Knight-field-enabled nuclear spin polarization in single quantum dots

We demonstrate dynamical nuclear-spin polarization in the absence of an external magnetic field by resonant circularly polarized optical excitation of a single electron or hole charged quantum dot. Optical pumping of the electron spin induces an effective inhomogeneous magnetic (Knight) field that determines the direction along which nuclear spins could polarize and enables nuclear-spin cooling by suppressing depolarization induced by nuclear dipole-dipole interactions. Our experiments constitute a first step towards a quantum measurement of the Overhauser field.     

Overhauser DNP and EPR in a Mobile Setup: Influence of Magnetic Field Inhomogeneity

Power-dependent Overhauser dynamic nuclear polarization (DNP) enhancements and continuous-wave electron paramagnetic resonance (EPR) spectra of nitroxide radicals were measured in the magnetic field of a mobile Halbach-array permanent magnet and compared with results from a commercially available electromagnet. DNP saturation factors for varying microwave power were obtained from both measurement series and used to investigate how the increased magnetic field inhomogeneity present in the Halbach magnet affects the saturation efficiency. An EPR detection system was designed to allow continuous-wave EPR measurements at microwave power up to 20?W. Our results show that despite the lower magnetic field homogeneity, a Halbach-array magnet can be used for EPR and DNP-enhanced nuclear magnetic resonance of high quality providing almost the same performance as a more homogeneous electromagnet.     

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.     

Local control of light polarization with low-temperature fiber optics

A fiber-optic-based polarization control system that uses a backreflection measurement scheme at low temperatures has been developed. This provides a stringent test of the light polarization state at the output of the fiber, allowing for determination and control of the degree of circular polarization; i.e., it can generate linear, right, or left circular polarization with cryogenic fibers. This polarization controller is paving the way toward the control and manipulation of nuclear spins in semiconductors via the optical Overhauser effect and could be used, for example, for the purpose of quantum information processing with the large nuclear spins of GaAs.     

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.     

Optical pumping of the electronic and nuclear spin of single charge-tunable quantum dots

We present a comprehensive examination of optical pumping of spins in individual GaAs quantum dots as we change the net charge from positive to neutral to negative with a charge-tunable heterostructure. Negative photoluminescence polarization memory is enhanced by optical pumping of ground state electron spins, which we prove with the first measurements of the Hanle effect on an individual quantum dot. We use the Overhauser effect in a high longitudinal magnetic field to demonstrate efficient optical pumping of nuclear spins for all three charge states of the quantum dot.     

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.     

Nuclear spin nanomagnet in an optically excited quantum dot

Linearly polarized light tuned slightly below the optical transition of the negatively charged exciton (trion) in a single quantum dot causes the spontaneous nuclear spin polarization (self-polarization) at a level close to 100%. The effective magnetic field of spin-polarized nuclei shifts the optical transition energy close to resonance with photon energy. The resonantly enhanced Overhauser effect sustains the stability of the nuclear self-polarization even in the absence of spin polarization of the quantum dot electron. As a result the optically selected single quantum dot represents a tiny magnet with the ferromagnetic ordering of nuclear spins-the nuclear spin nanomagnet.     

Combined Use of 2-D NMR Correlation Experiments, GIAO DFT 13C Chemical Shifts and 1-D NOESY Methods in Regioisomeric and Conformational Structure Determination of Cyclophanes in Solution

The combined application of two-dimensional nuclear magnetic resonance (2-D NMR) correlation experiments and gauge-including atomic orbital (GIAO) ¹³C NMR chemical shift calculations allowed reliable and simple determination of regioisomeric structure of heterocyclic substituents on the calix[4]arene lower rim. Moreover, the 1-D double pulsed field gradient nuclear Overhauser effect technique allows quick and efficient measurement of small nuclear Overhauser effects and, in doing so, establishes a 3-D structure of calix[4]arene simply and unequivocally. In general, these methods may find application in the regio- and stereoisomeric structure determination of complicated macrocyclic compounds.     

Portable X-band system for solution state dynamic nuclear polarization

This paper concerns instrumental approaches to obtain large dynamic nuclear polarization (DNP) enhancements in a completely portable system. We show that at fields of 0.35 T under ambient conditions and at X-band frequencies, 1H enhancements of >100-fold can be achieved using nitroxide radical systems, which is near the theoretical maximum for 1H polarization using the Overhauser effect at this field. These large enhancements were obtained using a custom built microwave transmitter and a commercial TE102 X-band resonant cavity. The custom built microwave transmitter is compact, so when combined with a permanent magnet it is readily transportable. Our commercial X-band resonator was modified to be tunable over a range of approximately 9.5-10 GHz, giving added versatility to our fixed field portable DNP system. In addition, a field adjustable Halbach permanent magnet has also been employed as another means for matching the electron spin resonance condition. Both portable setups provide large signal enhancements and with improvements in design and engineering, greater than 100-fold 1H enhancements are feasible.     

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.     

Enhancement of electron spin coherence by optical preparation of nuclear spins

We study a large ensemble of nuclear spins interacting with a single electron spin in a quantum dot under optical excitation and photon detection. At the two-photon resonance between the two electron-spin states, the detection of light scattering from the intermediate exciton state acts as a weak quantum measurement of the effective magnetic (Overhauser) field due to the nuclear spins. In a coherent population trapping state without light scattering, the nuclear state is projected into an eigenstate of the Overhauser field operator, and electron decoherence due to nuclear spins is suppressed: We show that this limit can be approached by adapting the driving frequencies when a photon is detected. We use a Lindblad equation to describe the driven system under photon emission and detection. Numerically, we find an increase of the electron coherence time from 5 to 500 ns after a preparation time of 10 micros.     

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.     

Dynamic nuclear polarization with single electron spins

We polarize nuclear spins in a GaAs double quantum dot by controlling two-electron spin states near the anticrossing of the singlet (S) and m(S)= +1 triplet (T+) using pulsed gates. An initialized S state is cyclically brought into resonance with the T+ state, where hyperfine fields drive rapid rotations between S and T+, "flipping" an electron spin and "flopping" a nuclear spin. The resulting Overhauser field approaches 80 mT, in agreement with a simple rate-equation model. A self-limiting pulse sequence is developed that allows the steady-state nuclear polarization to be set using a gate voltage.     

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.     

Hyperfine interaction-dominated dynamics of nuclear spins in self-assembled InGaAs quantum dots

We measure the dynamics of nuclear spins in a single-electron charged self-assembled InGaAs quantum dot with negligible nuclear spin diffusion due to dipole-dipole interaction and identify two distinct mechanisms responsible for the decay of the Overhauser field. We attribute a temperature-independent decay lasting ～100 sec at 5 T to intradot diffusion induced by hyperfine-mediated indirect nuclear spin interaction. By repeated polarization of the nuclear spins, this diffusion induced partial decay can be suppressed. We also observe a gate voltage and temperature-dependent decay stemming from cotunneling mediated nuclear spin flips that can be prolonged to ～30 h by adjusting the gate voltage and lowering the temperature to ～200 mK. Our measurements indicate possibilities for exploring quantum dynamics of the central spin model.     

Surface SelectiveH/Si CP NMR by NOE Enhancement from Laser Polarized Xenon

The surface proton spin polarization created by the spin-polarization-induced nuclear Overhauser effect from optically polarized xenon can be transferred in a subsequent step by solid-state cross polarization to another nuclear spin species such as²⁹Si. The technique exploits the dipolar interactions of xenon nuclear spins with high γ nuclei such as¹H, and is experimentally simpler than direct polarization transfer from¹²⁹Xe to heteronuclei such as¹³C and²⁹Si.     

1H dynamic nuclear polarization in supercritical ethylene at 1.4 T

(1)H dynamic nuclear polarization (DNP) has been measured in supercritical ethylene in the pressure range 60-300 bar in an external field of 1.4 T. A single-cell sapphire tube was used as a high-pressure cell, and powdered 1,3-bisdiphenylene-2-phenyl allyl (BDPA) free radicals were added and distributed at the wall of the cell. At all pressures the dominant DNP mechanism was a positive Overhauser enhancement, caused by proton-electron contact interactions at the fluid/solid radical interface. The observed enhancements varied from 12 at 60 bar to 17 at 300 bar. Besides the Overhauser enhancement, small solid state and thermal mixing enhancements also were observed, indicating that part of the ethylene was adsorbed at the radical surface for a prolonged time. The impacts of the experimental conditions on the Overhauser enhancement factors are discussed, and enhancements of at least 40-60 are estimated when the EPR saturation factor and the leakage factor become maximal. These data indicate that DNP-enhanced NMR has the potential of extending the impact of NMR in research areas involving supercritical fluids.     

Method of nuclear polarization measurement in a low-energy polarized target by means of the internal field

The experimental technique of a new type of polarization measurement especially for use with low-energy polarized targets is described. It is possible to derive the nuclear polarization as well as the nuclear spin-lattice relaxation time from measurements of the internal field.     

Dynamics of nuclear polarization in InGaAs quantum dots in a transverse magnetic field

The time-resolved Hanle effect is examined for negatively charged InGaAs/GaAs quantum dots. Experimental data are analyzed by using an original approach to separate behavior of the longitudinal and transverse components of nuclear polarization. This made it possible to determine the rise and decay times of each component of nuclear polarization and their dependence on transverse magnetic field strength. The rise and decay times of the longitudinal component of nuclear polarization (parallel to the applied field) were found to be almost equal (approximately 5 ms). An analysis of the transverse component of nuclear polarization shows that the corresponding rise and decay times differ widely and strongly depend on magnetic field strength, increasing from a few to tens of milliseconds with an applied field between 20 and 100 mT. Current phenomenological models fail to explain the observed behavior of nuclear polarization. To find an explanation, an adequate theory of spin dynamics should be developed for the nuclear spin system of a quantum dot under conditions of strong quadrupole splitting.