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Physical Review B

Influence of optical coherence on the electron spin in singly charged InP quantum dots excited by resonant laser pulses

Shinichi Tomimoto, Keisuke Kawana, Akira Murakami, Yasuaki Masumoto

Published Jun 26, 2012• 0 citations
Publisher

Abstract

We have experimentally studied the spin dynamics of excitons, electrons, and trions in charge-tunable InP/InGaP quantum dots (QDs) excited by picosecond resonant laser pulses by observing the time-resolved Kerr rotation. In singly charged QDs, inversion of the spin polarization direction of doped electrons is found to be caused simply by variation in the pulse intensity, which is accompanied by an abrupt change of the spin coherence time. This phenomenon is reproduced by density-matrix calculations allowing for the reaction on the QD electron-trion four-level system during its coherent radiation emission. This result means that the optical coherence is another critical factor affecting electron spin coherence.

DOI
10.1103/physrevb.85.235320

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We have experimentally studied the spin dynamics of excitons, electrons, and trions in charge-tunable InP/InGaP quantum dots (QDs) excited by picosecond resonant laser pulses by observing the time-resolved Kerr rotation. In singly charged QDs, inversion of the spin polarization direction of doped electrons is found to be caused simply by variation in the pulse intensity, which is accompanied by an abrupt change of the spin coherence time. This phenomenon is reproduced by density-matrix calculations allowing for the reaction on the QD electron-trion four-level system during its coherent radiation emission. This result means that the optical coherence is another critical factor affecting electron spin coherence.
In this work, we study the resonant nonlinear optical response obtained when optical fields are used to excite charged semiconductor quantum dots (QDs). The basic physics of charged excitons (trions) created by optical excitation of charged QDs is of interest from the point of view of optically driven spin based quantum computing (QC). Stimulated Raman excitation, resonantly enhanced by the optical dipole coupling to the trion state, was used to optically generate electron spin coherence in the ground state of charged QDs. The evolution of the spin coherence was monitored through quantum beats in the phase-sensitively detected four wave mixing signal. The decay of the beats is a measure of the spin coherence time, which was found to be at least an order of magnitude greater than either the trion dipole coherence, or the Raman coherence time between excitons in a single neutral QD. A fascinating outcome of the experiment was the first observation of a contribution to the spin coherence induced by the vacuum field, which is also responsible for spontaneous emission from the trion state, known as spontaneously generated coherence (SGC). QC demands that coherent optical manipulations should be performed within the spin coherence time. We performed coherent optical control experiments, with a pair of phase-locked pump pulses, that showed the quantum nature of the coherence through interference of different quantum mechanical pathways. We showed both in experiment and theory that we can manipulate the spin coherence on the time scale of the Larmor frequency, as well as on an ultrafast femtosecond time scale, corresponding to the optical frequency of the trion state. Finally, resonant optical excitation of both the bright and nominally forbidden transitions from a single electron spin in a QD to the trion state were demonstrated. This allows for direct optical access to all the transitions required for optically driven QC with QD electron spins. We used frequency-domain nonlinear spectroscopy measurements on single QD trions to obtain the trion dipole decoherence and decay rates. Further, we demonstrated that the single electron spin coherence could be generated and detected optically, and found that the spin coherence time was significantly greater than in ensemble measurements at the same magnetic field.
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Optical control of the spin coherence of quantum well electrons by short laser pulses with circular or linear polarization is studied experimentally and theoretically. For that purpose the coherent electron spin dynamics in a nnn-doped CdTe/(Cd,Mg)Te quantum well structure was measured by time-resolved pump-probe Kerr rotation, using resonant excitation of the negatively charged exciton (trion) state. The amplitude and phase shifts of the electron spin beat signal in an external magnetic field, that are induced by laser control pulses, depend on the pump-control delay and polarization of the control relative to the pump pulse. Additive and nonadditive contributions to pump-induced signal due to the control are isolated experimentally. These contributions can be well described in the framework of a two-level model for the optical excitation of the resident electron to the trion.
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Coherent optically driven semiconductor quantum dot systems are proposed for the implementation of quantum information processing devices. Fundamental quantum computation units, the quantum bits (qubits), are realized and optically manipulated in the exciton and spin bases. In this thesis, consecutive phase-sensitive rotations of a single qubit and their importance in the measurement of the full physical density matrix have been demonstrated experimentally in the exciton system in neutral GaAs/Al0:3Ga0:7As interface fluctuation quantum dots. The experimental work done on the exciton system serves as a foundation for consequent work on the long coherence lifetime spin-based qubits in charged quantum dots. In the spin-based system in the charged GaAs/Al0:3Ga0:7As interface fluctuation quantum dots, we demonstrate the selective excitation from the two spin ground states to the charged exciton (trion) state through phase sensitive control of the spin coherence in an ensemble of three-level spin-trion Lambda systems. This controlled excitation utilized the optically coupled and decoupled states of the electron spin in the presence of coherent transient excitation of the spin ground states in singly charged quantum dots. This progress lays the ground work for achieving complete ultrafast spin rotations.