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Physical review. B./Physical review. B

Efficiency enhancement of the coherent electron spin-flip Raman scattering through thermal phonons in (In,Ga)As/GaAs quantum dots

J. Debus, D. Kudlacik, P. Waldkirch, V. F. Sapega, Sven Scholz, Arne Ludwig, Andreas Dirk Wieck, M. Bayer

Published May 18, 2017• 3 citations
Publisher

Abstract

The spin-flip Raman scattering efficiency of the resident electron is thermally enhanced in singly charged (In,Ga)As/GaAs quantum dots, for probing the $s$- or $p$-shell trions. The Raman shift, polarization characteristics, and spectral position of the resonant scattering profile are insensitive to the sample temperature up to 50 K. This indicates a thermally robust mechanism of the coherent electron spin-flip based on exchange interaction. The background of the scattering spectra, whose intensity increases also by about one order of magnitude with temperature, is associated with acoustic phonon scattering. We propose that acoustic phonons enhance the spin-flip probability of the resident electron with growing temperature. The coherent spin-flip Raman scattering is ultimately suppressed at temperatures, which are a few times lower than that required for thermal trion dissociation.

DOI
10.1103/physrevb.95.201303

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The spin-flip Raman scattering efficiency of the resident electron is thermally enhanced in singly charged (In,Ga)As/GaAs quantum dots, for probing the sss- or ppp-shell trions. The Raman shift, polarization characteristics, and spectral position of the resonant scattering profile are insensitive to the sample temperature up to 50 K. This indicates a thermally robust mechanism of the coherent electron spin-flip based on exchange interaction. The background of the scattering spectra, whose intensity increases also by about one order of magnitude with temperature, is associated with acoustic phonon scattering. We propose that acoustic phonons enhance the spin-flip probability of the resident electron with growing temperature. The coherent spin-flip Raman scattering is ultimately suppressed at temperatures, which are a few times lower than that required for thermal trion dissociation.
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.
We study the role of electron-phonon scattering for a pulse-triggered quantum dot single-photon source which utilizes a modified version of stimulated Raman adiabatic passage and cavity coupling. This on-demand source is coherently pumped with an optical pulse in the presence of a continuous-wave laser drive, allowing for efficient generation of indistinguishable single photons with polarizations orthogonal to the applied fields. In contrast to previous studies, we explore the role of electron-phonon scattering on this semiconductor system by using a polaron master equation approach to model the biexciton-exciton cascade and cavity mode coupling. In addition to background zero-phonon-line decoherence processes, microscopic electron--acoustic-phonon coupling, which usually degrades the indistinguishability and efficiency of semiconductor photon sources, is rigorously taken into account. We study how different system parameters (including cavity and laser detunings, cavity spectral width, temperature) affect the device performance and contrast the relative influence of intrinsic phonon coupling with other dephasing mechanisms. We describe how this biexciton-exciton cascade scheme allows for true single photons to be generated with over 90% quantum indistinguishability and efficiency simultaneously using realistic experimental parameters. We also show how the double-field dressing can be probed through the cavity-emitted spectrum.
A single spin confined to a semiconductor quantum dot is a system of significant interest for quantum information science, as a potential optically-addressable qubit. In many respects, a quantum dot behaves like a single atom with high quality single photon emission. By controlling the light-matter coupling in such a system, it is possible to generate highly non-classical states of light and coherently control a single spin confined to the quantum dot. A departure from the ideal atomic picture appears once we consider the mesoscopic environment with which the quantum dot interacts. Charge fluctuations in the surroundings of the quantum dot affect the photon emission frequency leading to inhomogeneous broadening. Further broadening of the emission is caused by coupling to phonon modes of the host semiconductor material. Finally, coupling between the spin of a confined electron and a large bath of nuclear spins residing in the quantum dot leads to fast dephasing of the electron spin. All of these effects are typically considered detrimental to the potential use of quantum dots for quantum technologies. In this thesis, we develop the environmental coupling of a negatively charged quantum dot as a resource for quantum optics and spin control. First, the phonon-assisted fluorescence is shown to be a useful independent channel for feedback stabilisation of the quantum dot emission frequency, without requiring a measurement of the indistinguishable zero-phonon line. With stabilisation, the corresponding frequency broadening is drastically improved, and the sub-Hz frequency fluctuations are no longer resolved. Next, we show low-power resonance fluorescence emission spectra of the negatively charged trion transition. In the low power regime of resonance fluorescence, the excited state is not populated and most of the emission is coherent. In addition to elastic Rayleigh scattering, we observe coherent Raman sidebands, linked to an effective magnetic field created by the hyperfine interaction, the Overhauser field. This fluctuating effective field lifts the electron spin degeneracy in the absence of a magnetic field, and dictates the optical selection rules of the trion system. These spectra therefore allow for a measurement of the time-averaged distributions of in-plane and out-of-plane Overhauser field components. In the final part of the thesis, we use this hyperfine-generated Λ -scheme to optically create electron spin superpositions through two-colour excitation and coherent population trapping. We then show that rapid shifts in the relative phase of the lasers lead to initialisation of the electron spin into a rotated dark state.
The spin of an electron confined into a lateral semiconductor quantum dot has been proposed as a possible physical realization of a qubit. While the spin has the advantage of large decoherence times, operations with more than one qubit will necessarily involve orbital degrees of freedom, namely, charge, which is much more prone to decoherence. There are also alternative quantum dot qubit proposals that are entirely based on charge. We have used a realistic model to quantify the limitations imposed by acoustic phonons on the operation of quantum dot-based qubits. Our treatment includes essential aspects of the setup geometry, wave function profile and materials characteristics. The time dependence of the qubit density matrix is the presence of a phonon bath solved within the Born-Markov approximation. We find that the inclusion of geometric form factors makes the phonon-induced decoherence rates in double dot charge qubits nearly one order of magnitude lower than estimates previously in the literature. Moreover, our theoretical prediction for the quality factor of coherent charge oscillations based on phonon decoherence are higher than the values recently observed experimentally. This allows us to conclude that phonons are not the primary source of decoherence in double quantum dot qubits.
We report a study on temperature-dependent resonant fluorescence from InAs/GaAs quantum dots. We combined spectral and temporal measurements in order to identify sources of dephasing. In the spectral domain, we observed temperature-dependent broadening of the zero-phonon line as $0.3\phantom{\rule{0.28em}{0ex}}\ensuremath{\mu}\mathrm{eV}/\mathrm{K}$, and a temperature-dependent phonon broadband. Time-resolved autocorrelation measurements revealed temperature-dependent spin pumping times between T1,s=6{T}_{1,s}=6T1,s​=6 ns (4 K) and 0.50.50.5 ns (15 K). These results are compared against theoretical modeling with a master equation for a four-level system coupled to phonon and spin baths. We explained the results by phonon-mediated hole-spin scattering between two excited states, with the piezophonons as a dominant mechanism.
The ability to extend the time scale of the coherent optical response from large ensembles of quantum emitters is highly appealing for applications in quantum information devices. In semiconductor nanostructures, spin degrees of freedom can be used as auxiliary, powerful tools to modify the coherent optical dynamics. Here, we apply this approach to negatively charged (In,Ga)As/GaAs self-assembled quantum dots which are considered as excellent quantum emitters with robust optical coherence and high bandwidth. We study 3-pulse spin-dependent photon echoes subject to moderate transverse magnetic fields up to 1 T. We demonstrate that the timescale of coherent optical response can be extended by at least an order of magnitude by the field. Without magnetic field, the photon echo decays with T2T_ 2T2​ = 0.45 ns which is determined by the radiative lifetime of trions T1T_1T1​ = 0.27 ns. In the presence of the transverse magnetic field, the decay of the photon echo signal is given by spin dephasing time of the ensemble of resident electrons T2,eT_{2,e}T2,e​ ~ 4 ns. We demonstrate that the non-zero transverse g-factor of the heavy holes in the trion state plays a crucial role in the temporal evolution and magnetic field dependence of the long-lived photon echo signal.