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Journal of the Optical Society of America B

Linear and nonlinear pulse propagation at bound excitons in CdS

Marcus Jütte, H. Stolz, Wolf von der Osten

Published Jun 1, 1996• 27 citations
Publisher

Abstract

Pulse propagation experiments are performed with coherent picosecond laser pulses in resonance with the donor bound A-exciton (I2) state in CdS. Using bandwidth-limited time-resolved spectroscopy, we investigate the intensity of the transmitted laser pulse as a function of monochromator energy position and time. This method permits the determination of both the amplitude and the phase of the complex electric-field amplitude. Studying the dependence of pulse propagation on the input intensity, for small-area pulses we found at the rear of the sample the spectral hole formation and beating characteristic of a 0π pulse. At large pulse areas close to 2π the pulse propagates nearly unperturbed, showing no oscillatory reshaping or significant absorption losses. This provides clear evidence for self-induced transparency at an excitonic state in solids. Our interpretation is substantiated by an analysis within the framework of the combined Maxwell and optical Bloch equations.

DOI
10.1364/josab.13.001205

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Pulse propagation experiments are performed with coherent picosecond laser pulses in resonance with the donor bound A-exciton (I2) state in CdS. Using bandwidth-limited time-resolved spectroscopy, we investigate the intensity of the transmitted laser pulse as a function of monochromator energy position and time. This method permits the determination of both the amplitude and the phase of the complex electric-field amplitude. Studying the dependence of pulse propagation on the input intensity, for small-area pulses we found at the rear of the sample the spectral hole formation and beating characteristic of a 0π pulse. At large pulse areas close to 2π the pulse propagates nearly unperturbed, showing no oscillatory reshaping or significant absorption losses. This provides clear evidence for self-induced transparency at an excitonic state in solids. Our interpretation is substantiated by an analysis within the framework of the combined Maxwell and optical Bloch equations.
The propagation of small-area picosecond pulses of coherent light in resonance with the I 2 bound-exciton line in CdS is investigated. The observed strong reshaping of the pulses in form of propagation beats is consistent with the concomitantly measured hole formation in the pulse spectrum. By employing transform-limited time-resolved spectroscopy the complex amplitude of the transmitted optical field can be reconstructed. This allows to identify the beats as amplitude oscillations and phase changes by π characteristic of 0π pulse formation.
Abstract Measuring the transform‐limited time‐resolved spectrum of a coherent laser pulse allows one to determine the amplitude and phase of the pulse electric field. From the reshaping of pulses transmitted through a thin semiconductor platelet in resonance with an exciton transition in case of the donor bound exciton in CdS the effects of coherent exciton–photon interaction for different laser intensities can be studied. While at low intensities the expected polariton beating connected with the formation of a 0π‐pulse is observed, at sufficiently high intensities changes in the pulse shape occur that are ascribed to self‐induced transparency of the bound exciton states.
We report the first observation of quantum beats in the resonance fluorescence of a bound exciton in a semiconductor, the ionized-donor exciton complex in CdS. Measurements of the polarization behavior and magnetic-field dependence of the beats permitted a detailed investigation of strain effects and magneto-optical parameters of the states. From the damping of the beats, coherence times of the order of several hundreds of picoseconds are deduced. For the neutral-donor and -acceptor bound exciton states, very rapid dephasing with coherence times of the order of 20 ps is found.
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 form invariant coherent pulse propagation in semiconductors excited at 1s-exciton resonance is studied analytically using the reduced semiconductor Maxwell-Bloch equations. The sech-shaped pulse solution for excitonic self-induced transparency (SIT) is presented, showing significant difference in comparison with the well known SIT solution for non-interacting two-level systems. In contrast to 2π pulses in atomic systems, the phenomenon of SIT of interacting excitons in semiconductors occurs for the pulses of area 1.07π. Possible applications of the SIT solitons in semiconductor all-optical switching devices are discussed.
Summary form only given.Free-exciton resonances in semiconductors cannot be treated as bare two-level systems because Coulomb interaction and correlation/exchange effects between the carriers substantially modify the optical Bloch equations that describe the behavior of a two-level system under the influence of an external light field. The semiconductor Bloch equations (SBEs) give a more realistic description of the dynamic response of the system on ultrafast time scales. Therefore, the coherent transients known from two-level systems in atomic physics have been found to be substantially modified in semiconductors. Whereas self-induced transparency (SIT) on bound excitons, which are known to behave as atomiclike two-level systems, has been found, the question whether SIT could also appear on a free-exciton resonance is still subject of controversial discussions. We addressed this problem in a combined theory-experiment study.