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Physical Review A

Observation of new scattering orders in degenerate four-wave mixing with semiconductors

Brian P. McGinnis, Ewan M. Wright, S. W. Koch, Nasser N. Peyghambarian

Published Jan 1, 1990• 1 citation
Publisher

Abstract

New scattering orders in degenerate four-wave mixing with a bulk semiconductor have been observed due to spatial subharmonic bifurcation of the laser-induced grating. For the observation, wave mixing in the Raman-Nath regime was performed in a thin platelet of CdS that exhibited increasing absorption optical bistability. A qualitative theoretical model is presented that explains the appearance of new scattering orders.

DOI
10.1103/physreva.41.523

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New scattering orders in degenerate four-wave mixing with a bulk semiconductor have been observed due to spatial subharmonic bifurcation of the laser-induced grating. For the observation, wave mixing in the Raman-Nath regime was performed in a thin platelet of CdS that exhibited increasing absorption optical bistability. A qualitative theoretical model is presented that explains the appearance of new scattering orders.
A theory of degenerate four-wave mixing in the Raman-Nath approximation is developed that includes transverse effects and excitation-dependent optical material properties. A microscopic model is used for the nonlinear absorption and refractive-index changes of laser-excited semiconductors. Diffusion of the excitation density is assumed to be the dominant transverse coupling mechanism. Numerical simulations of the Raman-Nath scattering spectrum are presented for the example of room-temperature bulk GaAs using steady-state illumination. The shortcomings of the standard analysis at high excitation are demonstrated.
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.
Recently, the high speed of semiconductor materials was combined with the large optical nonlinearity of the Franz-Kelydish effect near the quantum confined exciton absorption within semi-insulating multiple quantum well structures (SIMQW)[1]. The diffraction efficiency of four wave mixing obtained in the SIMQW with an optical interaction length of 1.05 µm is comparable with the diffraction efficiency for a semiconductor bulk sample with an optical interaction length of several mm operating under similar conditions. Thus, SIMQW become a ideal candidate to study the diffraction process in the Raman-Nath regime[2]. Here, we report two effects of the second order diffraction in a SIMQW sample under applied field: 1) the direct observation of a strong second order diffraction signal; 2) the intensity of the degenerate four wave mixing signal depends on the direction of applied field when the fringe spacing becomes large.
Higher orders of diffraction observed in a transient four-wave mixing experiment with acceptor-bound exciton complexes in CdS are analyzed in terms of pulse propagation. The description is based on a mean-field correction to the driving electric field in the optical Bloch equations, which are shown to generally lack higher-order diffraction for two-pulse self-diffraction. A propagation-induced sequence of stimulated echoes diffracted at the population grating dominates at least the second order of diffraction. \textcopyright{} 1996 The American Physical Society.