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arXiv:0905.0297

All-Optical Ultrafast Control and Read-Out of a Single Negatively Charged Self-Assembled InAs Quantum Dot

Erik D. Kim, Katherine Smirl, Yanwen Wu, Alberto Amo, Xiao-Dong Xu, Duncan G. Steel, A. S. Bracker, D. Gammon, Lu Jeu Sham

Published May 3, 2009• 1 citation
arXivHTMLPDF

Abstract

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.

DOI
10.48550/arxiv.0905.0297

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quant-pharXiv:2604.07074•Apr 9, 2026
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.
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.
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.
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.
The ability to manipulate the spin states of charges confined in quantum dots (QDs) is essential for the realization of a quantum computer based on such spins. Here, we present experimentally realized electron spin qubit gates in a single self-assembled InAs QD using a combination of picosecond optical pulses, spin precession about an external DC magnetic field and optically generated geometric phases. Arbitrary unitary operations on the electron spin qubit may be constructed using a combination of optical pulses and either spin precession or the optically generated geometric phases.
We demonstrate complete coherent control of a single spin qubit confined in a self-assembled InAs negatively charged quantum dot subjected to an Oblique magnetic field, and directly compare this regime with the conventional Voigt geometry. In the Oblique-field configuration, the groundstate spin eigenstates are found to be unequal superpositions of the bare electron spin, with their composition tunable via the orientation of the applied field. This tunable spin mixing provides an additional degree of freedom to engineer the spin basis and associated optical couplings in the charged quantum dot system. Although this geometry has a distinct structure with important implications, it provides a regime in which we can fully and coherently control the tailored spin qubit. We observe Rabi oscillations and Ramsey fringes, and demonstrate arbitrary single-qubit rotations, enabling a direct comparison with the Voigt case. Our results establish that spin-qubit control does not necessarily require a pure Voigt geometry and can instead be achieved under Oblique magnetic fields. This relaxes constraints on device and field alignment and offers a versatile route to design and optimize quantum information processing architectures in semiconductor quantum dots.