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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.
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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.
Electrically detected magnetic resonance is used to identify recombination centers in a set of Czochralski grown silicon samples processed to contain strained oxide precipitates with a wide range of densities (~ 1e9 cm-3 to ~ 7e10 cm-3). Measurements reveal that photo-excited charge carriers recombine through Pb0 and Pb1 dangling bonds and comparison to precipitate-free material indicates that these are present at both the sample surface and the oxide precipitates. The electronic recombination rates vary approximately linearly with precipitate density. Additional resonance lines arising from iron-boron and interstitial iron are observed and discussed. Our observations are inconsistent with bolometric heating and interpreted in terms of spin-dependent recombination. Electrically detected magnetic resonance is thus a very powerful and sensitive spectroscopic technique to selectively probe recombination centers in modern photovoltaic device materials.
We report on the use of the LaAlO3 (LAO) high-k dielectric as a tunnel barrier in magnetic tunnel junctions. From tunnel magnetoresistance (TMR) measurements on epitaxial La2/3Sr1/3MnO3/LAO/La2/3Sr1/3MnO3 junctions, we estimate a spin polarization of 77% at low temperature for the La2/3Sr1/3MnO3/LAO interface. Remarkably, the TMR of La2/3Sr1/3MnO3/LAO/Co junctions at low bias is negative, evidencing a negative spin polarization of Co at the interface with LAO, and its bias dependence is very similar to that of La2/3Sr1/3MnO3/STO/Co junctions. We discuss possible reasons for this behaviour.
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 theoretically investigate a manipulation method of nonequilibrium spin accumulation in the paramagnetic normal metal of a spin pumping system, by using the spin precession motion combined with the spin diffusion transport. We demonstrate based on the Bloch-Torrey equation that the direction of the nonequilibrium spin accumulation is changed by applying an additional external magnetic field, and consequently, the inverse spin Hall voltage in an adjacent paramagnetic heavy metal changes its sign. We find that the spin relaxation time and the spin diffusion length are simultaneously determined by changing the magnitude of the external magnetic field and the thickness of the normal metal in a commonly-used spin pumping system.
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