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arXiv:cond-mat/0403260 · Journal of Applied Physics

Theory of ultrafast optical manipulation of electron spins in quantum wells

Jinshuang Jin, Xin-Qi Li

Published Dec 15, 2005• 3 citations
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Abstract

Based on a multiparticle-state stimulated Raman adiabatic passage approach, a comprehensive theoretical study of the ultrafast optical manipulation of electron spins in quantum wells is presented. In addition to corroborating experimental findings [Gupta et al., Science 292, 2458 (2001)], we improve the expression for the optical-pulse-induced effective magnetic field, in comparison with the one obtained via the conventional single-particle ac Stark shift. Further study of the effect of hole-spin relaxation reveals that, while the coherent optical manipulation of electron spin in undoped quantum wells would deteriorate in the presence of relatively fast hole-spin relaxation, the coherent control in doped systems can be quite robust against decoherence. The implications of the present results on quantum dots will also be discussed.

DOI
10.1063/1.2140868

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Based on a multiparticle-state stimulated Raman adiabatic passage approach, a comprehensive theoretical study of the ultrafast optical manipulation of electron spins in quantum wells is presented. In addition to corroborating experimental findings [Gupta et al., Science 292, 2458 (2001)], we improve the expression for the optical-pulse-induced effective magnetic field, in comparison with the one obtained via the conventional single-particle ac Stark shift. Further study of the effect of hole-spin relaxation reveals that, while the coherent optical manipulation of electron spin in undoped quantum wells would deteriorate in the presence of relatively fast hole-spin relaxation, the coherent control in doped systems can be quite robust against decoherence. The implications of the present results on quantum dots will also be discussed.
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.
The excitation of electron spin polarization and coherence by picosecond light pulses and their dynamics in a wide remotely doped quantum well are studied theoretically and experimentally. Assuming that all electrons in the quantum well are localized, the theory considers the resonant interaction of light pulses with the four-level system formed by the electron spins of the ground state and the hole spins of the trion excited state. The theory describes the effects of spontaneous emission, a transverse magnetic field and hole spin relaxation on the dynamics detected by the Kerr rotation of a probe pulse. Time resolved Kerr rotation experiments were carried out on a remotely doped 14nm14\phantom{\rule{0.3em}{0ex}}\mathrm{nm}14nm GaAs quantum well in the frequency range of optical transitions to the heavy hole (HH) trion and to the light-hole (LH) trion degenerate with the HH exciton. The experiments on the resonant excitation of the HH trion show a very slow heavy hole spin relaxation and, consequently, a weak electron spin polarization after the trion relaxation. In contrast, the resonant excitation of the LH trion/HH exciton results in a fast hole spin relaxation that increases electron spin polarization.
Individual electron and hole quantum dot spin qubits can be coherently manipulated using picosecond modelocked laser pulses; an all-optical spin-echo was implemented that decouples slow environmental changes. While dephasing and decoherence mechanisms for electrons and holes are intrinsically different, similar qualitative results are obtained, except for dynamic nuclear polarization effects that affect the controllability of electrons. In addition, we demonstrate spin-photon entanglement in a charged InAs quantum dot, using an ultrafast downconversion technique that converts a single, spontaneously emitted photon at 900 nm into a 1560 nm photon with picosecond timing resolution. This ultrafast conversion technique allows quantum erasure of which-path frequency information in the spontaneous emission process.
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.
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.
In this paper, we review our recent experimental studies on electromagnetically induced transparency (EIT) from electron spin coherences in semiconductor quantum wells. Coherent Raman resonances, manifestations of EIT from electron spin coherences at relatively low pump intensities, were demonstrated in both V-type and Λ-type three-level systems via heavy-hole exciton and trion transitions in undoped and doped quantum wells, respectively. Coherent Raman resonances from electron spin coherences via light-hole transitions were also demonstrated in a waveguide geometry that enables a long optical interaction length as well as a large absorption coefficient. Experimental approaches that can avoid or reduce detrimental many-body effects in quantum wells are suggested for the realization of nearly ideal EIT processes.