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Novel approach to nonlinear susceptibility

Odile Betbeder-Matibet, Kikuo Cho, Hiroshi Ajiki

Published Nov 17, 2003• 0 citations
OpenAlex

Abstract

The calculation of the third order susceptibility still is a long standing fundamental problem of particular importance in nonlinear nanooptics: Indeed, cancellation of size-dependent terms coming from uncorrelated excitations is expected, but up to now shown for very simple Hamiltonians only. Using a many-body theory recently developed to handle interacting close-to-bosons, we prove it here for \emph{arbitrary} H. This new formalism actually provides the first clean way to calculate nonlinear susceptibilities, with results different from previous ones.

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Novel approach to nonlinear susceptibility

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Jun 1, 1991•0 citations
The calculation of the third order susceptibility still is a long standing fundamental problem of particular importance in nonlinear nanooptics: Indeed, cancellation of size-dependent terms coming from uncorrelated excitations is expected, but up to now shown for very simple Hamiltonians only. Using a many-body theory recently developed to handle interacting close-to-bosons, we prove it here for \emph{arbitrary} H. This new formalism actually provides the first clean way to calculate nonlinear susceptibilities, with results different from previous ones.
The calculation of the third order susceptibility still is a long standing fundamental problem of particular importance in nonlinear nanooptics: Indeed, cancellation of size-dependent terms coming from uncorrelated excitations is expected, but up to now shown for very simple Hamiltonians only. Using a many-body theory recently developed to handle interacting close-to-bosons, we prove it here for \emph{arbitrary} H. This new formalism actually provides the first clean way to calculate nonlinear susceptibilities, with results different from previous ones.
We here propose a new procedure to derive a general expression of the third-order susceptibility valid for any semiconductor Hamiltonian. It relies on our theory for composite exciton many-body effects which is quite appropriate to this problem since all optical nonlinearities in semiconductors come from exchange scatterings with the virtual excitons coupled to photons. Our expression of χ (3) is sample volume free, as physically expected. It also contains a Pauli term (exchange without Coulomb) which is missed by all bosonized exciton approaches. This term, dominant at large detuning, is a direct manifestation of the exciton composite nature.
A new propagator approach for the calculation of nonlinear susceptibilities is proposed. In this approach a higher order susceptibility is generated by the functional derivative of a lower order susceptibility. The procedure is illustrated through a calculation of the third-order susceptibility. A diagram technique is employed to select and calculate the important contributions. The results are applied to the resonance fluorescence from a two-level atom in a gas. The existing results of the impact theory are generalized by taking proper account of the lower state interaction and by calculating the higher order collision corrections.
We revisit the approach proposed by Mukamel and coworkers to describe interacting excitons through infinite series of composite-boson operators for both, the system Hamiltonian and the exciton commutator -- which, in this approach, is properly kept different from its elementary boson value. Instead of free electron-hole operators, as used by Mukamel's group, we here work with composite-exciton operators which are physically relevant operators for excited semiconductors. This allows us to get \emph{all} terms of these infinite series explicitly, the first terms of each series agreeing with the ones obtained by Mukamel's group when written with electron-hole pairs. All these terms nicely read in terms of Pauli and interaction scatterings of the composite-exciton many-body theory we have recently proposed. However, even if knowledge of these infinite series now allows to tackle NNN-body problems, not just 2-body problems like third order nonlinear susceptibility χ(3)χ^{(3)}χ(3), the necessary handling of these two infinite series makes this approach far more complicated than the one we have developed and which barely relies on just four commutators.
We revisit the approach proposed by Mukamel and co-workers to describe interacting excitons through infinite series of composite-boson operators for both the system Hamiltonian and the exciton commutator---which, in this approach, is properly kept different from its elementary-boson value. Instead of free-electron-hole operators, as used by Mukamel's group, we here work with composite-exciton operators which are physically relevant operators for excited semiconductors. This allows us to get all terms of these infinite series explicitly, the first terms of each series agreeing with the ones obtained by Mukamel's group when written with electron-hole pairs. All these terms nicely read in terms of Pauli and interaction scatterings of the composite-exciton many-body theory we have recently proposed. However, even if knowledge of these infinite series now allows us to tackle NNN-body problems, not just two-body problems like third-order nonlinear susceptibility ${\ensuremath{\chi}}^{(3)}$, the necessary handling of these two infinite series makes this approach far more complicated than the one we have developed and which barely relies on just four commutators.