions address properties other than the energy, and also excited states and multireference CC and MBPT methods. The many-body algebraic and diagrammatic methods used in electronic structure theory have their origin in quantum field theory and in the study of nuclear matter and nuclear structure. The second-quantization formalism was first introduced in a treatment of quantized fields by Dirac (1927) and was extended to fermion systems by Jordan and Klein (1927) and by Jordan and Wigner (1928). This formalism is particularly useful in field theory, in scattering problems and in the study of infinite systems because it easily handles problems involving infinite, indefinite or variable numbers of particles. The diagrammatic approach was introduced into field theory by Feynman (1949a,b) and applied to many-body systems by Hugenholtz (1957) and by Goldstone (1957). Many-body perturbation theory and its linked-diagram formalism were first introduced by Brueckner and Levinson (1955) and by Brueckner (1955), and were formalized by Goldstone (1957). Other important contributions to the methodology, first in field theory and then in the theory of nuclear structure, are due to Dyson (1949a,b), Wick (1950), Hubbard (1957, 1958a,b) and Frantz and Mills (1960). Applications to the electronic structure of atoms and molecules began with the work of Kelly (1963, 1964a,b, 1968), and molecular applications using finite analytical basis sets appeared in the work of Bartlett and Silver (1974a, b).