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Quantum Optoelectronics

Coherent Nonlinear Optical Spectroscopy of Semiconductor Microcavities

Hailin Wang, Jagdeep Shah, Theo C. Damen, William Y. Jan, J. E. Cunningham

Published Jan 1, 1995• 0 citations
Publisher

Abstract

In semiconductor microcavities, quantization of the photon modes can lead to a unique system where excitons couple coherendy to a single mode of photons. In this paper we present the first coherent nonlinear optical study of a composite exciton-cavity system. The results reveal coherent dynamical behaviors that are not accessible to linear measurements.

DOI
10.1364/qo.1995.qwb2

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In semiconductor microcavities, quantization of the photon modes can lead to a unique system where excitons couple coherendy to a single mode of photons. In this paper we present the first coherent nonlinear optical study of a composite exciton-cavity system. The results reveal coherent dynamical behaviors that are not accessible to linear measurements.
We present a coherent nonlinear optical study of composite exciton-cavity systems in the strong-coupling regime. Quantum oscillations in a transient four-wave-mixing response show the creation of a coherent superposition state between the two normal modes of the composite system and demonstrate in the time domain the coherent energy exchange between the exciton and cavity. The deep oscillation persists when the cavity resonance is far detuned from the exciton resonance. The result shows that dynamics of the nonlinear response can be in a nonperturbative regime while dynamics of the linear response remains in a perturbative regime.
The normal modes in a nonperturbatively coupled quantum-well semiconductor microcavity are linear superpositions of the QW exciton and cavity mode when the QW exciton transition is resonant with the cavity mode. When the lower normal mode is excited by a phase-locked pair of optical pulses, the nonlinear response of a probe pulse tuned to the upper mode is controlled. Thus the normal modes are coupled in their nonlinear optical response due to the nonlinearity of the exciton underlying the two normal modes. The cavity enhancement of the excitonic nonlinearity gives rise to a large signal; modulating the relative phase of the excitation pulses produces a differential reflectivity of up to 10%. Besides the coherent control of normal modes which is explainable with in the frame of semiclassical models, we observe a purely quantum mechanical phenomenon in our system. The quantum correlations between the field and carrier density lead to intraband coherences which live much longer than the interband dephasing time.
Summary form only given. The optical coherent control of quantum mechanical systems enables the direct manipulation of quantum states, and has been demonstrated on excitonic transitions in semiconductors. We have demonstrated the coherent control of the nonlinear optical response of quantum-well excitons in a resonant high-Q microcavity. There are two significant advantages to using excitons in microcavities instead of bare quantum wells: first, the multiple reflections which occur in the cavity strongly enhance the optical nonlinearity, enabling large-signal coherent control, and second, 2-color coherent control may be implemented, where a pump pulse tuned to one of the normal modes of the coupled exciton-microcavity system can control the response of a probe tuned to the other normal mode. The nonlinear response of the normal modes is due to the nonlinearity of the underlying exciton transition.
Multi-dimensional coherent spectroscopy (MDCS) has become an extremely versatile and sensitive technique for elucidating the structure, composition, and dynamics of condensed matter, atomic, and molecular systems. The appeal of MDCS lies in its ability to resolve both individual-emitter and ensemble-averaged dynamics of optically created excitations in disordered systems. When applied to semiconductors, MDCS enables unambiguous separation of homogeneous and inhomogeneous contributions to the optical linewidth, pinpoints the nature of coupling between resonances, and reveals signatures of many-body interactions. In this review, we discuss the implementation of MDCS to measure the nonlinear optical response of excitonic transitions in semiconductor nanostructures. Capabilities of the technique are illustrated with recent experimental studies that advance our understanding of optical decoherence and dissipation, energy transfer, and many-body phenomena in quantum dots and quantum wells, semiconductor microcavities, layered semiconductors, and photovoltaic materials.
Nonlinear optical phenomena in both semiconductor microcavities and sodium vapor are investigated. Systems displaying atomic and excitonic coupling are studied in detail in order to unravel underlying physical principles. Possible applications for these systems are evaluated where appropriate. Normal-mode coupling (NMC) in a semiconductor microcavity is achieved when a narrow-linewidth quantum well exciton resonance is coincident with the cavity mode of a high-finesse microcavity. This interaction leads to a double-peaked spectrum in either transmission, reflection, or photoluminescence (PL). The high-quality microcavities studied here at liquid-Helium temperatures reveal intensity dependent behavior that has not previously been observed. Nonlinear saturation of the exciton leads to a spectral broadening of the excitonic absorption without a significant loss in oscillator strength. This results in a reduction of the two transmission peaks with almost no change in the splitting between the peaks. Such behavior is easily explained using phenomenological nonlinear dispersion theory. In this nonlinear regime, the luminescence from the microcavity shows a gradual transition from the nonperturbative regime of NMC to lasing with increasing excitation. The observed behavior is explained by density-dependent changes in both the transmission of the microcavity and the bare-exciton emission, rather than a boson-condensation of excitons which has been previously proposed. An intermediate-finesse microcavity also modifies the emission distribution from a bulk-semiconductor at room temperature. Angularly resolved emission spectra and quantum efficiency measurements show the PL is strongly dependent on the reflectivity of the microcavity. Unfortunately, the enhancement in the decay rate of excitons due to high-reflectivity mirrors seen previously by our group does not result in an increased quantum efficiency. High-gain optical-wavefront amplification in atomic sodium vapor is demonstrated via both the three-photon effect and stimulated Raman scattering (SRS). In both cases, single-pass weak-field gain of nearly 400 is achieved with only 800 mW of pump power near 589 nm. In the case of SRS, phase preservation of the amplified wavefront, which is necessary in adaptive imaging applications, is also demonstrated.