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Physical Review B

Ultrafast optical control of electron spin coherence in charged GaAs quantum dots

M. V. Gurudev Dutt, Jun Cheng, Yanwen Wu, Xiaodong Xu, Duncan G. Steel, A. S. Bracker, D. Gammon, Sophia E. Economou, Ren‐Bao Liu, Lu Jeu Sham

Published Sep 13, 2006• 43 citations
Publisher

Abstract

Impulsive stimulated Raman excitation with coherent optical fields is used for controlling the electron spin coherence in a charged $\mathrm{GaAs}$ quantum dot ensemble through an intermediate charged exciton (trion) state. The interference between two stimulated Raman two-photon quantum mechanical pathways leading to the spin coherence allows us to control the electron spin coherence on the time scale of the Larmor precession frequency. We also demonstrate, both theoretically and experimentally, that ultrafast manipulation of the spin coherence is possible on the time scale of the optical laser frequency, and analyze the limitations due to the trion and spin decoherence times.

DOI
10.1103/physrevb.74.125306

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Impulsive stimulated Raman excitation with coherent optical fields is used for controlling the electron spin coherence in a charged GaAs\mathrm{GaAs}GaAs quantum dot ensemble through an intermediate charged exciton (trion) state. The interference between two stimulated Raman two-photon quantum mechanical pathways leading to the spin coherence allows us to control the electron spin coherence on the time scale of the Larmor precession frequency. We also demonstrate, both theoretically and experimentally, that ultrafast manipulation of the spin coherence is possible on the time scale of the optical laser frequency, and analyze the limitations due to the trion and spin decoherence times.
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.
Abstract In this letter, we have discussed the two-dimensional diffraction pattern via electron spin coherence in a GaAs quantum dot. Impulsive stimulated Raman excitation utilizing coherent optical fields is employed for the purpose of regulating the electron spin coherence within a charged ensemble of GaAs quantum dots, by means of an intermediate charged exciton (trion) state. We show that for the coupling two-dimensional standing wave (SW) field in the x and y directions, the two-dimensional Fraunhofer pattern can be formed for a weak probe light. By using the experimental parameters and controlling the Rabi frequency of the SW field and relative phase between applied lights, the symmetry and asymmetry diffraction pattern are obtained for the weak probe light due to the four-wave mixing mechanism. Our proposed model may have potential applications in high-capacity optical communications and quantum information technologies.
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.
We demonstrate coherent optical control of a single hole spin confined to an InAs/GaAs quantum dot. A superposition of hole-spin states is created by fast (10-100 ps) dissociation of a spin-polarized electron-hole pair. Full control of the hole spin is achieved by combining coherent rotations about two axes: Larmor precession of the hole spin about an external Voigt geometry magnetic field, and rotation about the optical axis due to the geometric phase shift induced by a picosecond laser pulse resonant with the hole-trion transition.
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.
We demonstrate the all-optical ultrafast manipulation and read-out of optical transitions in a single negatively charged self-assembled InAs quantum dot, an important step towards ultrafast control of the resident spin. Experiments performed at zero magnetic field show the excitation and decay of the trion (negatively charged exciton) as well as Rabi oscillations between the electron and trion states. Application of a DC magnetic field perpendicular to the growth axis of the dot enables observation of a complex quantum beat structure produced by independent precession of the ground state electron and the excited state heavy hole spins.