Non-Linear Interactions in Pump-Probe Optical Phenomena for Moving Atomic Systems

V. L. Jacobs

V. L. Jacobs

V. L. Jacobs

Claude N. Cohen-Tannoudji

V. L. Jacobs

Linear and non-linear interactions in electromagnetically induced transparency and related pump-probe optical phenomena involving moving many-electron atomic systems are investigated using a reduced-density-matrix approach. Time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations are developed in a unified manner. The standard Born (lowest-order perturbation-theory) and Markov (short-memory-time) approximations are systematically introduced within the framework of the general non-perturbative and non-Markovian formulations. A preliminary semiclassical perturbation-theory treatment of the electromagnetic interaction is adopted. However, it is emphasized that a quantized-electromagnetic-field approach is essential for a self-consistent quantum-mechanical formulation. Our primary result is the derivation of compact Liouville-space operator expressions for the linear and the general (n'th order) non-linear macroscopic electromagnetic-response tensors. These expressions can be evaluated for coherent initial atomic excitations and for the full tetradic-matrix form of the Liouville-space self-energy operator representing the environmental interactions in the Markov approximation. Collisional interactions between atoms can be treated in various approximations for the self-energy operator, and the influence of Zeeman coherences on the electromagnetic-pulse propagation can be investigated by including an applied magnetic field on an equal footing with the electromagnetic fields.

V. L. Jacobs

Reduced density matrix descriptions are developed for linear and non-linear electromagnetic interactions of moving atomic systems, taking into account applied magnetic fields as well as atomic collisions together with other environmental decoherence and relaxation processes. Applications of interest include electromagnetically induced transparency and related pump-probe optical phenomena in warm atomic vapors. Time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations are developed in a unified manner. The standard Born (lowestorder perturbation-theory) and Markov (short-memory-time) approximations are systematically introduced within the framework of the general non-perturbative and non-Markovian formulations. A preliminary semiclassical treatment of the electromagnetic interaction is adopted. However, the need for a fully quantum mechanical approach is emphasized. Compact Liouville-space operator expressions are derived for the linear and the general (n'th order) non-linear macroscopic electromagnetic-response tensors occurring in a perturbation-theory treatment of the semiclassical electromagnetic interaction. These expressions can be evaluated for coherent initial atomic excitations and for the full tetradic-matrix form of the Liouville-space self-energy operator representing the environmental interactions in the Markov approximation. Collisional interactions between atoms can be treated in various approximations for the selfenergy operator, and the influence of Zeeman coherences on the macroscopic electromagnetic response can be investigated.