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Physical Review B

Resonant two-color high-resolution spectroscopy of a negatively charged exciton in a self-assembled quantum dot

Martin Kroner, K. M. Weiss, B. Biedermann, Stefan Seidl, Alexander W. Holleitner, A. Badolato, Pierre M. Petroff, Patrik Öhberg, Richard John Warburton, K. Karraï

Published Aug 21, 2008• 32 citations
Publisher

Abstract

We report high-resolution resonant two-color laser spectroscopy on single self-assembled InGaAs quantum dots. The negatively charged exciton in a quantum dot can decay radiatively into both electron-spin ground states, the states with an electron in the quantum dot with its spin parallel or antiparallel to an applied magnetic field. The two decay paths can be used for optical spin alignment via optical pumping. We apply two laser fields at two different colors resonant with the two Zeeman split optical transitions to study the properties of the spin of the resident electron in the quantum dot in both the Faraday and Voigt geometries. The resonant two-color signal is monitored as a function of the laser power as well as the applied magnetic and electric field allowing us to determine spin decay and dephasing rates. We find the rate at which the optical spin alignment can be performed depending on the direction and the magnitude of the applied magnetic field. Finally we demonstrate the feasibility of performing coherent all-optical spin manipulation of an electron spin in a quantum dot.

DOI
10.1103/physrevb.78.075429

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Applied Physics Letters•Jan 21, 2008•36 citations
We report high-resolution resonant two-color laser spectroscopy on single self-assembled InGaAs quantum dots. The negatively charged exciton in a quantum dot can decay radiatively into both electron-spin ground states, the states with an electron in the quantum dot with its spin parallel or antiparallel to an applied magnetic field. The two decay paths can be used for optical spin alignment via optical pumping. We apply two laser fields at two different colors resonant with the two Zeeman split optical transitions to study the properties of the spin of the resident electron in the quantum dot in both the Faraday and Voigt geometries. The resonant two-color signal is monitored as a function of the laser power as well as the applied magnetic and electric field allowing us to determine spin decay and dephasing rates. We find the rate at which the optical spin alignment can be performed depending on the direction and the magnitude of the applied magnetic field. Finally we demonstrate the feasibility of performing coherent all-optical spin manipulation of an electron spin in a quantum dot.
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.
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.
A single Mn atom in an InGaAs epitaxial quantum dot provides an effective spin JJJ=1, which couples optically to excitonic states, offering an original spin-based platform for applications in quantum photonics. The authors investigate here the coherence of this spin by using one- and two-laser resonant optical spectroscopy in continuous wave regime to evidence and probe the Autler-Townes splitting generated at high excitation power. From the careful analysis of these data with a model based on optical Bloch equations, the authors can infer the pure dephasing rate of the addressed spin states.
A pair of self-assembled InGaAs quantum dots filled with two electrons can act as a singlet-triplet spin qubit that is robust against nuclear spin fluctuations as well as charge noise. This results in a T2* coherence time two orders of magnitude longer than that of a single electron, provided the qubit is operated at a particular "sweet spot" in gate voltage. However, at this fixed operating point the ground-state splitting can no longer be tuned into resonance with e.g. another qubit, limiting the options for coupling multiple qubits. Here, we propose using a four-electron coupled quantum dot to implement a singlet-triplet qubit that features a magnetically tunable level splitting. As a first step towards full experimental realization of this qubit design, we use optical spectroscopy to demonstrate the tunability of the four-electron singlet-triplet splitting in a moderate magnetic field.
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.
The Rabi splitting of the negatively charged exciton in a single InGaAs quantum dot is observed in resonance transmission spectroscopy. We use a pump laser excitation to drive strongly the unpolarized trion transition in a quantum dot and detect its modified absorption spectrum with a second weak probe laser. By tuning the pump laser near resonance, we observe an ac-Stark effect dispersion, with a power dependent Rabi splitting on resonance, both signatures of a strongly coupled two level system. Although the pump and probe laser fields are resonant with the same transition, we do not observe all features in the Mollow spectrum. We combine the results of pump probe with saturation spectroscopy data to deduce the individual contributions to the low power linewidth.