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IEEE Journal of Quantum Electronics

Nonlinearity of the refractive index due to an excitonic molecule resonance state in CdS

R. Baumert, I. Broser, Klaus Buschick

Published Aug 1, 1986• 13 citations
Publisher

Abstract

We report the observation of an intensity-dependent refractive-index nonlinearity in CdS due to a resonance state where an excitonic molecule is created by induced absorption of light. The refractive indexnas a function of the incident laser photon energyEis measured directly by light refraction in thin crystal prisms. A renormalized dielectric function describes the measuredn(E)spectra well. This strong refractive-index nonlinearity is well suited to produce an optical bistability and to further strengthen the evidence of CdS to be an important material for laser-induced dynamic gratings.

DOI
10.1109/jqe.1986.1073125

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We report the observation of an intensity-dependent refractive-index nonlinearity in CdS due to a resonance state where an excitonic molecule is created by induced absorption of light. The refractive indexnas a function of the incident laser photon energyEis measured directly by light refraction in thin crystal prisms. A renormalized dielectric function describes the measuredn(E)spectra well. This strong refractive-index nonlinearity is well suited to produce an optical bistability and to further strengthen the evidence of CdS to be an important material for laser-induced dynamic gratings.
Optical bistability in the presence of an optically induced absorption is observed when a thin 13-μm CdS sample is inserted between two mirrors of 90 % reflectivity, in our experiment, a modulated cw laser of ~15-mW peak power is tuned on each side of the free exciton resonance in CdS, and the transmission characteristics are studied. A theoretical calculation including both absorptive and dispersive effects is presented and good agreement is obtained. The absorption coefficient and the index of refraction of the material are connected by Kramers-Kronig relations. Propagation effects are taken into account. Sufficiently long pulses (40 ms) are considered to allow the thermally induced absorption to occur. For detunings above the free exciton resonance, we predict that counterclockwise hysteresis loops will first be observed as the intensity rises; for detunings below the free exciton resonance, only clockwise hysteresis loops are predicted. These predictions were experimentally verified. Power levels of the order of 5–10 mW were sufficient to observe bistability. Cavity effects were also observed.
Transient optical nonlinearities of semiconductor quantum dots in the strongly confined regime are studied, in which the exciton, biexciton and magnetic field effects are taken into account. The photo induced band-to-band electronic transitions are considered from both the heavy-hole (hh) and light-hole (lh) valence bands to the lowest (1s) exciton state below the fundamental absorption edge. The time dependent perturbation technique for a three-level system, under the near band gap resonant excitation regime, has been employed; with the incorporation of the relaxation and dephasing mechanisms phenomenologically. The induced polarization is calculated from where the real and imaginary parts of the third-order nonlinear optical susceptibility, responsible for the occurrence of nonlinear refraction and nonlinear absorption respectively, have been derived. The temporal and detuning spectra of nonlinear refraction and absorption; and their dependence on density of biexcitons and a moderately strong magnetic field, have been analyzed. It is observed that the nonlinear refraction and nonlinear absorption enhance with increasing magnetic field in small CdS quantum dots.