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.     

Theoretical treatment of pulsed Overhauser dynamic nuclear polarization: Consideration of a general periodic pulse sequence

A general theoretical approach to pulsed Overhauser-type dynamic nuclear polarization (DNP) is presented. Dynamic nuclear polarization is a powerful method to create non-thermal polarization of nuclear spins, thereby enhancing their nuclear magnetic resonance signals. The theory presented can treat pulsed microwave irradiation of electron paramagnetic resonance transitions for periodic pulse sequences of general composition. Dynamic nuclear polarization enhancement is analyzed in detail as a function of the microwave pulse length for rectangular pulses and pulses with finite rise time. Characteristic oscillations of the DNP enhancement are found when the pulse-length is stepwise increased, originating from coherent motion of the electron spins driven by the pulses. Experimental low-field DNP data are in very good agreement with this theoretical approach.     

The theory of nuclear orientation via electron spin locking (NOVEL)

Nuclear orientation via electron spin locking (NOVEL) is a technique to orient nuclear spins embedded in a solid. Like other methods of dynamic nuclear polarization (DNP) it employs a small amount of unpaired electron spins and uses a microwave field to transfer the polarization of these unpaired electron spins to the nuclear spins. Traditional DNP uses CW microwave fields, but NOVEL uses pulsed electron spin resonance (ESR) techniques: a 90 degree pulse–90 degree phase shift–locking pulse sequence is applied and during the locking pulse the polarization transfer is assured by satisfying the Hartmann–Hahn condition. The transfer is coherent and similar to coherence transfer between nuclear spins. However, NOVEL requires an extension of the existing theory to many, inequivalent nuclear spins and to arbitrary, i.e. high electron and nuclear spin polarization. In this paper both extensions are presented. The theory is applied to the system naphthalene doped with pentacene, where the proton spins are polarized using the photo-excited triplet states of the pentacene molecules and found to show excellent agreement with the experimentally observed evolution of the polarization transfer during the locking pulse.     

Enhancement of efficiency in photo-excitation to the triplet state by laser-pulse reshaping

An optical system is proposed to enhance efficiency in photo-excitation to the triplet state by reshaping an original laser pulse into a train of pulses. This optical system can be used to improve the attainable nuclear spin polarization in dynamic nuclear polarization experiments using photo-excited triplet electron spins.     

Persistent narrowing of nuclear-spin fluctuations in InAs quantum dots using laser excitation

We demonstrate the suppression of nuclear-spin fluctuations in an InAs quantum dot and measure the timescales of the spin narrowing effect. By initializing for tens of milliseconds with two continuous wave diode lasers, fluctuations of the nuclear spins are suppressed via the hole-assisted dynamic nuclear polarization feedback mechanism. The fluctuation narrowed state persists in the dark (absent light illumination) for well over 1 s even in the presence of a varying electron charge and spin polarization. Enhancement of the electron spin coherence time (T2*) is directly measured using coherent dark state spectroscopy. By separating the calming of the nuclear spins in time from the spin qubit operations, this method is much simpler than the spin echo coherence recovery or dynamic decoupling schemes.     

Spin accumulation in forward-biased MnAs/GaAs Schottky diodes

We describe a new means for all-electrical generation of spin polarization in semiconductors. In contrast with spin injection of electrons by tunneling through a reverse-biased Schottky barrier, we observe accumulation at the metal-semiconductor interface of forward-biased ferromagnetic Schottky diodes, which is consistent with a theory of spin-dependent reflection off the interface. Spatiotemporal Kerr microscopy is used to image the electron spin and the resulting dynamic nuclear polarization that arises from the nonequilibrium carrier polarization.     

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.     

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.     

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.     

Scalable spin amplification with a gain over a hundred

We propose a scalable and practical implementation of spin amplification which does not require individual addressing nor a specially tailored spin network. We have demonstrated a gain of 140 in a solid-state nuclear spin system of which the spin polarization has been increased to 0.12 using dynamic nuclear polarization with photoexcited triplet electron spins. Spin amplification scalable to a higher gain opens the door to the single spin measurement for a readout of quantum computers as well as practical applications of nuclear magnetic resonance spectroscopy to infinitesimal samples which have been concealed by thermal noise.     

Dynamic Polarization and Relaxation of <Superscript>75</Superscript>As Nuclei in Silicon at High Magnetic Field and Low Temperature

We present the results of experiments on dynamic nuclear polarization and relaxation of ⁷⁵As in silicon crystals. Experiments are performed in strong magnetic fields of 4.6 T and temperatures below 1 K. At these conditions donor electron spins are fully polarized, and the allowed and forbidden electron spin resonance transitions are well resolved. We demonstrate effective nuclear polarization of ⁷⁵As nuclei via the Overhauser effect on the time scale of several hundred seconds. Excitation of the forbidden transitions leads to a polarization through the solid effect. The relaxation rate of donor nuclei has strong temperature dependence characteristic of Orbach process.     

Electron–Nuclear Spin Dynamics in Semiconductor QDs

This work presents an overview of investigations of the nuclear spin dynamics in nanostructures with negatively charged InGaAs/GaAs quantum dots characterized by strong quadrupole splitting of nuclear spin sublevels. The main method of the investigations is the experimental measurements and the theoretical analysis of the photoluminescence polarization as a function of the transverse magnetic field (effect Hanle). The dependence of the Hanle curve profile on the temporal protocol of optical excitation is examined. Experimental data are analyzed using an original approach based on separate consideration of behavior of the longitudinal and transverse components of the nuclear polarization. The rise and decay times of each component of the nuclear polarization and their dependence on transverse magnetic field strength are determined. To study the role of the Knight field in the dynamic of nuclear polarization, a weak additional magnetic field parallel to the optical axis is used. We have found that, only taking into account the nuclear spin fluctuations, we can accurately describe the measured Hanle curves and evaluate the parameters of the electron–nuclear spin system in the studied quantum dots. A new effect of the resonant optical pumping of nuclear spin polarization in an ensemble of the singly charged (In,Ga)As/GaAs quantum dots subjected to a transverse magnetic field is discussed. Nuclear spin resonances for all isotopes in the quantum dots are detected in that way. In particular, transitions between the states split off from the ±1/2 doublets by the nuclear quadrupole interaction are identified.     

Nonequilibrium nuclear-electron spin dynamics in semiconductor quantum dots

We study the spin dynamics in charged quantum dots in the situation where the resident electron is coupled to only about 200 nuclear spins and where the electron spin splitting induced by the Overhauser field does not exceed markedly the spectral broadening. The formation of a dynamical nuclear polarization as well as its subsequent decay by the dipole-dipole interaction is directly resolved in time. Because not limited by intrinsic nonlinearities, almost complete nuclear polarization is achieved, even at elevated temperatures. The data suggest a nonequilibrium mode of nuclear polarization, distinctly different from the spin temperature concept exploited on bulk semiconductors.     

Dynamic Nuclear Polarization in Solids: The Birth and Development of the Many-Particle Concept

A brief review is presented on historical aspects of the dynamic nuclear polarization (DNP) research in 1960–1970s of the last century. Much attention is given to development of the many-particle approach, from pioneering studies of the 3-spin electron–nuclear cross effect to development of spin-temperature concept and thermal mixing mechanism of DNP in solids. Applicability of different models to modern DNP data is briefly discussed.     

NMR probing of spin excitations in the ring structure of a two-subband system

Resistively detected nuclear magnetic resonance (NMR) is observed inside the ringlike structure, with a quantized Hall conductance of 6e(2)/h, in the phase diagram of a two-subband electron system. The NMR signal persists up to 470 mK and is absent in other states with the same quantized Hall conductance. The nuclear spin-lattice relaxation time T1, is found to decrease rapidly towards the ring center. A strong dynamic nuclear polarization by the biasing current has also been observed only inside the ring. These observations are consistent with the assertion of the ringlike region being a ferromagnetic state that is accompanied by collective spin excitations.     

Spin polarization of the neutral exciton in a single quantum dot

While efficient nuclear polarization has earlier been reported for the charged exciton in InAs/GaAs quantum dots at zero external magnetic field, we report here on a surprisingly high degree of circular polarization, up to ≈60%$\approx 60\%$, for the neutral exciton emission in individual InAs/GaAs dots. This high degree of polarization is explained in terms of the appearance of an effective nuclear magnetic field which stabilizes the electron spin. The nuclear polarization is manifested in experiments as a detectable Overhauser shift. In turn, the nuclei located inside the dot are exposed to an effective electron magnetic field, the Knight field. This nuclear polarization is understood as being due to the dynamical nuclear polarization by an electron localized in the QD. The high degree of polarization for the neutral exciton is also suggested to be due to separate in-time capture of electrons and holes into the QD.     

Observation of hysteretic transport due to dynamic nuclear spin polarization in a GaAs lateral double quantum dot

We report a new transport feature in a GaAs lateral double quantum dot that emerges for magnetic-field sweeps and shows hysteresis due to dynamic nuclear spin polarization (DNP). This DNP signal appears in the Coulomb blockade regime by virtue of the finite interdot tunnel coupling and originates from the crossing between ground levels of the spin triplet and singlet extensively used for nuclear spin manipulations in pulsed-gate experiments. The magnetic-field dependence of the current level is suggestive of unbalanced DNP between the two dots, which opens up the possibility of controlling electron and nuclear spin states via dc transport.     

电阻式核磁共振测量的最新进展

电阻式核磁共振(RDNMR)测量是1988年由德国马普所的von Klitzing研究小组针对GaAs二维电子气中少量核自旋的探测而提出的一种具有超高灵敏度的实验技术. 目前, RDNMR已经成为研究单层或双层GaAs二维电子气核自旋和电子自旋特性的重要手段. 由于为实现电阻式核磁共振测量所建立的动态核极化方法强烈依赖于GaAs特有的材料属性, 至今这一技术一直没有扩展应用到其他半导体低维系统中. 最近,本研究小组发展了一种动态核极化新方法,成功实现了对典型窄带半导体锑化铟(InSb) 二维电子气的电阻式核磁共振测量.本文在介绍电阻式核磁共振测量工作原理及已建立的典型动态核极化方法的基础上,着重讨论所提出的动态核极化新方法的机理、 实验结果以及对今后研究的展望.