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Applied Physics Letters

Low power optical saturation of bound excitons with giant oscillator strength

M. Dagenais

Published Oct 15, 1983• 28 citations
Publisher

Abstract

The optical saturation of the I2 bound exciton in cadmium sulfide, an exciton bound to a donor, is reported. This system, which decays radiatively in 500 ps, can be saturated with a cw power of only 3.6 μW, which is equivalent to a saturation intensity of 58 W/cm2. Good agreement is found with the predictions of an inhomogeneously broadened two-level system. Thermal effects appear to play a minimal role.

DOI
10.1063/1.94481

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Low Power Optical Bistability Near Bound Excitons in Cadmium Sulfide

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The I2 bound exciton in cadmium sulfide has a giant oscillator strength of 6. It decays mostly radiatively in 500 psec. Such a large oscillator strength leads to a very large transition dipole moment and to very large nonlinear effects off-resonance. At 2K, this sytem saturates like an inhomogeneously broadened system for intensities up to 30 times the saturation intensity. The transition linewidth is 7.5 GHz. In a tight focusing geometry, only 3.6 μW is required to see the onset of saturation. This corresponds to a measured saturation intensity of about 60 W/cm2. The linear absorption coefficient right at the resonance peak was measured to be 3.2 x 103 cm-1. At higher temperatures, the transition linewidth broadens and the line becomes more and more homogeneously broadened because of phonon interaction. At intensities above 50 times the saturation intensity, the absorption coefficient stops decreasing and then starts increasing. At these high intensities, thermal effects appear to play a significant role in shifting the free and bound exciton resonances toward lower energies. At intensities less than 20 times the saturation intensity, thermal effects are believed to be insignificant in our saturation measurements.

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Forward degenerate four-wave mixing near bound excitons in CdS

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

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.

Annual Meeting Optical Society of America•Jan 1, 1985•0 citations
The optical saturation of the I2 bound exciton in cadmium sulfide, an exciton bound to a donor, is reported. This system, which decays radiatively in 500 ps, can be saturated with a cw power of only 3.6 μW, which is equivalent to a saturation intensity of 58 W/cm2. Good agreement is found with the predictions of an inhomogeneously broadened two-level system. Thermal effects appear to play a minimal role.
The I2 bound exciton in cadmium sulfide has a giant oscillator strength of 6. It decays mostly radiatively in 500 psec. Such a large oscillator strength leads to a very large transition dipole moment and to very large nonlinear effects off-resonance. At 2K, this sytem saturates like an inhomogeneously broadened system for intensities up to 30 times the saturation intensity. The transition linewidth is 7.5 GHz. In a tight focusing geometry, only 3.6 μW is required to see the onset of saturation. This corresponds to a measured saturation intensity of about 60 W/cm2. The linear absorption coefficient right at the resonance peak was measured to be 3.2 x 103 cm-1. At higher temperatures, the transition linewidth broadens and the line becomes more and more homogeneously broadened because of phonon interaction. At intensities above 50 times the saturation intensity, the absorption coefficient stops decreasing and then starts increasing. At these high intensities, thermal effects appear to play a significant role in shifting the free and bound exciton resonances toward lower energies. At intensities less than 20 times the saturation intensity, thermal effects are believed to be insignificant in our saturation measurements.
Very large nonlinearities are observed in the vicinity of a bound exciton resonance in cadmium sulfide. Power levels of the order of 8 μW are sufficient for saturating the bound exciton resonance in a tight focusing geometry. In a more loosely focused geometry, power levels of the order of 250 μW are sufficient for saturating the bound exciton resonance and for observing optical bistability. Transverse effects are found to play a very important role. For all our measurements, no thermal contributions to the nonlinearity were observed. Since thermal effects are not playing a role and since the studied bound excitons decay radiatively in 500 psec, we infer subnanosecond switchoff and cycling times.
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.