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Annual Meeting Optical Society of America

Forward degenerate four-wave mixing near bound excitons in CdS

M. Dagenais, Michael E. Prise, Wayne F. Sharfin

Published Jan 1, 1985• 0 citations
Publisher

Abstract

Excitons bound to neutral donors in direct gap semiconductors are known to have remarkably large oscillator strengths (f ≠ 75). This leads to extremely fast radiative lifetime (τ ≠ 50 ps). We report here the observation of large resonant degenerate four-wave mixing signals near the l2 bound exciton in high purity (~1015/cc) CdS platelets. All the incident beams propagate in the forward direction. An electrooptically modulated cw dye laser operating single mode at 487 nm is used as the optical source. Optical pulses of 2 μs in duration are produced at a repetition rate of 10 kHz. The two incident beams responsible for generating the grating in the sample are mechanically modulated at frequencies ν1 = 1527 Hz and ν2 = 1349 Hz. Phase sensitive detection is used to detect the four-wave mixing signals at ν1 + ν2. Scattering efficiently larger than 1% for peak input power levels of ~5 mW in each beam is observed. The beam diameter on the sample is ~40 μm. Resonance enhancement of the four-wave mixing signal is observed as the laser is scanned across the bound exciton resonance. An anomalously large broadening of the four-photon signal is observed as the incident intensity is increased. The possible role of light trapping is discussed.

DOI
10.1364/oam.1985.thj2

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Excitons bound to neutral donors in direct gap semiconductors are known to have remarkably large oscillator strengths (f ≠ 75). This leads to extremely fast radiative lifetime (τ ≠ 50 ps). We report here the observation of large resonant degenerate four-wave mixing signals near the l2 bound exciton in high purity (~1015/cc) CdS platelets. All the incident beams propagate in the forward direction. An electrooptically modulated cw dye laser operating single mode at 487 nm is used as the optical source. Optical pulses of 2 μs in duration are produced at a repetition rate of 10 kHz. The two incident beams responsible for generating the grating in the sample are mechanically modulated at frequencies ν1 = 1527 Hz and ν2 = 1349 Hz. Phase sensitive detection is used to detect the four-wave mixing signals at ν1 + ν2. Scattering efficiently larger than 1% for peak input power levels of ~5 mW in each beam is observed. The beam diameter on the sample is ~40 μm. Resonance enhancement of the four-wave mixing signal is observed as the laser is scanned across the bound exciton resonance. An anomalously large broadening of the four-photon signal is observed as the incident intensity is increased. The possible role of light trapping is discussed.
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We perform two beam time integrated (TI) degenerate four wave mixing (DFWM) measurements on 8~nm GaAs quantum wells (QW). Pulses from a Ti-Sapphire laser resonantly excite only 1s heavy hole excitons. The power density of the leading pulse (I1) is increased, keeping that of the delayed pulse fixed and relatively small. We measure the TI-DFWM signal at different delays as well as the DFWM spectra at a fixed delay, as I1 is increased. We find that the dephasing rate, after an initial increase with I1, becomes independent of I1 for large I1. The spectrally integrated DFWM signal, which probes the coherent polarization of the resonantly excited QWs, initially increases with I1, reaches a peak and then decreases as 1/(root)I1 at large I1. The results are compared with theoretical models of exciton coherence.
Nearly degenerate four-wave mixing in Fabry–Perot semiconductor lasers is studied for pump–probe detunings that range from a few hundred megahertz to as high as 20 GHz. It is observed that the conjugate reflectivity and probe amplification decrease with slopes of −60 and −20 dB per frequency decade, respectively, when the detuning exceeds the relaxation-oscillation frequency. A resonance enhancement of the four-wave mixing signal is observed at both the relaxation-oscillation frequency and twice the relaxation-oscillation frequency. Cascade four-wave mixing signals are observed under a very weak (−37-dBm) input probe beam. A quantitative fit to the nearly degenerate four-wave mixing data is obtained, permitting the extraction of basic semiconductor-laser parameters by use of this technique.