Femtosecond-pulse propagation in resonantly excited semiconductors is investigated by numerically solving the semiconductor Maxwell-Bloch equations for plane waves. For excitation at the exciton resonance, it is shown that the pulse absorption exhibits a strongly nonlinear dependence on the input pulse area. Very long propagation distances for strong pulses are observed, but even when all dephasing processes have been neglected, no lossless propagation (self-induced transparency) was found. The influence of the electron-hole many-body effects, nonequilibrium carrier relaxation, and optical dephasing on the pulse-propagation dynamics is studied. The exchange interaction in the electron-hole plasma is shown to support large propagation distances. For excitation of the continuum states, the dependence of the absorption on the intensity of the input pulse is reduced due to the rapid carrier relaxation into quasiequilibrium distributions.
The dynamics of electrons and holes in semiconductors and semiconductor heterostructures have been extensively discussed in the literature, and are governed by their mutual Coulomb interaction, by their interaction with lattice vibrations (phonons) and by their radiative recombination (for an overview see e.g. Ref. [1]). A powerful technique to study the carrier dynamics in semiconductors utilizes short optical pulses to photoexcite electrons from the valence to the conduction band (i.e. to create electron-hole pairs) that subsequently relax until the photon energy stored in the medium is dissipated and the system has recovered the thermal equilibrium. The dynamics of the carriers photoexcited by the short optical pulse can be followed by monitoring two main optical observables: the interband population difference and the induced polarization. Both quantities decay with time after the photoexcitation due to the carrier dynamics. While the induced polarization (which is an ensemble average over many photoexcited dipole moments) is sensitive to scattering events that break the phase relationship among the individual dipoles and/or with the light field creating them (dephasing processes), the population difference is sensitive only to events that change the energy state of the carriers. Transient coherent optical spectroscopy addresses the time-evolution of the induced polarization in the time-regime during and immediately following the photoexcitation by a short laser pulse, in which the photoexcited dipoles have retained a defined phase relationship among each other and with the exciting coherent radiation.
In order to optimize opto-electronic applications of semiconductor nanostructures, a deep understanding of optical nonlinearities is essential.One fundamental method currently used within this field of research is ultrafast optical spectroscopy.This work presents a theoretical study of optical nonlinearities in semiconductor quantum wells in the coherent time regime.The theory is based on the equations of motion for the coherent exciton and biexciton transition amplitudes.These equations are derived using two different ways: Heisenberg equations of motion in combination with the dynamics-controlled truncation theory and alternatively the non-equilibrium Green´s function technique. For the coherent regime both approaches are equivalent and can be used to formulate a coupled set of equations for the coherent excitation dynamics that is correct up to the third order in the optical field.In contrast to the dynamics-controlled truncation theory the non-equilibrium Green´s function technique allows the inclusion of incoherent scattering processes into the description.The theory is evaluated to describe pump and probe as well as four-wave-mixing experiments with ZnSe quantum wells.Numerical calculations for the coherent control of the macroscopic polarization andthe dependence of transient four-wave-mixing on the light-polarization and intensity are both in good agreement with experiments.In order to correctly describe elevated excitation conditions for the latter investigation, the theory is self-consistently extended such that the included excitonic and biexcitonic nonlinearities contribute up to arbitrary order in the optical field.
Summary form only given. High-intensity pulse propagation of femtosecond laser pulses in optically thick semiconductor crystals can lead to self-induced transmission when the laser is tuned to a free exciton resonance. This effect means that at intensities on the order of MW/cm/sup 2/, pulses in the subpicosecond range lead to Rabi flopping of the carrier density. This causes the pulses to break up temporally after long-distance coherent propagation. The effect depends strongly on the coherence of the incident light field with the polarization of the exciton transition created in the semiconductor. Despite the expected excitation-induced dephasing, a large amount of coherent nonlinear transmission and a high contrast ratio of the Rabi flops are found at sample temperatures /spl les/10 K. In order to study the dynamics of the coherently driven polarization and the dependence on external dephasing, we introduced phonon-scattering by raising the temperature of our samples. The experiments were conducted with 800 fs pulses of an optical parametric amplifier in epitaxially grown CdSe. Our experiments clearly demonstrate that the coherent coupling of the free carrier polarization to the driving field of a high-intensity subpicosecond pulse with an area larger than /spl pi/ effectively prevents the expected dephasing by carrier-carrier scattering. Opening an additional dephasing channel by introducing phonon-scattering gradually weakens the coupling and suppresses characteristic features of self-induced transmission.
A new method of picosecond and femtosecond transient spectroscopy yielding information about ultrafast relaxation processes without requiring ultrashort light pulses is presented. It is based on the present theoretical analysis of the resonant degenerate four-wave-mixing process excited by two temporally incoherent light beams with wave vectors ${\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}}_{1}$ and ${\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}}_{2}$ which are originated from a single beam at frequency $\ensuremath{\omega}$ but have mutual time delay $\ensuremath{\tau}$. Under the assumption that the incoherent light field has Gaussian random complex amplitude and that the resonant material consists of the usual two-level atoms, the statistically averaged intensity of the output light field with ${\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}}_{3}=2{\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}}_{2}\ensuremath{-}{\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}}_{1}$ at $\ensuremath{\omega}$ is calculated as a function of $\ensuremath{\tau}$. Even with the light having a much longer duration than both
T1 (the longitudinal relaxation time) and
T2 (the transverse relaxation time), the correlation trace, i.e., output intensity versus $\ensuremath{\tau}$, represents a decay profile determined mainly by
T2 for both homogeneously and inhomogeneously broadened transitions, as long as the light correlation time ${\ensuremath{\tau}}_{c}$ is much shorter than the relaxation times. The correlation trace does not always represent a single-exponential decay but is sometimes slightly deformed by the
T1 effect. However, it does not cause a significant error in the determination of
T2. Moreover, as $\frac{{T}_{2}}{{T}_{1}}\ensuremath{\rightarrow}0$, the trace becomes a single-exponential decay curve determined only by
T2. The feature of the results obtained by the present method is similar to that obtained by the conventional coherent transient spectroscopy with short pulses, such as the photon echo. The time resolution in the present method, however, is limited only by ${\ensuremath{\tau}}_{c}$ much shorter than the light duration. By regarding the incoherent light as a series of random ultrashort pulses, the present four-wave-mixing process is also interpreted as the ensemble of numerous transient four-wave-mixing processes caused by various combinations of these pulses.
In this paper we develop a theoretical analysis which describes a coherent transient effect of two entering pulses---one laser and one Stokes---in a Raman-active medium. The field (Maxwell) and atomic (Schr\"odinger, density-matrix representation) equations are coupled in a self-consistent manner in time and space by virtue of the resultant second-order nonlinear macroscopic polarizations at the two frequencies. This treatment is accomplished under the circumstances where atomic coherence plays a predominant role. The equations derived here may be referred to as "Raman Bloch-Maxwell equations." The resultant equations yield a new aspect of transient stimulated Raman scattering and thus coherent Raman propagation. The transient-pulse behavior may be understood as self-induced modulation of coherent amplification and absorption. The self-induced modulation for the step-function input pulse is described by a combination of Jacobian elliptic functions depending on the input intensity. Computer calculations of transient-pulse evolution reveal interesting pulse breakup phenomena with peak amplification, energy transmission, pulse advance or delay, and pulse-narrowing effects.