J. van Tol

Quenching Spin Decoherence in Diamond through Spin Bath Polarization

We experimentally demonstrate that the decoherence of a spin by a spin bath can be completely eliminated by fully polarizing the spin bath. We use electron paramagnetic resonance at 240 GHz and 8 T to study the electron-spin coherence time T2 of nitrogen-vacancy centers and nitrogen impurities in diamond from room temperature down to 1.3 K. A sharp increase of T2 is observed below the Zeeman energy (11.5 K). The data are well described by a suppression of the flip-flop induced spin bath fluctuations due to thermal electron-spin polarization. T2 saturates at approximately 250 micros below 2 K, where the polarization of the electron-spin bath exceeds 99%.

A quasioptical transient electron spin resonance spectrometer operating at 120 and 240 GHz

A new multifrequency quasioptical electron paramagnetic resonance (EPR) spectrometer is described. The superheterodyne design with Schottky diode mixer/detectors enables fast detection with subnanosecond time resolution. Optical access makes it suitable for transient EPR (TR-EPR) at 120 and 240 GHz. These high frequencies allow for an accurate determination of small g-tensor anisotropies as are encountered in excited triplet states of organic molecules like porphyrins and fullerenes. The measured concentration sensitivity for continuous-wave (cw) EPR at 240 GHz and at room temperature without cavity is 1013spins∕cm3 (15 nM) for a 1 mT linewidth and a 1 Hz bandwidth. With a Fabry-Perot cavity and a sample volume of 30 nl, the sensitivity at 240 GHz corresponds to ≈3×109 spins for a 1 mT linewidth. The spectrometer’s performance is illustrated with applications of transient EPR of excited triplet states of organic molecules, as well as cw EPR of nitroxide reference systems and a thin film of a colossal magn...

Decoherence in crystals of quantum molecular magnets

Quantum decoherence is a central concept in physics. Applications such as quantum information processing depend on understanding it; there are even fundamental theories proposed that go beyond quantum mechanics, in which the breakdown of quantum theory would appear as an ‘intrinsic’ decoherence, mimicking the more familiar environmental decoherence processes. Such applications cannot be optimized, and such theories cannot be tested, until we have a firm handle on ordinary environmental decoherence processes. Here we show that the theory for insulating electronic spin systems can make accurate and testable predictions for environmental decoherence in molecular-based quantum magnets. Experiments on molecular magnets have successfully demonstrated quantum-coherent phenomena but the decoherence processes that ultimately limit such behaviour were not well constrained. For molecular magnets, theory predicts three principal contributions to environmental decoherence: from phonons, from nuclear spins and from intermolecular dipolar interactions. We use high magnetic fields on single crystals of Fe8 molecular magnets (in which the Fe ions are surrounded by organic ligands) to suppress dipolar and nuclear-spin decoherence. In these high-field experiments, we find that the decoherence time varies strongly as a function of temperature and magnetic field. The theoretical predictions are fully verified experimentally, and there are no other visible decoherence sources. In these high fields, we obtain a maximum decoherence quality-factor of 1.49 × 106; our investigation suggests that the environmental decoherence time can be extended up to about 500 microseconds, with a decoherence quality factor of ∼6 × 107, by optimizing the temperature, magnetic field and nuclear isotopic concentrations.

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.

Magnetic phase diagrams of

For the compound of wolframite structure three antiferromagnetic phases are known to exist in the absence of an external field. In this contribution we present the magnetic phase diagrams up to a field strength of 20 T. The plane spanned by the easy direction and the orientation of the twofold screw axes is exposed for the application of external magnetic fields, and the change in the topology of the phase diagrams with the variation of the specific field direction within this plane is described in detail. The application of an external magnetic field perpendicular to this plane hardly affects the stability ranges of any of the phases.

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.

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.

Pulsed electron paramagnetic resonance spectroscopy powered by a free-electron laser

Electron paramagnetic resonance (EPR) spectroscopy interrogates unpaired electron spins in solids and liquids to reveal local structure and dynamics; for example, EPR has elucidated parts of the structure of protein complexes that other techniques in structural biology have not been able to reveal. EPR can also probe the interplay of light and electricity in organic solar cells and light-emitting diodes, and the origin of decoherence in condensed matter, which is of fundamental importance to the development of quantum information processors. Like nuclear magnetic resonance, EPR spectroscopy becomes more powerful at high magnetic fields and frequencies, and with excitation by coherent pulses rather than continuous waves. However, the difficulty of generating sequences of powerful pulses at frequencies above 100 gigahertz has, until now, confined high-power pulsed EPR to magnetic fields of 3.5 teslas and below. Here we demonstrate that one-kilowatt pulses from a free-electron laser can power a pulsed EPR spectrometer at 240 gigahertz (8.5 teslas), providing transformative enhancements over the alternative, a state-of-the-art ∼30-milliwatt solid-state source. Our spectrometer can rotate spin-1/2 electrons through π/2 in only 6 nanoseconds (compared to 300 nanoseconds with the solid-state source). Fourier-transform EPR on nitrogen impurities in diamond demonstrates excitation and detection of EPR lines separated by about 200 megahertz. We measured decoherence times as short as 63 nanoseconds, in a frozen solution of nitroxide free-radicals at temperatures as high as 190 kelvin. Both free-electron lasers and the quasi-optical technology developed for the spectrometer are scalable to frequencies well in excess of one terahertz, opening the way to high-power pulsed EPR spectroscopy up to the highest static magnetic fields currently available.

Spin-dependent processes at the crystalline Si-SiO2 interface at high magnetic fields

An experimental study on the nature of spin-dependent excess charge-carrier transitions at the interface between (111)-oriented phosphorous-doped ([P]≈1015 cm−3) crystalline silicon and silicon dioxide at high magnetic field (B0≈8.5 T) is presented. Electrically detected magnetic-resonance (EDMR) spectra of the hyperfine split 31P donor-electron transitions and paramagnetic interface defects were conducted at temperatures in the range of 3 K≤T≤12 K. The results at these previously unattained (for EDMR) magnetic-field strengths reveal the dominance of spin-dependent processes that differ from the previously well investigated recombination between the 31P donor and the Pb state, which dominates at low magnetic fields. While magnetic resonant current responses due to 31P and Pb states are still present, they do not correlate and only the Pb contribution can be associated with an interface process due to spin-dependent tunneling between energetically and physically adjacent Pb states. This work provides an experimental demonstration of spin-dependent tunneling between physically adjacent and identical electronic states as proposed by Kane Nature (London) 393 133 (1998)] for readout of donor qubits.