Gate control of dynamic nuclear polarization in GaAs quantum wells

Gate control of dynamic nuclear polarization under optical orientation is demonstrated in a Schottky-gated n-GaAs/AlGaAs (110) quantum well by time-resolved Kerr rotation measurements. Spin relaxation of electrons due to mechanisms other than the hyperfine interaction is effectively suppressed as the donor induced background electron density is reduced from metallic to insulating regimes. Subsequent accumulation of photoexcited electron spins dramatically enhances dynamic nuclear polarization at low magnetic field, allowing us to tune nuclear spin polarization by external gate voltages.     

Dynamic Nuclear Polarization in III–V Semiconductors

We report on electron spin resonance, nuclear magnetic resonance and Overhauser shift experiments on two of the most commonly used III–V semiconductors, GaAs and InP. Localized electron centers in these semiconductors have extended wavefunctions and exhibit strong electron–nuclear hyperfine coupling with the nuclei in their vicinity. These interactions not only play a critical role in electron and nuclear spin relaxation mechanisms, but also result in transfer of spin polarization from the electron spin system to the nuclear spin system. This transfer of polarization, known as dynamic nuclear polarization (DNP), may result in an enhancement of the nuclear spin polarization by several orders of magnitude under suitable conditions. We determine the critical range of doping concentration and temperature conducive to DNP effects by studying these semiconductors with varying doping concentration in a wide temperature range. We show that the electron spin system in undoped InP exhibits electric current-induced spin polarization. This is consistent with model predictions in zinc-blende semiconductors with strong spin–orbit effects.     

Optical orientation of nuclei in nitrogen alloys GaAsN at room temperature

The intensity and giant circular polarization of edge luminescence in a longitudinal magnetic field have been measured in nitrogen alloys GaAsN under circularly polarized pumping. It has been found that these dependences are shifted with respect to zero field by a value B _eff. The magnitude of the internal field B _eff increases with the pumping intensity and reaches saturation (≈250 G) at large excitation densities. The saturation of the B _eff field with growth of pumping indicates that this is a field of nuclei, polarized dynamically due to hyperfine interaction with optically oriented deep paramagnetic centers, rather than a field of exchange interaction created on the center by spin-polarized photo-excited conduction electrons. The short time of nuclear polarization by electrons (<15 μs), measured under modulation of circular polarization of the exciting light with high frequency, points to a small number of nuclei undergoing hyperfine interaction with an electron localized at a center.     

Effect of the nuclear hyperfine field on the 2D electron conductivity in the quantum Hall regime

The effect of the nuclear hyperfine interaction on the dc conductivity of 2D electrons under quantum Hall effect conditions at filling factor ν=1 is observed for the first time. The local hyperfine field enhanced by dynamic nuclear polarization is monitored via the Overhauser shift of the 2D conduction electron spin resonance in AlGaAs/GaAs multiquantum-well samples. The experimentally observed change in the dc conductivity resulting from dynamic nuclear polarization is in agreement with a thermal activation model incorporating the Zeeman energy change due to the hyperfine interaction. The relaxation decay time of the dc conductivity is, within experimental error, the same as the relaxation time of the nuclear spin polarization determined from the Overhauser shift. These findings unequivocally establish the nuclear spin origins of the observed conductivity change. Pis’ma Zh. éksp. Teor. Fiz. 69, No. 1, 58–63 (10 January 1999) Published in English in the original Russian journal. Edited by Steve Torstveit.     

Analysis of correlation patterns in hyperfine sublevel correlation spectroscopy of<Emphasis Type="Italic">S</Emphasis>=1/2,<Emphasis Type="Italic">I</Emphasis>=3/2 systems

The properties of two-dimensional four-pulse electron spin echo envelope modulation spectra of nuclei with nuclear spinI=3/2 in disordered systems are discussed by means of calculated lithium hyperfine sublevel correlation spectra. Since a case of small coupling is treated, the multifrequency transition components appear only in the first quadrant of the two-dimensional spectra. The influence of the hyperfine and nuclear quadrupole interaction parameters on the cross peak ridges in the two-dimensional powder pattern is analyzed. Furthermore the possibility to determine the magnitude of the dipolar hyperfine and the nuclear quadrupole coupling from the cross peak line shapes is investigated. In this context the potential of those spectral features representing the so-called multiquantum transitions for the interpretation of the spectra is demonstrated.     

Theoretical aspects of dynamic nuclear polarization in the solid state - the solid effect

Dynamic nuclear polarization has gained high popularity in recent years, due to advances in the experimental aspects of this methodology for increasing the NMR and MRI signals of relevant chemical and biological compounds. The DNP mechanism relies on the microwave (MW) irradiation induced polarization transfer from unpaired electrons to the nuclei in a sample. In this publication we present nuclear polarization enhancements of model systems in the solid state at high magnetic fields. These results were obtained by numerical calculations based on the spin density operator formalism. Here we restrict ourselves to samples with low electron concentrations, where the dipolar electron-electron interactions can be ignored. Thus the DNP enhancement of the polarizations of the nuclei close to the electrons is described by the Solid Effect mechanism. Our numerical results demonstrate the dependence of the polarization enhancement on the MW irradiation power and frequency, the hyperfine and nuclear dipole-dipole spin interactions, and the relaxation parameters of the system. The largest spin system considered in this study contains one electron and eight nuclei. In particular, we discuss the influence of the nuclear concentration and relaxation on the polarization of the core nuclei, which are coupled to an electron, and are responsible for the transfer of polarization to the bulk nuclei in the sample via spin diffusion.     

Study of natural diamonds by dynamic nuclear polarization-enhanced C nuclear magnetic resonance spectroscopy

The results of a study of two types of natural-diamond crystals by dynamic nuclear polarization (DNP)-enhanced high-resolution solid-state ¹³C nuclear magnetic resonance (NMR) are reported. The home-built DNP magic-angle spinning (MAS) ¹³C NMR spectrometer operates at 54 GHz for electrons and 20.2 MHz for carbons. The power of the microwave source was about 30 W and the highest DNP enhancement factor came near to 10³. It was shown that in the MAS spectra the ¹³C NMR linewidths of the I_b-type diamond were broader than those of I_aB3-type diamond. From the hyperfine structure of the DNP enhancement as a function of frequency, four kinds of nitrogen-centred and one kind of carbon-centred free radicals could be identified in the I_b-type diamond. The hyperfine structures of the DNP enhancement curve that originated from the anisotropic hyperfine interaction between electron and nuclei could be partially averaged out by MAS. The ¹³C polarization time of DNP was rather long, i.e. 1500 s, and the spin—lattice relaxation time (without microwave irradiation) was about 300 s, which was somewhat shorter than anticipated. Discussions on these experimental results have been made in this report.     

Electron paramagnetic resonance study of the nuclear spin dynamics in an AlAs quantum well

The nuclear spin dynamics in an asymmetrically doped 16-nm AlAs quantum well grown along the [001] direction has been studied experimentally using the time decay of the Overhauser shift of paramagnetic resonance of conduction electrons. The nonzero spin polarization of nuclei causing the initial observed Overhauser shift is due the relaxation of the nonequilibrium spin polarization of electrons into the nuclear subsystem near electron paramagnetic resonance owing to the hyperfine interaction. The measured relaxation time of nuclear spins near the unity filling factor is (530 ± 30) min at the temperature T = 0.5 K. This value exceeds the characteristic spin relaxation times of nuclei in GaAs/AlGaAs heterostructures by more than an order of magnitude. This fact indicates the decrease in the strength of the hyperfine interaction in the AlAs quantum well in comparison with GaAs/AlGaAs heterostructures.     

Overhauser effect of 67Zn nuclear spins in ZnO via cross relaxation induced by the zero-point fluctuations of the phonon field

Hole burning in and displacements of the magnetic-resonance absorption line of the electron spin of the shallow hydrogen-related donor in ZnO are observed upon resonant irradiation with microwaves at 275 GHz and at 4.5 K in a magnetic field of 10 T. These effects arise from an almost complete polarization of the many 67Zn (I=5/2) nuclear spins that have an isotropic hyperfine interaction with the electron spin of the shallow donor. It is proposed that this huge dynamic nuclear polarization is caused by a spontaneous-emission-type cross relaxation in the coupled electron-spin nuclear-spin system induced by the zero-point fluctuations of the phonon field.     

Electron spin-echo envelope modulation at S-band. 3: Analysis of nuclear quadrupole interaction effects

In the present paper the nuclear modulation of electron spin echo signals at S-band is investigated in the case of interacting nuclei with a quadrupole moment high enough to cause nuclear quadrupole couplings not negligible with respect to the nuclear Zeeman and dipolar hyperfine couplings. Both the two-pulse and three-pulse electron spin echo envelope modulation (ESEEM) due to²⁷Al and¹⁴N are simulated at different values of the nuclear quadrupole coupling by numerical diagonalization of the nuclear Hamiltonians. The behavior of their amplitude and periods is discussed on the basis of the ratios between the strengths of the nuclear quadrupole interaction and the nuclear Zeeman and the dipolar hyperfine interactions. The interpretation of their trends in terms of the eigenfunctions and eigenvectors of the nuclear Hamiltonians is carried out by using analytical equations obtained by perturbation approaches. First order perturbation treatments for integer and half-integer nuclear spin quantum numbers are developed when the nuclear quadrupole coupling is the main interaction. A discussion on the limits of the interpretation based on the perturbation approach is also given by comparing the magnitude Fourier transform of the patterns calculated by exact diagonalization and analytical equations.     

Electron-nuclear cross polarization

We describe the coherent polarization transfer from an unpaired electron to neighboring nuclei via electron-nuclear cross polarization (eNCP) in a doubly, tilted rotating frame. Although the experiment superficially resembles the well-known Hartmann-Hahn cross polarization (CP) process introduced by Pines et al., that is widely used in solid-state nuclear magnetic resonance (SSNMR), it differs in significant respects. In particular, eNCP requires an alternative treatment due to the very different sizes of the specific terms in the spin Hamiltonian. We derive analytical expressions for the matching condition for optimal polarization transfer and verify their correctness with experimental results obtained with electron detected CP experiments performed on powder samples of BDPA radical dispersed in a protonated polystyrene matrix and with numerical simulations. We use fully protonated BDPA as an example of polarization transfer to strongly coupled nuclei. In contrast, perdeuterated BDPA serves as an example of the transfer of polarization from electrons to weakly coupled nuclei. In addition, we performed CP on a paramagnetic crystal to determine the influence of resolved hyperfine structure on the CP process. It is shown that almost no structure is observed in the corresponding electron-(1)H CP matching curve. It appears that only a restricted number of hyperfine coupled (1)H's contribute to the observed signal intensities in the CP experiment.     

Measurement of a heavy-hole hyperfine interaction in InGaAs quantum dots using resonance fluorescence

We measure the strength and the sign of hyperfine interaction of a heavy hole with nuclear spins in single self-assembled quantum dots. Our experiments utilize the locking of a quantum dot resonance to an incident laser frequency to generate nuclear spin polarization. By monitoring the resulting Overhauser shift of optical transitions that are split either by electron or exciton Zeeman energy with respect to the locked transition using resonance fluorescence, we find that the ratio of the heavy-hole and electron hyperfine interactions is -0.09 ± 0.02 in three quantum dots. Since hyperfine interactions constitute the principal decoherence source for spin qubits, we expect our results to be important for efforts aimed at using heavy-hole spins in quantum information processing.     

Stabilization of the electron-nuclear spin orientation in quantum dots by the nuclear quadrupole interaction

The nuclear quadrupole interaction eliminates the restrictions imposed by hyperfine interaction on the spin coherence of an electron and nuclei in a quantum dot. The strain-induced nuclear quadrupole interaction suppresses the nuclear spin flip and makes possible the zero-field dynamic nuclear polarization in self-organized InP/InGaP quantum dots. The direction of the effective nuclear magnetic field is fixed in space, thus quenching the magnetic depolarization of the electron spin in the quantum dot. The quadrupole interaction suppresses the zero-field electron spin decoherence also for the case of nonpolarized nuclei. These results provide a new vision of the role of the nuclear quadrupole interaction in nanostructures: it elongates the spin memory of the electron-nuclear system.     

Electron nuclear quadruple resonance for assignment of overlapping spectra

Multiple resonance methods are important tools in EPR for revealing the network of hyperfine levels of free radicals and paramagnetic centers. The variations of electron nuclear double resonance (ENDOR) or electron spin-echo envelope modulation (ESEEM) techniques help to correlate nuclear frequencies with each other. These methods have limited utility when there is extensive overlap or suspected overlap in the EPR spectrum between different species or different orientations. In the ENDOR spectrum, overlap and second-order shifts of lines also leads to ambiguity in assignment and interpretation. A new electron nuclear multiple resonance method is presented here that is based on population transfer ENDOR. It is a quadruple resonance method that correlates ENDOR lines and reveals the network of hyperfine levels in samples with unoriented paramagnetic species and in samples with overlapping EPR or ENDOR lines.     

Monolayer resolved oscillating hyperfine fields in epitaxial face-centered-tetragonal Co(001) films

Ultrahigh-quality thin fct-Co films grown on Cu(001) have been investigated by 59Co nuclear magnetic resonance. The influence of the spin-dependent electron scattering at the interfaces is observed for at least four Co atomic layers from the interface with monolayer resolution. An oscillatory effect on the Co hyperfine field with a period of several monolayers is measured, corresponding to the oscillating conduction electron polarization. The observation is exclusively possible in this system due to its very narrow resonance lines, corresponding to a virtually perfect Co structure.     

Influence of the anisotropic hyperfine interaction on the 14N ENDOR and the ESEEM orientation-disordered spectra

The influence of the anisotropic hyperfine interaction on the 14N electron-nuclear double resonance/electron spin echo envelope modulation spectra is studied by approximate analytical and graphical methods for the case of the isotropic g-factor. The suggested determination of the modified characteristic directions of the magnetic field due to anisotropy enhances the insight in the structural details of the system and analytical solutions of the secular equation for these conditions are derived. The graphical method, previously used for the analysis of the orientation dependence of the 14N nuclear-transition frequencies in orientation-disordered samples for isotropic hyperfine interaction is extended to the case of arbitrary anisotropic hyperfine tensor. The above analytical and graphical methods are illustrated and tested against exact simulations in two practically important cases: (i) isotropic hyperfine interaction (hfi) exceeding other nuclear interactions in nuclear spin Hamiltonian. (ii) Cancellation of the isotropic part of the hfi.     

Subsecond spin relaxation times in quantum dots at zero applied magnetic field due to a strong electron-nuclear interaction

A key to ultralong electron spin memory in quantum dots (QDs) at zero magnetic field is the polarization of the nuclei, such that the electron spin is stabilized along the average nuclear magnetic field. We demonstrate that spin-polarized electrons in n-doped (In,Ga)As/GaAs QDs align the nuclear field via the hyperfine interaction. A feedback onto the electrons occurs, leading to stabilization of their polarization due to formation of a nuclear spin polaron [I. A. Merkulov, Phys. Solid State 40, 930 (1998)]. Spin depolarization of both systems is consequently greatly reduced, and spin memory of the coupled electron-nuclear spin system is retained over 0.3 sec at temperature of 2 K.     

Nuclear polarization in muonic atoms of deformed nuclei

The treatment of nuclear polarization correction in muonic atoms belonging to deformed nuclei is analyzed. The geometrical factors involved are expanded into a series of multipoles and the exact expansion coefficients are calculated. It is shown that, using reasonable assumptions about the nuclear spectrum, the nuclear polarization correction may be expressed as a shift of all hyperfine components plus a renormalization of the even multipole hyperfine interaction constants. All nuclear excited states contribute to the shift, but the ground-state rotational band gives an over-whelming contribution to the multipole moment renormalization. The effect of the ground-state band is analyzed in detail. The radial coefficients are calculated and an approximate formula, applicable over a broad range of atomic numbers and deformations, is obtained. By comparing our results with exact calculations we conclude that this part of the nuclear polarization correction may be calculated with accuracy better than 10 %.     

Direct measurement of the hole-nuclear spin interaction in single InP/GaInP quantum dots using photoluminescence spectroscopy

We measure the hyperfine interaction of the valence band hole with nuclear spins in single InP/GaInP semiconductor quantum dots. Detection of photoluminescence (PL) of both "bright" and "dark" excitons enables direct measurement of the Overhauser shift of states with the same electron but opposite hole spin projections. We find that the hole hyperfine constant is ≈11% of that of the electron and has the opposite sign. By measuring the degree of circular polarization of the PL, an upper limit to the contribution of the heavy-light hole mixing to the measured value of the hole hyperfine constant is deduced. Our results imply that environment-independent hole spins are not realizable in III-V semiconductor, a result important for solid-state quantum information processing using hole spin qubits.     

Comparison of electron spin relaxation times measured by Carr-Purcell-Meiboom-Gill and two-pulse spin-echo sequences

Electron spin relaxation times obtained by two-pulse spin-echo and Carr-Purcell-Meiboom-Gill (CPMG) experiments were compared for samples with: (i) low concentrations of nuclear spins, (ii) higher concentrations of nuclear spins and low concentrations of unpaired electrons, (iii) higher concentrations of nuclear spins and of electron spins, and (iv) dynamic averaging of inequivalent hyperfine couplings on the EPR timescale. In each case, the CPMG time constant decreased as the time between the refocusing pulses increased. For the samples with low concentrations of nuclear spins (the E' center in irradiated amorphous SiO2) the limiting value of the CPMG time constant at short interpulse spacings was similar to the Tm obtained by two-pulse spin echo at small turning angle. For the other samples, the time constants obtained by CPMG at short interpulse spacings were systematically longer than Tm obtained by two-pulse spin echo. For most of the samples, the CPMG time constant decreased with increasing electron spin concentration, which is consistent with the expectation that the CPMG sequence does not refocus dephasing due to electron-electron dipolar interaction between resonant spins. Dynamic processes that average inequivalent hyperfine couplings contributed less to the CPMG time constant than to the spin-echo decay time constant. The impact of nuclear echo envelope modulation on CPMG time constants also was examined. For a Nycomed trityl radical in glassy D2O:glycerol-d8 solution, the CPMG time constant was up to 20 times longer when the time between pulses was approximately equal to integer multiples of the reciprocal of the deuterium Larmor frequency than when the time between pulses was an odd multiple of half the reciprocal of the deuterium Larmor frequency.