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Physical Review Letters

Dark States in Coherent Semiconductor Spectroscopy

Markus Lindberg, Rolf H. Binder

Published Aug 14, 1995• 74 citations
Publisher

Abstract

The possibility of creating dark states (a concept well known in atomic systems) in semiconductors is discussed. Based on the semiconductor Bloch equations, the analysis shows that, in spite of complications due to band-structure and strong excitonic many-body effects, signatures of dark states should be observable in femtosecond nonlinear optical excitation experiments.

DOI
10.1103/physrevlett.75.1403

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The possibility of creating dark states (a concept well known in atomic systems) in semiconductors is discussed. Based on the semiconductor Bloch equations, the analysis shows that, in spite of complications due to band-structure and strong excitonic many-body effects, signatures of dark states should be observable in femtosecond nonlinear optical excitation experiments.
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A microscopic many-body theory for the optical and electronic properties of semiconductors is reviewed with an emphasis on the role of correlation effects. At the semiclassical level, the semiconductor Bloch equations include many-body effects via bandgap and field renormalization as well as correlation contributions representing two electron-hole pair amplitudes, excitonic populations, and coupled interband and intraband coherences. These Coulomb interaction induced carrier correlations lead to characteristic signatures in nonlinear semiconductor spectroscopy. At the fully quantum mechanical level the dominant light-matter correlations are described by coupled semiconductor Bloch and luminescence equations. Excitonic emission properties of quantum well and microcavity systems are discussed, including effects such as coherent signatures in the secondary emission and coherent control of the emitted light.
The coherent response of a semiconductor three-state system to one or two intense light pulses is investigated experimentally on a 100 fs time scale. Three experiments constitute this dissertation: observation of excitonic Rabi oscillations, measurement of two-exciton coupled Stark shifting, and an attempt to observe dark states. Basic concepts of time-resolved ultrafast semiconductor spectroscopy are explained, followed by an analysis of semiconductor two- and three-state systems. Pure two- and three-state dynamics are derived from first principles, followed by the development of the appropriate semiconductor Bloch equations (SBE). Two-color pump-probe, two-color pump-pump, and pump-pump-probe techniques are explained in the context of three-state semiconductor experiments. The experimental setup is explained in detail. Resonant two-color pump-probe measurements resulted in the first observation of multiple excitonic Rabi oscillations. The common conduction band shared by the light-hole and heavy-hole excitons of an InGaAs multiple quantum well allowed us to measure hh-exciton density (Rabi) oscillations by probing lh-exciton absorption. By studying the intensity dependence of the Rabi frequency, we showed the important role of many-body effects in renormalizing the dipole energy. The shared conduction band also causes the lh-exciton resonance to Stark shift when the hh exciton is Stark shifted. We measured a transient Stark shifting of both resonances due to virtual hh-exciton transitions. We observed that the ratio of the hh-exciton shift to lh-exciton shift was 2:1 at large pump-exciton detuning, as predicted from a simple three-state dressed exciton picture. For smaller detunings we saw an increase in the ratio and a redshift of the non-dipole coupled exciton state. Both of these observations are consistent with the most recent theories and experiments on excitonic Stark shifting. For strong near-resonant pumping of both lh- and hh-exciton transitions, an intervalence-band Raman-type coherence follows from the SBE that results in a transparent eigenstate (dark state) when both pumps are equally detuned from resonance. The existence of this coherence is well-known in atomic-optical systems, but has been elusive in semiconductors. Our inconclusive experimental result is presented along with an evaluation of experimental shortcomings. In brief, the expected change is absorption was too small to see.
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.
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