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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Ultrafast and large nonlinear optical response of excitons weakly confined in a semiconductor thin film

Toshiro Isu, Koichi Akiyama, Nobuyuki Tomita, Yoshinori Nomura, Hajime Ishihara, Kikuo Cho

Published Jun 2, 2003• 1 citation
Publisher

Abstract

We observe ultrafast and large nonlinear optical responses of a semiconductor thin film where excitons are weakly confined and their center-of-mass motion is quantized. The observed degenerate four-wave mixing (DFWM) signal of a GaAs double-hetero-structure layer exhibits an anomalous thickness-dependence, and is much enhanced at the thickness of 110nm. The decay time of the response is the order of ps, which depends on the thickness of the layer and on the number of the layer. These phenomena are elucidated by the theory of the nonlocal interaction between excitonic states and the light beyond the long wavelength approximation regime. The enhancement at the thickness is due to the size-resonant enhancement of the internal field with a nano-scale spatial structure, where the second quantized level of the exciton center-of-mass motion mainly contributes to the large response at the thickness. We, furthermore, demonstrate ultrafast response in a reflective type nonlinear polarization rotation switch with the 110nm thick three double-hetero. The signal intensity of 20% for the reflective pulse was obtained at a pump intensity of 10nJ/cm2, and the decay time is 1.5ps at low temperatures. These results provide a novel design of a semiconductor structure in order to obtain both large and ultrafast nonlinear response that is suitable for device application.

DOI
10.1117/12.475705

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We observe ultrafast and large nonlinear optical responses of a semiconductor thin film where excitons are weakly confined and their center-of-mass motion is quantized. The observed degenerate four-wave mixing (DFWM) signal of a GaAs double-hetero-structure layer exhibits an anomalous thickness-dependence, and is much enhanced at the thickness of 110nm. The decay time of the response is the order of ps, which depends on the thickness of the layer and on the number of the layer. These phenomena are elucidated by the theory of the nonlocal interaction between excitonic states and the light beyond the long wavelength approximation regime. The enhancement at the thickness is due to the size-resonant enhancement of the internal field with a nano-scale spatial structure, where the second quantized level of the exciton center-of-mass motion mainly contributes to the large response at the thickness. We, furthermore, demonstrate ultrafast response in a reflective type nonlinear polarization rotation switch with the 110nm thick three double-hetero. The signal intensity of 20% for the reflective pulse was obtained at a pump intensity of 10nJ/cm2, and the decay time is 1.5ps at low temperatures. These results provide a novel design of a semiconductor structure in order to obtain both large and ultrafast nonlinear response that is suitable for device application.
In this paper, we experimentally demonstrate an ultrafast and large nonlinear optical response by controlling the thickness of the GaAs layers in a double hetero-structure through a degenerate four-wave mixing (DFWM) experiment. We show that the polarization corresponding to the second quantized level of the CM state (n = 2) induces a large nonlinear response although this is optically forbidden for ordinal treatment using LWA. We prepare very high quality samples of GaAs layers in order to properly measure the nonlinear optical response of excitons, which extend coherently over the sample. A calculation based on a nonlocal response theory is performed to explain the experimental result.
We study the size dependence of the nonlinear response of weakly confined excitons for the size region beyond the long wavelength approximation regime. The observed degenerate-four-wave mixing signal of GaAs thin layers exhibits an anomalous size dependence, where the signal is resonantly enhanced at a particular thickness region. The theoretical analysis elucidates that this enhancement is due to the size-resonant enhancement of the internal field with a spatial structure relevant to the nondipole-type excitonic state. These results establish the formerly proposed new type of size dependence of nonlinear response due to the nonlocality induced double resonance.
We demonstrate the possibility of ultrafast optical control of excitons confined in GaAs thin films. The intensity of a two-beam degenerate four-wave-mixing signal changes with an increase in the power of each pulse. The signal intensity monotonically decreases after reaching the maximum. Peaks appear at different excitation powers for k 1 and k 2 pulses, which suggests that the decrease in the signal intensity is caused by excitonic Rabi oscillations. Our results demonstrate the possibility of ultrafast control of the exciton population by using optical pulses.
A theoretical investigation is reported of the coherent nonlinear response of excitons and biexcitons in a thin semiconductor film subjected to resonant laser radiation. It is shown that saturation of an exciton transition results in an abrupt qualitative change in the nature of film transmission from total reflection of the incident pulse at low pump amplitudes to oscillatory reflection at high amplitudes. A new area theorem is derived for ultrashort pulses: it establishes a correspondence between the areas of the incident, transmitted, and reflected pulses. Anomalous transmission and reflection (area 'quantisation') is predicted for large values of the nonlinear parameter. The equations of state, describing bistable behaviour of the amplitudes of the fields of the transmitted and reflected radiation, are derived for quasi-cw operation.
The nonlinear response of single GaAs quantum dots is studied in femtosecond near-field pump-probe experiments. At negative time delays, transient reflectivity spectra show pronounced oscillatory structure around the quantum dot exciton line, providing the first evidence for a perturbed free induction decay of the excitonic polarization. Phase-disturbing Coulomb interactions between the excitonic polarization and continuum excitations dominate the optical nonlinearity on ultrafast time scales. A theoretical analysis based on the semiconductor Bloch equations accounts for this behavior.
A theoretical investigation is reported of the coherent nonlinear response of excitons and biexcitons in a thin semiconductor film subjected to resonant laser radiation. It is shown that saturation of an exciton transition results in an abrupt qualitative change in the nature of film transition from the regime of total reflection of the incident pulse at low pump amplitudes to oscillatory reflection at high amplitudes. A new area theorem is derived for ultrashort pulses: it establishes a correspondence between the areas of the incident, transmitted and reflected pulses. Anomalous transmission and reflection is predicted for large values of the nonlinear parameter. The equations of the state, describing bistable behavior of the amplitudes of the fields of the transmitted and reflected radiation, are derived for quasi-cw operation.