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Coherent optical manipulation of electron spin in charged semiconductor quantum dots.

Meenakshi Dutt

Published Jan 1, 2004• 0 citations
OpenAlex

Abstract

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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•Jan 1, 2011•0 citations
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.
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.
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.
Self-assembled quantum dots (QDs) containing a single electron are one of the leading candidate systems for the realization of a quantum computer. The spin states of charges confined in these dots have been shown to possess a number of qualities that are attractive for use as the quantum bits (qubits) in quantum computing implementations, particularly their long lifetimes and coherence times. In addition, these spin qubits may be controlled optically, offering the prospect of ultrafast qubit gate operations, a crucial necessity for the execution of quantum algorithms. Due to the weak interaction of self-assembled QDs with light, however, the coherent optical control and read-out of the spin states of charged self-assembled QDs has proven to be a considerable challenge. This thesis presents two sets of experiments demonstrating the coherent optical control and read-out of the quantum states of a self-assembled InAs QD containing a single electron. The first utilizes mode-locked picosecond optical pulses to control the optical transitions in the dot and to detect QD level occupations. These capabilities are used to observe transient phenomena in a singly charged InAs QD such as the generation and decay of excited state population and spin precession. Further, Rabi oscillations between the electron and the lowest-lying excited state are observed, demonstrating the ability to coherently control the optical transitions of the QD, a prerequisite for spin control. These results are built upon in the second set of experiments, in which a combination of optical pulses, an externally applied DC magnetic field and a continuous-wave (CW) optical field are employed to initialize and completely control the states of a QD confined electron spin. Spin control by the use of pulse-driven two-photon Raman processes, spin precession about the external magnetic field and geometric phases generated by CW-driven cyclic evolutions in the dot is demonstrated. A number of spin qubit gate operations are shown for these spin control mechanisms, forming a foundational set of single qubit gates required for the implementation of quantum computing with singly charged self-assembled QDs.
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.
The optically-induced coherent spin dynamics in a charged quantum dot (QD) is studied theoretically using a new dynamical model for rigorous description of circularly polarized ultrashort optical pulse resonant interactions with the electron-trion system. Generalized pseudospin master equation is derived for description of the time evolution of spin coherences and spin populations in terms of the real state pseudospin (coherence) vector including dissipation in the system through spin relaxation processes. The equation is solved in the time domain self-consistently with the vector Maxwell equations for the optical wave propagation coupled to it via macroscopic medium polarization. Using the model the long-lived electron spin coherence left behind a single resonant ultrashort optical excitation of the electron-trion transition in a charged QD is simulated in the lowand high-intensity Rabi oscillations regime. Signatures of the polarized photoluminescence (PL) resulting from the numerical simulations, such as the appearance of a second echo pulse after the excitation and a characteristic PL trace shape, specific for initial spin-up orientation, are discussed for realization of high-fidelity schemes for coherent readout of a single spin polarization state.
Optically driven self-assembled quantum dots are leading candidates for use in quantum computers because of their potential for high speed gate operations and relatively compact design. In this approach, each dot is charged with a single electron whose spin serves as the quantum bit (qubit). This thesis addresses the need for a universal set of gates to physically implement quantum computing and discusses initial steps toward spin-photon entanglement. Both are addressed through coherent control of the spin state in a magnetic field with optical pulses. This work experimentally demonstrates coherent rotations of the electron spin. First, the electron spin is rotated at up to 0.5 terahertz about the optical axis by a detuned picosecond optical pulse. The rotation occurs via a nearly resonant stimulated spin-flip Raman process involving a negatively charged exciton (trion). Second, rotation about an orthogonal axis is demonstrated due to electron spin precession about the magnetic field between two detuned optical pulses. The magnitude of the electron g factor is measured to be 0.4, and the rotation speed is 30 gigahertz in a 6.6 Tesla field. Geometric phases are detected in quantum dots for the first time due to cyclic Rabi oscillations driven by a resonant continuous-wave laser. These geometric phases provide another method of spin rotation and can be used in a gate. Any combination of these methods that provides spin rotation about two orthogonal axes can form an arbitrary rotation and together with a phase gate can form any unitary single qubit gate. Finally, this thesis also presents a detailed experimental procedure for creating a partial entanglement of internal variables within a quantum dot spin-exciton system, as a preliminary step to spin-photon entanglement. It has been proposed that entanglement between non-adjacent qubits in a large qubit network could occur via a photon, fueling research to demonstrate spin-photon entanglement. The experiment proposed here will create the precursor state in 25 picoseconds with a predicted fidelity of 0.985, and the precursor superposition state has a theoretical entropy of entanglement of 0.92.