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.     

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.     

Optical pump-probe measurements of local nuclear spin coherence in semiconductor quantum wells

We demonstrate local manipulation and detection of nuclear spin coherence in semiconductor quantum wells by an optical pump-probe technique combined with pulse rf NMR. The Larmor precession of photoexcited electron spins is monitored by time-resolved Kerr rotation (TRKR) as a measure of nuclear magnetic field. Under the irradiation of resonant pulsed rf magnetic fields, Rabi oscillations of nuclear spins are traced by TRKR signals. The intrinsic coherence time evaluated by a spin-echo technique reveals the dependence on the orientation of the magnetic field with respect to the crystalline axis as expected by the nearest neighbor dipole-dipole interaction.     

Voltage-selective bidirectional polarization and coherent rotation of nuclear spins in quantum dots

We propose and demonstrate that the nuclear spins of the host lattice in GaAs double quantum dots can be polarized in either of two opposite directions, parallel or antiparallel to an external magnetic field. The direction is selected by adjusting the dc voltage. This nuclear polarization manifests itself by repeated controlled electron-nuclear spin scattering in the Pauli spin-blockade state. Polarized nuclei are also controlled by means of nuclear magnetic resonance. This Letter confirms that the nuclear spins in quantum dots are long-lived quantum states with a coherence time of up to 1 ms, and may be a promising resource for quantum-information processing such as quantum memories for electron spin qubits.     

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.     

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.     

Controlling the interaction of electron and nuclear spins in a tunnel-coupled quantum dot

We present a technique for manipulating the nuclear spins and the emission polarization from a single optically active quantum dot. When the quantum dot is tunnel coupled to a Fermi sea, we have discovered a natural cycle in which an electron spin is repeatedly created with resonant optical excitation. The spontaneous emission polarization and the nuclear spin polarization exhibit a bistability. For a σ(+) pump, the emission switches from σ(+) to σ(-) at a particular detuning of the laser. Simultaneously, the nuclear spin polarization switches from positive to negative. Away from the bistability, the nuclear spin polarization can be changed continuously from negative to positive, allowing precise control via the laser wavelength.     

Optical polarization of nuclei and ODNMR in GaAs/AlGaAs quantum wells

Optical orientation of electrons was used to polarize the crystal lattice nuclei in quantum-size heterostructures and to study the effect of the conduction band spin splitting on the spin states of quasi-two-dimensional (2D) electrons drifting in an external electric field. High (～1%) nuclear polarization was registered using polarized luminescence and ODNMR in single GaAs/AlGaAs quantum wells. Measurement was made of the hyperfine interaction fields created by polarized nuclei on electrons and by electrons on nuclei. The spin-lattice relaxation of nuclei on the non-degenerate 2D electron gas was calculated. A comparison of the theoretical and experimental longitudinal relaxation times permitted the conclusion that the localized charge carriers are responsible for nuclear polarization in quantum wells in the temperature range of 2–77 K. A new effect has been studied, i.e. induction of an effective magnetic field acting on 2D electron spins when electrons drift in an external electric field in the quantum well plane. This effective field B_eff is due to the spin splitting of the conduction band of 2D electrons. The paper discusses possible registration of an ODNMR signal when the field B_eff is modulated by an electric current during optical orientation.     

Optical pumping of quantum-dot nuclear spins

Hyperfine interactions with randomly oriented nuclear spins present a fundamental decoherence mechanism for electron spin in a quantum dot, that can be suppressed by polarizing the nuclear spins. Here, we analyze an all-optical scheme that uses hyperfine interactions to implement laser cooling of quantum-dot nuclear spins. The limitation imposed on spin cooling by the dark states for collective spin relaxation can be overcome by modulating the electron wave function.     

Direct observation of the electron spin relaxation induced by nuclei in quantum dots

We have studied the electron spin relaxation in semiconductor InAs/GaAs quantum dots by time-resolved optical spectroscopy. The average spin polarization of the electrons in an ensemble of p-doped quantum dots decays down to 1/3 of its initial value with a characteristic time T(Delta) approximately 500 ps, which is attributed to the hyperfine interaction with randomly oriented nuclear spins. We show that this efficient electron spin relaxation mechanism can be suppressed by an external magnetic field as small as 100 mT.     

An endohedral fullerene-based nuclear spin quantum computer

We propose a new scalable quantum computer architecture based on endohedral fullerene molecules. Qubits are encoded in the nuclear spins of the endohedral atoms, which posses even longer coherence times than the electron spins which are used as the qubits in previous proposals. To address the individual qubits, we use the hyperfine interaction, which distinguishes two modes (active and passive) of the nuclear spin. Two-qubit quantum gates are effectively implemented by employing the electronic dipolar interaction between adjacent molecules. The electron spins also assist in the qubit initialization and readout. Our architecture should be significantly easier to implement than earlier proposals for spin-based quantum computers, such as the concept of Kane [B.E. Kane, Nature 393 (1998) 133].     

Polarization of nuclear spins from the conductance of quantum wire

We devise an approach to measure the polarization of nuclear spins via conductance measurements. Specifically, we study the combined effect of external magnetic field, nuclear spin polarization, and Rashba spin-orbit interaction on the conductance of a quantum wire. Nonequilibrium nuclear spin polarization affects the electron energy spectrum making it time dependent. Changes in the extremal points of the spectrum result in time dependence of the conductance. The conductance oscillation pattern can be used to obtain information about the amplitude of the nuclear spin polarization and extract the characteristic time scales of the nuclear spin subsystem.     

Quantum information processing and metrology with color centers in diamonds

The Nitrogen Vacancy （NV） center is becoming a promising qubit for quantum information processing. The defect has a long coherence time at room temperature and it allows spin state initialized and read out by laser and manipulated by microwave pulses. It has been utilized as a ultra sensi- tive probe for magnetic fields and remote spins as well. Here, we review the recent progresses in experimental demonstrations based on NV centers. We first introduce our work on implementation of the Deutsch- Jozsa algorithm with a single electronic spin in diamond. Then the quantum nature of the bath around the center spin is revealed and continuous wave dynamical decoupling has been demonstrated. By applying dynamical decoupling, a multi-pass quantum metrology protocol is realized to enhance phase estimation. In the final, we demonstrated NV center can be regarded as a ultra-sensitive sensor spin to implement nuclear magnetic resonance （NMR） imaging at nanoscale.     

Nuclear spins of ionized phosphorus donors in silicon

We demonstrate the coherent control and electrical readout of ionized phosphorus donor nuclear spins in (nat)Si. By combining time-programed optical excitation with coherent electron spin manipulation, we selectively ionize the donors depending on their nuclear spin state, exploiting a spin-dependent recombination process at the Si/SiO(2) interface, and find a nuclear spin coherence time of 18 ms for the ionized donors. The presented technique allows for spectroscopy of ionized-donor nuclear spins and enhances the sensitivity of electron nuclear double resonance to a level of 3000 nuclear spins.     

Direct observation of quantum coherence in single-molecule magnets

Direct evidence of quantum coherence in a single-molecule magnet in a frozen solution is reported with coherence times as long as T{2}=630+/-30 ns. We can strongly increase the coherence time by modifying the matrix in which the single-molecule magnets are embedded. The electron spins are coupled to the proton nuclear spins of both the molecule itself and, interestingly, also to those of the solvent. The clear observation of Rabi oscillations indicates that we can manipulate the spin coherently, an essential prerequisite for performing quantum computations.     

Stimulated and spontaneous optical generation of electron spin coherence in charged GaAs quantum dots

We report on the coherent optical excitation of electron spin polarization in the ground state of charged GaAs quantum dots via an intermediate charged exciton (trion) state. Coherent optical fields are used for the creation and detection of the Raman spin coherence between the spin ground states of the charged quantum dot. The measured spin decoherence time, which is likely limited by the nature of the spin ensemble, approaches 10 ns at zero field. We also show that the Raman spin coherence in the quantum beats is caused not only by the usual stimulated Raman interaction but also by simultaneous spontaneous radiative decay of either excited trion state to a coherent combination of the two spin states.     

Measurement of a heavy-hole hyperfine interaction in InGaAs quantum dots using resonance fluorescence

We measure the strength and the sign of hyperfine interaction of a heavy hole with nuclear spins in single self-assembled quantum dots. Our experiments utilize the locking of a quantum dot resonance to an incident laser frequency to generate nuclear spin polarization. By monitoring the resulting Overhauser shift of optical transitions that are split either by electron or exciton Zeeman energy with respect to the locked transition using resonance fluorescence, we find that the ratio of the heavy-hole and electron hyperfine interactions is -0.09 ± 0.02 in three quantum dots. Since hyperfine interactions constitute the principal decoherence source for spin qubits, we expect our results to be important for efforts aimed at using heavy-hole spins in quantum information processing.     

On the possibility of the dynamic self-polarization of nuclear spins in a quantum dot

The possibility of self-polarization of nuclear spins predicted by M.I. D’yakonov and V.I. Perel’ (JETP Lett. 16, 398 (1972)) has been investigated in the case of the electric current passing through a single quantum dot. The mechanisms of nuclear spin relaxation in the quantum dot leading to the polarization and depolarization of the nuclei are discussed. To make the nuclear polarization possible, it has been proposed to increase the nuclear polarization rate via the interaction of an electron localized in the quantum dot with electromagnetic oscillations in an electric circuit, whose proper frequency is tuned to a resonance with the Zeeman splitting of an electron level in the quantum dot.     

Gate control of quantum dot-based electron spin–orbit qubits

We investigate theoretically the coherent spin dynamics of gate control of quantum dot-based electron spin–orbit qubits subjected to a tilted magnetic field under electric-dipole spin resonance (EDSR). Our results reveal that Rabi oscillation of qubit states can be manipulated electrically based on rapid gate control of SOC strength. The Rabi frequency is strongly dependent on the gate-induced electric field, the strength and orientation of the applied magnetic field. There are two major EDSR mechanisms. One arises from electric field-induced spin–orbit hybridization, and the other arises from magnetic field-induced energy-level crossing. The SOC introduced by the gate-induced electric field allows AC electric fields to drive coherent Rabi oscillations between spin-up and -down states. After the crossing of the energy-levels with the magnetic field, the spin-transfer crossing results in Rabi oscillation irrespective of whether or not the external electric field is present. The spin–orbit qubit is transferred into the orbit qubit. Rabi oscillation is anisotropic and periodic with respect to the tilted and in-plane orientation of the magnetic field originating from the interplay of the SOC, orbital, and Zeeman effects. The strong electrically-controlled SOC strength suggests the possibility for scalable applications of gate-controllable spin–orbit qubits.     

金刚石纳米颗粒中氮空位色心的电子自旋研究

通过电子注入的方法制备了含氮空位色心单光子源的金刚石荧光纳米颗粒. 自旋回声测试结果表明, 纳米颗粒中氮空位色心的相干时间T₂很短, 介于0.86 μs至5.6 μs之间. Ramsey干涉条纹测试结果表明, 氮空位色心NV1点的退相干时间T₂^* 最大, 为0.7 μs, 其电子自旋共振谱可分辨的最小线宽为1.05 MHz. 并且NV1点的电子自旋共振谱可分辨氮空位色心本身的¹⁴N核自旋与 氮空位色心电子自旋之间的2.2 MHz超精细相互作用, 这对于在金刚石纳米颗粒中实现核自旋的操控和多个量子比特的门操作具有重要意义. 关键词： 纳米颗粒 氮空位色心 电子自旋