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Physical Review Letters

Coherent Control and Polarization Readout of Individual Excitonic States

Brian Patton, U. Woggon, W. Langbein

Published Dec 21, 2005• 97 citations
Publisher

Abstract

We present measurements and simulations of coherent control and readout of the polarization in individual exciton states. The readout is accomplished by transient four-wave mixing detected by heterodyne spectral interferometry. We observe Rabi oscillations in the polarization, which show half the period of the Rabi oscillations in the population. A decrease of the oscillation amplitude with pulse area is observed, which is not accompanied by a change in the dephasing time. This suggests the transfer of the excitation to other states as the origin of the Rabi-oscillation damping. Detuning of the excitation enables the control of the polarization in phase and amplitude and is in qualitative agreement with simulations for a two-level system. Additionally, simultaneous Rabi flopping of several spatially and energetically close exciton states is demonstrated.

DOI
10.1103/physrevlett.95.266401

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We present measurements and simulations of coherent control and readout of the polarization in individual exciton states. The readout is accomplished by transient four-wave mixing detected by heterodyne spectral interferometry. We observe Rabi oscillations in the polarization, which show half the period of the Rabi oscillations in the population. A decrease of the oscillation amplitude with pulse area is observed, which is not accompanied by a change in the dephasing time. This suggests the transfer of the excitation to other states as the origin of the Rabi-oscillation damping. Detuning of the excitation enables the control of the polarization in phase and amplitude and is in qualitative agreement with simulations for a two-level system. Additionally, simultaneous Rabi flopping of several spatially and energetically close exciton states is demonstrated.
We present a novel heterodyne‐detected four‐wave mixing technique, which determines the third‐order nonlinear polarization in phase and amplitude by spectral interferometry. It allows us to measure the resonant transient four‐wave mixing of single localized excitons, both frequency and time‐resolved. In the signal, the strength of the coupling between two probed exciton transitions is directly observable. Applying a strong optical pump pulse, we observe optical Rabi oscillations of the exciton polarization. Observing decay of the third‐order polarization after the pump pulse, we can exclude the presence of signi£cant excitation‐induced dephasing.
Biexcitonic polarization excited in a ZnSe quantum well is coherently controlled with a pair of phase-locked laser pulses. The coherent control of this four-particle correlation is directly verified by observing a spectrally resolved four-wave-mixing signal in direction of the first order of diffraction of the pulse pair. By using polarization selection rules for the generation of biexcitons and changing the interpulse delay of the pulse pair the oscillations of the four-wave-mixing signal are studied at the energetic position of the excitonic as well as the biexcitonic resonance. The excitonic and biexcitonic signals exhibit a phase shift in dependence on the interpulse delay which clearly indicates the separate coherent control of the excitonic and biexcitonic polarization.
The coherent control of excitonic and biexcitonic polarization in pulse-transmission and four-wave-mixing (FWM) experiments is analysed with real time resolution. As a model system a ZnSe single quantum well is exclusively excited at the heavy-hole exciton and exciton–biexciton resonance. In pulse-transmission experiments the coherent control of excitonic polarization is shown for low excitation intensities. At elevated excitation intensities the dephasing time of the polarization is found to be strongly dependent on the relative phase of two phase-locked laser pulses which perform the coherent manipulation of the polarization. In FWM experiments the separate coherent control of the excitonic and biexcitonic FWM polarization is demonstrated which enables a coherent manipulation of the amplitude and phase of exciton–biexciton beats which are observed on the FWM polarization transients.
Degenerate four-wave mixing (FWM) from individual localized excitonic transitions is measured using a dual-polarization extension of heterodyne spectral interferometry. A fine-structure splitting (FSS) of the localized excitons of $20--80\text{ }\ensuremath{\mu}\text{eV}$ is observed, revealing a spatially anisotropic localization in the quantum well plane, preferentially oriented along the [110] direction. The ratio of the transition dipole moments of the FSS transitions is in the range 0.7--1.4, with no significant correlation to the FSS. Retrieving both polarization components of the FWM in amplitude and phase we measure the time-resolved polarization state of the exciton after pulsed excitation, showing a coherent evolution oscillating between linear and virtually circular polarization. The polarization of the created FWM state is a result of the initial polarization state created by the first excitation pulse, its free evolution up to the arrival of the second pulse, and its conversion into the FWM controlled by the polarization of the second pulse.
Measurements of optical Rabi oscillations in the excited states of individual InGaAs are presented. Under pulsed resonant excitation we observe Rabi oscillations with increasing pulse area, which are damped after the first maximum and minimum. We show that the observed damping comes from an additional non-resonant generation of carriers in the quantum dot. The observation of Rabi oscillations provides an efficient way of directly measuring the excitonic transitions' dipole moments. A polarization anisotropy of the dipole moment is resolved in some of the quantum dots.