Electron-nuclear Spin Coupling Research Articles

Stabilization of an optical transition energy via nuclear Zeno dynamics in quantum-dot–cavity systems

We investigate the effect of nuclear spins on the phase shift and polarisation rotation of photons scattered off a quantum dot-cavity system. We show that as the phase shift depends strongly on the resonance energy of an electronic transition in the quantum dot, it can provide a sensitive probe of the quantum state of nuclear spins that broaden this transition energy. By including the electron-nuclear spin coupling at a Hamiltonian level within an extended input-output formalism, we show how a photon scattering event acts as a nuclear spin measurement, which when rapidly applied leads to an inhibition of the nuclear spin dynamics via the quantum Zeno effect, and a corresponding stabilisation of the optical resonance. We show how such an effect manifests in the intensity autocorrelation $g^{(2)}(\tau)$ of scattered photons, whose long-time bunching behaviour changes from quadratic decay for low photon scattering rates (weak laser intensities), to ever slower exponential decay for increasing laser intensities as optical measurements impede the nuclear spin evolution.

Modulated Continuous Wave Control for Energy-Efficient Electron-Nuclear Spin Coupling.

We develop energy efficient, continuous microwave schemes to couple electron and nuclear spins, using phase or amplitude modulation to bridge their frequency difference. These controls have promising applications in biological systems, where microwave power should be limited, as well as in situations with high Larmor frequencies due to large magnetic fields and nuclear magnetic moments. These include nanoscale NMR where high magnetic fields achieves enhanced thermal nuclear polarization and larger chemical shifts. Our controls are also suitable for quantum information processors and nuclear polarization schemes.

Magnetic and Electrical Control of Electron-Nuclear Spin Coupling in GaAs Double Quantum Dots

We magnetically and electrically control spin coupling between electrons and nuclei in a vertical GaAs double quantum dot in the Pauli spin blockade regime to characterize the two-electron exchange energy and the dynamic nuclear polarization (DNP). The Pauli blockade is lifted by a hyperfine-mediated transition from an electron triplet state to the singlet state. This transition progressively occurs when the triplet-singlet separation or exchange energy J is compensated by tuning either Zeeman energy with external magnetic field (i.e., magnetic control) or inter-dot energy detuning with bias voltage (i.e., electrical control). The blockade is then lifted with a current step for sweeping up an external magnetic field. The J value, which is evaluated from the step position for various inter-dot detuning values, is consistent with calculation. DNP takes place through the hyperfine coupling near the current step, leading to a shifted current step to lower external magnetic field for the down-sweep. For the electrical control, a similar current step appears for sweeping bias voltage. In this case we are able to control the two-electron state energies in a relevant manner based on real time before DNP is significantly influenced, because the voltage sweep is much faster than the magnetic field sweep. We use this technique to distinguish the current step with and without DNP contributions, and therefore quantify the nuclear Overhauser fields with external magnetic field as a parameter. We present a simple phenomenological model to reproduce the experiment and also discuss a possible approach to realize the full DNP.

Local detection of Knight shift around quantum‐Hall edge channels using resistively‐detected NMR

We develop a method for the observation of the Knight shift in nanometer-scale region in semiconductors using resistively detected nuclear magnetic resonance (RDNMR) in quantum Hall edge channels. Using a gate-induced decoupling of the hyperfine interaction between electron and nuclear spins, we obtain the RD-NMR spectra with and without the electron-nuclear spin coupling. By comparing these two NMR spectra, we obtain the values of the Knight shift for the nuclear spins polarized dynamically in the region between the relevant edge channels. (© 2006 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

Knight shift detection using gate-induced decoupling of the hyperfine interaction in quantum Hall edge channels

A method for the observation of the Knight shift in nanometer-scale region in semiconductors is developed using resistively detected nuclear magnetic resonance (RDNMR) technique in quantum Hall edge channels. Using a gate-induced decoupling of the hyperfine interaction between electron and nuclear spins, the authors obtain the RDNMR spectra with or without the electron-nuclear spin coupling. By a comparison of these two spectra, the values of the Knight shift can be given for the nuclear spins polarized dynamically in the region between the relevant edge channels in a single two-dimensional electron system, indicating that this method has a very high sensitivity compared to a conventional NMR technique.

Effects of Inversion Asymmetry on Electron-Nuclear Spin Coupling in Semiconductor Heterostructures: Possible Role of Spin-Orbit Interactions

We show that electron-nuclear spin coupling in semiconductor heterostructures is strongly modified by their potential inversion asymmetry. This is demonstrated in a GaAs quantum well, where we observe that the current-induced nuclear spin polarization at Landau-level filling factor nu=2/3 is completely suppressed when the quantum well is made largely asymmetric with gate voltages. Furthermore, we find that the nuclear spin relaxation rate is also modified by the potential asymmetry. These findings strongly suggest that even a very weak Rashba spin-orbit interaction can play a dominant role in determining the electron-nuclear spin coupling.

Resistance Oscillations by Electron-Nuclear Spin Coupling in Microscopic Quantum Hall Devices

We study electron-nuclear spin coupled systems implemented in microscopic fractional quantum Hall (FQH) devices. We find that the longtitudinal resistance in such systems oscillates with a period of about ∼200 s and is driven by a constant voltage instead of a constant current. This anomalous behavior suggests that an average nuclear spin polarization self-sustainingly oscillates between randomized and polarized states which reveal the nonlinear nature of the mesoscopic electron-nuclear spin coupled systems.

Self-sustaining resistance oscillations: Electron-nuclear spin coupling in mesoscopic quantum Hall devices

We study electron-nuclear spin coupled systems implemented in mesoscopic fractional quantum Hall devices. We find that longitudinal resistance in such systems, oscillates with a period of several hundreds of seconds driven by a constant voltage instead of a constant current. The anomalous behavior suggests that an average nuclear spin polarization self-sustainingly oscillates between randomized and polarized states, which reveal the nonlinear nature of the mesoscopic electron-nuclear spin coupled systems.

Fine and hyperfine structure in three low-lying 3Σ+ states of molecular hydrogen

The fine structure constant (electron spin-spin coupling) and the hyperfine structure parameters (electron-nuclear spin coupling, including spin-rotation and electron-nuclear quadrupole coupling) in the low-lying triplet states b3Σ+ u, a3Σ+ g and e3Σ+ u of molecular hydrogen and deuterium are calculated using a recently developed technique with full configuration interaction and multiconfiguration self-consistent field wave functions. The second-order spin-orbit coupling contribution to the 3Σ+ states splitting is negligible, and the calculations therefore provide a good estimate of the zero-field splitting based only on the electron spin-spin coupling values. For the bound a3Σ+ g state a negligible zero-field splitting is found, in qualitative agreement with the e-a spectrum. The zero-field splitting parameter is considerable for the repulsive b3Σ+ u state (≃1 cm−1) and of intermediate size for the bound e3Σ+ u state. The isotropic hyperfine coupling constant is very large not only for the valence b3Σ+ u state (1580 MHz) but also for the Rydberg a and e triplet states (≃1400 MHz). The quadrupole coupling constants for the deuterium isotopes are negligible (0.04–0.07 MHz) for all studied triplet states. The electric dipole activity of the spin sublevels in the triplet-singlet transitions to the ground state is estimated by means of the quadratic response technique.

A theoretical treatment of multiple quantum nuclear spin coherences in electron spin echo studies of polyacetylene

We present a theoretical investigation of the origin of the unusual 3-pulse electron spin echo envelope modulation (ESEEM) pattern obtained from 13C enriched polyacetylene, which exhibits modulation at multiple harmonics of the nuclear Larmor frequency ωn. ESEEM signals have been calculated for different models of the electron–nuclear spin coupling. It is shown that the local hyperfine tensors observed in electron nuclear double resonance (ENDOR) experiments on (13CH)x cannot account for the ESEEM results. These tensors have isotropic components which are too large to give narrow peaks at ωn, and there are too few nuclei to produce the large number of harmonics observed. Simulations for a point electron coupled to nuclei on a spherical shell, the spherical model, give insight into the conditions required to obtain narrow lines at multiple harmonics of ωn: The electron must be weakly coupled to a very large number of nuclei. Analytical results show that for the spherical model in the limit of small coupling, the intensity profile of the Fourier transform of the three-pulse ESEEM will be a Gaussian of width k̄ N, where k̄ is a function of the magnitude of the electron–nuclear coupling and N is the number of nuclei. Simulations assuming that the unpaired electron is delocalized in one dimension along the polyene chain and dipolar coupled to the 13C nuclei on neighboring chains give multiple harmonic patterns, at a reduced interchain distance. We conclude that the observed ESEEM pattern arises from nuclei on neighboring polyacetylene chains and is closely related to the matrix/distant ENDOR line observed for (13CH)x.

Measurement of the nuclear spin diffusion barrier around Eu 2+ ions in CaF 2

The NMR spectrum of discrete 19F nuclear spins surrounding paramagnetic Eu 2+ impurities in CaF 2 is observed at 1.6 K by high-sensitivity NMR. All but the very nearest nuclei are found to have an appreciable thermal contact with the bulk nuclei. A microscopic analysis of the electron-nuclear and nuclear-nuclear spin coupling mechanisms gives results in accord with this observation.

Low field electron-nuclear spin coupling in gallium arsenide under optical pumping conditions

In a semiconductor, absorption of circularly polarized light (optical pumping) leads to spin-oriented photoelectrons. In this situation, the nuclei of the crystal are dynamically polarized through their hyperfine interaction with the electronic spins. Consequently the electrons experience a hyperfine magnetic field due to the oriented nuclei which may reach several kilogauss. When this large nuclear field is driven obliquely with respect to the direction of the exciting light, the precession of the electronic spins around the nuclear field leads to a decrease of the electronic polarization along the light excitation: it is a nuclear Hanle effect. This work is an experimental and theoretical study of these effects in weak external magnetic fields, of the order of the local field which characterizes the nuclear spin-spin interactions (a few gauss). Large nuclear fields are obtained at 77\ifmmode^\circ\else\textdegree\fi{}K in strongly doped and compensated $p$-type GaAs samples. We present a model which includes the different effects of the hyperfine coupling when there is a nuclear spin temperature among all the nuclei of the sample: Dynamic polarization, nuclear field, but also, existence of an electronic field acting on the nuclei. We show that a small external field is able to drive the large nuclear field acting on the electrons; consequently the electronic polarization is very sensitive to external fields which are too small to have a direct effect on the electronic spin motion. We study experimentally the variation of the electronic polarization with the direction and magnitude of a small external magnetic field, by measuring the circular polarization of the luminescence light. The experimental results are in quantitative agreement with the theoretical predictions. The usual Hanle Lorentzian depolarization curve is strongly modified in low fields and $W$-like singularities appear around zero field. The experimental values of the average electronic and nuclear fields are in reasonable agreement with theoretical evaluations. These nuclear effects may strongly alter the measurement of the Hanle linewidth in standard optical pumping experiments.

Spin interactions in molecules

A critical discussion of the theory of spin interactions in molecules is presented. We emphasize that the conventional spin hamiltonian can only be used in first-order perturbation theory, otherwise a singular hamiltonian theory is obtained. The (singular) perturbation of atomic states by the contact operator and an inverse square potential is discussed in detail. The introduction of a spatially extended charge and magnetization for nuclei is suggested as a way of developing a mathematically satisfactory theory of electron-nuclear spin coupling effects; an analogous phenomenology for electrons alone however is not possible.