High-Field Phenomena of Qubits

Electron and nuclear spins are very promising candidates to serve as quantum bits (qubits) for proposed quantum computers, as the spin degrees of freedom are relatively isolated from their surroundings and can be coherently manipulated, e.g., through pulsed electron paramagnetic resonance (EPR) and nuclear magnetic resonance (NMR). For solid-state spin systems, impurities in crystals based on carbon and silicon in various forms have been suggested as qubits, and very long relaxation rates have been observed in such systems. We have investigated a variety of these systems at high magnetic fields in our multifrequency pulsed EPR/ENDOR (electron nuclear double resonance) spectrometer. A high magnetic field leads to large electron spin polarizations at helium temperatures, giving rise to various phenomena that are of interest with respect to quantum computing. For example, it allows the initialization of both the electron spin as well as hyperfine-coupled nuclear spins in a well-defined state by combining millimeter and radio-frequency radiation. It can increase the T ₂ relaxation times by eliminating decoherence due to dipolar interaction and lead to new mechanisms for the coherent electrical readout of electron spins. We will show some examples of these and other effects in Si:P, SiC:N and nitrogen-related centers in diamond.     

Quantum readout and fast initialization of nuclear spin qubits with electric currents

Nuclear spin qubits have the longest coherence times in the solid state, but their quantum readout and initialization is a great challenge. We present a theory for the interaction of an electric current with the nuclear spins of donor impurities in semiconductors. The theory yields a sensitivity criterion for quantum detection of nuclear spin states using electrically detected magnetic resonance, as well as an all-electrical method for fast nuclear spin qubit initialization.     

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.     

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.     

Matrix Line in Pulsed Electron-Nuclear Double Resonance Spectra

The intense line in Mims and Davies electron-nuclear double resonance (ENDOR) spectra due to the hyperfine interactions of an unpaired electron with distant matrix nuclei is shown to originate from a simultaneous inversion of a large number of nuclear spins by a radiofrequency pulse. Theoretical expressions describing the matrix ENDOR effect are derived and verified experimentally.     

ESR, ENDOR, and ESEEM investigations on UV-irradiated 2,4,6-tri-tert-butyl phenol crystals

Electron spin resonance (ESR), electron nuclear double resonance (ENDOR), and electron spin echo envelope modulation (ESEEM) measurements were carried out for UV-irradiated 2,4,6-tri-tert-butyl phenol in the polycrystalline state. The radical produced in the crystal was detected by ESR and identified to be the corresponding phenoxyl radical, which is well characterized in the chemical oxidations in solutions. ENDOR and ESEEM spectra were unambiguously analyzed in terms of the hyperfine coupling constants determined from well-resolved ESR in solutions. Radical pairs in the crystals were also ascertained, and together with the single-crystal study the analysis disclosed zero-field splitting parameters in the triplet states. ESEEM time decays gave relaxation timesT ₁ = 5.94 andT ₂ = 1.12 μs at room temperature. These appropriate values permit an easy detection of the spin echoes, and therefore this radical matrix can be used as a useful standard for pulsed ESR investigations.     

Room temperature electrical detection of spin coherence in C60

An experimental demonstration of electrical detection of coherent spin motion of weakly coupled, localized electron spins in thin fullerene C60 films at room temperature is presented. Pulsed electrically detected magnetic resonance experiments on vertical photocurrents through Al/C(60)/ZnO samples showed that an electron spin Rabi oscillation is reflected by transient current changes. The nature of possible microscopic mechanisms responsible for this spin to charge conversion as well as its implications for the readout of endohedral fullerene (N@C(60)) spin qubits are discussed.     

EPR and ENDOR Studies of Shallow Donors in SiC

Recent progress in the investigation of the electronic structure of the shallow nitrogen (N) and phosphorus (P) donors in 3C–, 4H– and 6H–SiC is reviewed with focus on the applications of magnetic resonance including electron paramagnetic resonance (EPR) and other pulsed methods such as electron spin echo, pulsed electron nuclear double resonance (ENDOR), electron spin-echo envelope modulation and two-dimensional EPR. EPR and ENDOR studies of the ²⁹Si and ¹³C hyperfine interactions of the shallow N donors and their spin localization in the lattice are discussed. The use of high-frequency EPR in combination with other pulsed magnetic resonance techniques for identification of low-temperature P-related centers in P-doped 3C–, 4H– and 6H–SiC and for determination of the valley–orbit splitting of the shallow N and P donors are presented and discussed.     

Generating entanglement and squeezed states of nuclear spins in quantum dots

We present a scheme for achieving coherent spin squeezing of nuclear spin states in semiconductor quantum dots. The nuclear polarization dependence of the electron spin resonance generates a unitary evolution that drives nuclear spins into a collective entangled state. The polarization dependence of the resonance generates an area-preserving, twisting dynamics that squeezes and stretches the nuclear spin Wigner distribution without the need for nuclear spin flips. Our estimates of squeezing times indicate that the entanglement threshold can be reached in current experiments.     

Optical detection and ionization of donors in specific electronic and nuclear spin States

We resolve the remarkably sharp bound exciton transitions of highly enriched 28Si using a single-frequency laser and photoluminescence excitation spectroscopy, as well as photocurrent spectroscopy. Well-resolved doublets in the spectrum of the 31P donor reflect the hyperfine coupling of the electronic and nuclear donor spins. The optical detection of the nuclear spin state, and selective pumping and ionization of donors in specific electronic and nuclear spin states, suggests a number of new possibilities which could be useful for the realization of silicon-based quantum computers.     

基于直接数字合成技术的电子自旋-核自旋双共振实验射频信号源设计

为了满足脉冲式电子顺磁共振谱仪中电子自旋-核自旋双共振模块的需要,利用直接数字合成器设计并制作了射频信号源. 该部件产生的射频脉冲具备对频率、幅度和相位快速精确调制的能力,对原子核自旋有较强操控能力.     

Indirect detection of selective nuclear spin-spin interactions in a hostile environment

We present a number of techniques which may be used to obtain precise values of selective spin-spin interactions between two nuclear spins in a hostile environment. Such an environment may be characterized by very fast relaxation and decoherence, e.g. due to the strong coupling of the two spins of interest to electron spins in their vicinity as well as other nuclei. Here, we used dilute paramagnetic Ce(3+) centers hosted in a single crystal of CaF(2). Selected (19)F internuclear interactions were measured indirectly by applying different electron nuclear double resonance (ENDOR) pulse sequences.     

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.     

ESR and ENDOR studies of solitons and polarons in conjugated polymers

Nonlinear excitations such as solitons and polarons in conjugated polymers carry spins. In this case electron spin resonance (ESR) and electron-nuclear double resonance (ENDOR) provide unique methods to determine their wave functions. In this review article, the case of solitons in polyacetylene, CH_x, and polarons in an electroluminescent polymer, poly(paraphenylene vinylene) (PPV) are discussed as typical examples. High-resolution proton ENDOR spectra, obtained with stretch-oriented samples, yield the half extension of the excitations of 18 carbon atoms and 4 phenyl rings for CH_x and PPV, respectively. These extensions are well described by the theories in the case of finite electron correlation. In addition, light-induced ESR technique is shown to be useful in obtaining site-selective information of spin distribution in the case of PPV derivatives, as well as the excitation spectra of polarons.     

Optical nuclear spin polarization in quantum dots

Hyperfine interaction between electron spin and randomly oriented nuclear spins is a key issue of electron coherence for quantum information/computation. We propose an efficient way to establish high polarization of nuclear spins and reduce the intrinsic nuclear spin fluctuations. Here, we polarize the nuclear spins in semiconductor quantum dot(QD) by the coherent population trapping(CPT) and the electric dipole spin resonance(EDSR) induced by optical fields and ac electric fields. By tuning the optical fields, we can obtain a powerful cooling background based on CPT for nuclear spin polarization. The EDSR can enhance the spin flip–flop rate which may increase the cooling efficiency. With the help of CPT and EDSR, an enhancement of 1300 times of the electron coherence time can be obtained after a 10-ns preparation time.     

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.     

Solid-state quantum computation—a new direction for nanotechnology

We review current proposals for six types of solid-state quantum computers. We discuss the general requirements for solid-state quantum computers and describe proposals which employ superconducting junctions, electron orbitals in quantum dots, electron spin resonance, nuclear spins of impurity atoms, and nuclear spins in a crystal lattice. We also describe our proposed nuclear spin quantum computer based on magnetic resonance force microscopy. Finally, we describe our numerical method for modeling quantum transformations with a large number (up to 1000) of qubits.     

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.