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Register a new userElectron-nucleus spin correlation conservation of the spin dependent recombination in Ga$^{2+}$ centers
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Spin dependent recombination in GaAsN offers many interesting possibilities in the design of spintronic devices mostly due to its astounding capability to reach conduction band electron spin polarizations close to 100% at room temperature. The mechanism behind the spin selective capture of electrons in Ga$^{2+}$ paramagnetic centers is revisited in this paper to address inconsistencies common to most previously presented models. Primarily, these errors manifest themselves as major disagreements with the experimental observations of two key characteristics of this phenomenon: the effective Overhauser-like magnetic field and the width of the photoluminescence Lorentzian-like curves as a function of the illumination power. These features are not only essential to understand the spin dependent recombination in GaAsN, but are also key to the design of novel spintronic devices. Here we demonstrate that the particular structure of the electron capture expressions introduces spurious electron-nucleus correlations that artificially alter the balance between the hyperfine and the Zeeman contributions. This imbalance strongly distorts the effective magnetic field and width characteristics. In this work we propose an alternative recombination mechanism that preserves the electron-nucleus correlations and, at the same time, keeps the essential properties of the spin selective capture of electrons. This mechanism yields a significant improvement to the agreement between experimental and theoretical results. In particular, our model gives results in very good accord with the experimental effective Overhauser-like magnetic field and width data, and with the degree of circular polarization under oblique magnetic fields.
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Similar to nitrogen-vacancy centers in diamond and impurity atoms in silicon, interstitial gallium deep paramagnetic centers in GaAsN have been proven to have useful characteristics for the development of spintronic devices. Among other interesting properties, under circularly polarized light, gallium centers in GaAsN act as spin filters that dynamically polarize free and bound electrons reaching record spin polarizations (100%). Furthermore, the recent observation of the amplification of the spin filtering effect under a Faraday configuration magnetic field has suggested that the hyperfine interaction that couples bound electrons and nuclei permits the optical manipulation of its nuclear spin polarization. Even though the mechanisms behind the nuclear spin polarization in gallium centers are fairly well understood, the origin of nuclear spin relaxation and the formation of an Overhauser-like magnetic field remain elusive. In this work we develop a model based on the master equation approach to describe the evolution of electronic and nuclear spin polarizations of gallium centers interacting with free electrons and holes. Our results are in good agreement with existing experimental observations. In regard to the nuclear spin relaxation, the roles of nuclear dipolar and quadrupolar interactions are discussed. Our findings show that, besides the hyperfine interaction, the spin relaxation mechanisms are key to understand the amplification of the spin filtering effect and the appearance of the Overhauser-like magnetic field. Based on our models results we propose an experimental protocol based on time resolved spectroscopy. It consists of a pump-probe photoluminescence scheme that would allow the detection and the tracing of the electron-nucleus flip-flops through time resolved PL measurements.
We demonstrate the detection of coherent electron-nuclear spin oscillations related to the hyperfine interaction and revealed by the band-to-band photoluminescence (PL) in zero external magnetic field. On the base of a pump-probe PL experiment we measure, directly in the temporal domain, the hyperfine constant of an electron coupled to a gallium defect in GaAsN by tracing the dynamical behavior of the conduction electron spin-dependent recombination to the defect site. The hyperfine constants and the relative abundance of the nuclei isotopes involved can be determined without the need of electron spin resonance technique and in the absence of any magnetic field. Information on the nuclear and electron spin relaxation damping parameters can also be estimated from the oscillations damping and the long delay behavior.
We have studied the nature and dynamics of spin-dependent charge carrier recombination in Tris(8-hydroxyquinolinato) aluminum (Alq$_3$) films in light emitting diodes at room temperature using continuous wave and pulsed electrically detected magnetic resonance (EDMR) spectroscopy. We found that the EDMR signal is dominated by an electron-hole recombination process, and another, weaker EDMR signal whose fundamental nature was investigated. From the pulsed EDMR measurements we obtained a carrier spin relaxation time, $T_2 = 45pm 25$ ns which is much shorter than $T_2$ in conjugated polymers, but relatively long for a molecule containing elements with high atomic number. Using multi-frequency continuous wave EDMR spectroscopy, we obtained the local hyperfine field distributions for electrons and holes, as well as their respective spin-orbit coupling induced g-factor and g-strain values.
We present experiments to systematically study the time constants of spin-dependent recombination processes in semiconductors using pulsed electrically detected magnetic resonance (EDMR). The combination of time-programmed optical excitation and pulsed spin manipulation allows us to directly measure the recombination time constants of electrons via localized spin pairs and the time constant of spin pair formation as a function of the optical excitation intensity. Using electron nuclear double resonance, we show that the time constant of spin pair formation is determined by an electron capture process. Based on these time constants we devise a set of rate equations to calculate the current transient after a resonant microwave pulse and compare the results with experimental data. Finally, we critically discuss the effects of different boxcar integration time intervals typically used to analyze pulsed EDMR experiments on the determination of the time constants. The experiments are performed on phosphorus-doped silicon, where EDMR via spin pairs formed by phosphorus donors and Si/SiO2 interface dangling bond defects is detected.
Understanding how the orbital motion of electrons is coupled to the spin degree of freedom in nanoscale systems is central for applications in spin-based electronics and quantum computation. We demonstrate this coupling of spin and orbit in a carbon nanotube quantum dot in the general multi-electron regime in presence of finite disorder. Further, we find a strong systematic dependence of the spin-orbit coupling on the electron occupation of the quantum dot. This dependence, which even includes a sign change is not demonstrated in any other system and follows from the curvature-induced spin-orbit split Dirac-spectrum of the underlying graphene lattice. Our findings unambiguously show that the spin-orbit coupling is a general property of nanotube quantum dots which provide a unique platform for the study of spin-orbit effects and their applications.
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