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arXiv:physics/0305131 · Journal of Optics B Quantum and Semiclassical Optics

A sum rule for nonlinear optical susceptibilities

Luciana C Dávila Romero, Davıd L. Andrews

Published Nov 3, 2003• 5 citations
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Abstract

It is explicitly shown, for optical processes arbitrarily comprising two-, three- or four-photon interactions, that the sum over all matter states of any optical susceptibility is exactly zero. The result remains true even in frequency regions where damping is prominent. Using a quantum electrodynamical framework to render the photonic nature of the fundamental interactions, the result emerges in the form of a traceless operator in Hilbert space. The generality of the sum rule and its significance as a thermodynamic limit are discussed, and the applicability to real systems is assessed.

DOI
10.1088/1464-4266/6/1/010

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It is explicitly shown, for optical processes arbitrarily comprising two-, three- or four-photon interactions, that the sum over all matter states of any optical susceptibility is exactly zero. The result remains true even in frequency regions where damping is prominent. Using a quantum electrodynamical framework to render the photonic nature of the fundamental interactions, the result emerges in the form of a traceless operator in Hilbert space. The generality of the sum rule and its significance as a thermodynamic limit are discussed, and the applicability to real systems is assessed.
We have formulated expressions providing the number of terms (Y-G diagrams)1contributing to an n-th order susceptibility of a non-linear optical process. Obtaining an accurate count of these terms is important for diverse reasons: a) To accurately specify the number of terms needed to evaluate the nonlinear optical susceptibility either analytically or numerically, b) To help develop sequences of diagrammatic contributions which can be summed to provide analytical results for the strong interaction limit. An example is the two-level system for semiclassical and quantized fields, c) To treat two or more processes (terms) which could give rise to interference, resulting, for example, in extra resonances due to a lack of complete coherence, d) To generalize results from quantum electrodynamics to situations for which multiple photon interactions and zero point fluctuations associated with non-vacuum states need to be considered. We shall discuss the number of possible diagrams in terms of three factors, which we call a permutation factor relating to the number of possible frequencies that can be assigned to each interaction vertex, a commutation factor relating to interaction vertex assignment on the two sides of the diagram, and a state factor relating to the number of diagrams generated from an enumeration of specific material state assignments between interaction vertices. We will discuss the application of these results to several situations of interest including second harmonic generation, degenerate four-wave mixing, and resonant CARS (coherent anti-Stokes Raman scattering) in a four-level system. The relevance of the present results to experimental results which have been obtained will be discussed along with future directions which need to be addressed including the summability of diagrams under specific approximations, the calculation of expectation values, and the nonperturbative representation of processes.
Abstract The Thomas–Reiche–Kuhn (TRK) sum rule is a fundamental consequence of the position–momentum commutation relation for an atomic electron, and it provides an important constraint on the transition matrix elements for an atom. Here, we propose a TRK sum rule for electromagnetic fields which is valid even in the presence of very strong light–matter interactions and/or optical nonlinearities. While the standard TRK sum rule involves dipole matrix moments calculated between atomic energy levels (in the absence of interaction with the field), the sum rule here proposed involves expectation values of field operators calculated between general eigenstates of the interacting light–matter system. This sum rule provides constraints and guidance for the analysis of strongly interacting light–matter systems and can be used to test the validity of approximate effective Hamiltonians often used in quantum optics.
The nonlinear oscillator model is useful to basically understand the most important properties of nonlinear optical processes. It has been shown to give the correct asymptotic behaviour and to provide the general feature of harmonic generation to all orders, in particular dispersion relations and sum rules. We investigate the properties of Pump and Probe processes using this model, and study those cases where general theorems based on the holomorphic character of the Kubo response function cannot be applied. We show that it is possible to derive new sum rules and new Kramers-Kronig relations for the two lowest moments of the real and imaginary part of the third order susceptibility and that new specific contributions become relevant as the intensity of the probe increases. Since the analitic properties of the susceptibility functions depend only upon the time causality of the system we are confident that these results are not model depemdent and therefore have a general validity, provided one substitutes to the equilibrium values of the potential derivatives the density matrix expectation values of the corresponding operators.
The linear and nonlinear dynamical susceptibilities of a two-level system are calculated as it undergoes a transition to a decoherent state. Analogously to the Glover-Tinkham-Ferrell sum rule of superconductivity, spectral weight in the linear susceptibility is continuously transferred from a finite frequency resonance to nearly zero frequency, corresponding to a broken symmetry in the thermodynamic limit. In this respect, the behavior of the present model (the Mermin model) differs from the spin-boson model. The third order nonlinear susceptibility, corresponding to two-photon absorption, has an unexpected nonmonotonic behavior as a function of the environmental coupling, reaching a maximum within the decoherent phase of the model. Both linear and nonlinear susceptibilities may be expressed in a universal form.
The topic of this thesis is a theoretical study of nonequilibrium transitions and quantum statistical properties of nonlinear quantum optical systems driven by an external radiation source. In certain limiting cases, a comparison is made between these transitions and the phase transitions found in equilibrium physical systems. In chapters one and two, the mathematical tools are introduced. In operator terms, the time development is described by a Markovian master equation in the interaction picture. This is equivalent to a corresponding time development equation or Fokker-Planck equation in a vector space of c-numbers. In order to deal with the type of Fokker-Planck equation that results, we introduce a quantum classical correspondence resulting in a distribution function over a complex phase-space, which is a generalisation of the Glauber-Sudarshan P-function. In chapter three this is applied to a model of a coherently driven mode with nonlinear dispersion and absorption. We find in the limit of zero temperature, that the spectrum is symmetric relative to the input frequency, and an exact solution is obtained for the distribution function. For a detuned driving field and nonlinear dispersion, optical bistability can occur. In chapter four a model of sub/second harmonic generation is introduced. This has several non-equilibrium transitions, including dispersive optical bistability, and bistable behaviour with coherent phase-locked input to both modes. Exact solutions occur in the limit of zero temperature and adiabatic elimination of one mode. In both chapters three and four, steady-state photon anti-bunching occurs with an absorptive nonlinearity. In chapter five we include interactions between the radiation mode and a fluorescent atomic system. In this case different behaviour occurs depending on the relative decay rates of the individual atoms and of the radiation mode. In the case of a high-Q interferometer, the atomic variables can be adiabatically eliminated. Both dispersive and absorptive bistability can occur. We show by analytic and numerical calculations (in the case of inhomogeneous broadening) that dispersive operation has advantages in requiring a lower atomic density and input field to observe bistability. When the input field has Gaussian (rather than coherent) photon statistics, there is no bistability, but enhanced photon bunching occurs. Finally, there is a different type of behaviour when the field mode decays rapidly and can be adiabatically eliminated. Within the cooperation lifetime the system can be described by a J²-invariant Hamiltonian, giving the special case of only collective damping. The result is a new type of critical point transition in the thermodynamic limit, with the appearance of a family of solutions like Lotka-Volterra cycles for a coherent driving field above threshold.