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physica status solidi (b)

Coherent Control of Two-Photon Transitions

N. Garro, Simon Kennedy, Albert P. Heberle, R. T. Phillips

Published Sep 1, 2000• 11 citations
Publisher

Abstract

Dipole-forbidden transitions have been investigated by means of coherent control techniques. The 2p heavy-hole excitonic transition of a GaAs/AlGaAs multiple quantum well system was excited by a pair of phase-locked pulses with their energy at half the transition energy. The temporal evolution of the amplitude of coherent control, monitored in the secondary emission at the 1s heavy-hole exciton energy, showed two different contributions: one at the frequency of the optical field, and a second one at twice that frequency, from the interference of the excitonic polarisation. The latter component contains, besides the energy of the dark transition, information about the dynamics of the state.

DOI
10.1002/1521-3951(200009)221:1<385::aid-pssb385>3.0.co;2-a

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Dipole-forbidden transitions have been investigated by means of coherent control techniques. The 2p heavy-hole excitonic transition of a GaAs/AlGaAs multiple quantum well system was excited by a pair of phase-locked pulses with their energy at half the transition energy. The temporal evolution of the amplitude of coherent control, monitored in the secondary emission at the 1s heavy-hole exciton energy, showed two different contributions: one at the frequency of the optical field, and a second one at twice that frequency, from the interference of the excitonic polarisation. The latter component contains, besides the energy of the dark transition, information about the dynamics of the state.
We have investigated the manipulation of the phase and amplitude of the state of a three-level exciton system by excitation with pairs of phase-locked optical pulses. We demonstrate coherent control over the phase of quantum beating between the light- and heavy-hole excitons which are the components of the system. The state of the system is monitored by time-resolved detection of the resonant secondary emission coupled out of the system in non-phase-matched directions by virtue of the static disorder. We show that the amplitude of the coherent manipulation must diminish as a function of time delay between the components of the pulse pair in a way which takes into account both the dephasing of the excitons and their unphasing which arises from inhomogeneous broadening.
Phase-locked pulse pairs are used for resonant excitation of excitons confined within GaAs/AlGaAs quantum wells. The time-resolved secondary emission displays strong dependence on the relative phases of the two pulses for inter-pulse delays of the order of 1ps or less. Constructive interference is combined with an increase in the rise time of the emission following the second pulse. For longer inter-pulse delays the different phases of inhomogeneous excitons complicate the effect of the second pulse, with the apparent effect changing with time after the second pulse. To model this, the optical Bloch equations for a line of three-level systems are integrated over time and the resulting polarisations summed over a range of angles. The importance of the inhomogeneity in descriptions of coherent control of secondary emission is shown.
Using a novel technique, we simultaneously study the femtosecond dynamics of the amplitude and the coherence of resonant secondary emission from GaAs quantum wells. Two phase-locked pulses resonantly excite excitons in the semiconductor and the subsequently emitted radiation is detected by femtosecond up-conversion. In experiments at various delays and phases between the excitation pulses we identify three different contributions to the secondary emission with different coherence properties in time.
Excitonic polarizations are coherently excited using two phase-locked pulses. By probing the linear propagation of the pulses through a GaAs/AlGaAs multiple quantum well sample, we directly demonstrate the intriguing interaction between the coherent exciton polarizations and the controlling pulses. It is shown that the second pulse can be either strongly amplified by taking up energy gained from the destruction of the exciton polarization or drastically decreased by giving up all its energy to excitons. The temporal signatures of the transmitted pulse shapes agree well with model calculations.
We demonstrate the presence of strong exciton-exciton correlations in GaAs-AlGaAs multiple quantum wells by using the polarization selection rules for four-wave mixing and a test that was originally designed to distinguish between quantum beats and polarization interference. We show that, when the four-wave-mixing signal is produced by two pulses that have the same circular polarization, dynamic beating behavior is observed at the heavy-hole-light-hole frequency that provides evidence of Coulomb-induced correlations that go beyond those expected from the semiconductor Bloch equations in the Hartree-Fock approximation and beyond the local field corrections used in simple phenomenological models. Moreover, this behavior cannot be explained by invoking biexcitonic effects. We demonstrate that this dynamic excitonic coupling can be explained in terms of a competition between quantum-beat-like and polarization-interference-like behavior, and we show that such behavior can be used to place quantitative limits on the coupling strength. In addition, we use a simple phenomenological model to show that excitation-induced-dephasing can produce such correlations.