Nuclear magnetic resonance inverse spectra of InGaAs quantum dots: Atomistic level structural information

A wealth of atomistic information is contained within a self-assembled quantum dot (QD), associated with its chemical composition and the growth history. In the presence of quadrupolar nuclei, as in InGaAs QDs, much of this is inherited to nuclear spins via the coupling between the strain within the polar lattice and the electric quadrupole moments of the nuclei. Here, we present a computational study of the recently introduced inverse spectra nuclear magnetic resonance technique to assess its suitability for extracting such structural information. We observe marked spectral differences between the compound InAs and alloy InGaAs QDs. These are linked to the local biaxial and shear strains, and the local bonding configurations. The cation-alloying plays a crucial role especially for the arsenic nuclei. The isotopic line profiles also largely differ among nuclear species: While the central transition of the gallium isotopes have a narrow linewidth, those of arsenic and indium are much broader and oppositely skewed with respect to each other. The statistical distributions of electric field gradient (EFG) parameters of the nuclei within the QD are analyzed. The consequences of various EFG axial orientation characteristics are discussed. Finally, the possibility of suppressing the first-order quadrupolar shifts is demonstrated by simply tilting the sample with respect to the static magnetic field.Comment: Published version, 17 pages, 18 figure

Direct measurement of the hole-nuclear spin interaction in single quantum dots

We use photoluminescence spectroscopy of ''bright'' and ''dark'' exciton states in single InP/GaInP quantum dots to measure hyperfine interaction of the valence band hole with nuclear spins polarized along the sample growth axis. The ratio of the hyperfine constants for the hole (C) and electron (A) is found to be C/A~-0.11. In InP dots the contribution of spin 1/2 phosphorus nuclei to the hole-nuclear interaction is weak, which enables us to determine experimentally the value of C for spin 9/2 indium nuclei as C_In~-5 micro-eV. This high value of C is in good agreement with recent theoretical predictions and suggests that the hole-nuclear spin interaction has to be taken into account when considering spin qubits based on holes.Comment: to be submitted to Phys Rev Let

Optically tunable nuclear magnetic resonance in a single quantum dot

We report optically detected nuclear magnetic resonance (ODNMR) measurements on small ensembles of nuclear spins in single GaAs quantum dots. Using ODNMR we make direct measurements of the inhomogeneous Knight field from a photoexcited electron which acts on the nuclei in the dot. The resulting shifts of the NMR peak can be optically controlled by varying the electron occupancy and its spin orientation, and lead to strongly asymmetric line shapes at high optical excitation. The all-optical control of the NMR line shape will enable position-selective control of small groups of nuclear spins inside a dot

Pumping of nuclear spins by the optical solid effect in a quantum dot

We demonstrate that efficient optical pumping of nuclear spins in semiconductor quantum dots (QDs) can be achieved by resonant pumping of optically "forbidden" transitions. This process corresponds to one-to-one conversion of a photon absorbed by the dot into a polarized nuclear spin, which also has potential for initialization of hole spin in QDs. Pumping via the "forbidden" transition is a manifestation of the "optical solid effect", an optical analogue of the effect previously observed in electron spin resonance experiments in the solid state. We find that by employing this effect, nuclear polarization of 65% can be achieved, the highest reported so far in optical orientation studies in QDs. The efficiency of the spin pumping exceeds that employing the allowed transition, which saturates due to the low probability of electron-nuclear spin flip-flop.Comment: 5 pages, 3 figures, submitted to Phys. Rev. Let

Overhauser effect in individual InP/GaInP dots

Sizable nuclear spin polarization is pumped in individual InP/GaInP dots in a wide range of external magnetic fields B_ext=0-5T by circularly polarized optical excitation. We observe nuclear polarization of up to ~40% at Bext=1.5T and corresponding to an Overhauser field of ~1.2T. We find a strong feedback of the nuclear spin on the spin pumping efficiency. This feedback, produced by the Overhauser field, leads to nuclear spin bi-stability at low magnetic fields of Bext=0.5-1.5T. We find that the exciton Zeeman energy increases markedly, when the Overhauser field cancels the external field. This counter-intuitive result is shown to arise from the opposite contribution of the electron and hole Zeeman splittings to the total exciton Zeeman energy

Overhauser effect in individual InP/GaInP dots

Sizable nuclear spin polarization is pumped in individual InP/GaInP dots in a wide range of external magnetic fields B_ext=0-5T by circularly polarized optical excitation. We observe nuclear polarization of up to ~40% at Bext=1.5T and corresponding to an Overhauser field of ~1.2T. We find a strong feedback of the nuclear spin on the spin pumping efficiency. This feedback, produced by the Overhauser field, leads to nuclear spin bi-stability at low magnetic fields of Bext=0.5-1.5T. We find that the exciton Zeeman energy increases markedly, when the Overhauser field cancels the external field. This counter-intuitive result is shown to arise from the opposite contribution of the electron and hole Zeeman splittings to the total exciton Zeeman energy

Suppression of nuclear spin diffusion at a GaAs/AlGaAs interface measured with a single quantum dot nano-probe

Nuclear spin polarization dynamics are measured in optically pumped individual GaAs/AlGaAs interface quantum dots by detecting the time-dependence of the Overhauser shift in photoluminescence (PL) spectra. Long nuclear polarization decay times of ~ 1 minute have been found indicating inefficient nuclear spin diffusion from the GaAs dot into the surrounding AlGaAs matrix in externally applied magnetic field. A spin diffusion coefficient two orders lower than that previously found in bulk GaAs is deduced.Comment: 5 pages, 3 figures, submitted to Phys Rev

Full coherent control of nuclear spins in an optically pumped single quantum dot

Highly polarized nuclear spins within a semiconductor quantum dot (QD) induce effective magnetic (Overhauser) fields of up to several Tesla acting on the electron spin or up to a few hundred mT for the hole spin. Recently this has been recognized as a resource for intrinsic control of QD-based spin quantum bits. However, only static long-lived Overhauser fields could be used. Here we demonstrate fast redirection on the microsecond time-scale of Overhauser fields of the order of 0.5 T experienced by a single electron spin in an optically pumped GaAs quantum dot. This has been achieved using full coherent control of an ensemble of 10^3-10^4 optically polarized nuclear spins by sequences of short radio-frequency (rf) pulses. These results open the way to a new class of experiments using rf techniques to achieve highly-correlated nuclear spins in quantum dots, such as adiabatic demagnetization in the rotating frame leading to sub-micro K nuclear spin temperatures, rapid adiabatic passage, and spin squeezing