Strong electronic correlation effects in coherent multidimensional nonlinear optical spectroscopy.

We discuss a many-body theory of the coherent ultrafast nonlinear optical response of systems with a strongly correlated electronic ground state that responds unadiabatically to photoexcitation. We introduce a truncation of quantum kinetic density matrix equations of motion that does not rely on an expansion in terms of the interactions and thus applies to strongly correlated systems. For this we expand in terms of the optical field, separate out contributions to the time-evolved many-body state due to correlated and uncorrelated multiple optical transitions, and use "Hubbard operator" density matrices to describe the exact dynamics of the individual contributions within a subspace of strongly coupled states, including "pure dephasing". Our purpose is to develop a quantum mechanical tool capable of exploring how, by coherently photoexciting selected modes, one can trigger nonlinear dynamics of strongly coupled degrees of freedom. Such dynamics could lead to photoinduced phase transitions. We apply our theory to the nonlinear response of a two-dimensional electron gas (2DEG) in a magnetic field. We coherently photoexcite the two lowest Landau level (LL) excitations using three time-delayed optical pulses. We identify some striking temporal and spectral features due to dynamical coupling of the two LLs facilitated by inter-Landau-level magnetoplasmon and magnetoroton excitations and compare to three-pulse four-wave-mixing (FWM) experiments. We show that these features depend sensitively on the dynamics of four-particle correlations between an electron-hole pair and a magnetoplasmon/magnetoroton, reminiscent of exciton-exciton correlations in undoped semiconductors. Our results shed light into unexplored coherent dynamics and relaxation of the quantum Hall system (QHS) and can provide new insight into non-equilibrium co-operative phenomena in strongly correlated systems.

Dynamics of inter-landau-level excitations of a two-dimensional electron gas in the quantum Hall regime.

The femtosecond inter-Landau-level dynamics of a two-dimensional electron gas in a large magnetic field is investigated by degenerate four-wave mixing on modulation doped quantum wells. We observe a large transfer of oscillator strength to the lowest Landau level, and unusual dynamics due to Coulomb correlation. We interpret the effects using a model based on shakeup of the electron gas.

From coherently excited highly correlated states to incoherent relaxation processes in semiconductors.

Recent theories of highly excited semiconductors are based on two formalisms, referring to complementary experimental conditions, the real-time nonequilibrium Green's function techniques and the coherently controlled truncation of the many-particle problem. We present a novel many-particle theory containing both of these methods as limiting cases. As a first example of its application, we investigate four-particle correlations in a strong magnetic field including dephasing resulting from the growth of incoherent one-particle distribution functions. Our results are the first rigorous solution concerning formation and decay of four-particle correlations in semiconductors. They are in excellent agreement with experimental data.

Polariton-biexciton transitions in a semiconductor microcavity.

The influence of four-particle correlations on the nonlinear optics of a semiconductor microcavity is determined by a pump-and-probe investigation. Experiments are performed on a nonmonolithic microcavity which contains a ZnSe quantum well. In this system the biexciton binding energy exceeds both the normal-mode splitting between exciton and cavity mode and all damping constants. Oscillatory spectral features below the excitonic resonance are observed in the response for counterpolarized beams. Comparison with model calculations shows that in this case the coherent nonlinearity is dominated by biexciton-exciton interactions beyond the Hartree-Fock approximation.