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Register a new userDynamic polarization of electron spins in indirect band gap (In,Al)As/AlAs quantum dots in weak magnetic field: experiment and theory
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A novel spin orientation mechanism - dynamic electron spin polarization has been recently suggested in Phys. Rev. Lett. $mathbf{125}$, 156801 (2020). It takes place for unpolarized optical excitation in weak magnetic fields of the order of a few millitesla. In this paper we demonstrate experimentally and theoretically that the dynamic electron spin polarization degree changes sign as a function of time, strength of the applied magnetic field and its direction. The studies are performed on indirect band-gap (In,Al)As/AlAs quantum dots and their results are explained in the framework of a theoretical model developed for our experimental setting.
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The band structure of type-I (In,Al)As/AlAs quantum dots with band gap energy exceeding 1.63 eV is indirect in momentum space, leading to long-lived exciton states with potential applications in quantum information. Optical access to these excitons is provided by mixing of the $Gamma$- and X-conduction band valleys, from which control of their spin states can be gained. This access is used here for studying the exciton spin-level structure by resonant spin-flip Raman scattering, allowing us to accurately measure the anisotropic hole and isotropic electron $g$ factors. The spin-flip mechanisms for the indirect exciton and its constituents as well as the underlying optical selection rules are determined. The spin-flip intensity is a reliable measure of the strength of $Gamma$-X-valley mixing, as evidenced by both experiment and theory.
The exciton spin dynamics are investigated both experimentally and theoretically in two-monolayer-thick GaAs/AlAs quantum wells with an indirect band gap and a type-II band alignment. The magnetic-field-induced circular polarization of photoluminescence, $P_c$, is studied as function of the magnetic field strength and direction as well as sample temperature. The observed nonmonotonic behaviour of these functions is provided by the interplay of bright and dark exciton states contributing to the emission. To interpret the experiment, we have developed a kinetic master equation model which accounts for the dynamics of the spin states in this exciton quartet, radiative and nonradiative recombination processes, and redistribution of excitons between these states as result of spin relaxation. The model offers quantitative agreement with experiment and allows us to evaluate, for the studied structure, the heavy-hole $g$ factor, $g_{hh}=+3.5$, and the spin relaxation times of electron, $tau_{se} = 33~mu$s, and hole, $tau_{sh} = 3~mu$s, bound in the exciton.
The dynamics of the coupled electron-nuclear spin system is studied in an ensemble of singly-charged (In,Ga)As/GaAs quantum dots (QDs) using periodic optical excitation at 1 GHz repetition rate. In combination with the electron-nuclei interaction, the highly repetitive excitation allows us to lock the electron spins into magnetic resonance in a transverse external magnetic field. Sweeping the field to higher values, the locking leads to an effective diamagnetic response of significant strength due to dynamic nuclear polarization, which shields the QD electrons at least partly from the external field and can even keep the internal magnetic field constant up to 1.3 T field variation. We model the effect through a magnetic field-dependent polarization rate of the nuclei, from which we suggest a strategy for adjusting the nuclear polarization through the detuning between optical excitation and electronic transition, in addition to tuning the magnetic field.
We show here the existence of the indirect coupling of electron and magnetic or nuclear ion spins in self-assembled quantum dots mediated by electron-electron interactions. With a single localized spin placed in the center of the dot, only the spins of electrons occupying the zero angular momentum states couple directly to the localized spin. We show that when the electron-electron interactions are included, the electrons occupying finite angular momentum orbitals interact with the localized spin. This effective interaction is obtained using exact diagonalization of the microscopic Hamiltonian as a function of the number of electronic shells, shell spacing, and anisotropy of the electron-Mn exchange interaction. The effective interaction can be engineered to be either ferromagnetic or antiferromagnetic by tuning the parameters of the quantum dot.
In III-V semiconductor nano-structures the electron and nuclear spin dynamics are strongly coupled. Both spin systems can be controlled optically. The nuclear spin dynamics is widely studied, but little is known about the initialization mechanisms. Here we investigate optical pumping of carrier and nuclear spins in charge tunable GaAs dots grown on 111A substrates. We demonstrate dynamic nuclear polarization (DNP) at zero magnetic field in a single quantum dot for the positively charged exciton X$^+$ state transition. We tune the DNP in both amplitude and sign by variation of an applied bias voltage V$_g$. Variation of $Delta$V$_g$ of the order of 100 mV changes the Overhauser splitting (nuclear spin polarization) from -30 $mu$eV (-22 %) to +10 $mu$eV (+7 %), although the X$^+$ photoluminescence polarization does not change sign over this voltage range. This indicates that absorption in the structure and energy relaxation towards the X$^+$ ground state might provide favourable scenarios for efficient electron-nuclear spin flip-flops, generating DNP during the first tens of ps of the X$^+$ lifetime which is of the order of hundreds of ps. Voltage control of DNP is further confirmed in Hanle experiments.
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