Nuclear Spin Dynamics Research Articles

Nuclear spin dynamics in [001] AlAs quantum well in the regime of integer and fractional quantum Hall effect

Relaxation of nuclear spins located in the vicinity of 2D electron system confined in a 16 nm [001] AlAs/AlGaAs quantum well was studied with the aid of electron spin resonance (ESR) in the regime of integer and fractional quantum Hall effect. Nuclear spin-lattice relaxation time τ was measured from the time decay of the Overhauser shift near different filling factors of the electron system. The resultant dependence of τ on filling factor turned out to be nontrivial. At the temperature 1.5 K τ reached its maximal value at the exact filling ν = 1 and decreased when ν was altered, yet this maximum vanished when the system was cooled down to 0.5 K. The fractional quantum Hall effect state at the filling of 2∕3 was formed at the temperature of 0.5 K, and the development of this state was accompanied by the slowing of the nuclear spin relaxation. This observation suggests the enhancement of energy gap in the spin excitation spectrum of two-dimensional electrons at 2/3 state.

Hybrid quantum-classical method for simulating high-temperature dynamics of nuclear spins in solids

First-principles calculations of high-temperature spin dynamics in solids in the context of nuclear magnetic resonance (NMR) is a long-standing problem, whose conclusive solution can significantly advance the applications of NMR as a diagnostic tool for material properties. In this work, we propose a new hybrid quantum-classical method for computing NMR free induction decay(FID) for spin $1/2$ lattices. The method is based on the simulations of a finite cluster of spins $1/2$ coupled to an environment of interacting classical spins via a correlation-preserving scheme. Such simulations are shown to lead to accurate FID predictions for one-, two- and three-dimensional lattices with a broad variety of interactions. The accuracy of these predictions can be efficiently estimated by varying the size of quantum clusters used in the simulations.

Spin pumping from nuclear spin waves

Various spintronic phenomena originate from the exchange of angular momentum between the spin of electrons and other degrees of freedom in crystalline materials. Many degrees of freedom, such as magnetization1 and mechanical motion2, have already been united into this exchange framework. However, the nuclear spin—a key angular momentum—has yet to be incorporated. Here we observe spin pumping from nuclear magnetic resonance (NMR), in which nuclear spin dynamics emits a spin current, a flow of spin angular momentum of electrons. By using the canted antiferromagnet MnCO3, in which typical nuclear spin-wave formation is established due to the reinforced hyperfine coupling, we find that a spin current is generated from an NMR. Nuclear spins are indispensable for quantum information technology3 and are also frequently used in various sensors, such as in magnetic resonance imaging4. The observed NMR spin pumping allows spin-current generation from nuclei and will enable spintronic detection of nuclear spin states. Spin current is generated by pumping from nuclear spin waves. The nuclear magnetic resonance is used to transfer angular momentum from the nuclei of an antiferromagnet to a propagating spin current that is subsequently collected in a distant electrode.

The Ortho-to-para Ratio of Water Molecules Desorbed from Ice Made from Para-water Monomers at 11 K

Abstract Water has two nuclear-spin isomers: ortho- and para-H2O. Some observations of interstellar space and cometary comae have reported the existence of gaseous H2O molecules with anomalous ortho-to-para ratios (OPRs) less than the statistical value of three. This has been often used to estimate the formation temperature of ice on dust, which is inferred to be below 50 K. The relation between the nuclear-spin dynamics of H2O in ice at low temperatures and the OPR of gaseous H2O desorbed from the ice has yet to be explored in a laboratory. Consequently, the true meaning of the observed OPRs remains debated. We measure the OPR of H2O photodesorbed from ice made from para-H2O monomers at 11 K, which was prepared by the sublimation of Ne from a para-H2O/Ne matrix. The photodesorbed H2O molecules from the ice have the statistical OPR value of three, demonstrating the immediate nuclear-spin-state mixing of H2O toward the statistical value of ice even at 11 K. The OPR of H2O thermally desorbed from the ice also shows the expected statistical value. Our results indicate that the OPR of H2O desorbed from interstellar ice should be the statistical value regardless of the formation process of the ice, which cannot be used to deduce the ice-formation temperature. This study highlights the importance of interstellar gas-phase processes in understanding anomalous abundance ratios of nuclear-spin isomers of molecules in space.

Electrically tunable dynamic nuclear spin polarization in GaAs quantum dots at zero magnetic field

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 are 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 Vg. Variation of ΔVg on the order of 100 mV changes the Overhauser splitting (nuclear spin polarization) from −30 μeV (−22%) to +10 μeV (+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 on the order of hundreds of ps. Voltage control of DNP is further confirmed in Hanle experiments.

New research progress of nuclear magnetic resonance quantum information processing

In the last 20 years, there have been lots of novel developments and remarkable achievements in quantum information processing theoretically and experimentally. Among them, the coherent control of nuclear spin dynamics is a powerful tool for the experimental implementation of quantum schemes in liquid and solid nuclear magnetic resonance (NMR) system, especially in liquid-state NMR. Compared with other quantum information processing systems, NMR platform has many advantages such as the long coherence time, the precise manipulation and well-developed quantum control techniques, which make it possible to accurately control a quantum system with up to 12-qubits. Extensive applications of liquid-state NMR spectroscopy in quantum information processing such as quantum communication, quantum computing and quantum simulation have been thoroughly studied over half a century. There are also many outstanding researches in the recent several years. So we focus on the recent researches in this review article. First, we introduce the basic principle of the liquid-state NMR quantum computing and two new methods reported in the pseudo-pure state preparation which has more advantages than the traditional methods. The quantum noise-injection methods and the quantum tomography technology in liquid-state NMR are also mentioned. Then we overview Horrow-Hassidim-Lioyd algorithm, quantum support vector machine algorithm, duality quantum computing and their implementations in liquid-state NMR system. Also, we report recent researches about quantum simulations, including quantum tunneling, high-energy physics and topological sequences. Then we display the quantum cloud platform of our group. In order to let more people, either amateurs or professionals, embrace and more importantly participate in the tidal wave of quantum science, we launch our NMR quantum cloud computing (NMRCloudQ) service. Through NMRCloudQ, we offer a direct access to a real, physical spectrometer in our laboratory and encourage users to explore quantum phenomena and demonstrate quantum algorithms. Finally, we discuss the development prospects and development bottlenecks of NMR, and point out the prospects for the future development direction.

Systematic investigations of transient response of nuclear spins in the presence of polarized electrons

We electrically probed the transient response of nuclear spins in an $n$-GaAs channel by performing Hanle signal and spin-valve signal measurements on an all-electrical spin-injection device having a half-metallic spin source of $\mathrm{C}{\mathrm{o}}_{2}\mathrm{MnSi}$. Furthermore, we simulated the Hanle and spin-valve signals by using the time evolution of nuclear-spin polarization under the presence of polarized electron spins by taking both ${T}_{1\mathrm{e}}$ and ${T}_{1}$ into consideration, where ${T}_{1\mathrm{e}}^{\ensuremath{-}1}$ is the polarization rate of nuclear spins through the transfer of angular momentum from polarized electron spins and ${T}_{1}^{\ensuremath{-}1}$ is the depolarization rate of nuclear spins through the interaction with the lattice. The simulation results reproduced our experimental results on all the nuclear-spin-related phenomena appearing in the Hanle and spin-valve signals at different measurement conditions, providing quantitative explanation for the transient response of nuclear spins in GaAs to a change in magnetic fields and an estimate of the time scales of ${T}_{1\mathrm{e}}$ and ${T}_{1}$. These experimental and simulated results will deepen the understanding of nuclear-spin dynamics in semiconductors.

Interplay of valley polarization and dynamic nuclear polarization in 2D transition metal dichalcogenides

The interplay of Ising spin-orbit coupling and non-trivial band topology in transition metal dichalcogenides (TMDs) produces anomalous transport and optical properties that are very different from a regular 2D electron gas. The spin-momentum locking of optically excited carriers near a valley point can give rise to an anomalous spin-valley Hall current under the application of an in-plane electric field. TMDs also exhibit strong electron-nuclear hyperfine interactions, but their effect on spin-valley-locked currents remains unknown. Here, we show that hyperfine interactions can create a feedback mechanism in which spin-valley currents generate significant dynamical nuclear polarization which in turn Zeeman shifts excitonic transitions out of resonance with an optical driving field, saturating the production of spin-valley polarization. We propose an experimental signature of dynamic nuclear polarization which can be detected via measurements of the anomalous Hall current. Our results help to elucidate the interplay of valley polarization and nuclear spin dynamics in TMDs.

Effects of Cd vacancies and unconventional spin dynamics in the Dirac semimetal Cd3As2.

Cd3As2 is a Dirac semimetal that is a 3D analog of graphene. We investigated the local structure and nuclear-spin dynamics in Cd3As2 via 113Cd NMR. The wideline spectrum of the static sample at 295 K is asymmetric and its features are well described by a two-site model with the shielding parameters extracted via Herzfeld-Berger analysis of the magic-angle spinning spectrum. Surprisingly, the 113Cd spin-lattice relaxation time (T1) is extremely long (T1 = 95 s at 295 K), in stark contrast to conductors and the effects of native defects upon semiconductors; but it is similar to that of 13C in graphene (T1 = 110 s). The temperature dependence of 1/T1 revealed a complex bipartite mechanism that included a T2 power-law behavior below 330 K and a thermally activated process above 330 K. In the high-temperature regime, the Arrhenius behavior is consistent with a field-dependent Cd atomic hopping relaxation process. At low temperatures, a T2 behavior consistent with a spin-1/2 Raman-like process provides evidence of a time-dependent spin-rotation magnetic field caused by angular oscillations of internuclear vectors due to lattice vibrations. The observed mechanism does not conform to the conventional two-band model of semimetals, but is instead closer to a mechanism observed in high-Z element ionic solids with large magnetorotation constant [A. J. Vega et al., Phys. Rev. B 74, 214420 (2006)].

Quantum dynamics of nuclear spins and spin relaxation in organic semiconductors

We investigate the role of the nuclear spin quantum dynamics in hyperfine-induced spin relaxation of hopping carriers in organic semiconductors. The fast hopping regime with a small carrier spin precession during a waiting time between hops is typical for organic semiconductors possessing long spin coherence times. We consider this regime and focus on a carrier random walk diffusion in one dimension, where the effect of the nuclear spin dynamics is expected to be the strongest. Exact numerical simulations of spin systems with up to 25 nuclear spins are performed using the Suzuki-Trotter decomposition of evolution operator. Larger nuclear spin systems are modeled utilizing the spin-coherent state $P$-representation approach developed earlier. We find that the nuclear spin dynamics strongly influences the carrier spin relaxation at long times. If the random walk is restricted to a small area, it leads to the quenching of carrier spin polarization at a non-zero value at long times. If the random walk is unrestricted, the carrier spin polarization acquires a long-time tail, decaying as $ 1/\sqrt{t}$. Based on the numerical results, we devise a simple formula describing the effect quantitatively.

Nuclear spin relaxation inn-GaAs: From insulating to metallic regime

Nuclear spin relaxation is studied in n-GaAs thick layers and microcavity samples with different electron densities. We reveal that both in metallic samples where electrons are free and mobile, and in insulating samples, where electrons are localized, nuclear spin relaxation is strongly enhanced at low magnetic field. The origin of this effect could reside in the quadrupole interaction between nuclei and fluctuating electron charges, that has been proposed to drive nuclear spin dynamics at low magnetic fields in the insulating samples. The characteristic values of these magnetic fields are given by dipole-dipole interaction between nuclei in bulk samples, and are greatly enhanced in microcavities, presumably due to additional strain, inherent to micro and nanostructures.

Landauer-Büttiker approach for hyperfine mediated electronic transport in the integer quantum Hall regime

The interplay of spin-polarized electronic edge states with the dynamics of the host nuclei in quantum Hall systems presents rich and non-trivial transport physics. Here, we develop a Landauer-B\"uttiker approach to understand various experimental features observed in the integer quantum Hall set ups featuring quantum point contacts. The approach developed here entails a phenomenological description of spin resolved inter-edge scattering induced via hyperfine assisted electron-nuclear spin flip-flop processes. A self-consistent simulation framework between the nuclear spin dynamics and edge state electronic transport is presented in order to gain crucial insights into the dynamic nuclear polarization effects on electronic transport and in turn the electron-spin polarization effects on the nuclear spin dynamics. In particular, we show that the hysteresis noted experimentally in the conductance-voltage trace as well as in the resistively detected NMR lineshape results from a lack of quasi-equilibrium between electronic transport and nuclear polarization evolution. In addition, we present circuit models to emulate such hyperfine mediated transport effects to further facilitate a clear understanding of the electronic transport processes occurring around the quantum point contact. Finally, we extend our model to account for the effects of quadrupolar splitting of nuclear levels and also depict the electronic transport signatures that arise from single and multi-photon processes.

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.

Introduction to average Hamiltonian theory. I. Basics

AbstractUnderstanding the dynamics of electron or nuclear spins during a magnetic resonance experiment requires to solve the Schrödinger equation for the spin system considering all contributions to the Hamiltonian from interactions of the spins with each other and their surroundings. In general, this is a difficult task as these interaction terms can be both time‐dependent and might not commute with each other. A powerful tool to analytically approximate the time evolution is average Hamiltonian theory, in which a time‐independent effective Hamiltonian is taking the place of the time‐dependent Hamiltonian. The effective Hamiltonian is subjected to the Magnus expansion, allowing to calculate the effective Hamiltonian to a certain order. The goal of this paper is to introduce average Hamiltonian theory in a rigorous but educational manner. The application to two composite pulses in NMR spectroscopy is used to demonstrate important aspects of average Hamiltonian theory.

Quadrupolar and anisotropy effects on dephasing in two-electron spin qubits in GaAs.

Understanding the decoherence of electron spins in semiconductors due to their interaction with nuclear spins is of fundamental interest as they realize the central spin model and of practical importance for using them as qubits. Interesting effects arise from the quadrupolar interaction of nuclear spins with electric field gradients, which have been shown to suppress diffusive nuclear spin dynamics and might thus enhance electron spin coherence. Here we show experimentally that for gate-defined GaAs quantum dots, quadrupolar broadening of the nuclear Larmor precession reduces electron spin coherence by causing faster decorrelation of transverse nuclear fields. However, this effect disappears for appropriate field directions. Furthermore, we observe an additional modulation of coherence attributed to an anisotropic electronic g-tensor. These results complete our understanding of dephasing in gated quantum dots and point to mitigation strategies. They may also help to unravel unexplained behaviour in self-assembled quantum dots and III–V nanowires.

Control of the nuclear spin of the 129Xe and 131Xe isotopes in the spin-exchange interaction with 87Rb atoms

Nuclear spin dynamics of the 129Xe and 131Xe isotopes in an external magnetic field B0 is considered. Nuclear spin is pumped by the laser through 87Rb, which transfers the electron spin to the 129Xe and 131Xe nuclei in the spin-exchange interaction. The nuclear spin dynamics is controlled with a transverse magnetic field that causes nuclear magnetic resonance in both 129Xe and 131Xe isotopes. Numerical calculations are performed to find conditions at which the transverse component of the nuclear spin in the established motion is of maximum and the slope angle relative to the vector of the constant magnetic field B0 is 45°. This regime is taken to be optimal for simulation of practical applications. It is also found that the pump of the nuclear spin of xenon is strongly attenuated when the rubidium polarization vector is turned to the plane perpendicular to the external magnetic field vector B0.

Transient analysis of oblique Hanle signals observed in GaAs

A transient response of nuclear spins in GaAs to a change in a magnetic field was analyzed based on the time evolution of nuclear spin temperature. Simulation results well reproduced our experimental results on transient oblique Hanle signals observed in an all-electrical spin injection device, enabling a quantitative understanding of nuclear spin dynamics in the presence of a hyperfine interaction between nuclei and polarized electrons. Analysis regarding the time evolution of nuclear spin temperature revealed that the hysteretic nature of a nuclear field with respect to the sweep direction of an external field was caused by the delay of time response of nuclear spin temperature to a change in the magnetic field. This analysis provides a deep understanding of nuclear spin dynamics in semiconductors.

P-shell carrier assisted dynamic nuclear spin polarization in single quantum dots at zero external magnetic field

Repeated injection of spin polarized carriers in a quantum dot leads to the polarization of nuclear spins, a process known as dynamic nuclear spin polarization (DNP). Here, we report the first observation of p-shell carrier assisted DNP in single QDs at zero external magnetic field. The nuclear field - measured by using the Overhauser shift of the singly charged exciton state of the QDs - continues to increase, even after the carrier population in the s-shell saturates. This is also accompanied by an abrupt increase in nuclear spin buildup time as p-shell emission overtakes that of the s-shell. We attribute the observation to p-shell electrons strongly altering the nuclear spin dynamics in the QD, supported by numerical simulation results based on a rate equation model of coupling between electron and nuclear spin system. DNP with p-shell carriers could open up avenues for further control to increase the degree of nuclear spin polarization in QDs.

Analysis of the transient response of nuclear spins in GaAs with/without nuclear magnetic resonance

As an alternative to studying the steady-state responses of nuclear spins in solid state systems, working within a transient-state framework can reveal interesting phenomena. The response of nuclear spins in GaAs to a changing magnetic field was analyzed based on the time evolution of nuclear spin temperature. Simulation results well reproduced our experimental results for the transient oblique Hanle signals observed in an all-electrical spin injection device. The analysis showed that the so called dynamic nuclear polarization can be treated as a cooling tool for the nuclear spins: It works as a provider to exchange spin angular momentum between polarized electron spins and nuclear spins through the hyperfine interaction, leading to an increase in the nuclear polarization. In addition, a time-delay of the nuclear spin temperature with a fast sweep of the external magnetic field produces a possible transient state for the nuclear spin polarization. On the other hand, the nuclear magnetic resonance acts as a heating tool for a nuclear spin system. This causes the nuclear spin temperature to jump to infinity: i.e., the average nuclear spins along with the nuclear field vanish at resonant fields of 75As, 69Ga and 71Ga, showing an interesting step-dip structure in the oblique Hanle signals. These analyses provide a quantitative understanding of nuclear spin dynamics in semiconductors for application in future computation processing.

Dicke model for quantum Hall systems

In GaAs quantum Hall (QH) systems, electrons are coupled with nuclear spins through the hyperfine interaction, which is normally not strong enough to change the dynamics of electrons and nuclear spins. The dynamics of the QH systems, however, may drastically change when the nuclear spins interact with low-energy collective excitation modes of the electron spins. We theoretically investigate the nuclear-electron spin interaction in the QH systems as hybrid quantum systems driven by the hyperfine interaction. In particular, we study the interaction between the nuclear spins and the Nambu–Goldstone (NG) mode with the linear dispersion relation associated with the U(1) spin rotational symmetry breaking. We show that such an interaction is described as nuclear spins collectively coupled to the NG mode, and can be effectively described by the Dicke model. Based on the model we suggest that various collective spin phenomena realized in quantum optical systems can also emerge in the QH systems.