Gavin W. Morley

Potential for spin-based information processing in a thin-film molecular semiconductor.

Organic semiconductors are studied intensively for applications in electronics and optics, and even spin-based information technology, or spintronics. Fundamental quantities in spintronics are the population relaxation time (T1) and the phase memory time (T2): T1 measures the lifetime of a classical bit, in this case embodied by a spin oriented either parallel or antiparallel to an external magnetic field, and T2 measures the corresponding lifetime of a quantum bit, encoded in the phase of the quantum state. Here we establish that these times are surprisingly long for a common, low-cost and chemically modifiable organic semiconductor, the blue pigment copper phthalocyanine, in easily processed thin-film form of the type used for device fabrication. At 5 K, a temperature reachable using inexpensive closed-cycle refrigerators, T1 and T2 are respectively 59 ms and 2.6 μs, and at 80 K, which is just above the boiling point of liquid nitrogen, they are respectively 10 μs and 1 μs, demonstrating that the performance of thin-film copper phthalocyanine is superior to that of single-molecule magnets over the same temperature range. T2 is more than two orders of magnitude greater than the duration of the spin manipulation pulses, which suggests that copper phthalocyanine holds promise for quantum information processing, and the long T1 indicates possibilities for medium-term storage of classical bits in all-organic devices on plastic substrates.

Electronic spin storage in an electrically readable nuclear spin memory with a lifetime >100 seconds.

Spin Control Controlling and manipulating the spin of an electron is a central requirement for applications in spintronics. Some of the challenges researchers are facing include efficient creation of spin currents, minimization of Joule heating, and extending the lifetime of electronic spins, which is especially important for quantum information applications. Costache and Valenzuela (p. 1645) address the first challenge by designing and fabricating an efficient and simple superconducting-based single-electron transistor that can produce spin current with controlled flow. Key to the design is asymmetric tunneling, which leads to a ratchet effect (or diode-like behavior), allowing the separation of up and down spins. Jonietz et al. (p. 1648) use electric currents five orders of magnitude smaller than those used previously in nanostructures to manipulate magnetization in a bulk material, MnSi, pointing the way toward decreased Joule heating in spintronic devices. This so-called spin-torque effect causes the rotation of the skyrmion lattice of spins, characteristic of MnSi, which is detected by neutron scattering. Finally, McCamey et al. (p. 1652) extend the short lifetime of an electronic spin of a phosphorous dopant by mapping it onto the much longer lived nuclear spin of the atom. Mapping the nuclear spin back onto the electronic spin allows production of a spin memory with a storage time exceeding 100s, which should prove useful for future practical applications. An electrically readable spin memory in silicon has been developed with storage times exceeding 100 seconds. Electron spins are strong candidates with which to implement spintronics because they are both mobile and able to be manipulated. The relatively short lifetimes of electron spins, however, present a problem for the long-term storage of spin information. We demonstrated an ensemble nuclear spin memory in phosphorous-doped silicon, which can be read out electrically and has a lifetime exceeding 100 seconds. The electronic spin information can be mapped onto and stored in the nuclear spin of the phosphorus donors, and the nuclear spins can then be repetitively read out electrically for time periods that exceed the electron spin lifetime. We discuss how this memory can be used in conjunction with other silicon spintronic devices.

The initialization and manipulation of quantum information stored in silicon by bismuth dopants

A prerequisite for exploiting spins for quantum data storage and processing is long spin coherence times. Phosphorus dopants in silicon (Si:P) have been favoured as hosts for such spins because of measured electron spin coherence times (T2) longer than any other electron spin in the solid state: 14 ms at 7 K with isotopically purified silicon. Heavier impurities such as bismuth in silicon (Si:Bi) could be used in conjunction with Si:P for quantum information proposals that require two separately addressable spin species. However, the question of whether the incorporation of the much less soluble Bi into Si leads to defect species that destroy coherence has not been addressed. Here we show that schemes involving Si:Bi are indeed feasible as the electron spin coherence time T2 is at least as long as for Si:P with non-isotopically purified silicon. We polarized the Si:Bi electrons and hyperpolarized the I=9/2 nuclear spin of (209)Bi, manipulating both with pulsed magnetic resonance. The larger nuclear spin means that a Si:Bi dopant provides a 20-dimensional Hilbert space rather than the four-dimensional Hilbert space of an I=1/2 Si:P dopant.

A multifrequency high-field pulsed electron paramagnetic resonance/electron-nuclear double resonance spectrometer.

We describe a pulsed electron paramagnetic resonance spectrometer operating at several frequencies in the range of 110-336 GHz. The microwave source at all frequencies consists of a multiplier chain starting from a solid state synthesizer in the 12-15 GHz range. A fast p-i-n-switch at the base frequency creates the pulses. At all frequencies a Fabry-Perot resonator is employed and the pi/2 pulse length ranges from approximately 100 ns at 110 GHz to approximately 600 ns at 334 GHz. Measurements of a single crystal containing dilute Mn(2+) impurities at 12 T illustrate the effects of large electron spin polarizations. The capabilities also allow for pulsed electron-nuclear double resonance (ENDOR) experiments as demonstrated by Mims ENDOR of (39)K nuclei in Cr:K(3)NbO(8).We describe a pulsed multi-frequency electron paramagnetic resonance spectrometer operating at several frequencies in the range of 110-336 GHz. The microwave source at all frequencies consists of a multiplier chain starting from a solid state synthesizer in the 12-15 GHz range. A fast PIN-switch at the base frequency creates the pulses. At all frequencies a Fabry-Perot resonator is employed and the pi/2 pulse length ranges from ~100 ns at 110 GHz to ~600 ns at 334 GHz. Measurements of a single crystal containing dilute Mn2+ impurities at 12 T illustrate the effects of large electron spin polarizations. The capabilities also allow for pulsed electron nuclear double resonance experiments as demonstrated by Mims ENDOR of 39K nuclei in Cr:K3NbO8.

Efficient dynamic nuclear polarization at high magnetic fields

By applying a new technique for dynamic nuclear polarization involving simultaneous excitation of electronic and nuclear transitions, we have enhanced the nuclear polarization of the nitrogen nuclei in 15N@C60 by a factor of 10(3) at a fixed temperature of 3 K and a magnetic field of 8.6 T, more than twice the maximum enhancement reported to date. This methodology will allow the initialization of the nuclear qubit in schemes exploiting N@C60 molecules as components of a quantum information processing device.

Long-lived spin coherence in silicon with an electrical spin trap readout

Pulsed electrically detected magnetic resonance of phosphorous (31P) in bulk crystalline silicon at very high magnetic fields (B0>8.5 T) and low temperatures (T=2.8 K) is presented. We find that the spin-dependent capture and reemission of highly polarized (>95%) conduction electrons by equally highly polarized 31P donor electrons introduces less decoherence than other mechanisms for spin-to-charge conversion. This allows the electrical detection of spin coherence times in excess of 100 mus, 50 times longer than the previous maximum for electrically detected spin readout experiments.

Matter-wave interferometry of a levitated thermal nano-oscillator induced and probed by a spin.

We show how the interference between spatially separated states of the center of mass (c.m.) of a mesoscopic harmonic oscillator can be evidenced by coupling it to a spin and performing solely spin manipulations and measurements (Ramsey interferometry). We propose to use an optically levitated diamond bead containing a nitrogen-vacancy center spin. The nanoscale size of the bead makes the motional decoherence due to levitation negligible. The form of the spin-motion coupling ensures that the scheme works for thermal states so that moderate feedback cooling suffices. No separate control or observation of the c.m. state is required and thereby one dispenses with cavities, spatially resolved detection, and low-mass-dispersion ensembles. The controllable relative phase in the Ramsey interferometry stems from a gravitational potential difference so that it uniquely evidences coherence between states which involve the whole nanocrystal being in spatially distinct locations.

Fast nuclear spin hyperpolarization of phosphorus in silicon

We experimentally demonstrate a method for obtaining nuclear spin hyperpolarization, that is, polarization significantly in excess of that expected at thermal equilibrium. By exploiting a nonequilibrium Overhauser process, driven by white light irradiation, we obtain more than 68% negative nuclear polarization of phosphorus donors in silicon. This polarization is reached with a time constant of approximately 150 sec, at a temperature of 1.37 K and a magnetic field of 8.5 T. The ability to obtain such large polarizations is discussed with regards to its significance for quantum information processing and magnetic resonance imaging.

Nanoscale solid-state quantum computing

Most experts agree that it is too early to say how quantum computers will eventually be built, and several nanoscale solid–state schemes are being implemented in a range of materials. Nanofabricated quantum dots can be made in designer configurations, with established technology for controlling interactions and for reading out results. Epitaxial quantum dots can be grown in vertical arrays in semiconductors, and ultrafast optical techniques are available for controlling and measuring their excitations. Single–walled carbon nanotubes can be used for molecular self–assembly of endohedral fullerenes, which can embody quantum information in the electron spin. The challenges of individual addressing in such tiny structures could rapidly become intractable with increasing numbers of qubits, but these schemes are amenable to global addressing methods for computation.

Laser writing of coherent colour centres in diamond

A negatively charged nitrogen–vacancy centre — a promising quantum light source — is created in diamond by laser writing (with pulses with a central wavelength of 790 nm and duration of 300 fs) with an accuracy of 200 nm in the transverse plane. Optically active point defects in crystals have gained widespread attention as photonic systems that could be applied in quantum information technologies1,2. However, challenges remain in the placing of individual defects at desired locations, an essential element of device fabrication. Here we report the controlled generation of single negatively charged nitrogen–vacancy (NV−) centres in diamond using laser writing3. Aberration correction in the writing optics allows precise positioning of the vacancies within the diamond crystal, and subsequent annealing produces single NV− centres with a probability of success of up to 45 ± 15%, located within about 200 nm of the desired position in the transverse plane. Selected NV− centres display stable, coherent optical transitions at cryogenic temperatures, a prerequisite for the creation of distributed quantum networks of solid-state qubits. The results illustrate the potential of laser writing as a new tool for defect engineering in quantum technologies, and extend laser processing to the single-defect domain.